review of the air quality directive...support services for the implementation of art. 32 vienna, 23...

Vienna, 23 February 2013

REVIEW OF THE AIR QUALITY DIRECTIVE

AND THE 4TH

DAUGHTER DIRECTIVE

Support Services for the implementation of Art. 32

of AQD and Art. 8 of 4th DD

Service Request No. 6 under framework contract

ENV.C.3/FRA/2009/0008

Final report

Iris Buxbaum

Beth Conlan

Chris Conolly

Sally Cooke

Brian Donovan

Marina Fröhlich

Dick van den Hout

Lorenz Moosmann

Christian Nagl

Jürgen Schneider

Wolfgang Spangl

Brian Stacey

John Stedman

Marita Voogt

Brigitte Winter

Project management

Christian Nagl

Authors

Iris Buxbaum, Umweltbundesamt

Beth Conlan, Ricardo - AEA

Chris Conolly, Ricardo – AEA

Sally Cooke, Ricardo – AEA

Brian Donovan, Ricardo – AEA

Marina Fröhlich, Umweltbundesamt

Dick van den Hout, TNO

Lorenz Moosmann, Umweltbundesamt

Christian Nagl, Umweltbundesamt

Jürgen Schneider, Umweltbundesamt

Wolfgang Spangl, Umweltbundesamt

Brian Stacey, Ricardo – AEA

John Stedman, Ricardo – AEA

Marita Voogt, TNO

Brigitte Winter, Umweltbundesamt

Review

Task 1:

Lorenz Moosmann, Umweltbundesamt



Task 2:

Iris Buxbaum, Umweltbundesamt

Brian Donovan, Ricardo – AEA

Marina Fröhlich, Umweltbundesamt




Marita Voogt, TNO

Task 3:


Jürgen Schneider, Umweltbundesamt


Task 4:

Beth Conlan, Ricardo – AEA

Sally Cooke, Ricardo – AEA


John Stedman, Ricardo – AEA

Task 5:

Dick van den Hout, TNO

Disclaimer

The orientation and content of this report cannot be taken as indicating the position of the European

Commission or its services.

For further information about the publications of the Umweltbundesamt please go to: http://www.umweltbundesamt.at/

http://www.umweltbundesamt.at/

Service Request 6 – final report – Content

Umweltbundesamt Vienna, 23 February 2013 3

CONTENT

SUMMARY ................................................................................................................... 7

1 INTRODUCTION ............................................................................................ 13

2 ASSESSMENT OF CURRENT AQ SITUATIONS, PROJECTIONS, REDUCTION POTENTIALS ........................................................................... 14

2.1 Key messages .............................................................................................................. 14

2.2 Introduction .................................................................................................................. 16

2.2.1 Basis .............................................................................................................................. 16

2.2.2 Data sources .................................................................................................................. 17

2.2.3 Comparison of monitoring data with limit values, target values and assessment thresholds .................................................................................................. 19

2.2.4 Report Structure ............................................................................................................. 19

2.2.5 Work covered by this task .............................................................................................. 20

2.3 PM10 ............................................................................................................................... 20

2.4 PM2.5 ............................................................................................................................... 21

2.4.1 Analysis of current (2010) ambient PM2.5 annual mean concentrations ........................ 22

2.4.2 Analysis of historic trends in ambient PM2.5 concentrations .......................................... 22

2.4.3 Analysis of historic trends in emission of PM2.5 ............................................................. 23

2.4.4 Calculation and assessment of the Average Exposure Indicator (AEI) ......................... 24

2.5 PM below PM2.5 and constituents ............................................................................... 26

2.6 Nickel ............................................................................................................................. 26

2.7 Cadmium ....................................................................................................................... 27

2.8 Arsenic .......................................................................................................................... 28

2.9 Benzo(a)pyrene ............................................................................................................ 29

2.10 Mercury ......................................................................................................................... 30

2.11 Reduction potentials.................................................................................................... 31

3 REVIEW OF ASSESSMENT METHODOLOGIES FOR РM10, PM2.5, HEAVY METALS AND PAHS ........................................................................ 33

3.1 Key messages .............................................................................................................. 33

3.2 Context .......................................................................................................................... 33

3.3 Scope and general approach ...................................................................................... 35

3.4 Review information provided ...................................................................................... 35

3.4.1 Does the data provided show inconsistencies which may be related to technical monitoring issues? .......................................................................................... 35

3.4.2 Do the datasets provided fulfil the basic requirements of the directives (data capture, QA/QC, etc)?.................................................................................................... 37

3.4.3 Is there any other monitoring undertaken by the member states (additional sites or additional pollutants) that is not submitted to DEM? ......................................... 37


4 Umweltbundesamt Vienna, 23 February 2013

3.5 Evaluate data quality objectives ................................................................................. 37

3.5.1 Analysis of reports available from network operators, including reports on equivalence testing ........................................................................................................ 37

3.5.2 Recommendations for improvements ............................................................................ 38

3.6 Siting criteria ................................................................................................................ 39

3.7 Reference methods ...................................................................................................... 40

3.7.1 Reference methods for PM ............................................................................................ 40

3.7.2 Reference methods for total gaseous mercury and heavy metals and PAH in PM10 ............................................................................................................................... 41

3.7.3 Deposition of heavy metals and PAH ............................................................................ 41

3.8 PM10 vs. PM2.5................................................................................................................ 42

3.8.1 Which PM fraction is the most relevant from the point of view of documented health effects? ................................................................................................................ 42

3.8.2 Is it feasible for monitoring network operators to monitor both fractions, taking into account the availability of new monitoring techniques? .......................................... 42

3.8.3 Is particle number a better metric than particle mass with respect to human health? ........................................................................................................................... 43

3.8.4 Is there a need for new reference methods? ................................................................. 43

3.8.5 Conclusions .................................................................................................................... 43

3.9 Reference method vs. near-real-time information .................................................... 44

3.9.1 Are there any implications associated with the fact that there is no standard method for continuous PM monitoring? ......................................................................... 44

3.9.2 Is there any information to suggest that the relationships between continuous and gravimetric samplers remains constant with time? ................................................. 45

3.9.3 Does this render information to the public more difficult? .............................................. 46

3.9.4 What would be the advantages/disadvantages of a separate, continuous standard method? .......................................................................................................... 46

3.10 Particle size fractions .................................................................................................. 47

3.11 Benzo(a)pyrene as marker .......................................................................................... 49

3.12 Relationships between pollutants .............................................................................. 50

4 DEVELOPING FUTURE OBJECTIVE(S) FOR PM2.5 ...................................... 52

4.1 Key messages .............................................................................................................. 52

4.2 Context .......................................................................................................................... 52

4.3 Identification possible new PM standards and selection for further investigation ................................................................................................................. 53

4.3.1 Criteria for air quality standards ..................................................................................... 53

4.3.2 Selection of possible new PM standards for further investigation ................................. 53

4.3.3 PM fraction ..................................................................................................................... 54

4.4 Evaluating the current state of implementation of the relevant provisions .......... 55

4.4.1 Implementation of assessment provisions ..................................................................... 55

4.4.2 Implementation of management provisions ................................................................... 56

4.4.3 Questionnaire on air quality management for PM2.5 reduction targets and exposure obligation ........................................................................................................ 64

4.5 Overview of current levels, projections, reduction potential and technical feasibility for attaining selected PM standards ........................................ 64



4.6 Detailed assessment of possible new standards, conclusions and recommendations ........................................................................................................ 66

5 DEVELOPING FUTURE OBJECTIVES FOR HEAVY METALS AND PAHS .............................................................................................................. 72

5.1 Key messages .............................................................................................................. 72

5.2 Context .......................................................................................................................... 73

5.3 Extent of exceedances for heavy metals ................................................................... 74

5.3.1 Current target values of the 4th Daughter Directive ....................................................... 74

5.3.2 Extent of exceedances of arsenic .................................................................................. 74

5.3.3 Extent of exceedances of cadmium ............................................................................... 76

5.3.4 Extent of exceedances of nickel .................................................................................... 78

5.4 Extent of exceedances of benzo(a)pyrene ................................................................ 80

5.5 Assessment of industrial facilities and related monitoring sites ........................... 82

5.6 Sources of exceedances ............................................................................................. 83

5.6.1 Sources causing exceedances of target values for heavy metals ................................. 84

5.6.2 Sources causing exceedances of the target value for B(a)P ......................................... 88

5.6.3 Necessary emission reductions ..................................................................................... 91

5.6.4 Technical feasibility of emission reductions ................................................................... 92

5.6.5 Cost of emission reduction ............................................................................................. 92

5.7 Impact on health and environment of changes to current standards of As, Cd, Ni and B(a)P .................................................................................................... 92

5.8 Thresholds for Hg ........................................................................................................ 94

5.8.1 Introduction .................................................................................................................... 94

5.8.2 Emissions, concentrations and deposition of Hg ........................................................... 95

5.8.3 Action to reduce Hg emissions ...................................................................................... 99

5.8.4 Possible thresholds for Hg ........................................................................................... 103

5.9 Deposition of Heavy Metals and PAHs .................................................................... 107

5.9.1 Quality of data .............................................................................................................. 107

5.9.2 Analysis of possible regulations ................................................................................... 111

6 INFORMATION OF THE PUBLIC UNDER THE 4TH DAUGHTER DIRECTIVE ................................................................................................... 114

6.1 Key messages ............................................................................................................ 114

6.2 Context – requirements for information of the public............................................ 114

6.3 Compiling reports and websites .............................................................................. 114

6.4 Reporting requirements under the Implementing Decision 2011/850/EC ............ 115

7 REFERENCES ............................................................................................. 117

8 ABBREVIATIONS ........................................................................................ 128

Service Request 6 – final report – Summary


SUMMARY

The Air Quality Directive (AQD) and the 4th Daughter Directive (DD4) to the Framework Direc-

tive both require a review of their provisions for PM2.5 and arsenic, cadmium, mercury, nickel

and polycyclic aromatic hydrocarbons (PAH), respectively. The European Commission set up a

service contract covering support in the review of these provisions. This report summarizes the

work under this contract. It takes into account discussions that took place at two meeting with

the European Commission, the PM workshop, which was held in Brussels in April 2012, the

Stakeholder Expert Group meetings and first resulfts by WHO and IIASA.

The services described in this contract include:

Assessment of the current air quality situation for PM2.5, PM10, arsenic, cadmium, mercury,

nickel and polycyclic aromatic hydrocarbons,

Assessment of current measurement practices of these pollutants,

Development of future objectives for these pollutants covered,

Assessment of information of the public and reporting.

Assessment of the current air quality situation for PM2.5, PM10, arsenic, cadmium,

mercury, nickel and polycyclic aromatic hydrocarbons

The analysis reported here was based on officially available datasets for PM10, PM2.5, As, Cd,

Ni, Hg and PAH (B(a)P) concentration and deposition levels as well as emissions. Other pollut-

ant specific issues, such as PM less than PM2.5, were investigated. Finally, any significant data

gaps were listed.

The aim of presenting these data is to gain an overview of how levels vary across the entire

area of Europe and to understand what conclusions can be drawn for each pollutant based on

the weight of evidence from the different data sources.

The analysis has shown that the PM2.5 target value is only likely to drive action in a small num-

ber of Member States (MS). The Exposure Concentration Obligation may drive action in around

eight MS. The National Exposure Reduction Target (NERT) may be challenging for many MS.

There are many issues in trying to assess Average Exposure Indicator (AEI) from data available

at the moment. In addition, there may be problems in calculating robust AEIs for 2010 (and

therefore setting reliable NERT for MS) and in reliably measuring NERT over the 10 year period.

According to the responses to the MS Questionnaire, no countries measured all of the chemical

species listed in the AQD for characterising the chemical composition of PM2.5.

For nickel, cadmium and arsenic there are very few stations where exceedance of the target

value is likely to drive action, as there are very few exceedances. There is more widespread ex-

ceedance of the target value for B(a)P than for the heavy metals. There are many exceedances

in Poland and other Member States to the east of Europe. There are also more exceedances of

the assessment thresholds than for the heavy metals.

For nickel, arsenic and B(a)P the main data gap was a lack of projections data. This is a signifi-

cant gap as it means that there is no available information on likely future changes.

There are not many data available for mercury, either concentration or deposition. Further in-

vestigation may be needed into the reasons why so many MS have not provided total gaseous

mercury data.

Many MS have not reported any deposition data for nickel, cadmium, arsenic, mercury or B(a)P.

The requirement and purpose of deposition measurements should be reviewed and either the



number of stations could be increased or it might be decided that deposition measurements are

not needed at all.

Assessment of current measurement practices of these pollutants

A review of information on pollutant levels, their trends and data coverage is presented, includ-

ing whether the data provided show inconsistencies which may be related to technical monitor-

ing. Whether the datasets provided fulfil the basic requirements of the Directives (data capture,

QA/QC) and whether there is any other monitoring undertaken by the Member States that is not

submitted to the Data Exchange Module of EIONET (DEM) is presented. The main issues re-

lated to meeting the data quality objectives are listed and suggestions for improvement are

made.

The reported monitoring stations are compared to macroscale siting criteria. Even though the

structure of the monitoring networks is quite heterogeneous the criteria are largely fulfilled.

However, the number of PM2.5 monitoring sites does not yet fulfil the requirements of the AQD.

Also, MS rarely share rural background monitoring sites.

The strengths, weaknesses and relevance of reference methods for PM2.5 and PM10 are dis-

cussed. These methods are not based on well defined measurands but on convention, and

even thoroughly standardized still comprise considerable variability in results. Unfortunately this

is also the case for all continuous methods (Automated Measurement Systems – AMS) currently

available. Procedures for equivalence demonstration of AMS may vary substantially between

Member States. Currently, a new standard is being developed by the European Committee for

Standardization (CEN) aiming at further normalization of equivalence procedures, taking into

account spatial and temporal variability. Relationships between and specific issues of PM,

heavy metals and PAH‘s are analysed, as is the suitability of B(a)P as a marker for the Interna-

tional Agency for Research on Cancer (IARC)1 Probable and Possible Carcinogenic PAHs.

The state of play in PM fractions is summarised, taking into account health effects, feasibility

and the strength and weaknesses of monitoring techniques. Whether there is a need for new

reference methods is discussed.

Specific information on the practical aspects of measurement of organic carbon, elemental car-

bon, inorganic carbon, black carbon, anions and cations are summarised. However, other as-

pects such as relevance from a health effects point of view or the further development of moni-

toring techniques play an important role.

Better understanding and definition of Black Carbon (BC) is needed. The measurement of BC is

potentially a very useful tool, for health, traffic related pollutant indicator, high-level source ap-

portionment (such as OC or ‗UV‘ carbon as a marker for biomass rather than fossil fuel combus-

tion) and climate change issues.

Benzo(a)pyrene, is still the only PAH with sufficient evidence to warrant classification as a hu-

man carcinogen. It has been used as a surrogate for all the other PAH, although there is insuffi-

cient evidence to say that it is not still valid as the marker. The additional PAH selected for as-

sessment within DD4 cover most, but not all, of the PAH in the IARC list and miss some addi-

tional PAH that can help with source apportionment studies. While some MS will measure a

wider range of PAH, this is not guaranteed.

1 http://www.iarc.fr/

http://www.iarc.fr/



Development of future objectives for PM

The AQD has set standards for particulate matter (PM) in ambient air and requires the Commis-

sion to review the PM2.5 standards. The study described in this report supports this review by

exploring possibilities for updating and improving the standards. This assessment also includes

considerations about other PM metrics such as PM10, ultrafine particles (UFP), Black Carbon

(BC) and further constituents of PM.

The study started with an inventory of the current state of implementation of the provisions relat-

ing to the PM2.5 standards regarding assessment and management. It included data reported

under the directive to the Commission and other information such as consultations of stake-

holders in questionnaires, a workshop on PM and experience from the US in managing PM2.5.

Most measures for PM10 and NO2 reduce PM2.5 levels as well with the exemption of few meas-

ures that address mechanical generated dust. Measures to reduce emissions of precursors

support the reduction of PM2.5 levels.

Important input to the investigation was the first results of the recent evaluation by WHO of the

health impacts of PM (WHO 2013).

The study aimed to identify possibilities for changing properties of the PM standards and to sys-

tematically assess the added value of such changes. To this end a set of evaluation criteria was

drawn up. All properties of the standards were considered: the PM fraction regulated, the bind-

ing nature, the level to be attained, the attainment year, other temporal aspects and spatial as-

pects.

The suitability of possible changes was analysed and where possible conclusions were drawn.

However it is difficult to objectively balance advantages and drawbacks, which are often differ-

ent in nature. Nevertheless, the analysis that has been compiled provides useful rationale for

the review process.

Reduction of PM is likely to be effective for reducing the health impact at all concentration levels

found in the EU. To avoid that a fully binding level to be attained everywhere will only drive

down levels at the most unfavourable locations, we recommend considering lower, more ambi-

tious levels in combination with flexibility provisions for locations where the standard cannot be

met (derogations such as the current time extension provisions, spatial differentiation to exclude

certain areas with persistent problems). We therefore also recommend strengthening the bind-

ing nature of the National Exposure Reduction Target for PM2.5.

Recommendations on the numerical level of the PM standards are not given in this report; they

should be based on detailed analysis of model projections taking into account the most recent

information.

Several refinements of more technical possibilities were investigated such as a possible three-

year compliance period for the limit values, a reduced averaging area of the Average Exposure

Indicator.

Options for new standards were also considered, in particular a 24-hour limit value for PM2.5 and

standards for black or elemental carbon and for ultrafine particulates.

WHO has stressed the importance of all existing PM standards, but in view of the desire of

Member States and other stakeholders to use the partial overlap of the standard for simplifying

the set of PM standards, possibilities were explored for withdrawing possibly redundant stan-

dards without decreasing the overall protection provided by the PM standards.



Assessment of objectives for heavy metals

The analysis of heavy metal concentrations has shown that reported exceedances of the exist-

ing target values are associated with a small number of industrial sources. There is some evi-

dence that the existing target values are ensuring that measures are being taken to tackle these

industrial exceedances by reducing emissions. However, detailed understanding of the relation-

ships between sources and ambient concentrations is scarce. Also information is missing on the

assessment and concentration levels around several sources that emit high quantities of heavy

metals. For those sources where exceedances have been reported only in very few cases de-

tailed information on the impact and costs of measures is available. More information on meas-

ures and their impact may become available once the existing target values come into force in

2013 and mandatory reporting by Member States on measures commences.

Assessment of objectives for benzo(a)pyrene

Exceedances of the target value for benzo(a)pyrene as a representative for PAH occur in sev-

eral Member States and affect several million people. Most of the reporting exceedances are

associated with domestic heating emissions; some are caused by industrial emissions. How-

ever, there is very little quantitative evidence available of the impact of the abatement measures

that have been and will be taken. A reduction of the target value to a much lower level would re-

sult in widespread exceedances across almost all of the EU.

Assessment of possible objectives for mercury

Measurement of mercury concentration in ambient air is scarce; the levels observed are in the

order of magnitudes below guideline values for ambient air. Exposure to ambient air concentra-

tions is not a significant contributor to human exposure to mercury, which is mainly driven by

dietary exposure and dental amalgam. Therefore it is recommended continuing of monitoring

ambient concentrations of Hg in both urban areas and industrial hotspots and continuing

abatement of emissions on international level. An implementation of a target value for mercury

would not result in a significant reduction of exposure to mercury.

Deposition of heavy metals and PAH

There is few deposition data available for heavy metals and PAH collected with the reference

measurement methods. Available data show a wide range between industrial sites and back-

ground sites; so a different sampling strategy is needed for these two different types of sites. As

there is a considerable influence in the use of different collector types to measured deposition

rates, it is recommended to gain more information on and experience with the current reference

measurements methods before setting target or limit values by additional deposition monitoring

on background and industrial sites.

Assessment of information of the public and reporting under DD4

To assess the information of the public and the reporting under DD4 the availability of the re-

quired information made available by the Member States via internet has been investigated.

The analysis has shown that the pollutants regulated by DD4 are published in annual reports.

The access to these reports is usually quite easy and straightforward. About two third of the

Member States comply fully with the requirements for information of the public, six Member

States either do not publish heavy metal and PAH data or do not monitor these pollutants.



Within this study also possible changes for reporting due to the Commission Implementing De-

cision laying down rules for Directives 2004/107/EC and 2008/50/EC of the European Parlia-

ment and of the Council as regards the reciprocal exchange of information and reporting on

ambient air quality 2011/850/EU were analysed. It is shown that this decision doesn‘t change

the present reporting requirements for the pollutants regulated by the DD4.

Service Request 6 – final report – Introduction


1 INTRODUCTION

According to Article 32 of Directive 2008/50/EC on ambient air quality and cleaner air for Europe

(―Air Quality Directive‖, AQD), the Directive‘s provisions related to PM2.5 and, as appropriate,

other pollutants shall be reviewed in 2013. In addition, a review is foreseen according to Article

8 of Directive 2004/107/EC relating to arsenic, cadmium, mercury, nickel and polycyclic aro-

matic hydrocarbons in ambient air (―4th Daughter Directive‖, DD4).

The European Commission set up a service contract with Umweltbundesamt, Ricardo – AEA

and TNO covering support in the review of the provisions related to PM2.5 and PM10 in the AQD

as well as the provisions related to all pollutants covered by the DD4 (specific contract number

070307/2011/599749/SER/C3). The contract came into force on 10 August 2011 and has a du-

ration of 16 months.

The services described in this contract include:

Assessment of the current air quality situation,

Assessment of current measurement practices,

Development of future objectives for the pollutants covered by the review,

Assessment of information of the public and reporting.

To provide these services, the work is divided into seven tasks:

Task 1: Assessment of current air quality situations, projections and reduction potentials in

the Member States (chapter 2).

Task 2: Review of assessment methodologies for РM10, PM2.5, heavy metals and PAHs with

particular emphasis on measurement practices (chapter 3).

Task 3: Developing future objective(s) for PM2.5 (chapter 4).

Task 4: Developing future objectives for heavy metals and PAHs (chapter 5).

Task 5: Addressing other aspects in the review of the 4th Daughter Directive (chapter 6).

Task 6: Consultation and updating of results (the results of this task are summarized in meet-

ing reports and further documentation).

Task 7: Meetings, preparation and follow-up (the results of this task are summarized in meet-

ing reports).

This final report is based on the specific reports for Task 1 to 5 (RICARDO – AEA 2012; RICARDO –

AEA, UMWELTBUNDESAMT & TNO 2012; TNO, UMWELTBUNDESAMT & RICARDO – AEA 2013;

UMWELTBUNDESAMT & RICARDO – AEA 2012; UMWELTBUNDESAMT 2012).

Service Request 6 – final report – Assessment of current AQ situations, projections, reduction potentials


2 ASSESSMENT OF CURRENT AQ SITUATIONS, PROJECTIONS, REDUCTION POTENTIALS

2.1 Key messages

PM10

In just over half of all MS all monitoring stations were in compliance with the PM10 annual limit

value in 2009. Most of the exceeding monitoring stations are in Eastern Europe or Italy.

Almost all MS had a least one monitoring station in exceedance of the PM10 daily limit value

in 2009.

The main data gap in the work on PM10 was that no data were available on PM10 concentra-

tions in 2010. These data were not in the 2010 questionnaires 2004/461/EC and the updated

version of AirBase that included 2010 data was not available during the timescale of Task 1

(summarized in this chapter) of this project.

PM2.5

The PM2.5 target value is only likely to drive action in a small number of MS. The Exposure

Concentration Obligation (ECO) may drive action in around eight MS. The National Exposure

Reduction Target (NERT) may be challenging to many MS, especially those with highest cur-

rent concentrations. There are many issues in trying to assess AEI from data available at the

moment. The Commission should scrutinise the 2011 Questionnaire 2004/461/EC in great

detail for Average Exposure Indicator (AEI) and it is likely that direct engagement with the MS

will be needed.

The compliance statistics for PM10 and PM2.5 presented in the current report (including AEI

and ECO) should help to inform the review as to which limits are more likely to drive action.

There may be problems in calculating robust AEIs for 2010 and therefore setting reliable

NERT for MS. In addition, there may be a potential problem in reliably measuring NERT over

the 10 year period.

AQUILA have published draft guidance on calculating the AEI (AQUILA 2012). However, there

is further work to do on the AEI and other bodies and projects such as AQUILA are likely to

be involved in further looking in to these issues.

PM less than PM2.5

According to the responses to the MS Questionnaire, no countries measured all of the spe-

cies listed in the AQD for characterising the chemical composition of PM2.5. Seven countries

measured only one of the species and four countries measured between four and six.

The reason for the lack of data on PM less than PM2.5 should be investigated. Possibly addi-

tional monitoring of PM1 or black carbon (for example) should be mandatory in new AQD.

However, it should be considered how this could be done without placing a large burden on

MS and without a specific environmental objective being set.

Nickel

There are very few stations where exceedances of the target value is likely to drive action, as

there are very few exceedances. The stations that are in exceedance are mostly industrial



stations (though one is a traffic station). In addition, there are only a small number of stations

with concentrations greater than the assessment thresholds for nickel.

Many MS have not reported any nickel deposition data. The reason for the lack of data

should be investigated. The requirement and purpose of deposition measurements should be

reviewed and either the number of stations could be increased or it might be decided that

deposition measurements are not needed at all.

The main data gap was a lack of projections data. This is a significant gap as it means that

there is no available information on likely future changes.

Cadmium

There are very few stations where exceedance of the target value is likely to drive action, as

there are very few exceedances. The exceedances are mostly at industrial stations, but there

are also exceedances at two background and one traffic station. There are also only a small

number of stations with concentrations greater than the assessment thresholds for cadmium.

Many MS have not reported any cadmium deposition data. The reason for the lack of data




Arsenic

There are very few stations where exceedance of the target value is likely to drive action, as

there are very few exceedances. The exceeding stations are mostly industrial, but there are

also four exceedances at background stations. However, there are more stations with con-

centrations greater than the assessment thresholds for arsenic than for nickel and cadmium.

Many MS have not reported any arsenic deposition data. The reason for the lack of data






B(a)P

There is more widespread exceedance of the target value for B(a)P than for the heavy met-

als. There are many exceedances in Poland and other Member States to the east of Europe.

There are exceedances of the target value at some industrial stations and traffic stations but

most of the exceedances are at background stations. The use of solid fuel for domestic heat-

ing is likely to be the main source associated with the exceedances. There are also more ex-

ceedances of the assessment thresholds than for the heavy metals.

Many MS have not reported any B(a)P deposition data. The reason for the lack of data








Mercury

There are not many data available for mercury; not many MS have provided total gaseous

mercury data in the 2010 Questionnaire 2004/461/EC. Further investigation may be needed

into the reasons why so many MS have not provided total gaseous mercury data.

Many MS have not reported any mercury deposition data. The reason for the lack of data




Reduction potentials

Data reported by MS in the Questionnaire 2004/461/EC and emissions data did not neces-

sarily indicate that the same sources are important. In addition, national emissions can only

provide an indication of possible sources. As the exceedances may be confined to small ar-

eas, on a local level further sources might be of relevance, which might not show a large con-

tribution to emissions on a national scale. Task 4 (section 5) will provide more detail on

sources.

The major data gap in completing the assessment of reduction potential was the lack of re-

cent source apportionment data for heavy metals and B(a)P.

2.2 Introduction

2.2.1 Basis

The basis of this assessment are the two Directives, ―Directive 2008/50/EC of the European

Parliament and of the Council of 21 May 2008 on ambient air quality and cleaner air for Europe‖,

this can be referred to as the Air Quality Directive (AQD) and ―Directive 2004/107/EC of the

European Parliament and of the Council of 15 December 2004 relating to arsenic, cadmium,

mercury, nickel and polycyclic aromatic hydrocarbons in ambient air‖, which can be referred to

as the Fourth Daughter Directive (DD4).

Specifically a review is required of the following topics:

Article 32 of AQD requires a review of the regulations for PM2.5 and, as appropriate, other pol-

lutants, Art 32.3 provides for the necessity to prepare a report of the experience of monitoring

PM10 and PM2.5.

Article 8 of DD4 requires a report about the implementation of the directive and a review of

the targets for arsenic (As), cadmium (Cd), nickel (Ni), mercury (Hg) and polycyclic aromatic

hydrocarbons (PAH).

This report forms part of the review under the provisions listed above. The environmental objec-

tives from these Directives pertinent to this report are given in Summary Table 1, with the ex-

ception of Hg, which does not have a prescribed target or limit value.



Table 1: Environmental Objectives of the Air Quality Directive and the 4th Daughter Directive.

Determinant Limit Type Short Name Description

PM10 Limit Annual LV A calendar year average concentration of 40 µg/m³

Daily LV A daily concentration of 50 µg/m³ not to be ex-ceeded more than 35 times in one calendar year

PM2.5 National Ex-posure Re-duction Tar-get

NERT A comparison of the three year mean (AEI) up to 2020 to the three year mean 2008 to 2010 where the future three year mean value is either less than 8.5 µg/m³ or other reduction target based on the initial concentration

Target TV A calendar year average concentration of 25 µg/m³

Exposure concentration obligation

ECO 20 µg/m³ (applies to the AEI) in 2015

As Target TV 6 ng/m³ for the total content in the PM10fraction averaged over a calendar year

Cd Target TV 5 ng/m³ for the total content in the PM10fraction averaged over a calendar year

Ni Target TV 20 ng/m³ for the total content in the PM10fraction averaged over a calendar year

Benzo(a)Pyrene (B(a)P)†

Target TV 1 ng/m³ for the total content in the PM10fraction averaged over a calendar year

† - B(a)P is a specific type of PAH that has been adopted within the framework of DD4 as representative of the fate and

behaviour of the other PAH.

The National Emissions Ceilings Directive (NECD) is not the focus of this report so, none of the

pollutants covered in NECD are directly assessed but emissions of those pertinent to PM pre-

cursors are provided alongside the sector type emissions data for the PM fractions that are the

focus of this report.

2.2.2 Data sources

2.2.2.1 AirBase and the annual Questionnaire

For historical and current data, two datasets were used, AirBase2 and the Questionnaire accord-

ing to Decision 2004/461/EC (in the following referred to as ―questionnaire 2004/461/EC‖). This

assessment uses available data in AirBase for 2001-2009 for the analysis of the ambient con-

centrations in the years 2001-2009 for all pollutants. The level of meta-data associated with the

concentration and exceedance statistics is reasonable for the AirBase data.

As the AirBase data for 2010 were not available on the timescale of Task 1 of this work, the

data from completed Member State (MS) annual assessment questionnaires 2004/461/EC for

2010 were used for all pollutants except PM10 for which only AirBase data were used (the year

2010 was not included in the analysis for this pollutant). This is because for PM10 only ex-

ceedances are reported in the Questionnaire and therefore annual average concentrations for

all stations were not available for 2010. The most recent available data for PM10 were the 2009

data from AirBase.

2 http://www.eea.europa.eu/data-and-maps/data/airbase-the-european-air-quality-database-6

http://www.eea.europa.eu/data-and-maps/data/airbase-the-european-air-quality-database-6



The Questionnaire 2004/461/EC data submitted by each MS contains a number of inconsisten-

cies, namely:

Concentration and deposition rates stored as text rather than as a number.

Deposition data given in different units to that requested.

Pollutants given in a different order to that requested.

Additional descriptions given, leading to a wide gulf between the prior data to 2009 reported

in AirBase and that reported in the Questionnaires.

Lack of data capture statistics in the Questionnaire.

The data have been taken at face value, with the assumption that the MS has made every en-

deavour to ensure that the data presented are, as far as can be reasonably expected, a true es-

timate of the concentration and deposition rates. A data capture threshold of 90 % has been

applied to the AirBase data, in line with required proportion of valid data of Annex XI of the

AQD. Where the data capture was reported in the Questionnaire data this information was used

and a 90 % data capture threshold was also applied, however in general no data capture infor-

mation was given, so 90 % data capture was assumed.

2.2.2.2 Emissions data

The historic trends in emission have been included for the years 2000 to 2009. These data have

been taken from the UNECE/EMEP Centre on Emission Inventories and Projections (CEIP3)

emissions database (WebDab4). The data are reviewed annually. The ‗emissions used in the

EMEP models‘ data were downloaded for each MS (and Croatia), the data for PM10 and PM2.5

were resolved by SNAP code. The ‗emissions used in the EMEP models‘ data for the DD4 pol-

lutants is held as MS emission totals only.

The SNAP sector totals of the ‗officially reported‘ emissions have been used for assessing the

reduction potential of heavy metals and B(a)P. For assessing the reduction potential of heavy

metals (chapter 2.11), data from the ESPREME5 project were also used. The project included

calculating emissions and concentrations projections for 2000 to 2010 for heavy metals (arse-

nic, cadmium, chromium, mercury, nickel and lead) disaggregated by sector. There are large

differences between these datasets for some MS and for some pollutants, so these data have

not been presented together. For most MS and pollutants the total from the ESPREME project

is larger than the total from WebDab, but this is not always the case (see Table 9.3 of the task 1

report, RICARDO – AEA 2012).

2.2.2.3 Projection data

The CCE Status report 2010 studied emissions and concentrations projections of cadmium,

mercury and lead and these concentrations projections are presented in this report (CCE 2010).

For the projections data presented in this report three of the scenarios from this report were

used:

CLE2010, which is the current legislation projection for 2010 from a base year of 2000.

FI20, which is a projection for 2020 that includes full implementation of the HM protocol in all

UNECE Europe MS.

3 http://www.ceip.at/

4 http://www.ceip.at/webdab-emission-database/

5 http://espreme.ier.uni-stuttgart.de/

http://www.ceip.at/

http://www.ceip.at/webdab-emission-database/

http://espreme.ier.uni-stuttgart.de/



FI20_op1, which includes the possible revision of the HM protocol due to the implementation

of measures outlined in the ―Draft possible amendments to the 1998 HM Protocol‖ (UNECE

2009). It includes the most stringent emission limit values for major stationary sources in An-

nex V.II of the 1998 protocol.

Recent data on projections of ambient concentrations of arsenic, nickel and benzo(a)pyrene are

not available.

2.2.2.4 Member State Questionnaire

A questionnaire was circulated to MS in February 2012 in order to request further information

that was not available from other data sources (such as the Questionnaire 2004/461/EC) in or-

der to assess the current scale and quality of monitoring measurements across MS (including

information on the AEI and measurements of PM less than PM2.5).

2.2.3 Comparison of monitoring data with limit values, target values and as-

sessment thresholds

The level of rounding of monitoring data that should be done before comparison with the limit

values, target values and assessment threshold is currently unclear. It appears from the 2010

Questionnaires 2004/461/EC that different MS have used different levels of rounding in their of-

ficially reported values. In order to use a consistent approach throughout this report, all meas-

ured data are rounded to 1 decimal place before comparing with the limit values, target values

and assessment thresholds. Therefore the exceedance numbers presented in this report might

be different to the officially reported data in some cases. The Commission has clarified that the

AEI should be rounded to 1 decimal place and also the initial AEI concentration threshold

should be rounded to 1 decimal place as well. Clarification on the level of rounding required for

the target values of DD4 is foreseen for the review of the AQD and a consistent approach from

all MS should be the case in the future.

2.2.4 Report Structure

The work presented here seeks to contribute to the review through an analysis of officially avail-

able datasets for PM10, PM2.5, As, Cd, Ni, Hg and PAH (B(a)P). Specific attention is given to:

Ambient concentration measured and reported by MS (current and historical levels) – fo-

cused on and limited to, metrics for which environmental objectives have been set within the

Directives. Where no environmental objectives exist, the annual average concentrations have

been considered. Data for the years up to and including 2009 have been used for the PM10

analysis and data for the years up to and including 2010 have been used for the analysis for

all other pollutants.

Annual Emission trends for MS up to and including 2009.

Deposition rates reported by MS for relevant pollutants.

Other pollutant specific issues.

The analysis is presented by pollutant, as this will provide a better synthesis of what the differ-

ent data sources show for each. Geographically, this report covers the reported data from the

EU27 MS and Croatia, collectively referred to as the MS.



The data are presented with the dual aims:

To gain an overview of how levels vary across the entire area of Europe covered by this re-

view.

To understand what conclusions can be drawn for each MS for each pollutant based on the

weight of evidence from the different data sources.

The focus of the analysis in this report will be at MS level. New analysis by EU reporting zone

will not be carried out since this type of analysis is routinely reported by the EEA. However, for

completeness, we will present a summary of the EEA findings where relevant.

An additional section is provided that addresses the relationship between the DD4 pollutants

measured and the relevant PM fraction in which these have been measured.

2.2.5 Work covered by this task

Table 2 provides a master summary of the topics to be covered for each of the pollutants to be

considered.

Table 2: Checklist of work covered by this task.

Topic PM10 PM2.5 PM below PM2.5

As, Cd, Ni, B(a)P

Hg NO2

Ambient concentrations: a snapshot of current levels

Ambient concentrations: Historic trends

Ambient concentrations: Projections

Emissions: Historic trends

Emissions: Projections

Average Exposure Indicator

PM below PM2.5

Deposition

Reduction potential for Member States

Specific dataset: Summary statistics for IIASA

Specific dataset: Population exposure

2.3 PM10

Three groups of analysis have been carried out for PM10:

Analysis of current (2009) ambient PM10 annual mean concentrations and daily exceedance

statistics.

Analysis of historic trends in ambient PM10 concentrations.



Analysis of historic trends in emission of PM10.

It should be noted that projections of PM10 have not been considered as part of this work.

In addition to the data presented here, summary statistics from AirBase for PM10 and PM2.5 in

2009 were also provided to IIASA. These data were provided for ―priority stations‖ only. Priority

stations were those with exceedances of PM10 annual or daily limit values in 2009, exceedances

of PM2.5 target value in 2009 or those stations that were listed as AEI stations in the 2009 ques-

tionnaire.

The annual mean limit value and upper/lower assessment thresholds given in the AQD for PM10

are:

Limit value: 40 µg/m³ in a calendar year.

Upper assessment threshold: 28 µg/m³.

Lower assessment threshold: 20 µg/m³.

In just over half of all MS all monitoring stations were in compliance with the PM10 annual limit

value in 2009. The largest compliance gap was 42.6 µg/m³ at a traffic station in Italy. Most of the

exceeding monitoring stations are in Eastern Europe or Italy. Bulgaria was the only MS with an

average concentration for PM10 above the limit value at 46.8 µg/m³, from a total of 37 stations

reported.

Almost all MS had a least one monitoring station in exceedance of the PM10 daily limit value in

2009. The largest compliance gap was 254 exceedances at a traffic station in Italy.

Almost all MS have had at least one exceedance between 2001 and 2009. For most MS these

exceedances are across the station types, but roadside stations sometimes dominate.

Only thirteen MS have a time series of PM10 monitoring data longer than seven years. For Ger-

many, Belgium and Austria there is a statistically significant downward trend in PM10 concentra-

tions between 2000 and 2009. For France there is a statistically significant upward trend (but is

likely to be due to a change in monitoring method). The measurement method used to gather

the French PM10 data was predominantly using TEOMs and the French authorities changed the

correction method in 2007. For the other MS there is no statistically significant trend.

The primary PM10 emissions decreased between 2000 and 2009 for almost all MS. For most MS

there is a decline in concentrations that is reasonably consistent with the decline in primary

emissions. However it is recognised that part of the trend in measured concentrations will be

associated with the trends in secondary PM, for which the precursor emissions of SO2 and NOx

also show declines in many MS.

The main data gap in the work on PM10 was that no data were available on PM10 concentrations

in 2010. These data were not in the 2010 questionnaires 2004/461/EC and the updated version

of AirBase that included 2010 data was not available during the timescale of Task 1 this project.

For most MS the trends in PM10 and PM2.5 concentrations are broadly consistent, though there

are generally less data available for PM2.5 than PM10.

2.4 PM2.5

Four groups of analysis have been carried out for PM2.5:

Analysis of current (2010) ambient PM2.5 annual mean concentrations

Analysis of historic trends in ambient PM2.5 concentrations



Analysis of historic trends in emission of PM2.5.

The calculation and assessment of the Average Exposure Indicator (AEI).

No PM2.5 projections have been included in this data analysis task. A projection prepared by

IIASA for the review is available.

In addition to the data presented here, summary statistics from AirBase for PM10 and PM2.5 in

2009 were also provided to IIASA. These data were provided for ―priority stations‖ only. Priority

stations were those with exceedances of PM10 annual or daily limit values in 2009, exceedances

of PM2.5 target value in 2009 or those stations that were listed as AEI stations in the 2009 Ques-

tionnaire 2004/461/EC.

The annual mean target value and upper/lower assessment thresholds for PM2.5 are:

Target value: 25 µg/m³.

Upper assessment threshold: 10 µg/m³.

Lower assessment threshold: 7 µg/m³.

2.4.1 Analysis of current (2010) ambient PM2.5 annual mean concentrations

In 2010, many monitoring stations in most MS were below the PM2.5 target value. However,

there were exceeding monitoring stations in Germany, France, Italy, Poland, Czech Republic,

Hungary, Bulgaria, Slovakia and Latvia. The majority of exceedances were at background sta-

tions. The largest compliance gap in 2010 was 36 µg/m³ at a traffic station in Poland (Figure 1).

Figure 1: Annual mean PM2.5 levels in 2010 (in µg/m³. Minimum, 10th

percentile, mean, 90th percentile,

maximum levels and target value. Source: 2010 Questionnaire 2004/461/EC).

Just over half of the MS have had at least one monitoring station exceeding the PM2.5 target

value between 2001 and 2010. However, many of those exceedances are only exceeding the

target value by a small amount.

2.4.2 Analysis of historic trends in ambient PM2.5 concentrations

Only thirteen MS have a time series longer than five years. For Italy there is a statistically sig-

nificant downward trend in PM2.5 concentrations at background stations only between 2001 and

2009. For Portugal there is a statistically significant downward trend over the same time period

for industrial stations only. For Hungary and Sweden there is a statistically significant downward



for traffic stations only. There are no statistically significant upward trends for PM2.5 concentra-

tions (for those MS that have a time series longer than 5 years). For the other MS there is no

statistically significant trend. There are not enough data available to find an overall picture in

trends. The German dataset is shown as an example (Figure 2).

Figure 2: Annual mean PM2.5 concentration trends for Germany (in µg/m³, 2001–2010. Source: AirBase).

2.4.3 Analysis of historic trends in emission of PM2.5

There is a decrease in primary PM2.5 emissions for most MS between 2000 and 2010 (Figure 3).

For those 22 MS for which emission data is available since 2000, the overall emissions de-

creased by 16 % from 2000 to 2010. An increase was reported for BG, DK, EE, FI, LV, PL, SI

and SE.



Figure 3: PM2.5 emissions in EU MS 2000 to 2010 (officially reported data. Source: CEIP).

2.4.4 Calculation and assessment of the Average Exposure Indicator (AEI)

Indicative AEIs were calculated for 2010 using 2010 Questionnaire according to Decision

2004/461/EC data, 2009 Questionnaire according to Decision 2004/461/EC data and 2009 Air-

Base data. Five MS have best estimate AEIs above 22 µg/m³ and therefore their indicative Ex-

posure Reduction Target (ERT) would be to take all appropriate measures to achieve 18 µg/m³.

Most MS have best estimate AEI of between 13 µg/m³ and 18 µg/m³ and therefore have an in-

dicative ERT of 15 % (see Table 3.6 of Task 1 report for details, RICARDO – AEA 2012).

Eight MS (Bulgaria, Cyprus, Czech Republic, Hungary, Italy, Poland, Slovakia and Slovenia)

have best estimate AEIs for 2010 that are above the Exposure Concentration Obligation

(20 µg/m³), which will be legally binding in 2015.

There is a lack of data related to the AEI reported in the 2010 Questionnaire 2004/461/EC.

However, these gaps were expected to be filled in the 2011 Questionnaire 2004/461/EC, when

all MS should have reported their final AEI 2010 values. Many MS reported a final AEI 2010

value in the 2011 Questionnaire 2004/461/EC, but there were still missing data. In addition

within this project a specific questionnaire was sent to MS on 11 September 2012, where the

PM2.5 exposure reduction obligation was requested. The information received from MS is de-

scribed in Task 3 (see specific report, TNO, UMWELTBUNDESAMT, RICARDO – AEA 2013, summa-

rized in section 4).

In addition, the MS highlighted issues with data capture, the moving of monitoring stations and

general issues related to measurement of PM2.5 in their responses to our previous question-

naire, which was sent out in February 2012. They also highlighted the requirement for clear

guidance on the methods that should be used to calculate the AEI.

It is important that a specific method of calculation is defined, including whether a data capture

threshold should be used (and if so what it should be) and guidance on whether all stations

should be included or whether there needs to be a minimum number of valid years for the sta-

tion to be included. Some guidance on this can be found in the IPR (Decision 2011/850/EU).

The method of calculation of the AEI has been considered by AQUILA and recommendations

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for the methodology for defining the requirements that stations that are used to monitor PM2.5

concentrations, in order to provide data that the AEI and its associated parameters, should con-

form to, including proposals for (AQUILA 2012):

Selection of the monitoring stations, as far as practical;

Procedure(s) for calculating the required annual averages from the individual daily or inte-

grated-hourly measured PM2.5 data at the selected monitoring stations;

Methods for averaging the annual datasets from the selected stations to produce the average

annual values from all the monitoring stations;

Determination of the Average Exposure Indicator (AEI) for a Member State by averaging all

the valid annual results at all the specified locations.

A recommendation that the procedure for forming the three-year averaged AEI by weighting

the concentrations from the selected measurement stations with their data capture should be

applied to all the AEI calculations - that is:

The AEI for the initial reference year AEI that is then used to define the NERT,

The AEI in years 2013-2015 necessary for an examination of whether the ECO is met,

The AEI in years 2018-2020 necessary to determine whether the NERT is achieved,

and the AEIs that are to be reported for all other three year periods that are required (see

specific report for Task 2 for further details, RICARDO – AEA, UMWELTBUNDESAMT & TNO

2012, summarized in section 3).

Uncertainties in the measurements and within the calculation of delta AEI may mean that it is

not possible to assess the delta AEI against the ERT. New analysers, service and maintenance,

variability in analyser performance and changes to the Reference Method could mean that the

uncertainty of measuring the delta AEI could be greater than that needed to robustly assess a

required reduction of 2.0 µg/m³ in PM2.5 concentrations between 2010 and 2020. However dif-

ferent groups have reached different conclusions on this (RICARDO – AEA 2011, MATTHIJSEN et.

al. 2009). Further investigation is needed on whether the delta AEI can be calculated with

enough confidence to assess it against the ERT. AQUILA has published guidance for improving

the consistency of the AEI between 2010 and 2020 (AQUILA 2012).

For most MS the trends in PM10 and PM2.5 concentrations are broadly consistent, though there

are generally less data available for PM2.5 than PM10. There are only limited data available for

PM2.5 (see also section 2.4.2).

The PM2.5 target value is only likely to drive action in a small number of MS. The ECO may drive

action in around eight MS. The NERT may be challenging to many MS, especially those with

highest current concentrations. There are many issues in trying to assess AEI from data avail-

able at the moment. The Commission should scrutinise the 2011 Questionnaire 2004/461/EC in

great detail for AEI and it is likely that direct engagement with the MS will be needed. Some ad-

ditional data and information is available from the replies to the specific questionnaire sent out in

September 2012.

The compliance statistics for PM10 and PM2.5 presented in this section (including AEI and ECO)

should help to inform the review as to which limits are more likely to drive action (RICARDO – AEA

2012). There is further work to do on the AEI and other bodies and projects such as AQUILA

are likely to be involved in further looking in to these issues.



2.5 PM below PM2.5 and constituents

The AQD states that the list of chemical species given below shall be included in the measure-

ment of concentrations of appropriate compounds to characterise the chemical composition of

PM2.5:

SO42–

NO3–

Na2+

K+

NH4+

Cl–

Ca2+

Mg2+

elemental carbon (EC)

organic carbon (OC)

Seven countries did not respond to the MS Questionnaire (Bulgaria, Croatia, Finland, Hungary,

Malta, Portugal and Slovakia). Cyprus, Greece, Lithuania, Luxemburg, Romania and Slovenia

reported only one of these species were measured. No countries measured all of the species,

the Czech Republic, France, Poland, Spain and the UK measured between four and six.

The reason for the lack of data on PM less than PM2.5 should be investigated. Possibly addi-

tional monitoring of PM1 or black carbon (for example) should be mandatory in new AQD. How-

ever, it should be considered how this could be done without placing a large burden on MSs

and without a specific environmental objective being set.

2.6 Nickel

Seven groups of analysis have been carried out for nickel:

Analysis of current (2010) levels of nickel annual mean concentrations.

Analysis of historic trends in ambient nickel.

Ambient concentration projections.

Analysis of historic trends in emissions of nickel.

Emission projections.

Deposition of nickel.

Reduction potential of MS for nickel.

The annual mean target value and upper/lower assessment thresholds for Ni are:

Target value: 20 ng/m³.

Upper assessment threshold: 14 ng/m³.

Lower assessment threshold: 10 ng/m³.

In 2010 all monitoring stations were below the nickel target value in most MS. A few stations in

Germany, Spain and Belgium were in exceedance. The largest compliance gap was 48.5 ng/m³

at an industrial station in Germany.



The vast majority of MS have no measured exceedances of the nickel target value between

2001 and 2010. Only Germany, France, United Kingdom, Italy, Spain and Belgium had meas-

ured exceedances during this period.

There were insufficient data for trend analysis on the ambient trends between 2001 and 2010

(due to a lack of data for the earlier years).

MS emissions of nickel decrease between 2000 and 2009 for all MS with data available except

three (Czech Republic, Croatia and Cyprus). The trends in nickel emissions are reasonably

consistent with trends in PM10 emissions for some MS.

There are not enough data on nickel deposition available to draw any conclusions on deposi-

tion. There are a lot more data available in 2009 and 2010, than in previous years, but most of

the additional data are from Germany.

There were a few data gaps for nickel:

No projections data (for emissions or concentrations).

No modelled deposition data.

Webdab emissions data are not available for all MS.

The lack of projections data is a significant gap as it means that there is no available information

on likely future changes.

There are very few stations where exceedances of the target value is likely to drive action. The

stations that are in exceedance are mostly industrial stations (though one is a traffic station). In

addition, there are only a small number of stations with concentrations greater than the assess-

ment thresholds for nickel.

Many MS have not reported any nickel deposition data. The reason for the lack of data should

be investigated. The requirement and purpose of deposition measurements should be reviewed

and either the number of stations could be increased or it might be decided that deposition

measurements are not needed at all.

2.7 Cadmium

Seven groups of analysis have been carried out for cadmium, being:

Analysis of current (2010) levels of cadmium annual concentrations.

Analysis of historic trends in ambient cadmium.


Analysis of historic trends in emissions of cadmium.


Deposition of cadmium.

Reduction potential of MS for cadmium.

The annual mean target value and upper/lower assessment thresholds for Cd are:


Upper assessment threshold: 3 ng/m³.

Lower assessment threshold: 2 ng/m³.



All monitoring stations in most MS are below the cadmium target value in 2010. There were ex-

ceeding monitoring stations in France, Spain, Belgium, Bulgaria and Finland. The largest com-

pliance gap was 20.4 ng/m³ at a background station in Bulgaria.

Most MS did not have any exceeding monitoring stations between 2001 and 2010, though there

are a large number of exceedances of the target value in Belgium in every year from 2001 to

2010. Many MS do not have a large amount of monitoring data for this period and there were

insufficient data for trend analysis on the ambient trends between 2001 and 2010 (due to a lack

of data for the earlier years).

There is a decrease in cadmium emissions between 2000 and 2009 in just over half of the MS,

with thirteen of these showing a steady reduction between the two years. However, there is a

significant number of MS that show an increase in emissions during this period.

According to the CCE Status Report 2010 data, cadmium concentrations are predicted to de-

crease between 2010 and 2020 for all MS (in the most ambitious scenario) (CCE 2010). How-

ever, for the least ambitious scenario emissions are only predicted to decrease for just over half

of the MS and increase for just under half of the MS.

There are not enough data on cadmium deposition available to draw any conclusions on depo-

sition. There are a lot more data available in 2009 and 2010, than in previous years, but most of


The problems and gaps encountered in the data are:


There are very few stations where exceedance of the target value is likely to drive action. The

exceedances are mostly at industrial stations, but there are also exceedances at two back-

ground and one traffic station. There are also only a small number of stations with concentra-

tions greater than the assessment thresholds for cadmium.

Many MS have not reported any cadmium deposition data. The reason for the lack of data


reviewed and either the number of stations could be increased or it might be decided that depo-

sition measurements are not needed at all.

2.8 Arsenic

Seven groups of analysis have been carried out for arsenic, being:

Analysis of current (2010) levels of arsenic annual concentrations.

Analysis of historic trends in ambient arsenic.


Analysis of historic trends in emissions of arsenic.


Deposition of arsenic.

Reduction potential of MS for arsenic.

The annual mean target value and upper/lower assessment thresholds for arsenic are:


Upper assessment threshold: 3.6 ng/m³.



Lower assessment threshold: 2.4 ng/m³.

In 2010 most MS had no exceedances of the arsenic target value measured at any monitoring

stations. However, exceedances were measured at some monitoring stations in Germany, Po-

land, Belgium, Czech Republic and Finland. The largest compliance gap was 38.2 ng/m³ at a

Belgian industrial station.

Like the other heavy metals, most MS have had all monitoring stations below the target value

throughout the period between 2001 and 2010. However, there are a large number of ex-

ceedances of the target value in Belgium in every year from 2001 to 2010. For many MS there

is a limited amount of data. There were insufficient data for trend analysis on the ambient trends

between 2001 and 2010 (due to a lack of data for the earlier years).

There is a decrease in arsenic emissions between 2000 and 2009 in the majority of the MS.

However, there is a significant number of MS that show an increase in emissions during this pe-

riod.

There are not enough data on arsenic deposition available to draw any conclusions on deposi-

tion. There are a lot more data available in 2009 and 2010, than in previous years, but most of



No projections data (emissions and concentrations).

No modelled deposition data.




There are very few stations where exceedance of the target value is likely to drive action. The

exceeding stations are mostly industrial, but there are also four exceedances at background sta-

tions. However, there are more stations with concentrations greater than the assessment

thresholds for arsenic than for nickel and cadmium.

Many MS have not reported any arsenic deposition data. The reason for the lack of data should




2.9 Benzo(a)pyrene

Seven groups of analysis have been carried out for benzo(a)pyrene:

Analysis of current (2010) levels of benzo(a)pyrene annual concentrations.

Analysis of historic trends in ambient benzo(a)pyrene.


Analysis of historic trends in emissions of benzo(a)pyrene.


Deposition of benzo(a)pyrene.

Reduction potential of MS for benzo(a)pyrene.



The annual mean target value and upper/lower assessment thresholds for B(a)P are:


Upper assessment threshold: 0.6 ng/m³.

Lower assessment threshold: 0.4 ng/m³.

Just over half of the MS have at least one monitoring station in exceedance of the B(a)P target

value in 2010. Some MS have many monitoring stations in exceedance; Poland, Czech Repub-

lic and Austria have more than ten. The largest compliance gap was 23.6 ng/m³ at a new station

(unknown station type) in Poland.

Just over half of the MS have had a least one monitoring stations exceeding the target value be-

tween 2001 and 2010. There were insufficient data for trend analysis on the ambient trends be-

tween 2001 and 2010 (due to a lack of data for the earlier years). In the case of the United

Kingdom risks to successful sampling were reduced by switching to daily sampling. The appar-

ent step change in the UK data is important to note, as other Member States may have used

USEPA TO4 based samplers previously and have changed to the compliant dust samplers op-

erating within the PM10 sampling convention.

There is a decrease in B(a)P emissions between 2000 and 2009 in the majority of MS, with

available data. However, there is a significant number of MS that show an increase in emissions

during this period.

There are not enough data on B(a)P deposition available to draw any conclusions on deposi-

tion.


No projections data (emissions and concentrations).

Webdab emissions data are not available for all Member States.



There is more widespread exceedance of the target value for B(a)P than for the heavy metals.

There are many exceedances in Poland and other Member States to the east of Europe. There

are exceedances of the target value at some industrial stations and traffic stations but most of

the exceedances are at background stations. The use of solid fuel for domestic heating is likely

to be the main source associated with the exceedances. There are also more exceedances of

the assessment thresholds than for the heavy metals.

Many MS have not reported any B(a)P deposition data. The reason for the lack of data should




2.10 Mercury

Six groups of analysis have been carried out for Mercury:

Analysis of current (2010) levels of Mercury annual concentrations.

Analysis of historic trends in ambient Mercury.


Analysis of historic trends in emissions of Mercury.




Deposition of Mercury.

According to DD4 the MS are required to report the concentration of mercury, but no target has

been prescribed. MS will have developed their own assessment criteria, predominately for use

for planning and industrial process permitting.

There are few data available on measured mercury concentrations for 2010 and for the period

2001 to 2010. Many MS have not reported any data and nineteen of the forty eight stations re-

porting total gaseous mercury in 2010 are in the UK. Typical concentrations measured in MS

with available data in 2010 were around 1 to 2 ng/m³, however the largest reported value in

2010 was 17.8 ng/m³ (at a UK station). This compares with the long term Environmental As-

sessment Level (EAL) published by the Environment Agency for England and Wales of an an-

nual concentration of mercury of 250 ng/m³.

There were insufficient data for trend analysis on the ambient trends between 2001 and 2010

(due to a general lack of data).

Emissions of mercury decreased between 2000 and 2009 for the majority of MS. However,

there is a significant number of MS that show an increase in emissions during this period.

According to the CCE Status Report 2010 data, mercury concentrations are predicted to de-

crease between 2010 and 2020 for all MS (in the most ambitious scenario) (CCE 2010). How-

ever, for the least ambitious scenario emissions are predicted to increase for almost all of the

MS and decrease for just one MS (UK).

There are not enough data on mercury deposition available to draw any conclusions on deposi-

tion.


Airbase and Questionnaire 2004/461/EC data are both very incomplete.

There are not many data available; not many MS have provided total gaseous mercury data in

the 2010 Questionnaire 2004/461/EC. Further investigation may be needed into the reasons

why so many MS have not provided total gaseous mercury data.

Many MS have not reported any mercury deposition data. The reason for the lack of data should




2.11 Reduction potentials

There is only very limited information on reduction potential is available from official sources.

The key issues for emissions reduction in decreasing order of priority are:

a) Emissions of B(a)P from residential combustion.

b) Emissions of B(a)P, arsenic, cadmium and nickel from industrial sources including power

production.

c) Emissions of B(a)P, arsenic and cadmium from road traffic.

d) Emissions of B(a)P and arsenic due to a combination of sources in an agglomeration.



Data reported by MS in the Questionnaire 2004/461/EC and emissions data do not necessarily

indicate that the same sources are important. In addition, national emissions can only provide

an indication of possible sources. As the exceedances may be confined to small areas, on a lo-

cal level further sources might be of relevance, which might not show a large contribution to

emissions on a national scale. Task 4 provides more detail on sources (UMWELTBUNDESAMT

2012, section 5).

The results from this section specifically feed into Task 4 (section 5).

Service Request 6 – final report – Review of assessment methodologies for РM10, PM2.5, heavy metals and PAHs


3 REVIEW OF ASSESSMENT METHODOLOGIES FOR РM10, PM2.5, HEAVY METALS AND PAHS

3.1 Key messages

The initial part of Task 2 (section 3) was to review the collective experiences of the MS, this

was a good opportunity for MS to share their information, which was met with varying suc-

cess.

As part of this task, some fundamental questions were asked about which PM metrics (frac-

tions) are important. All presently applied metrics provide useful data to health policy.

Generally, the Target and Limit Values have been derived from the evidence of epidemiologi-

cal and toxicological studies and by discussion with expert groups at MS, EU and Interna-

tional level.

The number of PM2.5 monitoring sites does not yet fulfil the requirements of the AQD. Coop-

eration is very rare between MS to share rural background monitoring sites.

According to present legislation, the PM assessment focuses on the measurement of PM10

and PM2.5 mass concentrations. This is based on the evidence for a strong linkage between

the mass concentrations and health effects; however, health-effects could not unequivocally

be attributed to certain PM fractions. Initial studies have shown that short time resolution

measurements of Black Carbon (measured as BC or as EC), and UFP could be the key met-

rics for acute effects. The heavy metals and PAH are important with regard to longer-term

exposure, but further work on metalloids and chromium speciation may be needed.

To broaden information on traceable PM properties or constituents of PM and their health ef-

fects, extended measurement requirements in the MS are necessary. For the selection of

new, additional measurands balance has to be found between the assumed health impact,

and the existence of preferably traceable but at least well defined methods of monitoring

method. BC is discussed as a pollutant with clear relation to health effects. Better under-

standing and definition of BC is needed, including the development of a reference method.

The reference methods for PM10 and PM2,5 are not based on well defined measurands but on

convention, and even thoroughly standardized still comprise considerable variability in re-

sults. Unfortunately this is also the case for all continuous methods currently available; con-

sequently, a change of the reference method to a continuous one only shifts the problem

without improving the situation.

Based on present legislation, benzo(a)pyrene is assessed as a marker for all PAH and their

carcinogenic potential. Further research is recommended to identify both the carcinogenic po-

tential as well as the atmospheric levels of the PAH in the IARC list of carcinogenic sub-

stances.

3.2 Context

Measurement of PM and speciated PM in the atmosphere is an extremely challenging task.

There are a number of different measurement techniques available. Measurement harmonisa-

tion is dictated by Directives and Standards within a defined level of uncertainty. When compar-

ing measurements of PM, this uncertainty needs to be considered, but it does provide a basis

for comparison of the measurement made using different sampling and analytical technologies.



The pollutants covered by the present review have seen various developments since

entry into force of the Directives:

For PM10 and PM2.5, ambient air measurement techniques must currently comply with

EN 12341:1998 and EN 14907:2005 respectively, or demonstrate equivalence to these

methods by reference to the equivalence guide6 (European Commission 2010). Various con-

tinuous monitoring techniques have been introduced, but their equivalence with the reference

method has only been recently demonstrated and only in a few locations across Europe. This

demonstration of equivalence is also being undertaken during a period where our under-

standing of the limitations and variability of the reference method are becoming clearer. This

is already a key discussion point and will continue to be so in the coming years.

In addition, there is a growing archive of data for concentrations of many different particle

size fractions and research into associated health effects. Couple this to the introduction of

measurement techniques allowing the simultaneous measurement of several particle size

fractions, the question arises as to which fraction(s) the focus for regulation should be laid on

in the future.

For heavy metals, ambient air assessment techniques used must comply with

EN 14902:2005 ambient air quality - method for the measurement of Pb, Cd, As and Ni in the

PM10 fraction. In addition monitoring instruments of these particulate metals must adopt a

sampling system that has been assessed by and is operated in accordance with

EN 12341:1998. Measurement uncertainty can be managed by appropriate calibration fre-

quencies, extraction of reference standards and maintaining stability of sample flow through-

out the sampling periods. Mercury techniques must comply with EN 15852:2010 which de-

scribes an automatic measurement method, however the standard allows for a manual

equivalent.

For polycyclic aromatic hydrocarbons (PAHs) in ambient air, monitoring techniques must

demonstrate their equivalence to EN12341:1998. The sampling techniques employed are

non-automatic sampling techniques which are generally high-volume systems. Since the in-

troduction of the reference method EN15549:2008 it is likely that there may have been addi-

tional validation of sampling techniques with ozone denuders. As with particulate metal

measurement, uncertainty can be managed by appropriate calibration frequencies, extraction

of reference standards and maintaining stability of sample flow throughout the sampling peri-

ods.

For polycyclic aromatic hydrocarbons (PAHs) in ambient air deposition, monitoring tech-

niques must demonstrate their equivalence to EN15980:2011. The validation trial demon-

strated that the funnel-bottle bulk collector provided the most reliable and robust results

hence this was chosen as the standard collector. Cylindrical gauges and wet only collectors

can be used to measure deposition of PAH provided equivalence can be demonstrated. In

addition, for all PAH measurements, the question arises whether benzo(a)pyrene is the most

appropriate marker or another PAH is a more suitable replacement. Also, is more re-

search/discussion required to identify whether PM2.5 is a more suitable particulate size frac-

tion to measure for PAH.

6 http://ec.europa.eu/environment/air/quality/legislation/assessment.htm

http://ec.europa.eu/environment/air/quality/legislation/assessment.htm



3.3 Scope and general approach

This task covers a wide range of technical questions as well as questions related to the selec-

tion of particle size fraction (for PM) and marker pollutant (for PAH). These questions are ad-

dressed by the following general approach:

Collection and review of available literature, such as papers in peer-reviewed journals, other

technical papers and reports by network operators.

Discussion of specific questions with members of expert groups such as AQUILA7 and CEN

8.

Contacting network operators in Member States with specific questions on their practical ex-

perience with monitoring techniques, data quality objectives, siting of stations, equivalence

testing, and other topics.

External review of the draft report by selected experts (AQUILA, CEN etc.)

In detail this task covers the following questions:

Review information provided (section 3.4) regarding inconsistencies due to monitoring issues,

fulfilment of the datasets of requirements of the AQD, additional monitoring not reported

Evaluate fulfilment of data quality objectives (section 3.5)

Comparison of reported monitoring stations to macroscale siting criteria (section 3.6)

Evaluate strength and weakness of the reference methods (section 3.7)

PM10 vs PM2.5: health effects and monitoring aspect (section 3.8)

Reference method vs. near-real-time information via non standardized continuous monitors

(section 3.9)

Availability of data for different particle size fractions and constituents (section 3.10)

Suitability of benzo(a)pyrene as marker for PAH concentrations (section 3.11)

Correlation between the pollutants of the AQD and DD4 (section 3.12)

A questionnaire was sent to Member States in February 2012 to get further information on these

topics.

3.4 Review information provided

3.4.1 Does the data provided show inconsistencies which may be related to

technical monitoring issues?

The meta data for monitoring techniques used to provide measurements has been provided by

MS alongside measurement data. This information has been extracted from AirBase, compiled

in one data set and assessed in order to discover the distribution of various methods across all

MS.

It is important that detailed information about monitoring techniques are provided if we are to

assess information relating to use of the reference method, equivalent methods and non-

equivalent methods used to measure the relevant species across all member states.

7 http://ies.jrc.ec.europa.eu/aquila-project/aquila-homepage.html

8 http://www.cen.eu/cen/pages/default.aspx

http://ies.jrc.ec.europa.eu/aquila-project/aquila-homepage.html

http://www.cen.eu/cen/pages/default.aspx



Using the limited information and resources available, an assessment was carried out to try to

further differentiate methods into further graded categories and an additional category where

the specific method was not provided.

Five categories were defined by an air quality expert, Brian Stacey, based on his understanding

of the methods (Table 3). The actual methods used could be divided into four categories, the

reference method, methods that have demonstrated equivalence criteria to demonstration of

equivalence criteria, methods that have not but are deemed ‗good‘ methods that have been

shown to fail by a relatively small margin i.e., just outside the 25% uncertainty detailed in the

guidance (e.g. 27%) and ‗poor‘ methods that have been defined not to be used even for indica-

tive measurements. Later, the information was amended using information taken from equiva-

lence testing campaigns across Europe in Belgium (20109), Germany (2009

10), Finland (2010

11),

The Netherlands (200812

) and the UK (201013

)

Table 3: Categories for evaluating equivalence of different PM monitoring methods.

Equivalence Categories

ID Description Example for PM10

1 Reference method Leckel sampler

2 Demonstrated to be equivalent MetOne BAM

3 Good, but not equivalent TEOM

4 Poor Turnkey Osiris

5 Unknown Not possible to determine method*

*This is either because the method has not been tested for equivalence or not enough information provided, i.e. ‘beta

attenuation’ which could relate to several different instruments

Using data with >= 90 % data capture uploaded to AirBase, it is possible to show that 7.5 % of

PM10 data sets in 2009 was measured using the reference method and 24.4 % using an equiva-

lent method. 40.2 % of the data sets were measured using a method that was outside the crite-

ria set out in the GDE for 2005 and 2010, and no member states were found to be measuring

PM10 or PM2.5 using a ‗poor‘ method (category 4). 27.9 % of meta data is not sufficient to deter-

mine a method.

19.1 % of PM2.5 data sets in 2009 with a data capture of ≥90 % were obtained using the refer-

ence method. 12.6 % and 25.3 % of PM2.5 data sets were measured using equivalent and non-

equivalent methods respectively. There were 43% of measurements that could be not be cate-

gorised as a result of data omission or limited information.

9 VMM (2011), Comparative PM10 and PM2.5 Measurements in Flanders, 2010 campaign.

10 TÜV Rheinland (2009), Report on suitability testing of the ambient air quality measurement system SWAM 5a dual

channel monitor with PM10 and PM2.5 pre-separators of the company FAI instruments s.f.l for the components sus-

pended particulate matter PM10 and PM2.5

11 Finnish Meteorological Institute (2010), Demonstration of the equivalence of PM2.5 and PM10 measurement methods

in Helsinki

12 GGD Amsterdam (2008), Field Experiment on 11 Automated monitors

13 Defra and the Devolved Administrations (2010) UK Particulate matter equivalence trials data re-processed in accor-

dance with the January 2010 version of the guide to demonstration of equivalence (GDE)



3.4.2 Do the datasets provided fulfil the basic requirements of the directives

(data capture, QA/QC, etc)?

The data submitted to AirBase almost completely fulfils the data quality objectives.

It is possible to determine the data capture in two different ways. In the first year of a measure-

ment it is often unlikely to have a full year of time coverage. It is clear that data capture provided

to AirBase should be obtained from data sets with at least 90% data capture. The question is,

what the data capture should be relevant to, for example for a first year sample starting on 1st

June until December (i.e. time coverage of 50%):

1) The actual time coverage obtained i.e. 100% of 6 months

2) The annual year in full i.e. 50% of the calendar year

Currently this decision is down to the interpretation of the MS and as such there is an inconsis-

tent approach for calculating the data capture when you assess the time coverage from the start

and end dates provided with the data.

Using the questionnaire it has been possible to determine, in part, if member states are covered

by ISO17025 accreditation for all measurements and across all networks if applicable. Only Cy-

prus, Greece, Ireland, Italy and Latvia are not covered by ISO17025 accreditation for any air

quality measurements as detailed in the questionnaire. The Czech Republic, Estonia, The UK,

Hungary, Luxembourg, Latvia, The Netherlands, Romania, Sweden and Slovenia are covered

by ISO17025 accreditation for all measurements relevant to the Task 2 assessment (HM, B[a]P,

PM10 and PM2.5). For the remaining countries, accreditation is either dependent upon the region

or is unknown because no information has been provided.

3.4.3 Is there any other monitoring undertaken by the member states (additional

sites or additional pollutants) that is not submitted to DEM?

This section has been covered in section 3.10, please refer to this section for information relat-

ing to additional measurements.

3.5 Evaluate data quality objectives

3.5.1 Analysis of reports available from network operators, including reports on

equivalence testing

3.5.1.1 Uncertainty

The uncertainty of sampling methods for PM10 and PM2.5 can be determined by initial field

measurements or during equivalence trials. To achieve a representative assessment to show

the spread of sites across MS that are below 25 % uncertainty and those that are not for PM10

and PM2.5 we would need to be able to determine the method used to obtain the data uploaded

to airbase. As the assessment of methods across all MS shows (see section 3.4), it is not pos-

sible to carry out an assessment in this way as there are currently too many methods catego-

rised as ‗unknown method‘ as a result of omissions or the lack of more specific information.



3.5.1.2 Time Coverage

There is no time coverage requirement in the AQD for PM10 and PM2.5 measurements; however

it is necessary to ensure that the data capture (%) for all measurements is consistent to ensure

that the data quality objectives are met. Recommendations have been made in light of a possi-

ble inconsistency that occurs with the provision of data capture in per cent as opposed to days.

3.5.1.3 Data Capture

For 2009, 69 % of 2,851 PM10 data sets achieved a data capture of 90 % or more. This is a 10%

increase compared to 2001. The highest percentage (71 %) of data sets with data capture

≥ 90 % appeared in 2006. Only 53% of 801 PM2.5 datasets achieved data capture ≥ 90 % in

2009, this is 10 % higher than in 200814

.

UK, Romania, Greece, Ireland, Latvia and Malta provided less than 50 % of PM10 datasets with

a data capture of ≥ 90 % for 2009. In Austria, Bulgaria, Finland, Lithuania, Estonia and Luxem-

bourg 90% or more of the PM10 data sets had ≥ 90 % data capture.

UK, Spain, Poland, Romania, The Netherlands, Bulgaria, Croatia, Latvia and Malta show less

than 50 % of PM2.5 data sets with ≥ 90 % data capture. In Hungary, Austria, Slovakia, Slovenia

and Cyprus all of the PM2.5 data sets provided had ≥ 90% data capture.

3.5.2 Recommendations for improvements

The findings surrounding missing documentation of sampling and analytical methods are a ma-

jor issue when determining the station compliance with the data quality objectives. The Com-

mission needs to police its own requirements for data provision thoroughly. Data sets without

documentation of measurement methods cannot be used for assessment.

MS should provide uncertainty information with the data; this could be checked with assump-

tions made using the first recommendation.

Specific details of sampler manufacturer, model and analysis method (if applicable) should be

provided for all measurements such that the equivalence can be categorised. It would also then

be possible to list the uncertainties from equivalence reports and similar information such that

assumptions could be made regarding the uncertainty of data sets. This could then be used as

a sense check with the quoted uncertainty provided.

Time coverage and data capture should be detailed in terms of days sampled as opposed to per

cent so there is less possibility for error. I.e. Time coverage 365 days, Data capture 286 days.

This has the following advantages:

Verify the start date and end date corresponds with the time coverage

Removes any potential inconsistency with the data capture

14

The comparably low fraction of PM2.5 stations with high data capture can be attributed to the large number of ―new‖

PM2.5 stations put into operation during the year.



3.6 Siting criteria

This task comprises a comparison of reported monitoring stations to macro-scale siting criteria

of the AQD as laid down in Annex III, V, VIII, and IX of the AQD for each pollutant:

Annex III: Macro-scale and micro-scale siting criteria for all pollutants covered by the AQD

except ozone

Annex V: Number of monitoring stations per zone (all pollutants covered by the AQD except

ozone), including ratio between traffic and background sites, and ratio between PM10 and

PM2.5 sites.

Annex VIII: Macro-scale and micro-scale siting criteria for ozone

Annex IX: Number of monitoring stations per zone for ozone.

In addition, the number of monitoring sites fulfilling the monitoring requirements laid down in

Art. 6 (5) and Annex IV of the AQD (background measurements of PM2.5 compounds) and

Art. 5 (9) of DD4 (background measurements of heavy metals and PAHs in PM10 and their

deposition) as well as cooperation with other MSs have been screened.

Data sources are both AirBase and the annual Questionnaires according to 2004/461/EC, as

well as replies from a questionnaire distributed to MSs.

The percentage of background monitoring sites for NO2 and PM10 varies considerably between

different zones, from around 30 % up to 100 %. The percentage of background PM2.5 sites is

generally higher, corresponding to the focus of the AQD on population exposure.

This reflects the quite different structure of monitoring networks even within one MS.

The number of PM2.5 monitoring sites does not yet fulfil the requirements of Annex V. It may be

considered that the installation of monitoring sites is not yet completed, and AEI sites, which per

definition are urban background sites, have been installed at first.

In case of heavy metals, which are monitored at few industrial sites, the percentage of hot spot

locations varies from 0 to 100 % per zone. This may be justified because background heavy

metal concentrations are below the lower assessment threshold in most parts of Europe.

Most MSs state in their replies to the questionnaire the complete fulfilment of the siting criteria

laid down in Annex III. The justification for non-compliance with the micro-scale siting criteria

mostly comprises technical reasons due to local circumstances, mainly concerning traffic-

related measurement at larger distance from kerb than 10 m.

The minimum requirements for the number of NO2 monitoring sites laid down in Annex V.A are

fulfilled in almost all zones.

The minimum requirements for the sum of the number of PM10 and PM2.5 sites are not fulfilled in

most MSs. In all cases of non-compliance with the ratio of PM10/PM2.5 monitoring sites (between

0.5 and 2.0 according to Annex V), this ratio is above 2, i.e. there is a broad ―lack‖ of PM2.5 sites.

The high amount of ―missing‖ PM2.5 monitoring stations may be attributed to a delay in the im-

plementation of AQD.

The requirement for the ratio of traffic and background sites (between 0.5 and 2.0 according to

Annex V) is fulfilled in all zones in only four small MS; it is not fulfilled in all zones in 14 of the in-

vestigated MS, in three MSs only 25 % of the zones comply with these requirement. In most

cases of non-compliance, this ratio is below 0.5, i.e. traffic sites are missing.

Annex V.C of the AQD lays down the minimum number of monitoring sites to assess compli-

ance with the critical levels for the protection of vegetation in non-agglomeration zones: one site

per 20,000 km² if the upper assessment threshold is exceeded, one site per 40.000 km² if the



concentration is between the lower and the upper assessment threshold; no measurement is

required if the concentration is below the lower assessment threshold.

The information derived from the 2004/461/EC questionnaires related to monitoring sites to as-

sess compliance with the critical levels for the protection of vegetation is inconsistent or incom-

plete in several MSs. Therefore a check of the fulfilment of Annex V.C based on a representa-

tive subset of MSs is not possible. The criteria of Annex V.C are fulfilled in eight MSs. Several

MSs do not designate ozone monitoring sites to assess compliance with the critical levels for

the protection of vegetation or designate only a small subset of non-agglomeration zones.

The criteria for the number of ozone monitoring sites per zone laid down in Annex IX are fulfilled

in all zones in nine MSs (out of the screened 19 MSs); eight MS fulfil the criteria in at least 50 %

of the zones, and two in fewer zones.

All 16 MSs, which replied to the questionnaire, monitor PM2.5 compounds as well as HM and

PAHs in PM10 at a sufficient number of rural background sites. PAH background deposition

measurements are performed in only 12 MSs, HM deposition measurements in 14 MS meas-

urements.

Cooperation with other MSs is very rare, it only concerns BE/NL and FI/SE.

3.7 Reference methods

This section discusses the strengths and weakness of the various reference methods standard-

ised by the European Committee for Standardization (CEN) for the measurement of concentra-

tions of PM, heavy metals and PAH‘s in ambient air and deposition rates. Information sources

are the documents and draft standards of CEN, reports and presentations of Member States

experience given at AQUILA meetings as well as reports and comparison reports by the Euro-

pean Commission‘s Joint Research Centre (JRC).

3.7.1 Reference methods for PM

Currently, the reference methods for PM10 (EN 12341:1998) and PM2.5 (EN 14907:2005) are

manual gravimetric methods and allow more than one volume flow rate. As the mass of the PM

material is determinded by weighing the filter at specified conditions before and after sampling,

an daily information update to the public is not possible.

At present the methodology for monitoring PM10 and PM2.5 in ambient air is being harmonised in

a single European Standard (prEN 12341:2012) which merges the earlier EN 12341:1998 and

EN 14907:2005. The main differences to the existing standards for PM10 or PM2,5 are:

sampling with a flow rate of 2.3 m³/h (low volume sampler) only;

method allows the use of sequential sampler equipped with automated filter changers;

stricter conditions required in the weighing room: 45 % - 50 % relative humidity;

required filter identification.

The major sources of uncertainty of gravimetric PM measurement are effects of humidity on fil-

ters, the sampling flow rate and the lack of criteria for the performance of filter materials used.

The stricter requirements for the weighing procedures of filters in prEN 12341:2012 are the re-

sult of filter tests to address the effects of exposure of filters to high or varying relative humid-

ities.



In most of the MS low volume samplers operating at a nominal flow rate of 2.3 m³/h are used,

also common is a flow rate of 1 m³/h which is neither reference according to EN 12341:1998 nor

EN 14907:2005 and 30 m³/h which is reference according EN 14907:2005 but not according

EN 12341:1998. All MS except one use samplers equipped with an automated filter changer,

suitable for stand-alone operation. The most common used filter types are filters made of quartz

fibre followed by filters made of glass fibre. The requirements of prEN 12341:2012 for

monitoring of temperature and relative humdity in the weighing room and the balance resolution

are at present not fulfilled in all MS.

3.7.2 Reference methods for total gaseous mercury and heavy metals and PAH

in PM10

The reference method for the measurement of total gaseous mercury (TGM) concentrations in

ambient air is an automated method based on atomic absorption spectrometry or atomic fluo-

rescence spectrometry (EN 15852:2010). The results of the validation programme by CEN

showed that the uncertainty in the calibration of the instruments is a key factor. Therefore the

CEN working group proposed the development of more accurate and repeatable calibration

techniques for automatic instruments in future. The uncertainty of the mercury vapour pressure

was not included because there is no scientific consensus on which is the best one to use.

The measurement of heavy metals (reference method EN 14902:2005) and PAH (reference

method EN 15549:2008) in PM10 consists of two parts. First the sampling in the field by

collecting the PM10 fraction according to EN 12341 and second the analysis in the laboratory.

Validation programmes by CEN included laboratory and field tests. The JRC intercomparison

exercises focused on the analysis of the filters and showed good results for the reference

methods of analysis for both, heavy metals and PAH. Degradation of benzo(a)pyrene during

sampling in the presence of reactive gases like ozone or nitrogen dioxide is still under

discussion. Up to the moment no ozone denuders applicable with the reference methods of

PM10 are commercially available. Consequently CEN recommends further measurements with

and without ozone denuders of benzo(a)pyrene in ambient air to inquire the effect of

degradation with respect to the complience of the limit value.

3.7.3 Deposition of heavy metals and PAH

The reference methods for the sampling and analysis of the deposition of arsenic, cadmium,

mercury, nickel and polycyclic aromatic hydrocarbons are standardised by CEN in three stan-

dard methods, EN 15841:2009 (arsenic, cadmium, nickel), EN 15853:2010 (mercury) and

EN 15980:2011 (PAH). As set out in DD4, Annex V, the reference method for the sampling of

the deposition shall be based on the exposition of cylindrical deposit gauges with standardised

dimensions. All three reference methods describe sampling with three different collectors (wet-

only, bulk and Bergerhoff type of gauge) and two different analytical methods. Laboratory and

field tests carried out by different CEN working groups showed the following results:

Sampling with different collector types and sample preparation are the main factors in the

uncertainty budget of deposition measurements.

A different sampling strategy is needed for rural and industrial sites.

The various analysis methods did not influence the results noticeable.

Deposition is highly influenced by coincidental effects.



3.8 PM10 vs. PM2.5

Four questions were considered in this task.

3.8.1 Which PM fraction is the most relevant from the point of view of docu-

mented health effects?

Epidemiology is limited by the data and statistical tools available. As time passes more informa-

tion and experimental evidence are provided and a greater understanding of the biological and

physiological processes within the human body is now available.

Acute morbidity and mortality may correlate with PM fractions and other pollutants (SO2, NOx

etc…); however, if all these components also correlate with each other it is difficult to ascertain

which are more important. It is known that there is a correlation between PM10 and health ef-

fects. PM10 has PM2.5 as a sub-fraction, which mainly contains primary aerosol species such as

elemental carbon (EC) and organic carbon (OC), and secondary aerosol species such as sul-

phate, nitrate, ammonia, and some secondary OC. It is therefore necessary to understand as

completely as possible the potential for health impacts associated with each size fraction or

component in order to best judge possible abatement measures.

Presently, both PM10 and PM2.5 sampling conventions are still important in relation to health ef-

fects. Black carbon (BC) is also important in relation to health effects. Ultrafine particulate (UFP)

particle size and number count concentration may be important in relation to health effects.

However, speciation of metals within PM10 and measurement of anions, cations and EC in PM2.5

will continue to be important as the knowledge base expands.

The UNECE/WHO Task Force on Health Aspects of Air Pollution are still firmly committed to the

need for a reduction in exposure to PM2.5, due to the presence of combustion derived compo-

nents to reduce population exposure and reduce the health effects seen (WHO 2012). The Task

Force recommended that PM2.5 remains the primary measure, with BC as a suitable additional

indicator, specifically for localised measures to reduce exposure to combustion PM but accepts

that work still needs to be done on standardisation of BC and EC measurements and that there

is still need of further toxicological studies on PM and BC.

3.8.2 Is it feasible for monitoring network operators to monitor both fractions,

taking into account the availability of new monitoring techniques?

The network operator has to gather measurements to cover a number of measurement metrics

required for PM10 and PM2.5 under the AQD; consistency in the approach is needed if the refer-

ence methods and the metrics in the AQD do not alter. However, if some of the measurement

metrics are no longer relevant for the assessment of the risk to health, then some consolidation

of instrumentation will occur.

Dual channel and multiple PM analysers are already in use in research and in some MS moni-

toring networks. This would, over time, make it possible to rationalise the physical instruments

that have multiple PM fraction and PM collection capability. Development of systems is driven

by legislative requirements.



3.8.3 Is particle number a better metric than particle mass with respect to hu-

man health?

On balance, measuring the particle number concentration for the UFP size ranges is important

complementary to measuring the mass concentration of PM2.5 and/or BC. Further studies may

help better define the data requirements for health assessment.

3.8.4 Is there a need for new reference methods?

The continued need for the combined PM10 and PM2.5 reference method is clear. Development

needs to continue on the current methods for BC and EC. The EC standard is at the Technical

Report Stage, there are a number of operationally determined definitions of EC, so there is still

a lack of standardisation. For BC, there is a predominant but evolving method, but not true

standardisation, with the existence of built-in sampling or artefact bias correction and post

measurement correction regimes in publication, this can reduce the ability to compare data from

researchers and current networks in operation in Europe and globally.

3.8.5 Conclusions

The current weight of medical evidence strengthen the link between PM and adverse health ef-

fects. Epidemiologists have been presented with different metrics to which mortality and morbid-

ity records can be compared, BS and SO2 in the early 20th Century, NOx, O3 metals, PAH and

PM10 in the later 20th

Century and more recently PM2.5, BC and UFP particle number and count-

ing. Each has seen varying evidence of chronic and acute effects. At times a general indicator

has been sought, such as BS, PM10 and PM2.5.

The challenge has always been to elucidate what in the PM is having this effect. Researchers

have hunted for a single factor, but in truth, there are many components of the PM that have the

potential to present a risk to human health due to toxicity or other effect. Significant effort has

been put into the operational definitions and sampling protocols for the constituent parts of the

PM.

Recent research has centred on understanding the effects of UFP, to understand the mecha-

nisms in play, this would add to the number of determinations needed. Combined toxicologi-

cal/epidemiological research is now picking apart this complex mix and may provide a means to

rationalise the number of required measurements. Considerable attention is now being placed

on Black Carbon, be it expressed as an optical property BC or as a thermal-optical property

(EC/OC analysis). BC is being actively promoted by UNEP and WHO as a component to under-

stand, measure and mitigate, to not only reduce localised health issues, but also to reduce the

risk of climate change as BC is a recognised short-lived climate forcer.

However, current scientific knowledge is not sufficient to implement standards for constituents

such as BC and UFP.

Presently, CEN is preparing a revision of the now combined PM10 and PM2.5 reference method

that will continue to be important especially for the subsequent speciation of the PM. CEN is

also preparing a standard for EC/OC to provide a platform for comparable data. The preparation

of a standard for BC does need to be considered. However it has to be kept in mind that all

these constituents are defined by convention of the measurement method.

WHO is preparing to report on further studies of BC as a health indicator, which coupled with

the climate change mitigation for control based on BC measurement and reduction could be a

potential game changer in the near future. The decrease in mortality expected in Europe due to



controls based on BC attenuation is reasonable, but on a global scale outside the EU in the de-

veloping world, this would have far reaching implications.

This does suggest that, in the medium term, PM2.5 would be a reasonable sampling convention

to retain for comparison with the derived limit values, and this is the current recommendation

from the WHO. The understanding and measurement of BC and EC/OC needs to be expanded

as does the toxicology of UFP; so that the standards and target values can be derived to aug-

ment or even replace the PM mass concentrations as the current measure in the future.

3.9 Reference method vs. near-real-time information

The reference methods given in the AQD for the measurement of particulate matter (PM) are

not commonly used for operation in routine monitoring networks. In order to fulfil the require-

ments of the Directive (information should be updated on an hourly basis), these networks usu-

ally apply Automated continuous Measurement Systems (AMS). The AQD allows the use of

such systems after demonstration of equivalence with the reference method, i.e., after demon-

stration that these systems meet the data quality objectives for continuous measurements.

Guidance on the demonstration of equivalence was provided by the European Commission

(EC) Working Group on Guidance for the Demonstration of Equivalence (most recent report

from 2010, EUROPEAN COMMISSION 2010).This means that there are requirements and guidance

for the use of AMS, but there is no standard method for continuous PM monitoring.

Given the fact that the allowed uncertainty for PM measurements is as high as 25%, that the

reference method itself is associated with uncertainties (see section 3.7), and that Member

States use different kinds of AMS in different configurations, it is evident that variation in PM

measurements is relatively high, both within and between Member States.

3.9.1 Are there any implications associated with the fact that there is no stan-

dard method for continuous PM monitoring?

A consequence of not having a standard method is that there is a lot of variation in the type and

configuration of AMS used in monitoring networks. There are differences between Member

States, but also within some Member States. Based on the information provided by Member

States to the dedicated questionnaire, some Member States apply many different types of AMS

within their monitoring networks (for example Austria and Spain). In the UK one type of AMS is

applied, but with different sampler dryer configurations (RICARDO – AEA 2011).

AMS may be based on the use of oscillating microbalances (TEOM) or ß-ray attenuation, and

on in-situ optical methods (e.g. Grimm dust monitor). Most Member States apply TEOM or ß-ray

monitors. The performance of AMS (and the deviation from the reference method) depends on

many variables:

Configuration of the system

e.g. inlet heating, filter material, either or not fitted in a conditioned housing

Composition of the aerosol

depending on the type of monitoring station (traffic, urban, industrial, rural)

share of volatile components

Meteorological conditions

temperature, relative humidity



wind speed (performance of the sampling head)

e.g. research in the UK (HARRISON et al. 2010) showed that the TEOM FDMS overesti-

mated the PM concentration especially on days with temperatures higher than 25 °C, but

not on all of those days. There may be a relation with relative humidity (inefficient drying).

Maintenance condition and age of the system

e.g. preliminary evidence collected to date suggests that the TEOM FDMS analyser base-

line responses can change by 4 μg/m³ when a new dryer is installed (RICARDO – AEA 2011)

The equivalence trials that are required to determine the instrument uncertainty, do not

give insight in long term operational roll out of a candidate method. This has been ac-

knowledged by the CEN TC 264 Working Group 15 that is in the process of developing a

standard (or technical specification), see under Question 4, section 3.9.4.

Data acquisition method

e.g. comparison of a large number of monitoring stations in the Netherlands (with ß-ray at-

tenuation systems) showed that data acquired digitally were more in line with data from the

reference method than analogue data. Deviations in the analogue data ranged from -2 to

+4 μg/m³ (RIVM 2007).

Apart from these, there may be other variables that we currently are not aware of.

The implication is that inevitably there is a lot of variation between raw measurement data from

AMS. The variation can be decreased by applying procedures for equivalence demonstration.

However, these procedures may vary substantially between Member States, e.g. in the number

and variation of monitoring locations that are taken into account, how often a procedure is re-

peated, the number of instruments, etc.

Also, Member States report that the availability of reliable AMS is limited. In the questionnaire,

the UK mentions: ―There are severe limitations in terms of the availability of automatic tech-

niques which are reliable, type approved, proven equivalent, are tried and tested in the field and

for which the monitoring method is transparent and well understood. … Experience has shown

that, over the long term (that is, outside the scope of equivalence trials) there are issues around

the intercomparability of different measurement methods and thus a mixed network, and that all

PM monitoring techniques have their own quirks and problems‖.

3.9.2 Is there any information to suggest that the relationships between con-

tinuous and gravimetric samplers remains constant with time?

Given the list of variables that the performance of AMS depends upon under question 1, and the

fact that those variables may vary over time, the answer to this question clearly is that the rela-

tionships are not constant with time.

In more detail, the following plays a role in the variation in the relationship with time:

Due to new insights, the configuration of AMS applied in monitoring networks changes with

time (e.g. RIVM 2007).

Due to new insights, the choices that are allowed by the EN 12341 for the reference method

may change with time (e.g. filter type material, conditioning of housing).

Replacement of analyzer‘s components following maintenance schemes may result in a

change of the signal (e.g. with respect to dryers). For an FDMS analyzer, changing even ap-

parently minor components (like rubber air seals) can materially affect performance (RICARDO

– AEA 2011).



When an analyzer needs to be replaced at the end of its lifetime, a direct like for like re-

placement will often not be possible (due to changes in the configuration by the manufac-

turer).

The share of volatile components varies over time.

Meteorological circumstances (temperature, humidity) vary over time.

Besides the temporal variation, the relationship between continuous and gravimetric samplers

also vary in space. The order of variation seems to depend on the type of monitoring station and

the type of analyzer. In an intercomparison study in Germany it was shown that for both PM10

and PM2.5 measured with TEOM FDMS, the relationship may vary drastically from site to site.

However, there was almost no variation in the results obtained with the SHARP monitor

(PFEFFER et al. 2011). An intercomparison study in the Netherlands also showed that the rela-

tionships vary more for certain types of analyzers (RIVM 2008). A further report by RIVM estab-

lished correction equations for PM10 measured with ß-ray attenuation analyzers in the Dutch

monitoring network (RIVM 2008a). They differ between the rural and urban stations.

It seems therefore important that Member States derive correction equations for the different

types of location. This requirement will likely be implemented in the new standard for AMS (for

traffic, urban, industrial and rural stations), developed by CEN TC 264, WG 15 (see under ques-

tion 4).

3.9.3 Does this render information to the public more difficult?

Daily mean PM10 concentrations, and the resulting number of exceedance days have to be pub-

lished every day. These data have not been validated following procedures of the monitoring

authorities. In most cases, the validation will only take place after the year has ended. This may

result in a substantial change in the number of exceedance days once the year has passed. It is

hard to explain this to the public, especially when the number of exceedance days decreases.

3.9.4 What would be the advantages/disadvantages of a separate, continuous

standard method?

As mentioned under question 1 (section 3.9.1), procedures for equivalence demonstration may

vary substantially between Member States. This has been acknowledged by the European

Commission. Currently, the CEN TC 264 Working Group 15 is in the process of developing a

standard (or technical specification), under the working title ―Ambient air quality — Automated

continuous systems for the measurement of the concentration of particulate matter (PM10;

PM2.5)‖. Currently, the standard aims at the following:

Laying down the minimum performance requirements and test procedures for the selection of

appropriate AMS for particulate matter (type approval). This includes the evaluation of

equivalence with the reference method.

Describing minimum requirements for ongoing quality assurance – quality control (QA/QC) of

AMS deployed in the field.

Describing requirements and procedures for the treatment and validation of raw measure-

ment data that are to be used for the assembly of daily or yearly average concentration val-

ues.

Especially the second aim seems important, since relationships between continuous and gra-

vimetric samplers do not remain constant with time (see question 2, section 3.9.2).



The disadvantage of a standard that only gives minimum requirements is that there will still be a

lot of variation in measurement results for PM. To minimize the variation, a standard would be

needed that also defines the measurement method and configuration of the AMS. However, the

still ongoing research into the performance of both AMS and the reference method on the one

side and the allowed uncertainty for PM measurements of 25% on the other, would not allow for

a standard that excludes certain types of AMS.

3.10 Particle size fractions

Data from the informal questionnaire circulated to Member States (section 2.2.2.4) was used to-

gether with data that had been supplied or obtained from Member States on measurements

other than PM10 and PM2.5. The level of detail provided by the Member States was not consis-

tent and ranged from very succinct descriptions to incomplete forms. Some Member States in-

cluded actual data along with their completed informal questionnaire. A summary of these re-

plies is given in Table 4.

Table 4: Summary of responses by MS to the informal questionnaire on PM other than PM10/PM2.5.

Member State PM1 UFP Particle Numbers OC EC

Inorganic Carbon BC Anions Cations

Austria y n n n y (nd) n n y (nd) y (nd)

Belgium y y (2011) y (nd) y (nd) y (nd) n y y (nd) y (nd)

Bulgaria unavailable

Croatia unavailable

Cyprus n n n n n n n n n

Czech Republic n n n y y n n y y

Denmark n n y n n n n n n

Estonia n n n y (2011) y (2011) n n n n

Finland unavailable

France n y n y y n y y y

Germany n n y (nd) n n n n n n

Greece n n n n n n n n n

Hungary unavailable

Ireland n n n y (2011) y (2011) n n y (2011) y (2011)

Italy y y (2012) y (2012) y (2012) y (2012) y (2012) y (2012) y (2012) y (2012)

Latvia n n n n n n n y (nd) y (nd)

Lithuania n n n n n n n n n

Luxemburg n n n n n n n n n

Malta unavailable

Netherlands n n n n n n y n n

Poland n n n y y n n y y

Portugal unavailable

Romania n n n n n n n n n

Slovakia unavailable

Slovenia n n n n n n n n n

Spain y n n y y n n y y

Sweden n n y (nd) y (nd) y (nd) n y (nd) n n

United Kingdom n y y y y n y y y

y = species measured and data available

y (2011) or y (2012) = measurements only started in 2011 or 2012

y (nd) = species listed as measured, but data not given

n = species not listed as measured



The following Member States did not reply to the informal questionnaire: Portugal (PT), Bulgaria

(BG), Slovakia (SK), Finland (FI), Croatia (HR) and Malta (MT)

The following Member States replied, but do not undertake any further PM size fraction or

speciation measurements other than the gravimetric assessment of PM10 and PM2.5 required

under the Directive. They currently do not possess any plans to change/amend this strategy in

future years: Romania (RO), Slovenia (SI), Cyprus (CY) and Luxemburg (LU).

The following measurements are being conducted by the remaining Member States:

PM1 – This is a dust sampling convention analogous to PM10 or PM2.5 but with a sampling

inlet with a 50 % efficiency cut off at 1 µm mean aerodynamic diameter. This is typically

measured by a light scattering technique rather than by direct manual measurement.

Ultrafine particle size (UFP) distribution and number count – typically for the observation of

particle numbers in size classes less than 1 µm in diameter (number concentration of parti-

cles)

Elemental carbon (EC) and organic carbon (OC) are measured by thermal -optical analysis

with transmittance or reflectance correction. EC/OC are required in the speciation of PM2.5 in

the Directive.

Black carbon (BC) is measured typically using an Aethalometer in the infrared range (wave-

length of 880 nm).

Black smoke measurement was an atmospheric dust pollutant method that pre-dates the cur-

rent BC measurements now in more common use.

UV carbon – UV carbon is not a true physical parameter but determined, using an Aethalom-

eter at a wavelength of 370 nm less the BC concentration. In the ultraviolet region below

400 nm increased absorbance is shown for some organic carbon and fine smoke (diesel, oil

fume, solid fuel emissions and tobacco fume).

Anion and cation speciation are determined using time-integrated filter sampling and by con-

tinuous denuder/ion chromatography systems of varying complexity (multiple PM2.5 systems

to large dual PM10/PM2.5/gas analysis systems). The AQD requires the speciation of SO42–

,

NO3–, Cl

– anions and Na

+, K

+, NH4

+, Ca

2+, Mg

2+ cations in PM2.5.

The following Member States provided information on PM monitoring other than PM10 and PM2.5:

Other PM fractions: Continual UFP measured at one location in Germany, France and Italy,

two sites in Belgium and Sweden, three locations in Denmark and four locations in the United

Kingdom. Where data was provided, this was included in the Task Chapter.

BC is measured at four locations in France (FR) and Sweden (SE), 20 locations in Belgium

(BE), 21 locations in the United Kingdom (GB); The Netherlands (NL) are currently measuring

Black Smoke.

PM1 is measured at one sites in Austria (AT), two sites in Italy (IT), multiple sites in Wallonia

in Belgium (BE), and 25 sites in Spain (ES),

Other species within the PM fractions: EC/OC were measured at one site in Spain (ES),

Poland (PL), Belgium (BE), the Czech Republic (CZ), Austria (AT) - EC only, Ireland (IE) and

Estonia (EE); two locations in Italy (IT) and Sweden (SE); four sites in the United Kingdom

(GB) and 15 urban measurement stations in France (FR).

Anions and cations were measured at one site in Spain (ES), Poland (PL), Belgium (BE), the

Czech Republic (CZ), Ireland (IE) and Latvia (LV), two sites in Italy (IT), four sites in the

United Kingdom (GB) seven sites in Austria (AT) and at 15 urban measurement stations in

France (FR).



3.11 Benzo(a)pyrene as marker

For the purposes of assessment under DD4, benzo(a)pyrene (B(a)P) was to be measured and

compared against the prescribed limit value of 1 ng/m³ – B(a)P is defined as a human carcino-

gen by the International Agency for Research on Cancer. In addition to B(a)P, ‗at least‘ six other

specified PAH were also to be measured: Dibenz(a,h)anthracene (DbA) - defined as a probable

human carcinogen and Benzo(a)anthracene (BaA), Benzo(b)fluoranthene (BbF),

Benzo(j)fluoranthene (BjF), Benzo(k)fluoranthene (BkF), and Indeno(1,2,3-cd)pyrene (IdP) –

these are all defined as possible human carcinogens.

Like B(a)P, the benzo fluoranthenes and dibenz(a,h)anthracene are all five ring PAH structures,

benzo(a)anthracene has four rings and Indeno(1,2,3-cd)pyrene has six (Figure 4).

B(a)P DbA BaA BbF

BjF BkF IdP

Figure 4: Chemical structure of PAH (source: Wikimedia Commons).

Benzo(a)pyrene was selected as a marker both by the EU and by other bodies. It has a long

history of characterisation and assessment. Data collected by the Member States could be used

to verify the selection of B(a)P.

The available annual mean data from all Member States was assessed for correlation between

B(a)P and the other reported PAHs, more significant correlations were found than significant

anti-correlations. However PAH has a strong seasonal variation, with the highest mass concen-

trations between early December and mid February, the summer months being at negligible

levels.

Data was taken from the United Kingdom from measurements using the DHA80 PM10 sampler.

Correlation between B(a)P and the six individual selected PAH is very good, out of 32 sites

where the monthly data from at least 2008 to end of 2011 was made available, using typically,

46 pairs of data, 30 sites had very significant correlations, with the remaining two with significant

correlations. The same calculations correlating BkF against each of the additional PAH gave a

very similar outcome.

It is by no means any validation of the use of B(a)P as a marker, as in the literature, the selec-

tion of B(a)P as the marker has come under scrutiny. Two key papers by Park and Saarnio pro-

vide good evidence on the probable list of minimum PAH that are useful to measure and also for



the use of benzo(k)fluoranthene as an alternative marker for the possible and probable carcino-

genic PAH (PARK et al. 2002 and SAARNIO et al. 2008).

However, Saarnio focuses on other factors, such as the relative difference in stability of B(a)P,

which is considered more reactive than BkF. For the UK dataset, we have substituted BkF for

B(a)P in the correlation calculations and was not really any different to the results obtained from

B(a)P against the required additional PAH.. So as far as a surrogate of the six PAH measured

under the Directive, B(a)P and BKF would both suffice, but a risk based limit value has already

been assigned to B(a)P.

Each PAH will have a relative toxicity relative to B(a)P, there are many in the published litera-

ture, but with some widely differing ranges and further complications of derived carcinogens

from the reactive lighter PAHs and PAH present in different particle fractions, a weighting sys-

tem for a range of PAH would be difficult.

From the AirBase data and the available high resolution data from the United Kingdom, there is

nothing to suggest that B(a)P is not a suitable marker with regards to overall apparent behav-

iour. This suggests that a marker is still appropriate.

The list of additional PAH does miss some commonly measured PAH, which are useful in ratio

profiling for source apportionment, a larger profile is also useful for the alternative method of

profile signatures. Although short term measurement campaigns may be better suited for local-

scale source apportionment, researchers have successfully used National Network datasets to

achieve useful national level source apportionment (TOBISZEWSKI et al. 2012, MARI et al. 2010.

DVOSKA et al., 2012, GALARNEAU 2008 and SAARNIO et al. 2008).

To facilitate the basic source apportionment ratios, this would suggest the inclusion of phenan-

threne, anthracene, pyrene, fluoranthene and benzo (ghi) perylene. The ratios of these selected

PAH species can be used to broadly characterise the possible influences from coal combustion,

diesel exhaust fume, petrol exhaust fume, natural gas combustion, oil combustion, vegetative

combustion and wood combustion. However, there are some overlaps between these various

PAH ratios.

3.12 Relationships between pollutants

Correlations between the pollutants PM10, PM2.5, As, Cd, Ni and B(a)P were calculated from the

data in AirBase. The significant correlations and anti-correlations are summarised in Table 5.

There were no significant correlations between the data for PM2.5 with B(a)P, Cd or Ni, or B(a)P

with Cd or Ni.

Table 5 provides a summary of the correlations, this shows the number of sites that are co-

located for each of the correlations, the number of sites having n years of paired data and the

number of results that are potentially significant correlations and anti-correlations (i.e. where the

correlation was at or above the 95% confidence interval) and also shows the number of sites

were there was a positive or negative tendency.



Table 5: Summary of correlating and anti-correlating measurement data (number of sites).

Assessment Correlating sites Anti-correlating sites

PM10 vs As AT: 1, DE: 1, DK: 1, IT: 1 AT: 1

PM10 vs B(a)P AT: 5; LT: 1 IT: 1

PM10 vs Cd AT: 1, DE: 2, DK: 1

PM10 vs Ni AT: 1, DK: 2, IT: 1 DE: 1, IT: 1

PM10 vs PM2.5 AT: 4; BE: 1; CZ: 16; DE: 6; ES: 2; FR: 2; GB: 1; HU: 1; IT: 6; LT: 1; PT: 4; SE: 1

BE: 1

PM2.5 vs As DE: 1

B(a)P vs As AT: 1

As vs Cd AT: 1; BE: 2; DE: 1; LT: 1; UK: 10 AT: 1; BE: 2; UK: 1

As vs Ni AT: 1; BE: 2; DE: 2; DK: 5; IT: 3; UK: 4 AT: 1

Ni vs Cd DK: 1; IT: 1; UK: 4 AT: 3; BE: 1

Where there was collocated data for multiple pollutants, these were also assessed together; it

was found that there are four sites where three measurement parameters all correlate strongly.

These were at two sites in the United Kingdom for As, Cd and Ni at GB0047R – Heigham

Holmes (rural background) and GB0792A – Sheffield Brinsworth (urban); and one site each in

Italy – IT1523A D‘Acquisto (urban background), Asti for Ni, As and PM10 and Denmark –

DK0051A Arhus (urban traffic) for Ni Cd and PM10.

It was hoped that the correlation of these pollutants would provide information on the sources

and to discuss how these sources may be addressed. Additional information and measurements

would be required to detail a complete source apportionment for each Member State. Possible

correlations between PM10, PM2.5, As, Ni, Cd and B(a)P can be attributable to multiple sources

and processes. Identification of individual sources would be a complex task requiring a much

more detailed assessment of each monitoring site and the industry and roads local to them, in-

cluding extensive source receptor modelling and finer resolution data. A more detailed analysis

of sources is undertaken in the specific report for Task 4, see a summary in chapter 5.6

(UMWELTBUNDESAMT 2012).

For PAHs other than B(a)P suggested in DD4, this list omits a number of PAH that can be used

for source apportionment as considered in Section 3.11 above.

Service Request 6 – final report – Developing future objective(s) for PM2.5


4 DEVELOPING FUTURE OBJECTIVE(S) FOR PM2.5

4.1 Key messages

The Air Quality Directive requires the review of the PM2.5 standards, including investigation of

the feasibility of a more ambitious limit value.

Changes of PM standards could improve the effectiveness of health protection, but such im-

provements should be carefully balanced against the importance of regulatory stability.

Possibilities of changing properties of current standards have been investigated, such as the

binding nature of the National Exposure Reduction Target and the spatial extent of the Aver-

age Exposure Indicator and recommendations have been given

Possibilities for new PM standards have been investigated, this is not recommended

Possibilities for simplifying the set of PM standards have been investigated. Withdrawal of

PM standards is however not in accordance with the WHO recommendations.

First results of the current evaluation of PM by WHO and model projections of PM concentra-

tions by IIASA results could be taken into account, but full analysis of attainable levels was

not possible.

4.2 Context

Article 32 of the AQD obliges the Commission to review the PM2.5 air quality standards in the

light of new information and to take into account the feasibility of adopting a more ambitious limit

value for PM2.5, to review the indicative limit value of the second stage for PM2.5 and to consider

confirming or altering that value. Task 3 of this project, which is summarized in this chapter,

aims to support this review (TNO, UMWELTBUNDESAMT & RICARDO – AEA 2013).

New scientific information about the health impact of PM was obtained from the recommenda-

tions by WHO (WHO 2012a, 2013). Data on air quality levels in Member States were based on

the review in Task 1 (section 2) and on model calculations by IIASA aimed at possible revisions

of the NEC. Task 1 also gave information on the progress made in the reduction of PM2.5 emis-

sions and ambient concentrations resulting from Community measures, and this information

was supplemented by the results of a recent questionnaire for the member of the Air Quality

Committee on the implementation of the PM2.5 provisions.

In response to a previous questionnaire to the Stakeholder Expert Group on the Air Policy Re-

view and in a recent workshop on PM, Member States and other stakeholders have suggested

considering revision of the PM standards. These suggestions included simplification of the set of

PM standards, options for including Black Carbon or Ultrafine Particles, and diverging possibili-

ties of making the standards more or less stringent and more or less flexible.

Based on this information and other relevant information, strengths and weaknesses of the ex-

isting and possible new PM air quality standards were evaluated and recommendations on pos-

sible revisions of the PM standards were developed.



4.3 Identification possible new PM standards and selection for further investigation

4.3.1 Criteria for air quality standards

In order to judge the feasibility of air quality standards, a substantial number of relevant criteria

needed to be taken into account:

Health protection – in particular the potential health benefits triggered by actions to achieve

the standard,

Cost-effectiveness of action driven by the standard,

Attainability and attainment costs,

Scientific robustness,

Environmental equity,

Fairness to regulators (e.g. differences in reduction potentials, in effort already undertaken,

differences in climate and topography)

Regulatory stability/continuity,

Possibilities to assess (measure/model) compliance ,

Coherence with other (EU) legislation (e.g. EURO regulations for mobile sources),

Synergy (or antagonism) regarding other (EU) policies,

Stability in relation to meteorological variability,

Comparability to international standards,

Implementation burden,

Redundancy,

Complexity,

Message conveyed and transparency.

The criteria were used to evaluate the added value of possible changes given the existence of

the current set of PM standards. Using the above criteria we discussed whether a change was

favourable, neutral or unfavourable. We did not attempt balancing the added value against the

regulatory stability criterion, which is always a reason for not changing the legislation. Changes

that we identified as possible improvements of the PM standards were recommended for con-

sideration, but the choice between improving the current provisions or leaving the system un-

changed was left to the political decision making process.

Acceptability for stakeholders, in particular Member States, is obviously another important crite-

rion. However, because the current investigation is intended to support the stakeholders in find-

ing an acceptable set of PM standards, this criterion was not considered explicitly.

4.3.2 Selection of possible new PM standards for further investigation

Air quality standards comprise a number of properties that together define the standard: the PM

fraction, the binding nature, the level to be attained, the attainment date, temporal aspects (av-

eraging period) and spatial aspects. In the Air Quality Directive most of these properties are ex-

plicitly written as part of the definition of the standards, but some other properties are defined

elsewhere in provisions that relate to the standard. In Task 3a (section 4.3) we selected for each

of these properties options for further investigation in Task 3d (section 4.6).



4.3.3 PM fraction

The options for PM fractions will primarily be based on the recommendations by the WHO; a PM

fraction will only be considered if there is sufficient evidence of its health risk. Stakeholders and

international scientific organisations have recommended considering regulating BC/EC (see

also section 3.8). In the USA a standard for ―coarse‖ particulate matter PM10-2.5 has been intro-

duced15

.

Indicators selected for further evaluation:

PM2.5

PM10

PM10-2.5

BC/EC.

4.3.3.1 Binding nature

The binding nature of a standard is closely linked to the level to be attained and to the levels

that are achievable under different scenarios for future emissions; the level to be attained can

be set lower when the binding level is reduced. In view of uncertainties in the attainability of new

standards, the binding nature may be very important for stakeholders. Therefore we will keep all

possibilities for further evaluation.

Binding options selected for further evaluation:

Binding standards‖ (limit values, the ECO), which set air quality levels that have to be at-

tained by a given date,

Derogations of binding standards,

Target value, which does not require measures entailing disproportionate costs,

Short-term alert and information thresholds Alert threshold,

―Stage 2‖ standard and timeline,

Long term objective,

Non-binding health indicator.

4.3.3.2 Level to be attained

The level to be attained can be a specified concentration or a specified change of the concen-

tration (an absolute change or a percentage change). Some stakeholders have suggested con-

sidering a standard for the national contribution to the concentration, excluding transboundary

contribution, which cannot be controlled by the responsible authorities. The level that can be at-

tained in 2015, 2020, 2025, 2030 and possibly 2050 will be based on calculations by IIASA.

Parameters of levels to be attained selected for further evaluation:

Concentration;

Percentage change in concentration;

National contribution to concentration;

Percentage change to national contribution to concentration.

Numerical values of levels to be attained:

No restrictions.

15

http://www.epa.gov/air/criteria.html

http://www.epa.gov/air/criteria.html



4.3.3.3 Attainment date

Data on attainability will be available for 2015, 2020, 2025, 2030 and possibly 2050. There is no

reason to exclude at the first stage any attainability date.

Attainability dates selected for further evaluation:

No restrictions.

4.3.3.4 Temporal aspects

The choice of the temporal aspects will in the first place be based on the WHO recommenda-

tions.

Temporal aspects preliminarily selected for further evaluation:

Annual averages

Multiyear averages;

Percentiles of daily averages.

4.3.3.5 Spatial aspects

The spatial extent of the current limit values is implicitly given by the siting requirements of

monitoring stations. The spatial extent of the NERT and ECO is defined in the AEI. When a

standard applies everywhere, the attainable level is high because it depends on the most unfa-

vourable locations in the EU; for the many other areas where such a high limit value would be

already met, the directive does not require action. Therefore more spatially differentiated limit

values should be considered.

Stakeholders have suggested relating standards more strongly to human exposure.

Spatial aspects selected for further evaluation:

Applying everywhere, as for the current limit values;

Depending on the type of location, particularly urban background;

Spatially averaged over certain types of area;

Related to human exposure.

4.4 Evaluating the current state of implementation of the relevant provisions

4.4.1 Implementation of assessment provisions

The current state of implementation of the provisions relevant to PM2.5 were evaluated in Task 1

of the current project. Data from Airbase, the annual questionnaire 2004/461/EC were consid-

ered along with emissions data. Responses to a questionnaire to Member States in February

2012 seeking further information were evaluated.

Five groups of analysis have been carried out for PM2.5:

Analysis of current (2010) ambient PM2.5 annual mean concentrations

Analysis of historic trends in ambient PM2.5 concentrations

Analysis of historic trends in emission of PM2.5.



The calculation and assessment of the Average Exposure Indicator (AEI).

Analysis of PM below PM2.5 and constituents.

The results of this analysis are summarized in section 2.4 and 2.5.

4.4.2 Implementation of management provisions

Since the introduction of the PM10 limit value, numerous measures have been implemented in

most Member States to achieve compliance with those limit values. These measures have inter

alia reported in time extension notifications. As the USA has had air quality standards in place

for PM2.5 for some years, as a starting point, we considered the extensive list of actions pub-

lished by the US EPA16

as reasonably available control measures for PM2.5. We then consid-

ered the EU management provisions for PM10 standards and mapped these onto those known

to deliver PM2.5 emission reductions, based on the US EPA experiences. Hence, we have ex-

amined those measures being implemented to reduce PM10 emissions according to:

Type of exceedance area, i.e. whether it is predominantly vehicular, industrial, or domestic

emissions that are responsible for potential non-attainment;

Source sector and type of measure applicable;

The timescale for implementation (short or long term)

Whether a source/measure combination is likely to assist with meeting a PM2.5 National

Emission Reduction Targets (NERT), the Target Values (TV) or limit values (LV) at the road-

side; (i.e. whether the measure targets a reduction in the urban background or at hot spots,

either roadside or industrial);

How the impact of the measure is being monitored.

We have also distinguished between options for PM10 control – and consequently PM2.5 levels –

according to whether they focus on reducing primary sources of PM or whether they reduce

secondary PM as well.

In addition we highlighted measures that mainly reduce PM10 but are of limited effect in the case

of PM2.5 such as street sweeping or winter sanding restrictions.

Where possible we have drawn on recently published examples from a limited number of Euro-

pean countries (selected from the TEN) to illustrate the range of approaches followed in the

wider EU. There is little context specific information on the cost effectiveness of measures – that

which is available is highly unsystematic and is illustrative mainly of the problems of collecting

sound financial information. The detailed description of measures can be found in the specific

report for Task 3 (TNO, UMWELTBUNDESAMT & RICARDO – AEA 2013).

4.4.2.1 Measures suitable for exceedance situations where vehicular exhaust emis-

sions dominate

In general, exhaust emissions occur in the fine fraction; therefore measures to reduce exhaust

emission reduce PM10 and PM2.5 emissions to the same amount.

16

http://www.epa.gov/pm/fs20091118.html

http://www.epa.gov/pm/fs20091118.html



Actions shown to reduce PM2.5 emissions from vehicles are given in Table 6. These actions

were mapped onto measures commonly deployed in the Member States to reduce PM10 emis-

sions and encompass the following measures:

Low Emission Zones

Public Procurement Policies

Traffic Management

Encouragement of Modal shift

Other transport measures e.g. provision of electric vehicle charging points.

Table 6: Additional actions that have been demonstrated to reduce PM2.5 emissions from vehicles

according to the US EPA.

Mobile Source Actions

On-road diesel engine retrofits for public service and heavy goods vehicles using Euro standards

Non-road diesel engine retrofit, rebuild/replace with catalysed particle filter

Diesel idling programs for HGV, locomotive, and other mobile sources

Transportation control measures including transportation demand management and transportation systems management strategies

Programs to reduce emissions or accelerate retirement of high emitting vehicles, boats, lawn and garden equipment

Emissions testing and repair/maintenance programs for on-road vehicles

Emissions testing and repair/maintenance programs for non-road heavy duty vehicles and equipment

Programs to expand use of cleaner burning fuels

Opacity/emissions standards for ``gross-emitting'' diesel equipment or vessels

NOTE: These actions are additional to those taken to meet extant legal obligations.

All of these actions also reduce PM10 and NOx emissions.

Low emission zones

Low Emissions Zones (LEZ) can be an effective way of reducing PM10 and soot emissions that

have the added value of reducing PM2.5. LEZs are in place in 11 European Countries17

. They

were first introduced in Sweden in 1996 and the first motorway LEZ was established in Austria

in 2007. An increasing number of cities are implementing them, either for all vehicles or for

heavy goods vehicles (HGVs) only. LEZs that are for HGVs will in general be less effective than

the LEZs for all vehicles at least in inner city areas. Also those zones which were introduced

early, covered a relatively large geographical area, set an ambitious emissions standards (Euro

4 and better), and which are strictly enforced are, of course, the most effective. A possible

downside is that banning of high emitters in one location may relocate them elsewhere instead

of reducing them and so might have an impact on ‗hot spots‘ without reducing overall back-

ground emissions; this would be a case where the action of a Member State would be unhelpful

with meeting a PM2.5 NERT. However, if the LEZ zone is large enough, vehicles will be affected

on a much larger area as most of the vehicles might have to pass through or enter the LEZ

sooner or later.

17

see e.g. http://www.lowemissionzones.eu/

http://www.lowemissionzones.eu/



Public procurement policies

Public procurement, either directly by Member States or by others as a condition of the receipt

of public subsidies, has been widely applied as a means of engineering the vehicle fleet. Mu-

nicipal vehicle fleets and buses cover large distances in cities and can be a relevant source of

air pollution. Also, they have a large share in heavy vehicles and diesel engines. In addition,

public bodies serve as a role model to the private sector and should set out policies on vehicle

procurement that can be widely promoted. Retrofitting existing vehicles with diesel particulate fil-

ters (DPFs) and furnishing new ones with effective filters or other clean technologies are rele-

vant solutions which we‘ve rewarded in this ranking. Cities have different strategies which in-

clude retrofitting existing vehicles, acquiring new ones, reducing the fleet or investing in alterna-

tive energy sources. As with other measures, the timeline for cleaning the municipal fleet is an

important aspect that we have taken into consideration.

Traffic management

These include measures to maximise the efficient and reliable operation of the existing road

network and to minimise the impact of planned interventions on the road network, including

those that have the potential to disrupt traffic flows, such as road works, which are being ad-

dressed by the London Permit Scheme among other measures.

Modal shift

Modal Shift Measures raise the share of public transport, reduce car use, increase cycling and

walking. They encouraging smarter choices and sustainable travel by e.g. network expansion

and modernisation of railway lines at city level, disabled-friendly bus stops and fleet renewal.

Also introduction of pedestrian zones, improvement for cyclists, increased parking fees and cy-

cle hire schemes are important elements.

Other transport measures

Other measures include inter alia promoting technological change and cleaner vehicles, provi-

sion of electrical vehicle charging points and reduction of idling periods

4.4.2.2 Measures for exceedance situations where industrial, heat and power produc-

tion emissions dominate

Actions shown to reduce PM2.5 emissions from industrial, heat and power production are given

in Table 7.



Table 7: Additional actions that have been demonstrated to reduce PM2.5 emissions from stationary

sources according to the US EPA.

Stationary Source Actions

Stationary diesel engine retrofit, rebuild or replacement, with catalysed particle filter

New or upgraded emission control requirements for direct PM2.5 emissions at stationary sources (e.g., bag-house or electrostatic precipitators; and improved monitoring methods)

New or upgraded emission controls for PM2.5 precursors at stationary sources (e.g., wet/dry scrubbers)

Energy efficiency measures to reduce fuel consumption

Measures to reduce fugitive dust from industrial sites


The actions, depending on the stringency of implementation are effective in avoiding, reducing

or abating emissions of PM and, in some cases, NOx; they also tend to reduce the background

emission and may assist in reducing average exposure (as measured by AEI) and NERTs.

These include:

Improved process design

Energy efficiency measures

Tightening existing emissions standards and permits as opportunity allows, by:

The use of less polluting fuels (natural gas, biogas, light oils etc)

Optimized facility maintenance programmes

Improved combustion plants efficiency and refurbishment of equipment

Establish procedures for pollution days

More stringent application of existing legislation.

Fostering of inspection

4.4.2.3 Measures for where agricultural18

, commercial, public and residential emis-

sions dominate

Actions shown to reduce PM2.5 emissions from agriculture, commercial, public and residential

sources are given in Table 8. These actions were mapped onto measures commonly deployed

in the Member States to reduce PM10 emissions and encompass measures which reduce com-

bustion emissions from commercial, public and residential buildings and activities.

18

Agriculture is included at here as it is usually rural and its contribution to background tends to be its most significant

impact.



Table 8: Additional actions that have been demonstrated to reduce PM2.5 emissions from agriculture,

commercial, public and residential sources according to the US EPA.

Area Source Actions

New open burning regulations and/or measures to minimize emissions from forestry and agricultural burning activities

Smoke management programs to reduce domestic coal use

Reduce emissions from woodstoves and fireplaces

Regulate charbroiling/other commercial cooking operations

Further reduce solvent usage or solvent substitution (particularly for organic compounds with 7 carbon atoms or more, such as toluene, xylene, and trimethyl benzene)


These actions also reduce the background emission and may assist in reducing average expo-

sure (as measured by AEI) and NERTs. These include:

Avoiding, reducing and/or abating combustion emissions (solid and liquid fuels)

Combined Heat and Power (CHP)

Energy efficiency, retrofitting public housing stock.

Clean air zones

Small combustion plant inspection systems

Additional requirements for planning consents

Improved policing of or extension to smoke control zones

National small combustion plant regulations are an important measure to control PM in the lo-

calised areas. For example, in the UK the Clean Air Act (CAA) regulates emissions from resi-

dential heating, commercial/institutional heating and, small industrial activity (heating and proc-

ess emissions). The recent revision to the Gothenburg protocol sets national emission ceilings

for PM2.5 . The contribution of small combustion activities to the new 2020 ceilings for PM2.5 are

about 20 % which indicates the importance of these activities when considering measures to

address the new ceilings for PM2.5 .

Part II of the CAA (Article 4) requires new non-domestic furnaces and boilers to be capable of

smokeless operation and to be notified and plans approved by the Local Authority Part II of the

CAA (Articles 14 to 16) includes provision for approval of chimney height for non-domestic fur-

naces

Part III (Article 18) of the CAA allows the designation of Smoke Control Areas (SCA). Article 20

prohibits emission of smoke from building chimneys and from chimneys serving furnaces of ‗any

fixed boiler or industrial plant‗ in an SCA.

Smoke Control Area provisions have been effective in controlling emissions from domestic solid

fuel combustion including significant impacts on national emissions of Benzo(a)pyrene, PM10

and PM2.5 . PM2.5 domestic fuel emissions are predicted to increase 5 times in smoke control ar-

eas if current authorised smokeless fuels were to be replaced with wood (AEA 2012).

In Germany19

an ordinance20

(―1. BImSchV‖) provides for stringent emission limit values for PM

(and other pollutants) for new heating systems. Limit values have also been set for existing

19

The Danish Environment ministry announced on 6 December 2012 to implement new, thighter emission limit values

for stoves, http://www.mim.dk/Nyheder/20121206_braendebkg.htm

20 www.bmu.de/luftreinhaltung/downloads/doc/39616.php

http://www.mim.dk/Nyheder/20121206_braendebkg.htm

http://www.bmu.de/luftreinhaltung/downloads/doc/39616.php



stoves and ovens, for which compliance has to be proven or a retrofitting or replacement has to

be undertaken until 2024 at the latest. In addition this ordinance stipulates that operators must

be advised on the proper handling of the heating systems and the solid fuels to be used. In ad-

dition, wood fuel will be checked regularly for quality in the framework of other monitoring tasks.

There is anecdotal evidence that fuel or energy poverty and increase in gas and oil prices might

lead to increased use of low quality solid fuel or waste for residential heating. This could result

in increased levels of PM and PAH in various areas in Europe. Fuel poverty in general is de-

fined as a situation where households cannot afford or have to use a high percentage of income

to heat their homes to an adequate level (see e.g. BOUZAROVSKI – BUZAR, S. 2011; BRUNNER ET

AL. 2011; THOMSON, H. & SNELL, C. 2012; CASE 2012). The reasons might be low incomes, high

fuel prices and/or energy-inefficient buildings (and heating systems). Improvements of building

insulations and heating systems in general result in a reduction of emissions as well.

4.4.2.4 Measures for agriculture – suitable for PM exceedance situations

The reductions achievable in PM levels (particularly for PM2.5) by local measures is limited due

to dominant regional background concentrations, it is recommended that consideration is given

to further decrease emissions by gaseous precursors (e.g. NOx, SO2 and NH3) at EU level (NEC

Directive) to further decrease the regional background of PM. Also, given their rural nature,

measures for agriculture have the greatest potential for influencing background concentrations

NH3. These measures include:

Reduce NH3 emissions

Control agricultural burning

Control dust emissions

Measures to reduce NH3 emissions are indicated inter alia in the UNECE Gothenburg protocol

and supporting documents for this protocol and the IPPC Directive. Within the Nitrates Directive

Member States established codes of good agricultural practice and developed specific action

programmes. Possible and effective measures include those that are part of good agricultural

practice, e.g. timing of manure application and low emission techniques (e.g. band spreading,

subsequent incorporation of manure, slurry injection,…), reduced application of urea or treat-

ment of exhaust air by scrubbers and biotrickling filters in pig housing.

Agricultural waste burning releases PM2.5 to the air and in the recent GAINS model agriculture

accounts for 13 % of PM2.5 emissions (IIASA 2012a, 2012b, 2012c). Projections to 2030 show

that the contribution of agriculture to PM2.5 is expected to grow as the current legislation base-

line does not foresee any additional legislation in this area. The Good Agricultural and Environ-

mental Condition (GAEC) of the Common Agricultural Policy (CAP) sets out a ban of burning of

straw and stubbles in most MS. In addition some MS also ban agricultural burning under na-

tional legislation, e.g., Denmark since 1991 and England since 1993. Consequently, many na-

tional emissions inventories21

show a decline in emissions of PM from agriculture. However,

IIASA reported evidence of continued burning in many MS from remote sensing data derived

from the Global Fire Emission Database (GFED22

) database.

The GAINS model assumes a complete removal of PM2.5 emissions following the implementa-

tion of a ban on agricultural waste burning. This measure is relatively low costs and therefore is

21

However, there is a incomplete reporting of emissions from this sector.

22 www.globalfiredata.org

http://www.globalfiredata.org/



presented as an attractive option. If enforcement difficulties are overcome, this measure is likely

to be cost effective across MS.

4.4.2.5 Other measures

There are further measures available that are helpful to reduce PM levels on the long run or that

are helpful to implement stringent measures. These measures are not source specific and in-

clude inter alia:

Development of forest on open areas in and adjacent to urban centres with high PM levels.

The establishment of vegetation barriers alongside busy roads and beside industrial plant.

Improved transparency and communication of air quality plans with ‗emittors‘ (i.e. airports,

large commercial organisations etc) and the public.

Strategic planning – tackling emissions associated with new developments.

4.4.2.6 Measures that mainly reduce PM10 but hardly PM2.5

In the time extension notifications for PM10 a considerable number of measures were listed that

aim to reducing the coarse fraction (PM10-2.5) but are of limited effectiveness for reducing PM2.5.

These are inter alia:

Street sweeping: In a review study on the effectiveness of street sweeping no clear evidence

was found for the reduction of PM10 (AMATO et al. 2010). In this study the ratio of exhaust to

non-exhaust vehicle emissions was named to be 1.2 for PM10 but 4 for PM2.5. Given the fact

that street sweeping is expected to affect mostly the coarse fraction, the impact on PM2.5 is

likely to be small.

Winter sanding: The PM2.5 fraction of street wear and winter sanding particles in PM10 is

about 10-15 % (KUPIAINEN et al. 2005, TERVAHATTU et al. 2006). This considerably limits the

impact on PM2.5 concentrations of measures to control winter sanding.

Chemical dust suppressants: In a recent study on the effectiveness of reduction of PM10 and

PM2.5 by applying Calcium Magnesium Acetate (CMA) on roads an effect of about 10 % for

PM10 and about 3% for PM2.5 was found (URS 2011). The authors also concluded that further

work is required to confirm these effects.

Construction work: Also in the case of construction work, for mechanical generated dust the

fraction of PM2.5 in PM10 is about 20 % (see e.g. WATSON & CHOW 2000). Therefore the effec-

tiveness of reducing dust at construction sites is 5 times lower for PM2.5 than for PM10. How-

ever, this would be improved with more measures to control exhaust emissions from con-

struction machinery and construction site traffic were put in place.

4.4.2.7 Overview

In the following table the effectiveness of the measures described above is summarized and

evaluated qualitatively for reducing various PM fractions and measurands. The actual impact is

dependent on the concrete definition and implementation of the measure. The qualitative

evaluation given in the table therefore reflects a subjective expert estimate for typical cases



Table 9: Qualitative evaluation of the effectiveness of different measures on various PM fractions and

constituents.

Type of measure Measure PM fraction Comment

PM10 PM2.5 PM10-2.5 UFP EC/BC

traffic

low emission zone +++ +++ +++ +++ +++

Public procurement policies + + + + + usually the num-ber of vehicles af-fected is small. However, locally the impact can be high (e.g. roads or places with high share of public buses)

traffic management +, ++ +, ++ +, ++ +, ++ +, ++

modal shift +, ++ +, ++ +, ++ +, ++ +, ++

other transport measures +, ++ 0, + ++ 0 0, +

industry Avoiding, reducing, and abat-ing emissions

+ + + + +

agriculture NH3 emissions + + + 0 0

agricultural burning + + + + +

commercial, public, residential

Misc. measures + + + + +

other

e.g. forests, vegetation barri-ers

+ 0 + 0 0

strategic planning + + + + +

PM10

street sweeping, winter sand-ing

0, + 0 + 0 0

chemical dust suppressants + 0, + + 0 0

construction + 0 + 0 0

In principle, a target aim is to set policy and legislation so that the majority of pollution issues

are addressed with Community wide measures, with more difficult issues being addressed via

national measures. For isolated issues set in local circumstances, then local measures should

be relied upon to reduce emissions in these instances, but on the whole these should not arise

in the norm.

The implementation of this principle, has in recent years proved difficult to deliver as Community

wide measures such as the EURO standards in meeting emission standards in real world driv-

ing conditions has resulted in higher emissions that what was expected.

At this point, it is difficult to predict the impact of European Community wide measures com-

pared with national/local measures in relation to PM but it is important that we should ade-

quately assess the uncertainties in these measures and compare with standard compliance.

The uncertainties in the deliverance of Euro 6 standards have been assessed by IIASA (IIASA

2012d). While it is noted that PM impact is related to the concentrations of total PM2.5 in the air

and this comprises both directly emitted particles and secondary particles (PM2.5 formed in the

air by chemical reaction), NOx and NH3 are important to examine as they contribute to secon-

dary PM2.5 .

The GAINS model has been used by IIASA to show that if we assume Euro VI/6 emissions cal-

culated with COPERT 4 for PM reduction then Euro VI only delivers a 50 % improvement over

Euro V. However, if the baseline NOx emissions were adjusted in each MS to account for the

greater transport NOx emissions before the optimisation scenarios were run then the results as-



suming a future Euro VI delivers a 50% improvement over Euro V and Euro 6 is the same as

Euro 5.

Clearly, some uncertainty remains over the real world deliverance of the Community wide

measures already in place. It important that a close watching brief is maintained in this area to

monitor the compliance gap, and the ability of various measures to close this gap year on year.

4.4.3 Questionnaire on air quality management for PM2.5 reduction targets and

exposure obligation

In September 2012 an informal questionnaire on air quality management for the PM2.5 reduction

targets and exposure obligation was sent on behalf of the Commission to the members of the

Air Quality Committee. It was aimed at national and regional authorities responsible for PM2.5

management. The questionnaire addressed the following themes:

1. The National Exposure Reduction Target (NERT) and the Exposure Concentration Obligation

(ECO) for PM2.5;

2. Information on PM2.5 projections and measures, as well as accompanying studies;

3. Suggestions by Member States for alternative approaches than those laid down in Annex XIV

of the AQD.

Fourteen replies were received, of which ten came from representatives of a national authority

(Hungary, Ireland, Lithuania, Luxembourg, Malta, Netherlands, Norway, Poland, Spain, Swe-

den, United Kingdom) and three came from the three regions in Belgium. All replies have been

made available to the Commission.

Most respondents had not yet analysed the need of measures to achieve the NERT or ECO.

Seven respondents gave suggestions about alternative concepts to reduce exposure to PM2.5.

Suggestions given by more than one respondent are:

Four respondents suggested giving more attention to black carbon or combustion aerosol.

Three respondents pointed out that the NERT and ECO levels are dominated by large scale

pollution and should in the first place be addressed by EU-wide policies.

Two respondents suggested to adopt a population weighted AEI.

4.5 Overview of current levels, projections, reduction potential and technical feasibility for attaining selected PM standards

Under the service contract Monitoring and Assessment of Sectorial Implementation Actions a

consortium led by IIASA has developed projections of emissions and air quality.

The most relevant results in relation to the PM standards are given in recent report by IIASA

(IIASA 2012e). Several scenarios are considered: a baseline scenario (current legislation – CLE),

the Maximum Technical Feasible Reduction (MTFR) Scenario, in which all possible technical

measures, irrespective of costs, are assumed in force, and three policy scenarios in which

emission reductions are assumed of low, medium and high ambition, corresponding to closure

of the gap between CLE and MTFR of respectively 25%, 50% and 75%.

In model calculations projections of ambient concentrations in 2020, 2025, 2030 and 2050 were

done for rural as well as urban background levels in Europe. Using a scaling method for the

measured concentration difference between hotspot stations and nearby urban background sta-

tions estimates could also be made of the future concentrations at hotspot stations.



Table 10 shows the expected non-compliance with the current PM10 limit values in 2030 in the

various scenarios. Compared to the non-compliance of today (around 2010, 25% of the stations

did not comply with the PM10 limit values), a considerable progress towards compliance is be

expected, but in all scenarios a significant number of stations are predicted to not achieve com-

pliance: For the baseline scenario this number is of the order of 10% of the stations, which goes

down to roughly 5% in the most ambitious policy scenarios.

Table 10 Estimated percentage of stations in compliance with the current PM10 limit values in 2030. The

three scenario cases reflect low, medium and high ambition. The three columns indicate the

likeliness of the percentages (IIASA 2012e).

Scenario Percentage of stations in compliance with the current PM10 limit values

Likely Uncertain Unlikely

Baseline 84% 13% 3%

Low case 86% 11% 3%

Mid case 88% 10% 3%

High case 89% 9% 2%

Maximum Technical Feasible Reduction

92% 6% 2%

Other information on PM levels was obtained from the work in Task 1 of the service contract

and the questionnaire for the Air Quality Committee on PM2.5, see Table 11.



Table 11: Maximum levels of PM10 and PM2.5 in and around 2010. Exceedances of limit values and ECO in

bold (source: AirBase; AEI levels either from questionnaire 2004/461/EC or reply to specific

questionnaire for Task 3). Self-reported data are taken from the answers to the questionnaire

on PM2.5.

Member State/Country

PM10 exc. days

PM10 annual mean

PM2.5 annual mean

AEI AEI self-reported NERT NERT self-reported

*

Austria 87 38 24 17.6 15%

Belgium 69 36 23

19 20% 20%

Bulgaria 214 76 35 36 18

Cyprus 124 58 23

Czech Republic 159 66 50

Denmark 19 27 18 14 15%

Estonia 35 22 12

Finland 24 25 11 8.3 0%

France 167 52 26

Germany 104 44 27 16 15%

Greece 99 49 15 17 15%

Hungary 109 44 23 21 22 18 µg/m³ 18 µg/m³

Ireland 10 23 12 .. 10.2 10% 10%

Italy 161 51 33

Latvia 59 39 27 18 20%

Lithuania 54 34 20 12.3 12.3 10% 10%

Luxembourg 15 25 16 17.4 16 15% 15%

Malta 84 45 20

13.2 15%

Netherlands 35 32 20 .. 17 15% 15%

Poland 184 71 61 28 26 18 µg/m³ 18 µg/m³

Portugal 94 43 14

Romania 87 47 27

Slovakia 144 51 31

Slovenia 69 36 24 20.5 20%

Spain 106 43 20 .. 14.1 15% 15%

Sweden 54 33 14

6.6 0% 0%

* Or derived from the self-reported AEI value

4.6 Detailed assessment of possible new standards, conclusions and recommendations

4.6.1 Options for changes

The options considered for changing in the current standards, for introducing new PM standards

and for simplifying the current set of standards by withdrawing one or several standards are

listed below.



Possible changes of the current standards

Binding nature

Fully binding

Making the NERT binding

Binding with use of the Commission‘s discretional power

Derogations for locations where the standard cannot be met

Further time extension for attainment of PM standards

Streamlining the time extension procedure

Derogations/exemptions for designated areas

Target values

Enforcing Member States to take all proportionate measures required by the NERT

Complementing the limit values with a target value and enforcing that proportionate

measures are taken to achieve the target value

Target values for new PM fractions

Alert and information thresholds

Timeline, ―Stage 2‖ standards

Long term objectives

Non-binding health indicator

Parameter

Redefining the NERT as a concentration target

Applying the NERT and ECO to the national contribution to AEI only

Numeric values

Changing the levels to be attained

Smoothing the NERT table

Attainment dates

Harmonising attainment dates with emission legislation

Long term objective

Stage 2 standards or a timeline for standards

Temporal aspects other than the attainment date

Hourly standard

Introducing a 24-hour standard for PM2.5

Multiyear limit values

Percentiles of 24-hour averages

Spatial aspects

Further specifying the spatial application of the limit values

Defining the spatial application as properties of the standards

Changing the averaging area of the AEI

Statistical form

Improving the relation to exposure

Improving the application of the limit values to locations where people live

Weighting the Average Exposure Indicator by population density

Relating standards directly to actual exposure



a. Possible standards for new PM fractions

Elemental Carbon and Black Carbon

Ultrafine Particles

PM10-2.5

Other PM fractions

b. Simplification of the set of PM air quality standards

Withdrawing one of the PM10 limit values

Replacing both limit values for PM10 by an equivalent or stricter limit value for PM2.5

Replacing the limit value for PM2.5 by an equivalent or stricter limit value for PM10

Withdrawing the ECO while keeping the NERT

Farther going simplifications

Keeping a binding NERT in combination with a reduced number of PM limit values

4.6.2 Analysis of options for change

For these possibilities advantages and disadvantages of changes were systematically dis-

cussed. The purpose of the analysis was not to give final answers, but to present the most rele-

vant considerations for decisions on changes. We attempted balancing pros and cons and to

draw conclusions on desirability, but a fully objective trade-off between pros and cons of

changes was not possible. Before summarising our conclusions and recommendations, we dis-

cussed some considerations that should be leading in the final decision making process.

Regulatory stability and improvement of standards

Based on the set of criteria set out above, we identified several possibilities for improving the

PM standards. If standards are indeed changed to bring about the expected improvements, the

implementation process in Member States – currently still not without problems – will to some

extent be disturbed; a change of a standard may also reduce the effectiveness of planned or al-

ready implemented policies and measures; it may cause an extra administrative burden to

Member States. In our recommendations we left the balance between the added value of im-

provement options and the weight of regulatory stability up to the decision making process; we

only recommended considering changes.

Complexity and refinement of standards

Virtually all standards relate to a simplified representation of the real world. Annual mean air

quality limit values apply to outdoor locations even though nobody will ever be actually exposed

there for a whole year.

Standards may be refined by setting different requirements for different situations. Differentia-

tion can make standards more rational and precise, but it will usually also make the standards

more complicated and difficult to understand. For standards that are only used by specialists,

e.g. standards for medical equipment, complexity is more acceptable than for standards such as

speed limits, which need to be understood by the general population. Air quality standards are

in an intermediate position: it is not necessary for everyone to understand them, but it is impor-

tant that they can be communicated and understood by the public and stakeholders participat-



ing in air quality policy. The current set of PM standards is more complicated than most stan-

dards for other pollutants, which makes communication difficult. Therefore complexity should be

an important consideration.

Health protection and costs of attainment

In our analysis projections of attainable levels by IIASA were included. We evaluated the con-

nection between the binding nature of the standards and the level to be attained, the main de-

terminants of the ambition in the health protection provided by the standards. We did not give

recommendations on the ambition level and left this to the realm of decision making.

Compliance assessment and refinement of standards

There are still important differences in the assessment practice between Member States. Espe-

cially the limit value, with a high spatial resolution and to be attained everywhere, is problematic

in this respect: exceedances at hotspot locations identified in one Member State may go unde-

tected in other Member States due of differences in station siting strategies and/or modelling

capabilities. The expected health protection of refinements of the standards will in practice not

be gathered when the refinements are not reflected in the compliance assessment practice

within Member States.

4.6.3 Changes in the PM standards proposed for consideration

In the recommendations we distinguished three groups of possibilities mentioned above:

1) Optimising the existing standards;

2) Adding standards;

3) Withdrawing standards.

4.6.3.1 Optimising the existing standards

Options for optimising the existing standards are arranged under three headings:

a. Binding nature, flexibility arrangements and spatial differentiation,

b. Changes in the levels to be attained,

c. Refinements of a more technical nature.

a. Binding nature, flexibility arrangements and spatial differentiation

Air quality standards that set a fixed level to be attained everywhere, provide a minimum protec-

tion. Because PM is harmful at all levels and because the levels that can be attained vary con-

siderably over EU, standards are desirable that drive levels down everywhere where this is pos-

sible. The local reduction potential can be taken into account by including flexibility in the bind-

ing nature of the standard or by setting different objectives for different designated areas. Flexi-

bility options considered are:

Making the NERT more binding. Enforcing Member States to take all proportionate measures

The NERT is as target value a weak driver for action. To strengthen it we recommended

considering making the NERT binding, by introducing an enforcement mechanism for taking

proportionate measure or by making it binding with derogation possibilities.



Derogations (possibly streamlined) of otherwise binding standards

The existing time extension procedure could be re-introduced. Widespread derogations

should not be foreseen however. Possibilities for streamlining the derogation procedures

have been suggested.

Spatial differentiation of standards

Instead of ad hoc derogations on request, structural exemptions may be set for specified

types of areas, e.g. cities larger than some size. Because transboundary air pollution is an

important contributor to attainability problems, clear and simple physical or administrative cri-

teria for exemption of areas do not seem feasible. The NERT, specifying different targets per

Member State, has an implicit spatial differentiation but it does not take the reduction poten-

tial into account.

Also for the limit values, flexibility can be achieved by derogations or spatial differentiation or,

alternatively, by complementing the limit values with a target value for which taking propor-

tionate measures is enforced.

b. Changes in the level to be attained

The projections of PM levels in future years and the scenarios for reduction policies developed

by IIASA show that reductions of PM concentrations are possible everywhere in the EU. In cer-

tain areas the existing limit values will not be attained, even in the most ambitious scenarios. A

large share of the possible reductions is due to emission reduction under EU legislation (na-

tional emission ceilings and sectoral emission standards). This is particularly the case for the

projected AEI levels. The scenarios do not include all possible local measures, but it is likely

that local measures cannot bring the levels much further down than the levels calculated. We

did not give recommendations on changes in the levels to be attained. We recommend however

considering setting (or maintaining) lower levels than those attainable everywhere, in combina-

tion with flexibility arrangements (see above).

Attainment dates obviously relate to the levels to be attained. In order to convey to stakeholders

and citizens the message that levels to be attained are far above healthy levels, we recommend

considering setting out a timeline for PM standards. A long-term objective, such as exists al-

ready for ozone, does not seem a viable option.

c. Refinements of a more technical nature

The definition of the reduction objective of the NERT may be improved by smoothing the

NERT table and redefining it as a target concentration.

In order to reduce compliance fluctuations from year to year due to meteorological fluctua-

tions when the PM levels are very close to the level to be attained, three-year averaging for

the limit values could be considered. The number of compliance fluctuation cases is esti-

mated to be almost halved, but this may not be a significant improvement compared to draw-

backs.

We considered possibilities to reduce the averaging area of the AEI, but on balance do not

deem this an improvement.

To improve the representativeness of the AEI for the average exposure, the concentration at

each station contributing to the AEI could be weighted by the population represented by the

station. We deem the pros and cons approximately in balance.

The limit values could be exclusively related to locations where people live, but we do not

recommend this.



The spatial extent of the limit values is currently partly described in siting requirements. Some

clarity may be gained by defining the spatial application as properties of the limit values.

4.6.3.2 Adding standards

24-hour PM2.5 limit value

In its answers, WHO has proposed regulation of short-term average concentrations (such as the

24 hour mean), in addition to the existing annual limit value for PM2.5 and the two PM10 limit val-

ues. The additional health protection in relation to the indirect protection provided by the overlap

with existing limit values strongly depends on the level to be attained, which is not investigated

here. Because a new PM2.5 would increase the already substantial complexity of the current set

of standards, it will be important to carefully balance the added protection against the draw-

backs of a new 24 hour limit value for PM2.5.

New PM fractions

For new PM fractions, in particular black carbon and ultrafine particles, evidence on the health

impact has emerged. Because of uncertainties in attainable levels of possible standards and

immaturities in methods for assessing exceedance, binding standards for these fractions are

deemed premature. For black carbon synergy of air quality policy with climate change policy

would best be achieved in emission legislation. For the option of target values with a weak bind-

ing nature the added value is considered insufficient to counterbalance the disadvantage of the

higher complexity of the set of PM standards, but guidance on the use of black carbon as health

indicator would be useful for local policy making.

In anticipation of possible future standards for black, elemental or organic carbon and/or UFP

we recommend requiring more extensive monitoring in order to acquire data on ambient con-

centrations and to improve monitoring practice for these PM fractions.

4.6.3.3 Withdrawing standards

With health protection being the primary criterion for its recommendations, WHO is not recom-

mending withdrawing any of the PM standards. Many stakeholders on the other hand regard the

current set of standards as very complex and difficult to understand and communicate in the

policy making process. Because the various PM standards overlap to a considerable extent, it

was appropriate to investigate the possibility of withdrawing one of more standards without los-

ing substantial health protection, possibly by strengthening other standards.

We identified several possible options for reducing the number of PM standards. For all options

the remaining set of standards need to be tightened in order to fully or approximately achieve

the same level of protection against health effects given by the existing set of PM standards. In

addition, these options are not in accordance with the WHO recommendations.

Service Request 6 – final report – Developing future objectives for heavy metals and PAHs


5 DEVELOPING FUTURE OBJECTIVES FOR HEAVY METALS AND PAHS

5.1 Key messages

Heavy metals

Reported exceedances of the existing target values are associated with a small number of

industrial sources.

There is some evidence that the existing target values are ensuring that measures are being

taken to tackle these industrial exceedances by reducing emissions.

There is limited detailed understanding available of the relationships between sources and

ambient concentrations.

There is also information missing on the assessment and concentration levels around several

sources that emit high quantities of heavy metals.

Resuspension of contaminated soil was shown to be a major source of cadmium in one

Member State. However, no information was available on the contribution of resuspension in

other areas. Contributions from resuspension could make compliance difficult in some loca-

tions even if emissions to air are largely abated.

There is very little quantitative evidence available of the impact of the abatement measures

that have been taken.

More information on measures and their impact may become available once the existing tar-

get values come into force on 31 December 2012 and mandatory reporting by MS on meas-

ures commences.

The draft answers by WHO to answers concerning current target values for heavy metals

suggest not changing the provisions for arsenic and nickel.

However, for cadmium strengthened evidence on health impacts and still too high input levels

to agricultural soils suggest adapting the target value and/or emission legislation.

Polycyclic aromatic hydrocarbons

Most of the reporting exceedances are associated with domestic heating emissions.

There is some evidence that the existing TV are ensuring that measures are being taken to

tackle industrial exceedances by reducing emissions.

There is very little quantitative evidence available of the impact of the abatement measures

that have been taken.

Especially, there is very little information available on measures taken to reduce emissions

from domestic heating, which is the predominant source of emissions in most areas. This

situation might improve in the next few years when compliance with the target value is aimed

for from 2013 onwards.

The detailed information required for assessing the effort for compliance, which is currently

not available, suggests that the current target value approach is more appropriate than bind-

ing limit values.

A reduction to a much lower value would result in very widespread exceedances across al-

most all of the EU, which would mean that it would be hard to target measures at the worst

affected areas.



It might be considered applying an exposure reduction approach to urban background con-

centrations of B(a)P in a similar way to the treatment of PM2.5 in the AQD. This might be one

way to tackle the widespread nature of exceedances of the current target value.

Mercury

Exposure to ambient air concentrations is not a significant contributor to human exposure to

mercury.

Therefore it is recommended continuing of monitoring ambient concentrations of Hg in both

urban areas and industrial hotspots and continuing abatement of emissions on international

level.

An implementation of a target value for mercury would not result in a significant reduction of

exposure to mercury.

The draft answers by WHO to questions concerning mercury indicate that there is no new

evidence that would impact on the air quality policy for mercury.

Deposition

At the present only few deposition data for heavy metals and PAH collected with the refer-

ence measurement methods is available.

Available deposition data show a wide range between deposition data at industrial sites and

background sites; so a different sampling strategy is needed for rural and industrial sites.As

there is a considerable influence in the use of different collector types to measured deposition

rates, it is recommended to gain more information on and experience with the current refer-

ence measurements methods before setting target or limit values.

This gap of knowledge could be closed by additional deposition monitoring on background

and industrial sites.

5.2 Context

Article 8 of the DD4 states that a report has to be prepared by the Commission, which should be

the basis of a possible revision of the target values for Ni, As, Cd and B(a)P as well as possible

further action for mercury. This report has to be based on the latest scientific findings and tech-

nological developments. In addition, it has to take into account:

Current air quality trends and projections;

Scope for further emission reduction; technical feasibility, cost-effectiveness and additional

health and environment protection of these reductions as well as secondary effects;

Combined strategies and relationships between pollutants;

Information of the public and reporting (covered by section 6)

Experience in the Member States;

Secondary economic benefits for the environment and health

Adequacy of current sampling and suitability of B(a)P as a marker for PAH (see chapter 3);

Merits for further action for Hg.

The focus of the analysis lies on the 27 European Member States. Where available, data for

Croatia was included.



5.3 Extent of exceedances for heavy metals

5.3.1 Current target values of the 4th Daughter Directive

The current target values for the DD4 pollutants are shown in the table below.

Table 12: Target values for arsenic, cadmium, nickel and benzo(a)pyrene (source: DD4).

Pollutant Target value* in ng/m³

Arsenic 6

Cadmium 5

Nickel 20

Benzo(a)pyrene 1

* For the total content in the PM10 fraction averaged over a calendar year

These target values should not be exceeded from 31 December 2012 onwards. Member States

shall take all necessary measures not entailing disproportionate costs to ensure compliance.

5.3.2 Extent of exceedances of arsenic

The analysis summarized in chapter 2 has shown that in 2010 exceedances of the target value

for arsenic of 6 ng/m³ occurred in five MS (Table 13). It has to be noted that no data is available

for Greece and Malta as well as for Croatia.

Table 13: Maximum level of arsenic in 2010, number of stations affected, name of cities (source: annual

questionnaire 2004/461/EC).

MS max. As level (ng/m³) # of stations name of cities, regions

BE 44.2 4 Hoboken

CZ 9.4 2 Kladno-Švermov, Stehelčeves

FI 14.3 1 Harjavalta

DE 8.6 1 Braubach

PL 9.2 2 Bydgoszcz, Nakło nad Notecią

Table 14 shows the area and population affected by exceedances of the target value for arse-

nic. Overall the area affected is 9.8 km²; 10,550 people23

are estimated to be exposed accord-

ing to questionnaire 2004/461/EC.

23

Without PL



Table 14: Area and population affected by exceedances of the target value for arsenic in 2010 (source:

annual questionnaire 2004/461/EC).

MS city area (km²) population

BE Hoboken 0.84 2650

CZ Kladno-Švermov* 3 3050

Stehelčeves* 3 3050

FI Harjavalta 1 1500

DE Braubach 2 300

PL Bydgoszcz, Nakło nad Notecią (17,971) +

(2,069,575) +

* both stations are located close to the city of Kladno

+ according to the reply to the questionnaire. Numbers provided cover whole Voivodeship; however, for several stations

levels were reported that were below the target value.

The station type is given as industrial in Germany, Finland and Belgium, in Poland and Czech

Republic as background.

Figure 5 shows a map of monitored annual mean concentrations24

of arsenic for 2010. No mod-

elled data is available for arsenic.

Figure 5: Annual mean concentration of arsenic in 2010 in ng/m³ (source: EEA 2012).

24

According to Figure 5 one Slovakian site showed an arsenic concentration above 6 ng/m³, which was not reported in

questionnaire 2004/461/EC. The site Prievidza – Malonecpalska had an arsenic level of 6.4 ng/m³. If given as an inte-

ger number this means no exceedance of the target value.



5.3.3 Extent of exceedances of cadmium


for Cd of 5 ng/m³ occurred in five MS (Table 15). It has to be noted that no data is available for

Greece and Croatia.

Table 15: Level of cadmium in 2010, number of stations affected, name of cities (source: annual

questionnaire 2004/461/EC).

MS max. Cd level (ng/m³) # of stations name of cities, regions

BE 13.8 3 Andenne, Beerse (2 stations)

BG 25.4 3 Kardjaly, Dolny Voden, Plovdiv

FI 6.6 1 Harjavalta

FR 13.0 2 Viviez*

ES 6.1 1 Córdoba

* Prefecture Aveyron in Midi Pyrénées according to the answer to the questionnaire to the French authorities.

The station type is given as industrial in Belgium, Finland, France (answer to questionnaire to

French authorities) and Spain, as background and traffic (Plovdiv) in Bulgaria.

Table 16 shows the area and population affected by exceedances of the target value for cad-

mium as given in questionnaire 2004/461/EC. Overall the area affected is about 130 km²; about

445,000 people are estimated to be exposed. For Bulgaria no information on urban background

levels is available from the cities affected by exceedances. The numbers provided for area and

population comprise the whole city. Therefore the number provided should be used with care

and can be regarded as an upper bound.

In the surroundings of the industrial facilities for which more detailed information is available, the

area affected in BE, FI and FR amounts to about 8 km² where about 3,300 people are living.



Table 16: Area and population affected by exceedances of the target value for cadmium in 2010 (source:



BE Beerse 0.084 84

Andenne 0.2 274

BG

Kardjaly 31 62,970

Dolny Voden 2 2,000

Plovdiv 102 381,109

FI Harjavalta 1 1,500

FR Viviez* >7 >1,400

ES Córdoba (141)+ (328,547)

+

* according to the answer to questionnaire the numbers provided are the lower limit.

+ whole city of Córdoba. However, an urban background station shows Cd levels well below the target value.

Figure 6 shows a map of annual mean concentrations of cadmium for 2010, based on monitor-

ing data; Figure 7 shows model results of cadmium concentrations in air in 2009. The modelled

concentrations are in most parts of Europe a factor of 10 below the target value. This indicates

that there are no exceedances of the target value for cadmium on regional scale.

Figure 6: Annual mean concentration of cadmium in 2010 in ng/m³ (source: EEA 2012).



Figure 7: Annual mean concentration of cadmium in 2009 in ng/m³ in the regional background(source:

EMEP MSC-E).

A comprehensive analysis of transboundary fluxes of cadmium, mercury and lead was recently

published by EMEP MSC-E (EMEP MSC-E 2012).

5.3.4 Extent of exceedances of nickel

The analysis done under Task 1 has shown that in 2010 exceedances of the target value for Ni

of 20 ng/m³ occurred in four MS (Table 17). It has to be noted that no data is available for

Greece and Croatia.

Table 17: Level of nickel in 2010, number of stations affected, name of cities (source: annual questionnaire

2004/461/EC).

MS max. Ni level (ng/m³) # of stations name of cities, regions

BE 28.6 2 Genk (2 stations)

DE 68.5 1 Krefeld

ES 25 1 Santa Cruz de Tenerife

FR 24.5 1 Clermont-Ferrand



Table 18 shows the area and population affected by exceedances of the target value for nickel.

Overall the area affected is about 30 km²; about 7,200 people25

are estimated to be exposed.

Table 18: Area and population affected by exceedances of the target value for nickel in 2010 (source:



BE Genk 1.16 417

FR Clermont-Ferrand 21 1,812

DE Krefeld 7 5,000

ES Santa Cruz de Tenerife (173) +

(346,879) +

+ Exceedance at one site only; further monitoring sites do not show exceedances.

The station type is given as industrial in Belgium, France and Germany, traffic in Spain.

Figure 8 shows a map of monitored annual mean concentrations of nickel for 2010. No mod-

elled data is available for nickel.

Figure 8: Annual mean concentration of nickel in 2010 in ng/m³ (source: EEA 2012).

25

The numbers given do not include the city of Santa Cruz de Tenerife in Spain. In the questionnaire 2004/461/EC the

whole city is included even though eight further monitoring sites in Santa Cruz de Tenerife show levels below the tar-

get value.



N.B.: In Northern Italy a nickel concentration of 20.5 ng/m³ is given in AirBase, which was not

reported in questionnaire 2004/461/EC as an exceedance.

5.4 Extent of exceedances of benzo(a)pyrene


for benzo(a)pyrene of 1 ng/m³ occurred in twelve MS (Table 19).

It has to be noted that no data is available for Greece, Romania and Croatia. No data about the

area and population affected is available for Austria, Finland and Poland. For the other coun-

tries the area amounts to about 35,500 km² and the population to 17.7 millions.

This number can be compared with population affected that is derived with the help of modelling

calculations by MSC-E, which provide regional background concentrations on a 50x50 km²

scale (Figure 9). These model calculations can of course provide only information on regional

scale. Especially in mountainous areas the model cannot reflect a possible high variability on a

smaller spatial scale. In addition, the uncertainties of PAH emissions have to be considered.

Nevertheless, the calculations show that even in the regional background almost 18.5 Mio peo-

ple might be exposed to levels above 1.0 ng/m³ (Table 19). The area amounts to 77,500 km².

When combining these two sources of information we come up with a very rough estimate of

population affected of about 35.5 Mio people.

The calculations of MSC-E also show that exceedances might be expected in countries for

which no data or exceedances were reported such as Latvia, Portugal26

, and Romania.

Furthermore, it has to be noted that the number of exceeded stations derived from AirBase is

higher than that provided in questionnaire 2004/461/EC. The higher number is partly due to

rounding rules applied differently in the MSs.

Monitoring station types affected are mostly (sub-)urban background (134 out of 185 stations),

16 stations are labelled industrial (mostly urban) and 35 traffic (mostly urban).

26

The high B(a)P concentrations in Portugal are due to relatively high overall emissions, wherefrom 75 % stem from the

sector ―4F Field Burning of Agricultural Waste‖ (APAMBIENTE 2012). However, these numbers are not correct (pers.

communication Teresa Costa Pereira, Agência Portuguesa do Ambiente). Therefore also the model calculations

shown are not correct for Portugal.



Table 19: Level of benzo(a)pyrene in 2010, number of stations, area and population affected (source:

annual questionnaire 2004/461/EC; EMEP MSC-E, specific questionnaire to MS).

MS max. B(a)P level (ng/m³) # of stations area (km²) population population MSC-E

AT 5.4 5 unavailable unavailable no exc.

BG 4.8 5 374 1,866,038 600

CZ 7.2 23 11,272 6,567,900 254,000

DE 8.6 7 22,810 8,495,035 no exc.

FI 1.5 1 unavailable unavailable no exc.

FR 2.6 9 14 (one station) 1,030 (one

station) no exc.

HU 3.0 11 46 49,950 2,000

IT* 2.6 9 854* 357,622* 4,175,000

LT 1.4 3 14 8,940 no exc.

LV + + + + 929,000

PL 24.6 81

Kraków: 327 Niepołomice: 27.4

Proszowice: 7.2

756,000 10,000 6,000

4,084,000

PT + + + + 4,840,000

RO + + + + 4,210,000

SI 1.1 2 36 240,000 no exc.

UK 2.0 5 40 85,976 no exc.

sum

161 35,460 17,672,491 18,494,600

* no data available for Piemonte and Lombardia

+ no exceedances reported in questionnaire 2004/461/EC

Figure 9: Modelled annual mean B(a)P concentrations in 2009 in ng/m³ (source: MSC-E,

http://www.msceast.org).

http://www.msceast.org/



Figure 10: Annual mean B(a)P levels in 2010 in ng/m³ (Source: EEA: http://www.eea.europa.eu/data-

and-maps/figures/airbase-exchange-of-information-3).

5.5 Assessment of industrial facilities and related monitoring sites

The European Pollutant Release and Transfer Register (E-PRTR) data for 2010 was used to

assess whether the existing monitoring network covers areas close to industrial facilities show-

ing high emissions of heavy metals and PAH. The analysis was done in three steps:

1. Identification of main economic activity type causing exceedances;

2. Identification of facilities with equal or higher emissions than those for which nearby monitor-

ing data is available;

3. Identification of distance to nearest monitoring site. This was done with the help of a GIS pro-

gram.

In the following the results of this analysis is shown for As, Cd, Ni and B(a)P.

It has to be noted that his analysis can only provide a first glance at areas to be looked at for

several reasons:

In the E-PRTR for some facilities several entries are provided for different aggregates or

parts of the facility. Even though we did have a look at the sum of emissions in the surround-

ing (2 km diameter) of each monitoring site, some facilities might have been overlooked.

The release height of the pollutants is not known.

Fugitive emissions are often an important source but are hardly quantified or included.

http://www.eea.europa.eu/data-and-maps/figures/airbase-exchange-of-information-3

http://www.eea.europa.eu/data-and-maps/figures/airbase-exchange-of-information-3



The coordinates given do have two digits only and are sometimes erroneous.

No analysis of the actual exposure was undertaken.

No information is readily available on whether an air quality assessment was undertaken by

the MS.

A more detailed analysis would have been beyond the scope of this study. Especially, aggregat-

ing and correcting the E-PRTR datasets require some additional effort.

According to the replies to the specific questionnaire sent to MS within Task 4 metal processing

plants are responsible for the exceedances of arsenic, nickel and cadmium, for nickel in addition

oil refineries. Therefore the analysis of E-PRTR focused on these two types of facilities.

In the case of arsenic for 12 metal processing plants emissions above 300 kg have been re-

ported27

. Only one reported exceedance of the target value for arsenic can be related to one of

these facilities. Also in the case of cadmium only one exceedance was reported nearby a facility

for which considerable emissions are reported. In the case of nickel, two facilities do cause ex-

ceedances at nearby monitoring sites out of about 30 that have been analysed.

One reason why no further emissions are monitored lies in the fact that simply no monitoring

site is situated within a reasonable distance. However, in some cases low concentration levels

are reported nearby facilities showing high emissions.

High emissions of heavy metals are reported for power plants as well. Whereas the pollutants

from metal processing facilities are released mostly at low height either via stacks or from fugi-

tive sources, power plants usually have high stacks and therefore a distinct dispersion charac-

teristics. Due to the high stacks of power plants the maximum pollutant level can be expected to

occur at a distance of some km from the facility. In few cases only a monitoring station lies

within this distance. For the majority of power plants no nearby station, which might be affected,

could be identified. It has to be noted that the E-PRTR database does not contain detailed in-

formation about the release of the pollutants such as stack height. Nevertheless, a rough esti-

mate indicates that at least for arsenic and Ni an exceedance of the target value cannot be ex-

cluded in a distance of about 5 km around the highest emitting power plants under certain con-

ditions.

Also in the case of B(a)P the analysis of the E-PRTR database reveals several facilities showing

rather high emissions but either no nearby monitoring site or no clear influence.

A detailed analysis of the reasons for the large variations in monitored concentrations on the

one hand and the extent of exceedances to be expected on the other hand, goes beyond the

scope of this study.

5.6 Sources of exceedances

The analysis undertaken in Task 1 of this project and summarized in chapter 5.3 has shown that

the extent of the exceedances and the sources for those are rather different for the heavy met-

als and benzo(a)pyren. Whereas for heavy metals in most cases the exceedances are limited to

small areas due to emissions from individual industrial facilities, for B(a)P extensive ex-

ceedances have been observed, which were caused by different sources. In some cases ex-

ceedances of limit values for two different pollutants were caused by a single source. Therefore

27

This threshold was chosen considering the extent of exceedance for arsenic in Hoboken, Belgium, and the reported

emissions.



in the following chapters the sources for heavy metals emissions are analysed collectively in

chapter 5.6.1, whereas B(a)P is analysed in chapter 5.6.2.

5.6.1 Sources causing exceedances of target values for heavy metals

Information on the sources of exceedances can partly be found in questionnaire 2004/461/EC

on an aggregated level. The information provided in this questionnaire is summarized in Table

20. In addition, MS affected by exceedances were asked for more detailed information with the

help of individual questions. The type of industrial facility is given in Table 20 as well. In most

cases non-ferrous metals or steel plants are responsible for the exceedances; in one case a re-

finery.



Table 20: Exceedances of heavy metal target values in 2010, cities, sources codes and possible sources

(source: annual questionnaire 2004/461/EC, reply to questionnaire to Member States).

MS pollutant name of cities, re-gions

source (2004/461/EC)

+

source (replies from MS)

Belgium

As Hoboken S3 non-ferrous metal plant

Cd

Andenne S3 metal plant

Ath1 chemical plant

Charleroi: Lodelinsart, Dampremy

1

two steel plants

Beerse S3 non-ferrous metal plant

Ni Genk2 S3 iron and steel

Bulgaria Cd

Kardjaly S3 no information provided

Dolny Voden S3 no information provided

Plovdiv S2, S5 no information provided

Czech Republic As Kladno-Švermov

various sources iron and steel plants, coke plants, combustion plants

Stehelčeves

Finland As, Cd Harjavalta S3 metal plant

France

Cd Viviez, Midi-Pyrenees S3 battery plant, Al and Mg

smelter

Ni Les Ancizes-Comps (Auvergne)

S3 iron and steel plant

Germany As Braubach S3 secondary lead smelter

Ni Krefeld S3 steel plant3

Poland As Bydgoszcz S5, S2

4

Nakło nad Notecią S1, S5 4

Spain Cd Córdoba S3 copper and brass plants

Ni Santa Cruz de Tenerife S3 oil refinery

+ S1: Heavily trafficked urban centre

S2: Proximity to a major road

S3: Local industry including power production source related

S5: Domestic heating

1 concentrations above the target value 1994 to 2009 in AirBase; however, these data are not correct according to the

Agence Wallonne de l’Air et du Climat. The target value was exceeded only in 2008 in Ath. Information on

sources provided in the answer to the specific questionnaire.

2 values in AirBase showing further exceedance in Genk are not correct according to the Belgian authorities

3 steel plant has been sold and will probably be closed. Therefore no further information could be provided by the

German authorities

4 according to the reply to the specific questionnaire none of these companies are responsible for the exceedances. The

main reason for the exceedances is emissions from the residential sector.

The share of different sectors to emissions of arsenic, cadmium and nickel on a national level is

shown in Figure 11, Figure 12 and Figure 13, respectively. Obviously, these numbers on a na-

tional scale can be completely different from the local scale.



For arsenic, overall industrial combustion has the highest share (56 %), followed by public

power plants (19 %) and small combustion (13 %). There is however, a considerable variation

between MS.

For cadmium, small combustion has the highest share (39 %), followed by industrial combustion

(30 %) and industrial processes (15 %). As for arsenic, the numbers vary considerably between

MS.

As for arsenic, the sector industrial combustion contributes most to nickel emissions (45 %), fol-

lowed by small combustion (24 %) and public power (18 %). Again, there are large differences

between MS.

Figure 11: Arsenic emissions in EU27 in 2010 (source: CEIP, webdab).

0%

10%

20%

30%

40%

50%

60%

70%

80%

90%

100%

BE

BG

HR

CY

CZ

DK

EE FI

FR

DE

HU IE IT LV

LT

MT

NL

PL

PT

RO

SK

SL

SE

UK

tota

l

Q_AgriWastes

N_WasteIncin

I_OffRoadMob

H_Shipping

G_RoadRail

F_Solvents

E_Fugitive

D_IndProcess

C_SmallComb

B_IndustrialComb

A_PublicPower



Figure 12: Cadmium emissions in EU27 in 2010 (source: CEIP, webdab).

Figure 13: Nickel emissions in EU27 in 2010 (source: CEIP, webdab).

Next to actual emissions there might be a substantial contribution from resuspension by con-

taminated soils, which is not included in emission inventories (EMEP-MSC-E 2012a).

To get more detailed information on specific sources causing the exceedances of target values

for heavy metals and/or B(a)P a questionnaire was sent to MS asking specific questions on de-

tails of the sources, measures to reduce emissions resulting in compliance and costs of these

measures.

The results of this specific questionnaire are summarized in chapter 5.6.3, 5.6.4 and 5.6.5 be-

low.

0%

10%

20%

30%

40%

50%

60%

70%

80%

90%

100%

AT

BE

BG

HR

CY

CZ

DK

EE FI

FR

DE

HU IE IT LV

LT

MT

NL

PL

PT

RO

SK

SL

ES

SE

UK

tota

l

T_IntAviCruise

Q_AgriWastes

N_WasteIncin

L_OtherWasteDisp

K_CivilAviCruise

J_AviLTO

I_OffRoadMob

H_Shipping

G_RoadRail

F_Solvents

E_Fugitive

D_IndProcess

C_SmallComb

B_IndustrialComb

A_PublicPower

0%

10%

20%

30%

40%

50%

60%

70%

80%

90%

100%

BE

BG

CY

CZ

DE

DK

EE

ES FI

FR

HR

HU IE IT LT

LV

MT

NL

PL

PT

RO

SE

SK

UK

tota

l

T_IntAviCruise

R_Other

Q_AgriWastes

N_WasteIncin

L_OtherWasteDisp

K_CivilAviCruise

J_AviLTO

I_OffRoadMob

H_Shipping

G_RoadRail

F_Solvents

E_Fugitive

D_IndProcess

C_SmallComb

B_IndustrialComb

A_PublicPower



5.6.2 Sources causing exceedances of the target value for B(a)P

In contrast to heavy metals the sources causing the exceedances of the target value for B(a)P

are in most cases not related to single installations. In addition, a much larger area and popula-

tion are affected by the exceedances. The information provided in questionnaire 2004/461 is

summarized in Table 21.

Table 21: Level of benzo(a)pyrene in 2010, number of stations, area and population affected (source:


MS source code description

AT S5 Domestic heating

BG S1, S2, S3, S5 Traffic, industry, domestic heating

CZ

S1, S2, S3, S4, S5, S10, S12, S15, S16, S17, S19, S21 Traffic, mining, industry, domestic heating, transboundary

DE S2, S3, S5, S10 Traffic, industry, domestic heating, transboundary

FI S3 Industry

FR S3, S5 Industry, domestic heating

HU S1, S2, S3, S5, S10, S15 Traffic, industry, domestic heating, transboundary

IT* S1, S3, S5, S7 Traffic, industry, domestic heating, accidental emissions

LT S5 Domestic heating

PL S1, S2, S3, S5, S10, PL4 Traffic, industry, domestic heating, transboundary

SI S1, S5 Traffic, domestic heating

UK S3, S5 Industry, domestic heating

* no data available for Piemonte and Lombardia

Table 21 shows that domestic heating, industry and traffic are the three source categories

named most often in the annual questionnaire 2004/461/EC.

Overall emissions of B(a)P from domestic heating are cited as a contributory factor to 120 of the

154 exceedances of the target value. Emissions of this sector are responsible for about 80 % of

emissions of B(a)P in Europe.

This is corroborated by the emission data reported by MS (Figure 14). In all countries the sector

small combustion has the largest share. Overall, small combustion is reported to contribute by

84 % to B(a)P emissions.

The share of traffic is above 10% in CZ (12 %), FR (21 %) and MT (25 %).

According to a report from concawe in 2005, PAH emission from road traffic mostly stems from

old diesel vehicles (CONCAWE 2005). Gasoline cars with three-way catalysts and diesel vehicles

equipped with after-treatment systems showed very low PAH emissions.



Figure 14: Source categories of B(a)P in 2010 as reported by MS (source: CEIP, webdab).

An analysis done in UK shows a clear correlation between overall emissions and median con-

centration despite uncertainties in both emission calculations and monitoring (Figure 15, NPL

2012a).

Figure 15: Comparison of UK B(a)P estimated emissions and UK median B(a)P measured concentrations

from 1990 to 2009 (source: NPL 2012a).

The large reduction until 1996 came from legal restrictions to agricultural waste burning and

emission reductions in aluminium production (NPL 2012a).

5.6.2.1 Exceedances of B(a)P due to domestic heating

As described above, domestic heating of solid fuel is the major source for exceedances of the

B(a)P target value in most MS.

The costs and the effectiveness of options to reduce emissions from small scale combustion

sources were studied for the CAFE programme by AEA Technology in 2004 (AEAT 2004).

0%

10%

20%

30%

40%

50%

60%

70%

80%

90%

100%

BG

HR

CY

CZ

DK

EE

FR

DE

HU IE LV

LT

LU

MT

NL

PL

RO

SK

SL

SE

UK

tota

l

Other sectors

G_RoadRail

F_Solvents

E_Fugitive

D_IndProcess

C_SmallComb

B_IndustrialComb

A_PublicPower



The study suggested several options to reduce PM emissions and analysed the cost effective-

ness of various policy options.

For the review of the AQD IIASA conducted a study on the reduction potential for households

and other small scale combustion sources (IIASA 2012).

Both studies focused on PM and did not touch on B(a)P. However, a reduction of PM emissions

also reduces B(a)P approximately to the same relative extent. Therefore the results of these

studies can be applied to B(a)P as well.

IIASA concluded that PM2.5 emissions could substantially be reduced if Eco-design28

standards

would be implemented, which are still under discussion. Of relevance in this respect are Eco-

design standards for Solid Fuel Small Combustion Installations29

(Lot 15) and Local room heat-

ing products30

(Lot 20). From 2005 to 2020 emissions would decline by 38 % (current baseline:

21 %).

Emission control costs amount to 4.9 billion €/a in 2020 in the baseline scenario and to

8.8 billion €/a in the Eco-design scenario.

Table 22 shows emissions of PM2.5 from the domestic sector in the year 2005 and for the base-

line scenario and the Eco-design scenario in 2020 for those countries that reported ex-

ceedances of the B(a)P target value in 2010 (see Table 19, chapter 5.4).

Table 22 indicates that in the exceeded areas in most countries a larger reduction of PM2.5 and

B(a)P has to be undertaken than on average national level.

For Northern Ireland a detailed study has been undertaken on sources of B(a)P exceedances,

necessary emission reductions and costs (NPL 2012a). In 2010 B(a)P levels of about 2 ng/m³

were observed; the exceedances are caused by solid fuel heating systems.

The study concluded that a complete replacement of these heating systems and an enforce-

ment of ―smokeless zones‖ would far outweigh the damage costs. However, enforcement of ex-

isting smoke control areas would cost around the same amount as the damage cost and may

deliver reduced B(a)P concentrations.

Further studies are currently not available. As for heavy metals the target values should not be

exceeded from 31 December 2012 onwards. Therefore it can be expected that further informa-

tion on exceeded areas, measures and costs of this measures will become available in near fu-

ture.

28

http://ec.europa.eu/enterprise/policies/sustainable-business/ecodesign/index_en.htm

http://ec.europa.eu/energy/efficiency/ecodesign/eco_design_en.htm

http://ec.europa.eu/energy/efficiency/studies/ecodesign_en.htm

http://www.ecodesign-info.eu/

29 Lot 15 (Solid Fuel Small Combustion Installations): http://www.ecosolidfuel.org/

30 Lot 20 (Local room heating products): http://www.ecoheater.org/lot20/

http://ec.europa.eu/enterprise/policies/sustainable-business/ecodesign/index_en.htm

http://ec.europa.eu/energy/efficiency/ecodesign/eco_design_en.htm

http://ec.europa.eu/energy/efficiency/studies/ecodesign_en.htm

http://www.ecodesign-info.eu/

http://www.ecosolidfuel.org/

http://www.ecoheater.org/lot20/



Table 22: PM2.5 emissions from the domestic sector in 2005 and 2020 in the baseline and Eco-design

scenario for MS that reported exceedance of the B(a) target value in 2010 (source: IIASA 2012;

AirBase, questionnaire 2004/461/EC).

PM2.5 emissions in kt B(a)P concentration

2005 2020 2010

baseline Eco-Design max. B(a)P level ng/m³

Austria 8.2 5.3 3.1 5.4

Bulgaria 14.1 11.6 8.8 4.8

Czech Rep. 15.7 14.8 11 7.2

Finland* 9.1 8.6 6.6 1.5

France 144.6 87.8 62 2.6

Germany 23.2 23.7 19.2 8.6

Hungary 10.3 11.2 9.5 3.0

Italy 29.8 28.4 23.8 2.6

Latvia 14.2 11.4 8.8 1.1

Lithuania 6.3 4.7 3.6 1.4

Poland 171.5 147.8 125.5 24.6

Slovenia 3 2.9 2.1 1.1

UK 8.7 7.6 6.6 2.0

* exceedance caused solely by industrial facilities according to questionnaire 2004/461/EC

5.6.2.2 Exceedances of B(a)P target value due to industrial sources

The Member States that have named industry to be (partly) responsible for the exceedance of

the B(a)P target value were asked for specific facilities, aggregates and costs of emission re-

ductions. According to their replies, coke ovens, sintering plants and carbon cathodes plants are

the main industrial sources of B(a)P.

5.6.3 Necessary emission reductions

Different installations are responsible for the exceedances of heavy metals and/or B(a)P in the

different member states. MS sometimes only reported emission loads (kg emission parame-

ter / year) without further information (total capacity, ...) in the reply to the specific questionnaire.

In this case a comparison with Best Available Techniques Associated Emission Levels (BAT-

AEL) was not possible. For some facilities adaption of the Emission Limit Value (ELV) will be

necessary to be in line with the BAT Conclusions (e.g. BAT Conclusions on Iron and Steel). In

other cases BAT-AELs are reached and there is still an exceedance of the relevant target val-

ues.

In these cases companies together with competent authorities are elaborating programmes or

action plans to further reduce the emissions.

Stack emissions are reduced to a great extent and often reach the BAT-AELs. Diffuse emis-

sions contribute to a rather high amount to the overall emissions. They have to be further re-

duced.



In some cases parts of plants have been closed or will be closed in the near future; therefore lo-

cal authorities assume to reach compliance with the target values.

5.6.4 Technical feasibility of emission reductions

The specific questionnaires and further information sent from the member states provide hardly

any data on measures and costs that would result in compliance with the target values.

In general the installation of filters (fabric filters; Electrostatic precipitator, ESP) is applicable to

new and existing plants. The combination of emission reduction techniques depend on the flue

gas characteristics. Measures to reduce diffuse emissions will vary from site to site, but are ap-

plicable to all installations. Building ventilation can be installed; house in house concepts for the

reduction of diffuse emissions are available.

5.6.5 Cost of emission reduction

From a lead company estimated costs for a new filter system are € 1,000,000 for each installa-

tion, which amounts to € 3,000,000 for the three furnaces (reply to specific questionnaire).

Another plant gives information on costs for the reduction of one third of its emission of 12 Mil €.

(reply to specific questionnaire).

The relevant BREFs, in especially the BREF Iron and Steel give some data on costs:

Investment for revamping two existing ESPs to last generation electrostatic precipitators was

estimated in 2002 at € 10 – 15 million for a sinter plant with a 1.4 million Nm³/h gas flow (ex-

ample plants: ArcelorMittal, Fos sur Mer, France).

When estimating the costs of bag filter with a flow-injection unit, it should be borne in mind

that these installations are not only used for dust separation but also for reducing PCDD/F,

heavy metals and acid gases such as HF, HCl and SO2. The investment is in the range of

€ 16 to 35/Nm³/h (for new and existing plants). Decisive cost factors are pressure drop, the

waste gas flow, fabric material and filter loading. The operating cost is around € 0.3 –

0.6/t sinter and mostly depends on the costs of supplying activated carbon and limestone,

and the extra energy.

It can be calculated that a dry ESP for treatment of a waste gas flow of 300,000 Nm³/h will

require an investment of approximately € 2 million (1996 prices) for a pelletisation plant with

an annual production of 4 Mt and a drying mill waste gas flow of 300,000 Nm³/h (EUROPEAN

COMMISSION 2012).

A variety of measures exist to reduce diffuse emissions, general costs are depending of the kind

of measure or combination of measure (all cost data from BREF Iron and Steel 2012, EUROPEAN

COMMISSION 2012).

5.7 Impact on health and environment of changes to current standards of As, Cd, Ni and B(a)P

For the review of the AQD and DD4, WHO is currently conducting the REVIHAAP project (WHO

2012a). This project inter alia has the objective to provide the Commission and the stakeholders

with an evidence-based response to specific questions regarding health aspects of amongst

others PM, As, Cd, Hg, Ni and PAH. For these heavy metals and PAH the main question is,



whether there is any new evidence on the health effects, that would impact upon current target

values.

Draft results of the REVIHAAP project were published in October 2012 (WHO 2012a). Concern-

ing arsenic WHO concluded that there is some new evidence on the cancer risk of arsenic;

however, this is insufficient to impact upon the current EU target value.

Also for cadmium there is new and strengthened evidence on health effects. There is strong

evidence that even low level Cd exposure decreases bone mineral density and increases the

risk of skeletal fractures. Cd input to agricultural soil is still larger than the output; typically half of

the Cd in agricultural soil originates from air. Present levels in air still lead to an increase in soil

levels. WHO concludes that this should be taken into account in the review of the DD4.

The studies published on occupational epidemiology for nickel in recent year do not change the

unit risk estimate substantially. Therefore it is concluded that there is no significant impact on

the present target value. Evidence on the effect of nickel on cardiovascular risk is still too lim-

ited.

The analysis of the exceedances of the target values for arsenic, cadmium and nickel has

shown that these are confined to rather limited areas and affecting a limited number of people.

The reasons for these exceedances are specific industrial installations, mostly metal processing

plants, in one case an oil refinery. There is however some uncertainty whether the current moni-

toring network for heavy metals covers all areas at risk. There are a number of sources showing

high emissions but no nearby monitoring of concentration levels. A more detailed analysis would

be beyond the scope of this study.

The information provided by MS as a reply to specific requests did not allow identifying in most

cases the costs and the additional benefit of measures with which compliance could be

achieved. However, even in those cases were detailed analysis were undertaken by MS, some

ambiguities and uncertainties remain about the actual sources and possible measures. This is

due to the complex configuration of the facilities concerned, the large number of emission

sources and complexity of these sources, which might be a stack, fugitive or diffuse.

It was noted by MSs that measures have been implemented and further measures will be im-

plemented irrespective of whether the target values will be converted to limit values. Therefore

no additional benefit would arise in these cases.

A lower numerical threshold for arsenic and nickel equivalent to the lower end of the proposed

levels in the Position Paper (the threshold for cadmium is already equal to the lower end), would

increase the number of MS, zones and cities affected to some extent.

Currently, the concentration levels of heavy metals are determined as a fraction of PM10. A

change of metric to PM2.5 would affect the assessment of nickel concentrations to some extent,

as nickel has a relative high share in the coarse fraction.

Concerning PAH the draft REVIHAAP results concluded that there is some new evidence to link

PAH exposure to cardiovascular endpoints. However these effects cannot be separated from

that of particles. Therefore these findings cannot impact on the current target value. Neverthe-

less, WHO once again noted that the existing target value is associated with a lifetime cancer

risk of approximately 1 x 10-4

. In addition, a recent analysis concluded that B(a)P is a suitable

marker for PAH mixtures (DELGADO-SABORIT et al. 2011).

Contrary to heavy metals exceedances of the B(a)P target value are widespread in some coun-

tries. In addition in most cases no specific industrial installation is responsible for the ex-

ceedance but domestic heating resulting in emissions of many different small sources.



Similar however to heavy metals, in those cases where industrial facilities contribute to the ex-

ceedance or are responsible for it, the information on sources, measures and costs is rather

sparse.

A lowering of the threshold for B(a)P would have a large impact on the extent of exceedances.

A threshold according to the recommendations by WHO of 0.1 ng/m³ would result in ex-

ceedances in about 90 % of the air quality zones according to the current monitoring network.

The current gaps in knowledge to assess the exceedances on an European level for both heavy

metals and B(a)P can be summarised as following:

Assessment of concentration levels to cover relevant sources;

Assessment of population and area affected;

Sources of emissions;

Measures to achieve compliance;

Cost of these measures.

5.8 Thresholds for Hg

5.8.1 Introduction

The goal of this chapter is to analyse information of the Community Mercury Strategy31

, the

UNEP Global Atmospheric Mercury Assessment32

, the LRTAP framework33

and further source

in order to present pros and cons of different concepts to reduce mercury emissions and expo-

sure (EUROPEAN COMMISSION 2005, AMAP/UNEP 2008, UNEP 2008, 2008a, 2009, 2010,

COM(2005) 20 final, COM(2010) 723 final, BIO INTELLIGENCE SERVICE 2010)..

Mercury exists in different forms: most mercury is emitted to the atmosphere as gaseous ele-

mental mercury (GEM, sometimes name total gaseous mercury, TGM) and minor amounts of

reactive (or oxidized) gaseous mercury (RGM) or as particulate oxidized mercury (TPM, total

particulate mercury, AMAP-UNEP 2008). Whereas GEM has a rather long lifetime around one

year, RGM and TPM are much more short-lived with lifetimes in the order of hours to days.

Therefore RGM and TPM are more of regional concern, whereas GEM is a global issue.

Figure 16 gives an overview of mercury sources and pathways, wherefrom especially primary

and secondary anthropogenic sources are of interest, but also remobilisation and re-emissions

might be considered.

31

http://ec.europa.eu/environment/chemicals/mercury/index.htm

32 http://www.unep.org/hazardoussubstances/Mercury/GlobalMercuryPartnership/tabid/1253/Default.aspx

33 http://live.unece.org/env/lrtap/welcome.html

http://ec.europa.eu/environment/chemicals/mercury/index.htm

http://www.unep.org/hazardoussubstances/Mercury/GlobalMercuryPartnership/tabid/1253/Default.aspx

http://live.unece.org/env/lrtap/welcome.html



Figure 16: Pathways of mercury emissions (source: UNEP 2008).

5.8.2 Emissions, concentrations and deposition of Hg

5.8.2.1 Concentration levels of Hg

Monitoring of mercury is comparable scarce in Europe; in 2010 a total of about 40 measurement

stations in 11 Member States were reported in questionnaire 2004/461/EC, a large proportion of

these are from the United Kingdom that operates two metals monitoring networks.

Figure 17 shows concentration levels of Total Gaseous Mercury (TGM) in ambient air for the

year 2010. A large proportion is below 3 ng/m³, with only two higher measurements of 6.5 ng/m³

for an industrial station in Belgium, 18 ng/m³ at one station in the United Kingdom.



Figure 17: Summary of ambient concentrations of Hg at all monitoring station types for each Member State

for which data is available for 2010 (source: AirBase).

Figure 18 shows modelled concentrations of Hg. The highest concentrations can be found in the

Po valley, in Eastern Europe and around point sources. The concentration range is rather nar-

row; over large areas in Europe the levels vary only between 1.4 and 1.8 ng/m³. This range of

concentrations has been found in the UNEP assessment as well (AMAP/UNEP 2008).

Figure 18: Modelled annual mean Hg concentrations in 2009 in ng/m³ (source: MSC-E,

http://www.msceast.org).

0

2

4

6

8

10

12

14

16

18

20

Be

lgiu

m

Fin

lan

d

Fran

ce

Ire

lan

d

Lith

uan

ia

Mal

ta

Po

lan

d

Spai

n

Swe

de

n

Un

ite

d

Kin

gdo

m

Hg

in n

g/m

³

http://www.msceast.org/



5.8.2.2 Emissions of Hg

The Hg emissions34

in EU27 and Croatia decreased between 1990 and 1999 by about 40 %

and by additional 25 % between 2000 and 2010 (Figure 19).

It has to be noted that assessment of reported data indicate relative high uncertainty of emission

estimates in a number of countries and reporting of Hg emissions might be not complete (EMEP

Msc-E 2012).

The highest national total emissions in 2010 are reported by Poland (18 % of overall emissions),

followed by Italy and Germany (both 11 %).

Figure 19: Hg emissions reported to EMEP in EU27 and Croatia 2000 to 2010 in Mg (source: CEIP).

In Europe the most important sources for Hg emission are power plants (34 %), industrial instal-

lations (41 %) and small scale combustion sources (10 %). Significant Hg emissions are also

reported for waste incineration and shipping, see Figure 20.

34

For Greece, Luxembourg and Romania (2000-2004) emissions are shown as used in EMEP models.

0

20

40

60

80

100

120

140

2000 2001 2002 2003 2004 2005 2006 2007 2008 2009 2010

Hg

em

issi

on

s in

Mg

Hg emissions SK SI

SE RO

PT PL

NL MT

LV LU

LT IT

IE HU

HR GR

GB FR

FI ES

EE DK

DE CZ

CY BG

BE AT



Figure 20: Relevant source categories for Hg emissions in 2010 (source: CEIP).

5.8.2.3 Deposition of Hg

Figure 21 shows the spatial distribution of Hg deposition. High levels are found in Poland,

Greece, Bulgaria, BeNeLux, Germany and UK. The highest ones were calculated for Greece,

followed by Poland, Czech Republic, Slovakia and Luxembourg.

Figure 21: Spatial distribution of Hg deposition in 2009, g/km²/y (source: EMEP MSC-E).

A detailed analysis of mercury level in fish was done in Finland, Norway and Sweden (IVL 2007,

NIVA 2009). It showed that in northern Europe the mercury concentrations in pike exceed the

recommended limit for human consumption of 0.3-1.0 mg/kg (Figure 22). On average the mer-

cury concentrations were 0.73 mg/kg. The environmental quality standard of 0.02 mg/kg of the

Water Framework Directive is exceeded throughout these countries.

public electricity; 34%

industrial combustion;

21%small

combustion; 10%

industrial processes; 20%

shipping; 4%

waste incineration; 4%

remaining sectors; 6%



Figure 22: Map of northern Europe showing site-specific arithmetic means of observed mercury

concentrations in mg/kg in pike collected in 1965 to 2004 in 2517 lakes and rivers. The dot

size indicated the number of pikes analysed (source: IVL 2007).

5.8.3 Action to reduce Hg emissions

5.8.3.1 European Union

In 2005 the European Union launched the Mercury strategy35

, a comprehensive plan to reduce

mercury pollution within the EU and addressing global challenges as well (EUROPEAN

COMMISSION 2005). 20 specific actions have been decided in order to reach the following objec-

tives:

i. reducing mercury emissions,

ii. reducing the entry into circulation of mercury in society by cutting supply and demand,

iii. resolving the long-term fate of mercury surpluses and societal reservoirs (in products still in

use or in storage),

iv. protecting against mercury exposure,

v. improving understanding of the mercury problem and its solutions and

vi. supporting and promoting international action on mercury.

In 2010 the Commission has reviewed the Mercury strategy by assigning a study on implemen-

tation of the strategy and a stakeholder consultation process. Besides the assessment of im-

35

http://ec.europa.eu/environment/chemicals/mercury/

http://ec.europa.eu/environment/chemicals/mercury/



plementation of the strategy, possible additional actions and further assessment of selected ac-

tions including their environmental, economic and social impacts and administrative costs were

compiled and discussed. Within the annexes a compilation of EU legislation concerning mer-

cury, key policies and best practice on European and global level, additional data on mercury

emissions, mercury in energy-saving light bulbs and a screening assessment of possible addi-

tional policy actions were given. The review report, composed by Bio Intelligence Service SAS

summarizes the progress of the strategy as follows (Table 23, BIO INTELLIGENCE SERVICE 2010).

Table 23: Assessment of the strategy implementation (source: DG ENV, BIO INTELLIGENCE SERVICE 2010).

A new Communication on the review of the Community Strategy Concerning Mercury was

adopted by the Commission on 7 December 2010. Finally the European Council concluded on

the Review of the Community Strategy concerning Mercury in March 2011 (COUNCIL OF THE

EUROPEAN UNION 2011), reaffirming the overall goal to protect human health and the environ-

ment, highlighting the efforts undertaken so far and reiterating the need for further European

and global action.

On behalf of the European Commission a study on the potential to reduce mercury pollution

from dental amalgam and batteries has been conducted describing environmental, economic

and social impacts of different options (BIO INTELLIGENCE SERVICE 2012). Dental amalgam has

been the second largest mercury use in the EU in 2007, contributing 23- 25% to overall EU

mercury emissions to air and 9-13% of overall EU emissions to water and will be the largest use

after phasing out chlor–alkali plants in 2020. It has been concluded that improving enforcement



of EU waste legislation regarding dental amalgam and banning of amalgam in dentistry would

achieve the highest effectiveness with reasonable costs for stakeholders. In the case of batter-

ies a ban of the placing on the market of mercury containing button cells has been suggested as

best option reducing mercury, which could also have global impact. The European Commission

has now asked the Scientific Committee on Emerging and Newly Identified Health Risks

(SCENIHR) and on health aspects of the use of dental amalgam, expecting results in February

2013. It should be clarified if there is any new scientific evidence that justifies reason for con-

cern from the health point of view, also taking into considerations alternative materials and their

potential risks (SCENIHR 2012).

Currently, IIASA is implementing mercury and its abatement options into the GAINS model

(pers. communication Markus Amann). Indicative results point to large co-benefits with climate

change abatement measures.

5.8.3.2 UNECE

The Executive Body of the United Nations Economic Commission of Europe (UNECE) imple-

mented the Aarhus Protocol on Heavy Metals in 1998, which targets three particularly harmful

metals: cadmium, lead and mercury. Parties will have to reduce their emissions for these three

metals below their levels in 1990 (or an alternative year between 1985 and 1995) specified by a

party upon ratification, acceptance, approval or accession. The Protocol aims to cut emissions

from industrial sources (iron and steel industry, non-ferrous metal industry), combustion proc-

esses (power generation, road transport) and waste incineration. It lays down stringent limit val-

ues for emissions from stationary sources and suggests best available techniques (BAT) for

these sources, such as special filters or scrubbers for combustion sources or mercury-free

processes. It also introduces measures to lower heavy metal emissions from other products,

such as mercury in batteries, and proposes the introduction of management measures for other

mercury-containing products, such as electrical components (thermostats, switches), measuring

devices (thermometers, manometers, barometers), fluorescent lamps, dental amalgam, pesti-

cides and paint.

The Heavy Metals Protocols is currently under revision (UNECE 2011, 2011a). The UNECE aims

for an adoption of the revised protocol in December 2012. The largest impact of the protocol

and the revised protocol will be in countries outside the EU. For the EU the impact will be mostly

due to a reduction of transboundary contributions. The emissions of heavy metals in EU27 will

not be affected to a large extent due to the regulations and strategies already in place. How-

ever, there might be some influence also in EU27 due to proposed product regulations for use

of mercury (WGSR 2012). As the negotiations are ongoing the actual impact cannot be foreseen.

5.8.3.3 United States

The US-EPA provides comprehensive information on mercury regulation, pollution and personal

protection on its website36

. Under certain Federal environmental statutes, such as the Clean Air

Act, Clean Water Act, and Resource Conservation and Recovery Act, regulations to control

some mercury emissions to air, water, or from wastes and products have been developed by

US-EPA37

. In addition, states also remit regulations to address mercury emissions. The federal

‗‗Mercury Export Ban Act of 2008‘‘ includes provisions on mercury exports and on long-term

mercury management and storage. Because the United States is ranked as one of the world's

36

http://www.epa.gov/hg/index.html

37 http://www.epa.gov/hg/regs.htm#other

http://www.epa.gov/hg/index.html

http://www.epa.gov/hg/regs.htm#other



top exporters of mercury, implementation of the act will remove a significant amount of mercury

from the global market. However, the mercury export ban covers only elemental mercury. EPA

has published a report on congress concerning potential export of mercury compounds to fulfil

one requirement of the Mercury Export Ban Act (EPA 2009). A study on the impact of the long-

term storage program on mercury recycling and a report on global supply and trade of elemental

mercury (to be submitted by EPA no later than January 1, 2017) are actions, among others,

foreseen to implement the mercury export ban act. The Mercury-Containing and Rechargeable

Battery Management Act of 1996 (Battery Act) requires the phase-out of the use of mercury in

batteries and the efficient and cost-effective disposal of used nickel cadmium (Ni-Cd) batteries,

used small sealed lead-acid (SSLA) batteries, and certain other regulated batteries. The newly

enforced Toxic Substances Control Act requires persons who intend to manufacture, import or

process elemental mercury for an activity that is designated as a significant new use by the rule

to notify EPA at least 90 days before commencing that activity. The required notification will

provide EPA with the opportunity to evaluate the intended use and, if necessary, to prohibit or

limit that activity before it occurs (EPA 2012a). EPA also recently incorporated revised American

Society for Testing and Materials (ASTM) standards that provide flexibility in using alternatives

to mercury-containing industrial thermometers (EPA 2012b).

5.8.3.4 UNEP

United Nations Environment Programme (UNEP) stated the need for a global assessment of

mercury in 2001, published the UNEPs Global Mercury Assessment (UNEP 2002) and started

the Mercury Programme in 2003. In 2005 UNEP Mercury Partnerships between governments

and stakeholder were established, identifying 5 partnership areas and published the report on

dynamics of mercury pollution on regional and global scales (UNEP 2005). In 2007 UNEP devel-

oped a two track approach based on voluntary actions and legally binding instruments and also

an overarching framework for strengthening the UNEP Global Mercury Programme partner-

ships. Further reports were published by UNEP and partners in 2008 (Mercury Fate and Trans-

port in the Global Atmosphere: Emissions, Measurements and Models‖ and ―The Global Atmos-

pheric Mercury Assessment: Sources, Emissions and Transport―; UNEP 2008, 2009; AMAP/UNEP

2008). AMAP - the Arctic Monitoring Assessment Programme contributed considerably to the

global mercury assessment; data sets on mercury pollution are available since 200538

.

UNEP will also support the negotiations of an internationally legal instrument for control of mer-

cury, which development has been agreed on in February 2009. All documents and reports are

available at the UNEP mercury website39

.

In the fourth session of the Intergovernmental Negotiating Committee (INC) in Uruguay, from

June 27th to July 2

nd 2012 a revised draft text for a comprehensive and suitable approach to a

global legally binding instrument on mercury has been agreed40

.

UNEP will compile a report for the governmental council in 2013.

The World Health Organization (WHO) and Health-Care-Without-Harm (HCWH) are contributing

to the UNEP Global Mercury Partnership through the Global Mercury Free Health Care Initia-

tive41

. Notes on selecting mercury reduction activities were released by UNEP in the frame of

38

http://amap.no/Resources/HgEmissions/

39http://www.unep.org/hazardoussubstances/mercury/tabid/434/default.aspx

40 http://www.unep.org/hazardoussubstances/Portals/9/Mercury/Documents/INC4/4_3_text.pdf

41 http://www.mercuryfreehealthcare.org/

http://amap.no/Resources/HgEmissions/

http://www.unep.org/hazardoussubstances/mercury/tabid/434/default.aspx

http://www.unep.org/hazardoussubstances/Portals/9/Mercury/Documents/INC4/4_3_text.pdf

http://www.mercuryfreehealthcare.org/



the Global Healthcare Waste project. Within this project overall environmental impact, cost ef-

fectiveness and ease of implementation beside other parameters for different replacement

measures have been calculated. The results of the analysis imply that replacement of esophag-

eal dilators and fluorescent lamps are effective measures to reduce mercury, costs and in the

case of fluorescent lamps also energy (UNEP 2009). The WHO also published a report on dental

amalgam, suggesting phasing down due to environmental concerns on one hand and not phas-

ing out due to various practical reasons on the other hand (WHO 2010).

5.8.4 Possible thresholds for Hg

5.8.4.1 Approaches for thresholds

Different approaches to derive thresholds for atmospheric Hg have been examined in detail (see

below). Note that there are other approaches appropriate for monitoring environmental Hg pollu-

tion, which however fall outside the scope of DD4. Such approaches include, e.g., the monitor-

ing of environmental media other than air (e.g. water for dental amalgam residues) or pertain to

other legistic instruments (e.g. emission monitoring).

For easier appraisal, the approaches have been grouped by spatial scope:

A. approaches which monitor close to sources, with thresholds set to identify objects and/or epi-

sodes of excessive Hg releases

B. approaches which monitor normal (in the statistical sense; comparable attributes are ―refer-

ence‖ or ―background‖) atmospheric Hg levels as an indicator for the efficiency of interna-

tional abatement measures, with thresholds set to achieve environmental targets

Within the spatial categories A and B, approaches have further been distinguished by monitor-

ing technique, following DD4 which suggests the following methods:

1. air sampling

2. deposition sampling

3. bioindication

Examples of the above categorisation are:

air sampler operating close to a coal-fired power station A.1

Hg-data from the European moss monitoring network B.3

urban blood samples A.3

The above grouping already suggests that the suitability of a given threshold mainly depends on

its intended geographic extent. Table 24 lists the spatial, temporal and some other

characteristics for quick reference.



Table 24: Characterization of monitoring approaches.

A B

polluter defined local source(s) collective of long-distance source type(s) in-cluding non-anthropogenic sources

spatial scope local, regional national, international

monitoring rationale

tactical: identification / monitoring of sources

strategic: trend monitoring

efficacy short-term, local, executive long-term, international/global, legislative

monitoring frequency

daily–monthly monthly–yearly

character of threshold

limit limit or target

derivation of threshold

statistical (e.g. ―normal‖ or ―reference‖ value) or – characteristic for biomonitoring – risk based (environmental quality standards, human exposure…)

1 2 3 1 2 3

compartment air depo bioind. air depo bioind.

examples of existing in-frastructure

EMEPd)

, national pro-grammes

national surveys

CAMNete)

, EMEP

d)

AMAPf),

EMEPd)

ICP For-ests

g), ICP

Vegetationh)

, COPHES

i)

(human bio-mon.)

link between threshold and human health

+

a)

++

b)

+++

c)

+

a)

++

b)

+++

c)

monitoring expenses (equipment, maintenance, analyses…)

+++ ++ + +++ ++ +

Note: ranks (indicated with +, ++, +++) are a rough estimate only and vary considerably with monitoring design

a) Gaseous Hg in ambient air is assumed to contribute only negligibly to total human Hg exposure. Although gaseous

Hg actually dominates total exposure (followed by dietary exposure) in these estimates, this quantity evaporates

from dental fillings (see Table 25)

b) Deposition is a more direct measure of the load entering the ecosystem and food web from polluted air. This load

contributes more to total human exposure from the surroundings (see dietary vs. respiratory exposure above).

c) Biomonitoring, particularly human biomonitoring, is a close indicator of human Hg exposure.

d) Co-operative Programme for Monitoring and Evaluation of the Long-range Transmission of Air Pollutants in Europe,

http://www.nilu.no/projects/ccc/network/index.html

e) Canadian Atmospheric Mercury Measurement Network

(http://www.ec.gc.ca/natchem/default.asp?lang=en&n=4285446C-1)

f) Arctic Monitoring and Assessment Programme, http://www.amap.no/

g) International Cooperative Programme on Assessment and Monitoring of Air Pollution Effects on Forests, http://icp-

forests.net/

h) International Cooperative Programme on Effects of Air Pollution on Natural Vegetation and Crops,

http://icpvegetation.ceh.ac.uk/

i) Consortium to Perform Human Biomonitoring on a European Scale, http://www.eu-hbm.info/cophes

http://www.nilu.no/projects/ccc/network/index.html

http://www.ec.gc.ca/natchem/default.asp?lang=en&n=4285446C-1

http://www.amap.no/

http://icp-forests.net/

http://icp-forests.net/

http://icpvegetation.ceh.ac.uk/

http://www.eu-hbm.info/cophes



5.8.4.2 Considerations for selection of threshold(s)

The selection of environmental Hg thresholds should consider the following:

For the protection of human health (apart from occupational exposure), Hg deposition or

(human) biomonitoring are more significant than atmospheric concentration because

respiratory exposure from surrounding air contributes little to total human exposure compared

to dietary exposure (Table 25). Dietary exposure, in turn, is directly affected by the deposition

of airborne Hg to the terrestric and aquatic food web. Also the much larger intake by dental

amalgam compared to airborne Hg has to be considered.

Despite the above, more regulatory values exist for atmospheric Hg concentrations than for

Hg levels in deposition or biota.

Deposition sampling and (human) biomonitoring put lesser demands on infrastructure than

active air sampling.

Biomonitoring, and especially human biomonitoring, give the most immediate indication of

dietary and/or total exposure and, thus, risk (for the deduction of risk-based thresholds).

Deposition measurements have the advantage of being highly standardisable, but

measurements of dry deposition still suffer from considerable uncertainty (see Table 27).

To cap local atmospheric releases, emission limits allow closer control than stationary air

quality measurements (for ambient atmospheric concentrations, deposition etc.), especially

so because atmospheric dispersion may vary considerably with weather conditions.

Existing regulatory thresholds for workplace safety, environmental impact assessments and

WHO guidelines exceed ambient atmospheric Hg concentrations (background as well as

urban/industrial) by orders of magnitude (see Table 26).

Draft results of the WHO REVIHAAP concludes that there is no new evidence that should

influence current air quality policy of mercury (WHO 2012a).

Table 25: Estimated average daily intake (retention is shown in parentheses) of total mercury (ng/day) in

the general population not occupationally exposed to mercury (source: WHO 2007).



Table 26: Existing thresholds for, and characteristic ambient concentrations of atmospheric mercury

(examples).

medium / protection target remarks source

regulatory concentra-tions: ng/m³

environmental as-sessment of industry 250 annual average; Environmental Assessment Level

Environment Agency of England and Wales

outdoor air quality 1000 annual average WHO (2000)

workplace safety

10000 for mercury aryl cmpds., 8 hour weighted average ENVIRONMENT AUSTRALIA

(2011)1

100000 for mercury aryl and inorganic cmpds., 8 hour weighted average

100000 acceptable ceiling conc. US-OSHA (2006)

environmental concentrations

EU background and urban/industrial 1.35–3.57 range of medians from various studies since 1995

compiled in European Communities (2001)

background worldwide 1.5 various authors compiled in European Communities (2001)

EU industrial 0.5–20 LAHMANN ET AL. 1986

EU urban 0.1–5

LAHMANN ET AL. 1986

EU remote areas 0.001–6

LAHMANN ET AL. 1986

background levels < 2.5

background atmospheric Hg levels, i.e. those gov-erned by long-range transport rather than local or regional emissions remain below 2.5 ng/m³ UNEP (2008)

background, industrial and traffic monitoring < 3

(< 3 ng/m³) annual average for 45 out of 47 Euro-pean stations

2010 annual question-naire according to Deci-sion 2004/461/EC

deposition levels: g/m²/a

36.5 German guidance value (1 µg/km²/d) TA-LUFT 2002

7–20 across most EMEP countries; in regions with sig-nific. emissions: > 20 g / km2 /a (status 2008) EMEP MSC-E (2010a)

1) http://www.environment.gov.au/atmosphere/airquality/publications/sok/mercury.html

5.8.4.3 Gaps in knowledge

Table 27 lists the main gaps in knowledge that have to be taken into account when setting

thresholds for the concentration and/or deposition of Hg.

http://www.environment.gov.au/atmosphere/airquality/publications/sok/mercury.html



Table 27: Gaps in current knowledge to set thresholds.

item source

general Well designed experiments and carefully controlled and performed field campaigns must be undertaken to provide understanding that will allow fluxes to be estimated with far greater certainty than they are at present.

UNECE (2010)

deposition Improved data to determine deposition velocities for GEM, RGM, and TPM to vegetation and other surfaces. Improved information on heterogeneous chemistry, including surface oxidation of GEM, and surface reduction of RGM and TPM.

AMAP/UNEP (2008)

deposition measurements

In terms of estimating deposition, it is the dry deposition flux of gaseous oxidized Hg that is mostly poorly constrained. Methods and measurements are needed to advance understanding and improve estimation. However, as wet deposition measurements are regionally focused in the developed world, more measurement and better estimation of deposition fluxes are needed globally.

UNECE (2010)

deposition Campaigns evaluating deposition should also include emission measurements to allow for an estimation of the magnitude and direction of the net flux.

UNECE (2010)

Technical aspects of deposition measurements

There is yet a lack of sufficient experience with the reference measurement method (EN 15853:2010).

see chapter 5.9

Technical aspects of concentration measurements

There is yet a lack of sufficient experience with the reference measurement method (EN 15852:2010), especially the uncertainty in the calibration of the automatic instruments.

see specific report for Task 2, Subtask 2d (RICARDO - AEA, UMWELTBUNDESAMT & TNO 2012)

5.9 Deposition of Heavy Metals and PAHs

For assessing possible regulations for the deposition of As, Cd, Hg, Ni and PAHs the following

topics were analysed:

Measurement methods and quality of datasets, see chapter 5.9.1.

Analysis of possible regulations based on available datasets and deposition levels as well as

strength and weaknesses of different schemes (chapter 5.9.2).

5.9.1 Quality of data

5.9.1.1 Current reference methods

According to Annex V of DD4 the reference method for the sampling of the deposition shall be

based on the exposition of cylindrical deposit gauges with standardised dimensions. The use of

wet-only collectors instead of bulk sampling is permitted if the Member States show that the re-

sults using these samplers do not differ more than 10 % from bulk deposition sampling. The

DD4 recommends a sampling period of weeks or months throughout the year for the measure-



ment of deposition (Annex IV). The combined uncertainty (expressed at a 95 % confidence

level) of the measurement of total deposition rates may be up to 70 %. The uncertainty of depo-

sition measurements depends on the sampling method, on the methods of analysis, on the

deposition load and on different meteorological conditions (GLADTKE et al. 2012).

The reference methods for the sampling and analysis of the deposition of arsenic, cadmium,

mercury, nickel and polycyclic aromatic hydrocarbons are standardised by the European Com-

mittee for Standardization (Comité Européen de Normalisation, CEN) in three standard meth-

ods. Only in the absence of a CEN method, the DD4 allows the use of a national standard

method. With the 2011 standard published for PAH deposition standard methods are now avail-

able for all pollutants regulated in the DD4:

EN 15841:2009 ―Ambient air quality – Standard method for determination of arsenic,

cadmium, lead and nickel in atomospheric deposition‖

EN 15853:2010 ―Ambient air quality – Standard method for the determination of mercury

depositon‖

EN 15980:2011 ―Air quality – Determination of the deposition of benz[a]anthracene,

benzo[b]fluoranthene, benzo[j]fluoranthene, benzo[k]fluoranthene, benzo(a)pyrene,

dibenz[a,h]anthracene and indeno[1,2,3-cd]pyrene‖

EN 15841:2009 specifies three methods for the determination of deposition of arsenic (As),

cadmium (Cd), nickel (Ni) and lead (Pb) that can be used in the framework of the AQD and the

DD4.

5.9.1.2 Weaknesses and strengths of reference methods for the deposition of heavy

metals

The CEN TC 264 working group 20, ―Standard method for the determination of Pb, Cd, As and

Ni in depositions‖ conducted laboratory and field tests to create a standard method for the

measurement of the deposition of As, Cd, Ni and Pb (EN 15841:2009). The field tests were car-

ried out on four different European sites (two rural, one urban and on industrial). The working

group compared three different collectors (wet-only, bulk and Bergerhoff type of gauge) and two

analytical methods (GF-AAS and ICP-MS). Sampling with various types of collectors and sam-

ple preparation (e.g. filtration) were proved to be the main factors in the uncertainty budget of

deposition measurements. The main conclusion was that a different sampling strategy is

needed for rural and industrial sites (AAS et al. 2012).

At industrial or high-polluted sites it is necessary to use Bergerhoff samplers or a bulk bot-

tle+funnel method. For analysis both methods, GF-AAS and ICP-MS, are suitable. The ex-

panded uncertainty at 95 % confidence level was estimated to be 52 % and fulfils the data qual-

ity requirements of the DD4. At rural sites bulk or wet-only collector should be used. For analy-

sis only ICP-MS worked well with low concentration samples.

For developing a standard method for the determination of mercury deposition the CEN TC 264

Working Group 25 carried out a validation programme including laboratory test, preparation of

field tests and field tests. The working group tested different types of deposition collectors (bulk,

Bergerhoff and wet-only) at two European sites (one coastal/rural and one local/industrial) over

a period of twelve months to obtain parallel precipitation samples for mercury analysis. Analysis

of samples was performed following the analytical methods described in EMEP reference

method (EMEP manual chapter 4.18.1; EMEP 2002) or ISO 17852. Mercury in precipitation

samples were oxidized by adding bromine monochloride (BrCl), followed by UV irradiation,

SnCl2 reduction, gold amalgamation and detection by CVAAS. The working group concluded

that the collection efficiency of Bergerhoff samplers can be affected by windy weather condi-

tions. Therefore an increased uncertainty component for sampling efficiency should be em-



ployed when using this sampler. With an expanded uncertainty of 40 % and 44 % for the two

field trials the method fulfils the data quality objectives of the DD4.

5.9.1.3 Weaknesses and strengths of reference methods for the deposition of PAH

The working group 21, ―Ambient air – measurement method for B(a)P‖, of CEN TC 264 carried

out laboratory and field tests to establish the above mentioned standard method for the meas-

urement of the deposition of seven non-volatile PAH (EN 15980:2011). The technical method

validation programme comprised three parts: laboratory tests, degradation test and field tests.

The validation results showed that sample preparation and analysis methods did not influence

the results of PAH deposition rates. The different work-up and analysis methods proved to be

equivalent. Also the degradation of PAH in the bottles of the collectors during sampling was

proven to be negligible. Instead the use of different collector types influenced the measured

PAH deposition rates considerably (GLADTKE et al. 2012).

In the field test three different collector types at four sampling sites were used: bulk funnel-bottle

collectors, bulk open-jar collectors (Bergerhoff) and wet-only collectors. The test results showed

that the funnel-bottle bulk collector is the most appropriate sampling device for fulfilling the re-

quirements of DD4. The highest deposition rates and a low measurement uncertainty were ob-

tained with the funnel-bottle collector. Therefore the funnel-bottle collector is the reference sam-

pler in EN 15980. The wet-only collectors showed the lowest deposition rates at industrial sites

and should only be used at remote sites in a cold and humid climate. The uncertainties for the

open-jar/Bergerhoff collectors did not meet the 70% criterion of the DD4. They can only be used

in the case of high PAH deposition rates like at industrial sites.

5.9.1.4 DD4 versus EMEP

In compliance with Article 4 of the DD4, where appropriate, monitoring shall be coordinated with

the EMEP monitoring strategy and measurement programme (UNECE 2009). However, the DD4

and EMEP have different requirements for methodology. The objective of the DD4 is to measure

the ―total or bulk deposition‖ which is defined in Article 2 as ―the total mass of pollutants which is

transferred from the atmosphere to surface in a given area within a given time‖. The reference

method for the deposition sampling shall be based on the exposition of cylindrical deposit

gauges with standardised dimensions. The directive permits the use of wet-only samplers in-

stead of bulk sampler if it is shown that the difference between them is within 10%.

The EMEP Manual for Sampling and Analysis describes the standard recommended methods

for sampling and chemical analysis for the EMEP measurement network (EMEP 2002). In the

EMEP programme only the wet deposition of heavy metals is monitored, the dry deposition is

not measured (see Table 28).



Table 28: Monitoring requirements for HM and PAH specifed by the EMEP Manual for Sampling and

Analysis (EMEP 2002).

Components in precipitation

Measurement period

Measurement frequency

Sampling methods in field

Methods in laboratory

Heavy metals (Cd, Pb, Cu, Zn, As, Cr, Ni)

weekly weekly wet-only ICP-MS GF-

AAS

Mercury weekly (1 sampler)

monthly (2 samplers)

weekly

(or monthly)

wet-only

IVS sampler CV-AFS

PAHs to be decided to be decided wet-only

The Manual recommends using a wet-only collector for precipitation sampling of heavy metals.

Bulk samplers are recommended only if it can be shown that the contamination by dry deposi-

tion of dust and gases is negligible, and during periods when the precipitation is mainly in the

form of snow.

According to the EMEP Manual mercury has to be collected in special precipitation samplers

(see Table 29).

Table 29: Recommendations for sampling mercury in precipitation by the EMEP Manual for Sampling and

Analysis (EMEP 2002).

Recommendation Alternatives

Material Borosilicate glass Halocarbon materials, quartz

Sampler design Bulk samplers or wet-only sam-plers with gaseous Hg prevention and light shield. Heating and/or cooling of sample bottle depending on climatic conditions.

Event sampling using funnels and bottles or jars.

Sampling time 1 week to 1 month

Preservation of sam-ples

Monthly sampling 5 ml/l HCl (Su-prapur) prior to sampling.

Adding 10 ml/l HCl after sampling in sampling periods of < 2 weeks and samples are cooled if neces-sary.

The EMEP data quality objectives states that the uncertainty in the rural background measure-

ments of heavy metals should be less than 30 % in the annual averages. The DD4 states that

the data quality objective for total deposition of heavy metals and PAH should have an uncer-

tainty less than 70 %, expressed at a 95 % confidence level.

For the Member States who are affected by the requirements of DD4 and EMEP it is important

to have proper guidelines on which collectors and methods are suitable to use in which envi-

ronments (CEN TC 264 WG 20 2007). This will ensure that the deposition measurements are

valid for the different monitoring purposes. At remote sites (EMEP-type) with cold and humid

climate the results with wet-only collectors are comparable to the results of bulk samplers. At

EMEP-sites with considerable rates of dry deposition different sampling devices for monitoring

according to EMEP and DD4 are necessary.



5.9.2 Analysis of possible regulations

5.9.2.1 Existing regulations

Of the EU member states currently Germany and Austria have legally enforceable deposition

standards for a few heavy metals (see Table 30).

Some Member States apply non-legally binding target values for the assessment of deposition

of heavy metals (EUROPEAN COMMUNITIES 2001). Belgium (Flanders) uses a deposition target

value of 20 μg/(m²d) for cadmium.

For deposition of PAH there are no existing limit or target values in Europe.

Table 30: National air quality objectives for deposition of As, Cd, Hg and Ni for the protection of the human

health.

Country Objectives measured as standard Regulation

AT Cd 2 μg/(m²d) annual mean limit value Immissionsschutzgesetz-Luft (IG-L)

DE As 4 μg/(m²d)

Cd 2 μg/(m²d)

Hg 1 μg/(m²d)

Ni 15 μg/(m²d)

annual mean

annual mean

annual mean

annual mean

limit value Technische Anleitung zur Reinhaltung der Luft (TA-Luft)

CH Cd 2 μg/(m²d) annual mean limit value Luftreinhalte-Verordnung (LRV)

In Austria and Germany the limit values for heavy metal deposition were only exceeded at some

industrial sites (UMWELTBUNDESAMT 2011, LAU SA 2011). These exceedances are due to local

industrial emission sources. In rural or urban sites the deposition values are well below the limit

values.

5.9.2.2 Available datasets and deposition levels

A look at the deposition rates reported by the Member States in the Annual Questionnaire ac-

cording to Decision 2004/461/EC for 2007, 2008, 2009 and 2010 show that many Member

States have not reported any deposition data. More detailed information can be found in the

specific report for Task 1 (RICARDO – AEA 2012).

Deposition of arsenic, cadmium and nickel

Of the 101 stations reporting 2010 the deposition of arsenic 73 of these are from Germany. The

annual average data for individual stations ranges from below 0.01 µg/m²/day to a maximum of

3.4 µg/m²/day reported by Germany. The annual mean given for all stations for each MS ranges

from 0.01 µg/m²/day to 1.6 µg/m²/day. For Germany the annual mean for all stations is

0.61 µg/m²/day.

For cadmium deposition rates the reported stations vary from year to year and of the 83 stations

2010 reported 55 of these are from Germany. The annual average data for individual stations

ranges from 0.01 µg/m²/day to a maximum of 2.12 μg/m²day reported by Italy in 2010. The an-

nual mean given for all stations for each MS ranges from 0.01 μg/m²day to 0.62 μg/m²day again

for Italy from a total of five reported deposition stations. The German dataset, with 55 stations

currently reported showed a decrease from 0.21 μg/m²day to 0.13 µg/m²/day from 2009 to 2010.



The number of stations reported in the Annual Questionnaire for nickel deposition has risen

from two in 2007 to 99 stations reported across all Member States in 2009. Of the 100 individual

monitoring locations reported in 2010, 72 of these are from Germany alone. The data for the

first two years of reporting by Germany has shown a minor decrease in the annual average for

all stations from 3.1 μg/m²day to 2.7 µg/m²/day but a larger decrease in the maximum reported

value in 2009 of 38 µg/m²/day to 10 µg/m²/day for 2010. Most of the individual station data

spread for Germany is between 1 and 10 µg/m²/day for both years. On face value Latvia has

reported the greatest MS annual average, reducing from 7.6 μg/m²day in 2008 to 5.6 μg/m²day

in 2010, but this is based on a single station.

As many Member States have not reported any arsenic, cadmium and nickel deposition data or

reported data based on a single site, it is not possible to draw any conclusions on deposition

levels across the area of EU 27. The actual uncertainty over the station types (background or

industrial) limits the assessment to the overall annual average deposition rate for each Member

State. There are a lot more data available in 2009 and 2010, than in previous years, but most of


Mercury deposition

For mercury there are far fewer deposition measurements compared to the other metals meas-

ured according to DD4. Therefore is not possible to draw any conclusions on mercury deposi-

tion.

Deposition of benzo(a)pyrene

As for the heavy metals measured according to DD4 there are not enough data on

benzo(a)pyrene deposition available to draw any conclusions on Europe wide deposition levels.

The reported stations vary from year to year, with two stations reported in 2007, 22 stations in

2008 and 70 in 2009 and 20 stations in 2010. There is a reasonable spread of stations through-

out the different Member States but in many there is just one monitoring site.

The annual average data for individual stations range from below 0.01 μg/m²day to a maximum

of 62 µg/m²/day reported by the United Kingdom from a single station in 2008. It could be con-

sidered that this extremely high deposition rate, relative to the other measurements, could well

be an incorrect value caused by a units error, the data for 2009 and 2010 appear more realistic.

5.9.2.3 Possible regulations

Recommendations for deposition limit values are made by the European Commission Working

Group on Arsenic, Cadmium and Nickel Compounds in a Position Paper (EUROPEAN

COMMUNITIES 2001).

Depending on the commodities to be protected, the majority of the Working Group recommends

to set a limit value for cadmium deposition for local scales (in urban and industrialized areas)

within the following range: 2.5 – 5 μg/m²day.

The Working Group derived upper and lower assessment thresholds by analyzing the interan-

nual variability from time-series. For cadmium deposition, values of 40 % for the upper assess-

ment threshold and 20 % for the lower assessment threshold have been found.



The current gap in knowledge of deposition measurement and deposition data prevents us from

expanding or altering the recommendations given in the Position Paper. The main gaps are as

following:

Lack of experiences with the reference measurement methods for heavy metals and PAH

(published between 2009 and 2011);

Lack of deposition data for heavy metals and PAH at the present in many MS. Therefore no

information throughout the EU is available;

Available deposition data show a wide range between deposition data at industrial sites and

background sites;

Differences in methods for deposition sampling between DD4 and EMEP;

Considerable influence in the use of different collector types to measured deposition rates.

Service Request 6 – final report – Information of the public under the 4th Daughter Directive


6 INFORMATION OF THE PUBLIC UNDER THE 4TH DAUGHTER DIRECTIVE

6.1 Key messages

The majority of environmental information websites provide the data on heavy metals and

PAH in annual air quality reports. The access to these reports is usually quite easy.

The Commission Implementing Decision 2011/850/EC does not change the present reporting

requirements for the pollutants regulated by the DD4.

6.2 Context – requirements for information of the public

Current and future requirements of reporting to the public and to the Commission are addressed

in Article 8, paragraph 2 (d) of the DD4.

The provisions for the information of the public itself are laid down in Art. 7 of the DD4. They re-

quire information about the concentrations and deposition rates of Arsenic, Cadmium, Mercury,

Nickel, B(a)P and other polycyclic aromatic hydrocarbons (PAH) listed in Art. 4. In any case, it

has to cover information about exceedances of target values, including reasons of the ex-

ceedances and health effects. Besides the general public, the information shall especially be

made available to environmental protection organizations and organizations representing sensi-

tive population.

As the target values are laid down as annual mean values, the respective information is usually

provided in annual reports.

The subject of the review goes beyond the information reported routinely to the Commission. In-

formation from Member States‘ websites as well as the Commission Implementing Decision for

Reporting (2011/850/EU) has been assessed.

6.3 Compiling reports and websites

The availability of the required information made available by the Member States via internet

has been investigated.

Recent work done for the Task Force on Health on how health effects of air pollution is pre-

sented at selected websites is taken into account (BERKEMEYER et al. 2011). From the 26 web-

sites of national, regional or municipal authorities, covered in this study, only five provide data

on heavy metals. PAHs are included in ―others‖ (eleven websites) in the Task Force on health

study.

Altogether information was compiled from the following sources:

the results of the Task Force on health study,

web links provided by the competent authorities in the MSs after being contacted,

internet search.



A detailed list of the websites and an overview of the content is provided in the specific report

for Task 5 (UMWELTBUNDESAMT 2012).

The pollutants regulated by DD4 are published in annual reports, in most cases as annual mean

values, corresponding to the target values, in some cases also monthly mean values are given.

The results of the analysis of the websites and the reports available can be summarized as fol-

lowing:

17 MSs fully comply with the requirements for information of the public about heavy metal and

PAH concentrations; in two MSs, data are provided by regional authorities, but not by all within

the MS; six MSs either do not publish HM and PAH data or do not monitor these pollutants.

Data on HM and B(a)P are provided on national websites in 16 MSs in an official report;

Data on HM and B(a)P are provided on websites of all regional administrations for one MS

(BE);

Data on HM and B(a)P are provided on websites of some but not all regional administrations

for three MSs, but not on the website of an institution on the national level;

One MS states that there are no measurements

No data on HM and B(a)P could be identified on the national environmental information web-

sites of five MSs.

Health impact information could be identified on websites in eleven MSs.

Comments on the data presentation and accessibility:

There are in principle two different options for the presentation of HM and B(a)P data.

The majority of environmental information websites provide these data in annual air quality re-

ports, which are presented as pdf-documents. The access to these reports is usually quite easy

and straightforward; within the reports, the HM and B(a)P data are usually easily found.

Alternatively, tables or graphs of HM and B(a)P data are directly presented on the websites, in

some cases as excel files to be downloaded. On these websites, the data can be searched for

by selecting stations, pollutants and time periods, i.e. they are accessible in principle similar to

gaseous pollutants or PM10. For users who do not know at which station a specific pollutant is

measured it is not easy to find the data especially in CZ, PT and UK.

PT presents daily HM and B(a)P data as excel tables for each hour, i.e. most lines are empty,

and values are not easily read. In most cases, values are given as ―0‖, it is not clear if these are

below detection limit.

6.4 Reporting requirements under the Implementing Decision 2011/850/EC

The Commission Implementing Decision laying down rules for Directives 2004/107/EC and

2008/50/EC of the European Parliament and of the Council as regards the reciprocal exchange

of information and reporting on ambient air quality 2011/850/EU lays down the requirements for

the data and information to be made available to the Commission.

Article 10 of the Implementing Decision gives the provisions on the reporting of primary valid

assessment data and primary up-to-date assessment data. The latter does not refer to the pol-

lutants regulated by the present DD4 (heavy metals and PAHs), as these are not measured in



near-real-time, i.e. from continuous monitoring devices with hourly data transmission, but origi-

nate from sampling and later laboratory analyses.

In the context of DD4, primary validated assessment data according to Art. 10 are to be made

available by end of September of the year following the year of measurement. The relevant

meta-information is specified in Part E of Annex II of 2011/850/EC, the technical details will be

specified in the Guidance, which is being drafted by the Commission at present.

Aggregated valid assessment data according to Art. 11 are, in the case of the pollutants regu-

lated presently by the DD4, annual mean values.

The information about attainment (or exceedance) of environmental objectives to be made

available according to Art. 12 also refers to annual mean values.

Therefore, the Commission Implementing Decision 2011/850/EC does not change the present

reporting requirements for the pollutants regulated by the DD4.

Service Request 6 – final report – References


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Service Request 6 – final report – abbreviations


8 ABBREVIATIONS

AEI ........... Average Exposure Indicator

AMS ......... Automated continuous Measurement Systems

AQD ......... Air Quality Directive

AQUILA ... European Network of National Air Quality Reference Laboratories

As ............ Arsenic

B(a)P ....... Benzo(a)pyrene

BaA .......... Benzo(a)anthracene

BAT-AEL .. Best Available Techniques Associated Emission Levels

BbF .......... Benzo(b)fluoranthene

BjF ........... Benzo(j)fluoranthene

BkF .......... Benzo(k)fluoranthene

CAA ......... Clean Air Act

Cd ............ Cadmium

CEIP ........ Centre on Emission Inventories and Projections (http://www.ceip.at/)

CEN ......... Comité Européen de Normalisation (http://www.cen.eu/)

CVAAS .... Cold Vapour Atomic Absorption Spectrometry

CVFAS ..... Cold Vapour Atomic Fluorescence Spectrometry

DbA .......... Dibenz(a,h)anthracene

DD4 ......... 4th Daughter Directive

DEM ......... Data Exchange Module

EAL .......... Environmental Assessment Level

ECO ......... Exposure Concentration Obligation

EIONET ... European environment information and observation network

(http://www.eionet.europa.eu)

EMEP ...... Co-operative programme for monitoring and evaluation of the long-range transmis-

sions of air pollutants in Europe (http://www.emep.int/)

E-PRTR ... European Pollutant Release and Transfer Register (http://prtr.ec.europa.eu/)

ETC/ACM European Topic Centre for Air Pollution and Climate Change Mitigation

(http://acm.eionet.europa.eu/)

FDMS ...... Filter Dynamics Measurement System

GC-MS ..... Gas Chromatography – Mass Spectrometry

GEM ........ Gaseous Elemental Mercury

GF-AAS ... Graphite Furnace – Atomic Absorption Spectrometry

Hg ............ Mercury

HPLC-FLD High Performance Liquid Chromatography – Fluorescence Detection

http://www.ceip.at/

http://www.cen.eu/

http://www.eionet.europa.eu/

http://www.emep.int/

http://prtr.ec.europa.eu/

http://acm.eionet.europa.eu/

Service Request 6 – final report – abbreviations


IARC ........ International Agency for Research on Cancer, http://www.iarc.fr/

IdP ........... Indeno(1,2,3-cd)pyrene

ICP-MS .... Inductively Coupled Plasma – Mass Spectrometry

LRTAP ..... Convention on Long-range Transboundary Air Pollution

(http://live.unece.org/env/lrtap/welcome.html)

MS ........... Member States

MSC-E ..... Meteorological Synthesizing Centre-East (http://www.msceast.org/index.html)

MSC-W .... Meteorological Synthesizing Centre-West

(http://www.emep.int/mscw/index_mscw.html)

NERT ....... National Exposure Reduction Target

Ni ............. Nickel

PAH ......... Polycyclic Aromatic Hydrocarbons

Pb ............ Lead

POP ......... Persistent Organic Pollutant

RGM ........ Reactive Gaseous Mercury

SCA ......... Smoke Control Areas

TEOM ...... Tapered Element Oscillating Microbalance

TFHM ....... Task Force on Heavy Metals

(http://live.unece.org/env/lrtap/taskforce/tfhm/welcome.html)

TPM ......... Total Particulate Mercury

UFP ......... Ultra Fine Particles

UNECE .... United Nations Economic Commission for Europe (http://unece.org/Welcome.html)

WHO ........ World Health Organization (http://www.who.int, http://www.euro.who.int/en/what-

we-do/health-topics/environment-and-health/air-quality)

http://www.iarc.fr/

http://live.unece.org/env/lrtap/welcome.html

http://www.msceast.org/index.html

http://www.emep.int/mscw/index_mscw.html

http://live.unece.org/env/lrtap/taskforce/tfhm/welcome.html

http://unece.org/Welcome.html

http://www.who.int/

http://www.euro.who.int/en/what-we-do/health-topics/environment-and-health/air-quality

http://www.euro.who.int/en/what-we-do/health-topics/environment-and-health/air-quality