control of landfill leachates contaminated groundwater by a ...ni, cr (vito) o-xylene, p-xylene,...
TRANSCRIPT
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Control of landfill leachates contaminated groundwater by a MULTIBARRIER approach
L. Diels, J. Dries, L. BastiaensFlemish institute for technological research, Vito
Mol, Belgium
NATO-CCMS Pilot StudyPrevention and Remediation in Selected Industrial Sectors:
Rehabilitation of old landfills Cardiff, May 23 – 26, 2004
NATO-CCMS, 11 juli 2004, Cardiff 2004
No measures
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Landfill leakage: Multifunctional treatment zone or Multibarrier for removal of mixed pollutants
NATO-CCMS, 21 juli 2004, Cardiff 2004
Evaluation of several combinations– Chemical transformation (Fe°), – Biotransformation (aerobic/anaerobic),– Bioprecipitation– Sorption
Two solutions:
-Installation of a new landfill(20 – 40 million EURO)
-Installation of a MULTIBARRIER(2 - 4 million EURO)
Groundwater flow
GW level
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EU-project MULTIBARRIER
NATO-CCMS, 31 juli 2004, Cardiff 2004
Microorganismsbacteria, fungi
Carrier material
Fe 0, Carbon,
Sand
Growth
addi
tives
Nutrien
ts, O
RC, com
post
Mixed pollution
heavy metalsVOCls
aromatics
PARTNERS:
Vito, MolUniversity of WageningenUniversity of InnsbruckTUniversity of MunchenIBA, HeiligenstadtBIOTECs, BerlinUniversity of PragueDEC, ZwijndrechtUniversity of Latvia, RigaUnivesity of Mining, Sofia, Bulgaria
ENDORSERS:Montgomery Watson Harza, BrusselsIntercommunale Hooge Maey, Antwerp
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Mixed contamination plumes• Mixed contamination plumes require:
– a combination of different pollutant removal processes (biotic & physico-chemical)– a combination of barrier types = MULTIBARRIER
• Design and optimisation of multibarriers is more complex than single-barriers– Concept: sequential or mixed multibarrier?– Effect of the pollutants on the removal process (inhibition, stimulation or no effect)?– Effect of one pollutant removal process on an other one?
NATO-CCMS, 41 juli 2004, Cardiff 2004
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MULTIBARRIER Key-components• Groundwater:
0.5 mM NaHCO3
0.5 mM KHCO3
0.5 mM CaCl2.2H2O0.5 mM MgCl2.6H2O
+ growth supporting additives (Nutrients, O2, compost,..)
• Carrier materials:Filter sand (1-2 mm)Zerovalent iron FeA4 (0.3-2 mm)Activated carbon
GAC F400GAC Ind. React. (landfills)
(Aquifer material)MetasorbZeolitesWood chips
•Mixed pollution:VOCls: 2 mg/l PCE
5 mg/l TCEMetals: 5 mg/l Zn as ZnCl2
0.2 mg/l As(V) as Na2HAsO4
BTEX: 2 mg/l benzene2 mg/l toluene2 mg/l m-xylene
Extra: AOX (LFU)DCM, 11 DCA (UW)Ni, Cr (Vito)o-xylene, p-xylene,Ethylbenzene (Vito)
•Micro-organisms:Aquifer material Enrichment culturesAxenic strains
NATO-CCMS, 51 juli 2004, Cardiff 2004
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MULTIBARRIER materials
Filtersand
Specific surface [m2/g] (measured)
FiltersandEverzitMetasorbGAC F400Zerovalent Iron
1,9294,1
3,0764,4
1,0Everzit Metasorb GAC F400
magnitude: 500x
Zero Valent IronFiltersand
+ Aquifer as source of micro-organisms
NATO-CCMS, 61 juli 2004, Cardiff 2004
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Design of multibarriers
NATO-CCMS, 71 juli 2004, Cardiff 2004
• Different multibarrier concepts:
• Concept = Site specific and depending on the pollutants present• Sorption barrier = polishing step
SorptionBiodegradationReduction - Fe0
Mix
ed p
ollu
tion
g
SorptionBiodegradation Reduction - Fe0
...Mixed multibarrier
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MULTIBARRIER concepts: Sequential vs mixed
BIO
Fe0
TEA SEQUENTIAL MIXED
O2
NO3- ?
Fe3+
SO42-
CO2
NATO-CCMS, 81 juli 2004, Cardiff 2004
TEA
SEQUENTIAL MIXED
O2 +
NO3- +
SO42- + +
Fe3+ + +
CO2 + +
As +
VOCls + +
Bio/Fe0
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System A (O2) & System B (NO3)
NATO-CCMS, 91 juli 2004, Cardiff 2004
Biocolumns
Ironcolumns
Influent
PCETCE
Mixingvessel
N2
B T m-X
Aerobic/anoxicmedium
A
B
C2 1 3 4
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Benzene removal in a denitrifying sequential system
NATO-CCMS, 101 juli 2004, Cardiff 2004
PCE+TCE
metals
BTX
1,2-cisDCE
BTX
NO3-
(1 mM)
BIO
Fe0 0
20
40
60
80
100
0 100 200 300 400 500
t (d)
% b
enze
ne r
emov
a
Fe(0)BioMB
[NO3] (mM): 1 0 1
HRTx 1.3
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Systems D & E: Strictly anaerobic systems
1 2 3 4
Bio Bio
Bio
Bio+Fe
Fe
Fe
SR: 0.5 mM SO42-
IR: 2.5 mM Fe(III)EDTA
NATO-CCMS, 111 juli 2004, Cardiff 2004
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System D: PCE & TCE degradation (SR columns)1 2 3 4
Bio Bio
Bio
Bio+Fe
Fe
Fe
NATO-CCMS, 121 juli 2004, Cardiff 2004
initial sorption
incomplete PCE degradation
complete TCE degradation
0
25
50
75
100
0 50 100 150 200
t (d)%
PC
E re
mov
al
C1 aqC2A FeC2B aqC2 MBC3A aqC3B FeC3 MBC4 mix
0
25
50
75
100
0 50 100 150 200
t (d)
% T
CE
rem
oval
C1 aqC2A FeC2B aqC2 MBC3A aqC3B FeC3 MBC4 mix
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System D & E: Benzene removal
1 2 3 4
Bio Bio
Bio
Bio+Fe
Fe
Fe
NATO-CCMS, 131 juli 2004, Cardiff 2004
SR: no degradation
IR:- all MB- not in C2aq
0
25
50
75
100
0 50 100 150 200
t (d)%
ben
zene
rem
oval
C1 aqC2A FeC2B aqC2 MBC3A aqC3B FeC3 MBC4 mix
0
25
50
75
100
0 50 100 150 200
t (d)
% b
enze
ne re
mov
al
C1 aqC2A FeC2B aqC2 MBC3A aqC3B FeC3 MBC4 mix
SR
IR
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System C: Partially mixed MB system
Columns (L = 50 cm)K1: test columnK2: abiotic control
Layers:L1: FS/Aq/Fe0 = 60/20/20 (W)L2:FS/Aq = 78/22 (W)
Monitoring:chemical analysesmicrobial ecology
NATO-CCMS, 141 juli 2004, Cardiff 2004
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Partially mixed MULTIBARRIER: results
0123456789
10
0 100 200 300 400 500 600
Distance in column (mm)
pH
-500
-400
-300
-200
-100
0
100
200
300
ORP (mV)
pHORP
0
500
1000
1500
2000
2500
3000
3500
4000
0 200 400 600
Distance in column (mm)
PCE,
TC
E (p
pb)
0
5
10
15
20
25
30
35
40
45
50
cDC
E (p
pb)
PCETCEcDCE
0500
10001500200025003000350040004500
0 200 400 600
Distance in column (mm)
(ppb
) BTm-X
NATO-CCMS, 151 juli 2004, Cardiff 2004
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NATO-CCMS, 161 juli 2004, Cardiff 2004
System 1-5: Results DCM &11DCA
100%
50%
10%
0% Noand
50% (2nd)
No
50%
No
>50%
Complete
Complete
No
Fe(0)
redox conditioningelectron donor
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Results (% removal)
NATO-CCMS, 171 juli 2004, Cardiff 2004
Column trains
Characteristics (TEA) Acro-nym PCE TCE Benzene Toluene m-xylene
System A: Zerovalent iron wall followed by a micro-aerobic biobarrier 1
A1 1 – Fe(0)column A1-1 60-80 90-99 4-13 10-53 NA
2 – Bio column (O2) A1-2 80-100 92-100 99-100 99-100 > 90
System B: Zerovalent iron wall followed by a denitrifying biobarrier 1
B1 1 – Fe(0)column B1-1 66-99 97-100 6-18 16-54 NA
2 – Bio column (NO3-) B1-2 80-93 97-100 89-100 99-100 > 90
System C: Partially mixed Fe(0)/biowall followed by anaerobic biowall 2, 1
C1 1 – mixed zone C1-1 95-100 1 95-100 1 20 2 30 2 40 2
2 – bio zone C1-2 95-100 1 95-100 1 20 2 30 2 50 2
System D: sequential and mixed barriers under sulfate reducing conditions 1
D1 1 – Bio column (SO42-) D1-1 0-11 0-15 11-44 97-100 NA
D2 1 – Fe(0)column D2-1 55-71 88-98 4-54 0-36 NA
2 – Bio column (SO42-) D2-2 55-78 89-98 23-67 12-36 < 25
D4 1 – Mixed column (SO42-) D4-1 76-89 99-100 18-62 7-23 > 90
System E: sequential and mixed barriers under iron reducing conditions 1
E1 1 – bio column (Fe3+) E1-1 0-11 9-18 24-29 100 NA
E2 1 – Fe(0)column E2-1 53-67 85-92 50-68 72-91 NA
2 – Bio column (Fe3+) E2-2 54-67 86-92 52-71 77-90 > 90
E4 1 – Mixed column (Fe3+) E4-1 58-73 94-97 55-64 94-98 > 90
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Conclusions
NATO-CCMS, 181 juli 2004, Cardiff 2004
• Mixed contamination plumes are omnipresent.
• Remediation of mixed contamination plumes using barriersMULTIBARRIERs are required
• Fungi do not play a big role in a Multibarrier
• In lab-scale columns different Multibarrier-concepts have been shown to be effective for the remediation of a mixed plume (PCE, TCE, BTmX, Zn, As).
• Behaviour of AOX in a Multibarrier is under study
• No toxicity detected in effluent (toxicity reduction) • The design and optimisation of multibarriers is more complex in
comparison with ‘single barriers’Many influencing parameters have to be taken into accountMixed Multibarrier under iron or sulfate reducing conditions
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Conclusions
NATO-CCMS, 191 juli 2004, Cardiff 2004
• Sequential Multibarrier: ZVI + Micro-aerofilic biobarrier– PCE, TCE dehalogenation in ZVI– Zn, As removal in ZVI– BTX degradation in biobarrier– No degradation of cDCE
• Sequential Multibarrier: ZVI + Anaerobic biobarrier(denitrifying)– PCE, TCE dehalogenation in ZVI– Zn, As removal in ZVI– T, X degradation in biobarrier– B partially degraded in biobarrier– No degradation of cDCE
• Mixed Multibarrier: filtersand, aquifer materiaal, ZVI + Anaerobic biobarrier in aquifer– PCE, TCE dehalogenation– Zn, As removal in ZVI– BTX degradation in mixed zone– No formation of cDCE or VC
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NATO-CCMS, 201 juli 2004, Cardiff 2004
Upscaling promising multibarrier concept
Aquifer AquiferReactive materials
Groundwater
Closed system
Pollutant-mixing& monitoring unit Posttreatment
A: coarse zone (25 cm)
B: Aquifer material
C: mixed Bio/Fe0 barrier : FeA4/Aq/HM = 30/60/10
D: Biobarrier Aq/ HM (90/10)
E: Biobarrier Aq
E: coarse zone (25 cm)
F: Sorption barrier
0.5 m 1 m 3 m
BIOFe0/BIO
PCE, TCE, Zn, As, BTEX Polishing
BTEX?
A B C D E F G
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Set-up of MB on pilot scale
NATO-CCMS, 211 juli 2004, Cardiff 2004
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NATO-CCMS, 221 juli 2004, Cardiff 2004
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MULTIBARRIER Monitoring System (MMS)
NATO-CCMS, 231 juli 2004, Cardiff 2004
• On-line measuring and logging system pH, T, ORP, conductivity, O2 and pressure :
– Tested in the pilot system– Focus on EC-measurement
• in-well mixing system has been tested:– Works very well
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Pilot MULTIBARRIER system: First experiment
• Monitoring strategy:
10-20 cm bgs170-180 cm bgs
90-100 cm bgs 90-100 cm bgs
10-20 cm bgs170-180 cm bgs
EC-measurementsStirred electrode set
Non-stirred electrode set
NATO-CCMS, 241 juli 2004, Cardiff 2004
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NATO-CCMS, 251 juli 2004, Cardiff 2004
Monitoring of PRBs
A
B
B
B
C
C
C
D
E
E
E
F
G
G
Plume
Gravel
Reactive material
Monitoring well
100 m
- UK guidelines- US EPA guidelines- Flanders (OVAM) guidelines- Germany (in preparation?)
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In situ mesocosm-systemsMonitoring of microbiology (molecular biology)
NATO-CCMS, 261 juli 2004, Cardiff 2004
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WP3: HM + Mesocosms containerPearson correlation (Opt:0.90%) [0.0%-100.0%]MB
100
90807060504030
MB
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
MESO A1 T0 AMESO A2 T0 A
MESO A2 T0 BMESO A1 T0 B
MESO A5 T0 A
MESO A5 T0 BMESO A7 T0 A
MESO A7 T0 Bmengsel HM/AqDEC (bulk) B
mengsel HM/AqDEC (bulk) A
AqDEC (bulk) BAqDEC (bulk) A
mengsel HM/AqDEC/FeA4 (bulk) Bmengsel HM/AqDEC/FeA4 (bulk) A
MB Aquifer
HM (bulk) BHM (bulk) A
JD 112JD 112
JD 107JD 106
JD 104
JD 105
HMHM
Aëroob 2 onderAëroob 2 (REF) boven
Aëroob 1 (MB) boven
Aëroob 1 onder
NATO-CCMS, 271 juli 2004, Cardiff 2004
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MULTIBARRIER Modelling System: salt injection
new gage3
new gage2
new gage1
X
Y
Z
new gage3
new gage2
new gage1
X
Y
Z
NATO-CCMS, 281 juli 2004, Cardiff 2004
new gage3
new gage2
new gage1
X
Y
Z
new gage3
new gage2
new gage1
X
Y
Z
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Modelled salt-peaks• Permeability: 24.17 m/dag• Dispersivity: 0.3 m• Monitoring wells: filter 100 cm bgs,• Result: migration of pollutant initally faster, afterwards slower in comparsion with
measured values
NATO-CCMS, 291 juli 2004, Cardiff 2004
0
10
20
30
40
50
60
70
80
90
0 5 10 15 20 25 30 35 40
d = 5 md = 3,5 md = 1,5 m
Time (days)
Conc%
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NATO-CCMS, 301 juli 2004, Cardiff 2004
Pilot scale Multibarrier:Curilo deposit
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Installation at Curilo deposit
3 m
2 m0.1 m0.6 m
1.5 m
2.0 m
1.5 m
1.0 m
5.0 m
0.8 m
1.0 m
12
34
5
0,5 m
3
4
17.5 m
15.0 m
1.6 m
NATO-CCMS, 311 juli 2004, Cardiff 2004
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Curilo deposit: constructed wetland + Multibarrier
NATO-CCMS, 321 juli 2004, Cardiff 2004
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Thanks to all the partnersand the European Commission
QLK3-CT-2000-00163+
QLRT-2001-02916
NATO-CCMS, 331 juli 2004, Cardiff 2004
www.multibarrier.vito.be