chemical contaminants entering the marine …review chemical contaminants entering the marine...

Marine Pollution Bulletin 112 (2016) 17–38

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Marine Pollution Bulletin

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Review

Chemical contaminants entering the marine environment fromsea-based sources: A review with a focus on European seas

Victoria Tornero ⁎, Georg HankeEuropean Commission, Joint Research Centre (JRC), Institute for Environment and Sustainability (IES), Water Resources Unit, Enrico Fermi 2749, 21027 Ispra, Italy

⁎ Corresponding author.E-mail address: [email protected] (V. T

http://dx.doi.org/10.1016/j.marpolbul.2016.06.0910025-326X/© 2016 The Authors. Published by Elsevier Ltd

a b s t r a c t
a r t i c l e i n f o
Article history:Received 8 April 2016Received in revised form 22 June 2016Accepted 27 June 2016Available online 18 July 2016

Anthropogenic contaminants reach the marine environment mostly directly from land-based sources, but thereare cases in which they are emitted or re-mobilized in the marine environment itself. This paper reviews the lit-erature, with a predominant focus on the European environment, to compile a list of contaminants potentiallyreleased into the sea from sea-based sources and provide an overview of their consideration under existing EUregulatory frameworks. The resulting list contains 276 substances and for some of them (22 antifouling biocides,32 aquaculturemedicinal products and 34warfare agents) concentrations and toxicity data are additionally pro-vided. The EUMarine Strategy Framework Directive Descriptor 8, together with theWater Framework Directiveand the Regional Sea Conventions, provides the provisions against pollution of marine waters by chemical sub-stances. This literature review should inform about the current state of knowledge regardingmarine contaminantsources and provide support for setting-up of monitoring approaches, including hotspots screening.

© 2016 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license(http://creativecommons.org/licenses/by-nc-nd/4.0/).

Keywords:ContaminantsPollutantsSea-based sourcesMarine Strategy Framework DirectiveRegional Sea ConventionsReview

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 172. Approach . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 183. Sea-based activities resulting in the release of contaminants into the marine environment . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18

3.1. Shipping . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 183.1.1. Accidental spillage . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 183.1.2. Operational discharges . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 193.1.3. Emissions from antifouling paints . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19

3.2. Mariculture . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 203.2.1. Medicinal products . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 203.2.2. Food additives and contaminants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 213.2.3. Antifouling biocides . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 21

3.3. Offshore activities . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 213.3.1. Offshore oil and gas exploration and production . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 213.3.2. Other offshore installations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 22

3.4. Seabed mining. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 233.5. Dredging of sediment and dumping at sea . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 23

3.5.1. Emissions from historical dumping sites . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 233.6. Other sea-based activities . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 24

4. Results and conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 24References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 35

ornero).

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1. Introduction

Contamination caused by hazardous substances is a major environ-mental concern in European waters and consequently is addressed bya number of EU legislativemeasures and policies. TheWater Framework

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18 V. Tornero, G. Hanke / Marine Pollution Bulletin 112 (2016) 17–38

Directive (WFD, 2000/60/EC) provides for measures against chemicalpollution of surface waters. There are two components – the selectionand regulation of substances of EU-wide concern (priority substances,PS) as a means to assess the chemical status of water bodies up to 12nautical miles from the straightened coastline, and the selection byMember States of substances of national or local concern (river basinspecific pollutants, RBSP), which form part of the quality elements for“good ecological status”. In 2001 a first list of 33 PS was adopted (Deci-sion 2455/2001) and in 2008 the Environmental Quality Standards(EQSs) for those substances and eight other pollutants already regulat-ed at EU level were set in the Directive 2008/105/EC (or EQS Directive),which was amended by the Directive 2013/39/EU.

TheMarine Strategy Framework Directive (MSFD, 2008/56/EC) aimsto provide an integrative marine environment status assessment andconsiders both coastal and offshore environment, thus overlappingwith WFD for some parts of the marine environment. The approachtaken on contaminants under MSFD Descriptor 8 “Concentrations ofcontaminants are at levels not giving rise to pollution effects” should,therefore, be properly integrated and alignedwith thework on identifi-cation and review of PS and EQS under the WFD. The identification ofsubstances which are not listed as WFD PS or RBSP, but entail a signifi-cant risk to the marine environment is part of the MSFD provisions(Commission Decision 2010/477/EU).

It has been suggested that harmonization in MSFD Descriptor 8 im-plementation would be improved by compiling a list of contaminantswhich pose a risk to, or via, the marine environment (Tornero et al.,2015). This process has to take into consideration the relevant provi-sions of theWFD for territorial and/or coastal waters, but also the activ-ities of the Regional Sea Conventions (RSCs), which cover EU marineregions or sub-regions: OSPAR (Convention for the Protection of theMarine Environment in the North-East Atlantic), HELCOM (Conventionon the Protection of theMarine Environment in the Baltic Sea), Barcelo-na Convention (Convention for the Protection of Marine Environmentand the Coastal Region of the Mediterranean), and Bucharest Conven-tion (Convention for the Protection of the Black Sea).

This paper reviews the available literature to provide a list of chem-ical substances that have been, are being or might be released into themarine environment through sea-based human activities, with an over-view of the policies and regulations in place for their management andcontrol within the EU. This review should improve the knowledge re-garding substances that might occur in the marine environment. How-ever, it is important to note that the substances have been listedwithout considering their toxicological properties and/or marine con-centrations, and therefore this paper does not provide a risk assess-ment. The resulting list might support the setting-up of monitoringapproaches, e.g. through target screening schemes, and thus helpguide the selection of relevant substances for MSFD Descriptor 8implementation.

2. Approach

The information has been gathered through an extensive review ofthe existing literature, mainly peer-reviewed papers and books, butalso reports, assessments and proposals from RSCs and research pro-jects, conference proceedings, and other literature regarding the occur-rence of contaminants in marinewaters, andwith a special focus on theEuropean environment. The paper first compiles the relevant contami-nants on the basis of the sea-based human activities potentiallyresulting in their release into the marine environment. Contaminantsentering the marine environment through atmospheric transport arebeyond the scope of this review. For selected groups of identified sub-stances (biocides in ship antifouling paints, medicinal products in themarine aquaculture industry, andmain constituents of warfarematerialdumped at sea), specific information on their concentrations and toxic-ity in the marine environment is also compiled.

The gathered information is used to create a list of marine-relevantcontaminants, which includes their chemical identity and major sea-based sources. This list also gives information on the relevant interna-tional regulations/legislations and RSC monitoring programmes whichdeal with those substances, thus allowing the analysis of their coveragein European marine waters.

3. Sea-based activities resulting in the release of contaminants intothe marine environment

3.1. Shipping

Maritime traffic on the world's oceans has increased dramaticallyover the past 20 years, thus increasing the risk of pollution caused byshipping (Tournadre, 2014). Although environmental regulations arestrict, particularly under the MARPOL Convention (International Con-vention for the Preventionof Pollution fromShips), polluting substancescontinue to be discharged into the sea, often illegally (EMSA, 2012).

3.1.1. Accidental spillage

3.1.1.1. Chemical spills. Shipping is themost importantmode of transportfor a significant number of chemicals, referred to as Hazardous andNox-ious Substances (HNS), and defined as any substance other than oil,which if introduced into themarine environment is likely to create haz-ards to human health, to harm living resources and other marine life, todamage amenities and/or to interfere with other legitimate uses of thesea (IMO, 2000).

It is estimated that about 2000 different chemicals used by man areregularly transported by sea, either in bulk or in packaged form, and thechemical seaborne trade is estimated to reach 215 million tonnes by2015 (Purnell, 2009). According to the data compiled by the EuropeanMaritime SafetyAgency (EMSA), incidents resulting inHNS release hap-pen regularly in European waters (EMSA, 2007, 2008, 2009, 2010). Theecological hazards involved in these spills are less recognized and un-derstood than those involving oil pollution (Neuparth et al., 2011). Itseems logical to think that the most commonly transported chemicalsare the onesmost likely to be involved in one incident, so updated infor-mation about transported chemicalswould be a first step to be preparedfor and reduce the risk from possible incidents (Sheahan et al., 2015).However, putting together a comprehensive list of chemicals such asthis is complicated due to the high number and diversity of HNS. More-over, the data on the chemical transportation volumes in the EU is lim-ited and decentralized, and the exact quantities of different chemicalstransported and spilled are often not available and/or accessible (Postiand Häkkinen, 2012; EMSA, 2013a). Despite this, there are some studiesthat have gathered very valuable information. Cunha et al. (2015) col-lected information on the behavior, fate, weathering, and impact ofHNS spilled at sea around the world and converted it into a databasethat can be accessed by the general public. In Europe, the HASREP pro-ject (Response to Harmful Substances spilled at sea) identified the top100 chemicals being transported in and along European waters andfound that the 15 bulk HNSsmost handledwere palm and other vegeta-ble oils, methanol, benzene and its mixtures, sodium hydroxide solu-tion, xylenes, styrene, methyl tert-butyl ether (MTBE), molasses,ammonia, ethanol, phenol, phosphoric acid, sulphuric acid, acetic acid,and animal fat (HASREP, 2005). These chemicals were mostly thesame as those most transported/handled in the Baltic Sea according tothe Chembaltic project (Risks of Maritime Transportation of Chemicalsin Baltic Sea) (Posti and Häkkinen, 2012). According to the EMSA anal-ysis of significant HNS incidents, the most released substances during1978–2013 in European waters were styrene, sulphuric acid, benzene,and phosphoric acid. Other released substances include methyl-ketone,propane, phenols, isopropyl alcohol, acrylonitrile, acetone, and com-pounds of potassium, zinc, calcium, barium, lead, and sodium (EMSA,2013a).

19V. Tornero, G. Hanke / Marine Pollution Bulletin 112 (2016) 17–38

Many of those chemicals do have environmental hazard potential,although marine toxicological data are scarce for most of them(Neuparth et al., 2013; Häkkinen and Posti, 2014). It would be imprac-tical to consider a full scientific ecotoxicological data survey for all thosechemicals, so the prioritization of those HNS posing the highest risk tothe marine environment would be needed to assist the preparednessand emergency response planning to a potential incident (Neuparthet al., 2012; Sheahan et al., 2015 ). A priority list of 23 chemicals wasestablished in EU Atlantic waters in the context of the ARCOPOL plat-form (Atlantic Region-Coastal Pollution Response), based on the HNSvolumes transported, the reported HNS incidents, the HNS physico-chemical properties and the toxicity to marine organisms (Neuparthet al., 2011). A similar survey was conducted through the RAMOCS pro-ject (Implementation of risk assessment methodologies for oil andchemical spills in the European marine environment), resulting in theidentification of the top 20 ranking of HNS in European waters(Radovic et al., 2012).

3.1.1.2. Oil spills. Marine pollution caused by accidental spills is a well-known global concern. Oil tanker accidents account for 10–15% of allthe oil that enters the ocean world-wide every year. Although there isevidence for decrease in number of maritime incidents, major acciden-tal oil tanker spills (i.e. those N20,000 tonnes) still occur at irregular in-tervals in European waters (EEA, 2008).

The degree of the damage caused by an oil spill event will dependupon the quantity spilled, the chemicals involved and the sensitivityof themarine area impacted aswell as thewind andweather conditionsat themoment of the accident. Crude oil is not a single substance but it iscomposed of thousands of chemicals and its chemical compositionchanges dynamically after release into the environment. Moreover,there are thousands of different kinds of crude and refined oils(Coppock and Dziwenka, 2014). The polycyclic aromatic hydrocarbons(PAHs) often comprise up to 10% of the organic compounds in crudeoil and can be used as tracer for the general distribution of petroleumhydrocarbons in the environment associated with a spill. Oil spills arealso an importance source of Volatile Organic Compounds (VOCs)such as hexane, heptane, octane, nonane, benzene-toluene-ethylben-zene-xylene isomers (BTEX), and other lighter substituted benzenecompounds (Sammarco et al., 2013).

In recent years, there has been an increased interest in other compo-nents of petroleum, such as compounds containing nitrogen, sulfur, andoxygen, acids, esters, ketones, phenols and metals such as iron, nickel,copper, chromium and vanadium (NRC, 2003). Despite their relativelylow abundance, they may also cause harmful effects on the marine en-vironment (Bennett and Larter, 2000).

Following an oil spill, several means of cleanup are used to reducethe overall impacts on marine ecosystems. While the primary spill re-sponse tool usually is to recover oil from the sea surface with variousmechanical recovery devices, chemical dispersants can be used to trans-fer the oil from the sea surface to the water column, in the form of verysmall droplets and subsequent dilution into a very large volume ofwater, which facilitates the natural biodegradation process (EMSA,2016). Chemical dispersant use can be regarded as adding another pol-lutant to themarine environment and, despite improvements in disper-sant formulations, the toxicity of the dispersant/oil mixture to marinebiota is often a major environmental concern (ITOPF, 2005).

Within the EU, the decision to apply dispersants as an oil spill re-sponse strategy lies entirely with the affected coastal Member State(s)and a number of countries may consider the option of using dispersantsin an oil spill with certain reservations. Since 2005, EMSA publishes an“Inventory of national policies regarding the use of oil spill dispersantsin the EU Member States”, which is updated in regular intervals. Basedon latest inventory published (EMSA, 2014), there are approximately75 brands of dispersants approved for use in the EU/EFTA (EuropeanFree Trade Association) countries. However, only 34 different disper-sant brands are currently in stockpiles in Europe (EMSA, 2016).

All oil spill dispersants are composed of surfactants and solvents.Surfactants allow oil and water to mix easily and can be made bychemically combining fatty materials (e.g. vegetable oils) withmore water-soluble materials (e.g. sugars). Typical surfactants intoday's formulations include fatty acid esters or sorbitan esters(e.g. sorbitan, mono-(9Z)-9-octadecenoate), ethoxylated fatty acidesters (polyethylene glycols, PEGs) or ethoxylated sorbitan esters,and sodium di-isooctyl sulphosuccinate (DOSS). Solvents help keepthe chemicals mixed and help them dissolve into the oil. Typical sol-vents include light petroleum distillates and glycol ethers (e.g. pro-pylene glycol, 2-butoxyethanol, di-propylene glycol monomethylether, and di-propylene glycol monobutyl ether) (EMSA, 2010;Graham et al., 2016).

3.1.2. Operational dischargesOperational discharges relate to ship-based pollution that is not re-

stricted to accidents and can to a very large extent be effectively avoidedby the enforcement of existing regulations and the control, monitoringand surveillance of maritime traffic (Ferraro et al., 2009). Vessel-relatedoperational pollution include releases of bilge water from machineryspaces and ballast water of fuel oil tanks. Although environmental reg-ulations for these operations are quite strict, operational dischargesare still frequent (EMSA, 2008; OSPAR, 2010a; Hassler, 2011).

The chronic pollution resulting from operational discharges is moredifficult to assess than that caused by large catastrophic spills. Dis-charges are not limited to oil but also involve other contaminants suchas detergents and cleaners, lubricants, and chemicals from refrigeratingequipment and fire-extinguishers. The inventory of pollutants emittedcan be valuable for evaluating their environmental impacts. However,this issue seems to have been practically overlooked byboth researchersand the shipping industry and information on this regard is rather lim-ited (Honkanen et al., 2013; McLaughlin et al., 2014). A survey conduct-ed in 1988 in the North Sea found that the concentrations of certaintarget chemicals due to operational discharges from chemical tankerswere extremely low and lower than prior the implementation ofAnnex II of MARPOL (Hurford et al., 1990). A later study, however,found very high dissolved concentrations of nonylphenol ethoxylatesfar offshore the Dutch coastal zone and related them to theuse of surfac-tants to clean cargo ships at open sea (Jonkers et al., 2005).

The United States Environmental Protection Agency (US EPA) ana-lyzed different operational discharge types from various vessel classesand provided a list with the detected pollutants that may have the po-tential to pose a risk to human health or the marine environment. Thisstudy found that copper and arsenic represented the greatest environ-mental concern in vessel discharges. Other contaminants includedmetals such as aluminum, iron, manganese, cadmium, lead and zinc,semivolatile organic compounds (SVOCs) such as bis(2-ethylhexyl)phthalate, VOCs such as benzene, and long- or short-chain nonylphenoland octylphenol ethoxylates (USEPA, 2010).

3.1.3. Emissions from antifouling paintsThe accumulation of organisms on ships' hulls can reduce the perfor-

mance of vessels and increase fuel consumption and so, biocides havebeen traditionally used in antifouling paints to prevent the growth ofpotential fouling organisms. However, the biocide release from a ship'shull can be harmful to non-target organisms. For many years the mostwidely used active component in antifouling paints was the organotintributyltin (TBT), which has an endocrine disrupting effect, particularlyon shellfish (Dafforn et al., 2011). A global prohibition on the applicationof TBT-paints was ratified in 2008, although TBT impacts are still of con-cern in some localized European coastal ecosystems (Sousa et al., 2009).

Biocides such as copper(I) salts, mainly in the form of copper oxide(Cu2O) and copper thiocyanate (CuCHNS), have been the main alterna-tives to TBT inmany antifouling coatings. Copper losses at sea from coat-ings of moving ships are considered as a significant and increasinganthropogenic source of copper to the aquatic environment (OSPAR,


2010a). Although much less toxic than TBT, copper may also negativelyaffect organisms at concentrations higher than physiologically neces-sary and its risks on the marine ecosystem should not be neglected(Karlsson et al., 2010; Ytreberg et al., 2010).

Cu-based paints have now been supplemented by additional bio-cides, called “booster biocides”, to improve their performance againstcertain more resistant algal fouling (Cima and Ballarin, 2012). The listof potential booster biocides used or promoted as agents in antifoulingpaints is considerable, but not all compounds are marketed (Price andReadman, 2013). Typical candidates of the tin-free booster biocidewide-ly used in recent years include non-metallic organic compounds (irgarol,diuron, sea-nine 211, dichlofluanid, chlorothalonil, thiram, busan, densil,pyridine-triphenylborane, capsaicin, econea, medetomidine andtolylfluanid), and organometallic compounds (copper pyrithione, zincpyrithione, zineb and maneb) (Dafforn et al., 2011; Diniz et al., 2014).

However, precise current information about quantities and types ofthemost used biocides around the world or even at national territory isscarce. A picture of booster biocide distributions and concentrations inEuropean waters emerged from the Assessment of Antifouling Agentsin Coastal Environments (ACE) project, which ran from 1999 to 2002(ACE, 2002; Readman, 2006). Of these products, diuron presented thehighest mean concentrations, with maximum levels reported in north-western Europe. Irgarol 1051 was found at lower mean concentrationsthan diuron, with Mediterranean coastal environments the most con-taminated. Other biocides, such as chlorothalonil, dichlofluanid andsea-nine 211, were sporadically encountered, principally in the Medi-terranean Sea, but sometimes at very high concentrations (Price andReadman, 2013).

Information on the marine concentrations and toxicity of the mostcommon biocides in antifouling paints is provided in the Supplementa-ry Material, Table S1.

3.2. Mariculture

The European Commission is intending to boost growth of theaquaculture industry as a means to meet future seafood demandsand as a potential source of employment and economic development(EC, 2012). Even though significant progress has been made to im-prove the aquaculture's environmental performance, the rapid ex-pansion of this sector can also have a significant impact on thesurrounding environment. Farmers use a wide range of chemicalsto enhance productivity and growth, including antibiotics to controldisease, pesticides to control parasites and algae, and antifoulants(Guardiola et al., 2012).

The highest amounts of chemicals used in aquaculture are associ-ated with intensive finfish production, mainly salmonids, and seabass and sea bream, sectors which have experienced the highestgrowth rate in recent years. The pressures associated with the culti-vation of shellfish are generally considered to be less severe. As by farthe majority of marine finfish farms culture the fish in sea cages, anychemical that may be used is discharged into the open water andsediments (EEA, 2011). Many of these chemicals may exert toxico-logical effects on non-target organisms. However, accurate informa-tion on the quantities of chemicals actually applied within theaquaculture industry is not always available, thus the compilationof a complete and quantitative list of chemicals is basically unattain-able. Nevertheless, there are some overviewswhich provide valuableinformation (e.g. GESAMP, 1997; Costello et al., 2001; Johnston andSantillo, 2002; OSPAR, 2009a). It has been seen that the use ofchemicals varies between different types of aquaculture farms, be-tween countries and between individual operations within thesame country (Rodgers and Furones, 2009). Therefore, it is unclearwhich chemicals would be the most important to screen for in aqua-culture environments and aquaculture products (Burridge et al.,2010; Grigorakis and Rigos, 2011).

3.2.1. Medicinal productsFish farmers must have access to a variety of properly authorized

medicines to ensure animal health. There are only 14 medicinal prod-ucts fully authorized and approved for use in sea farming in Europe(amoxicillin, azamethiphos, bronopol, cypermethrin, emamectin ben-zoate, florfenicol, flumequine, hydrogen peroxide, oxolinic acid, oxytet-racycline, sarafloxacin, sulfadiazine:trimethoprim, teflubenzuron, andtricaine methane sulphonate). The number is limited because of thehigh cost of development and licensing for a small market relative toother markets for pesticides and medicinals. Furthermore, the list ofpharmaceuticals licensed varies a lot among countries. Despite the reg-ulatory possibilities, it appears that many compounds are still legallyavailable and even if not fully licensed, they can be used on an off-label basis (Daniel, 2009; Rodgers and Furones, 2009).

Information on the main medicinal products in the marine aquacul-ture industry is summarized below and data on their marine concentra-tions and toxicity are provided in the SupplementaryMaterial, Table S2.

3.2.1.1. Antibiotics. Despite the use of antibiotics having been reduceddrastically in recent years following the introduction of vaccines and im-proved husbandry practices, antibacterial therapy still remains the lastrecourse to combat bacterial fish infections in aquaculture (OSPAR,2009a; EEA, 2011). Antibiotics commonly used include oxytetracycline,oxolinic acid and flumequine, although the pattern of medicinal use inaquaculture is constantly changing (Marine Institute for SWRBD,2007). Typically, antibiotics are administered orally with feed but directinjection and/or immersion in antibiotic bath solutions are also used. Inboth cases, these substances, their metabolites and/or their degradationproducts are likely to pass to the surrounding environment. For exam-ple, in intensive fish farming, approximately 70–80% of the antibacte-rials given as medicated feed pellets end up in the environment(Ferreira et al., 2007). Concerns regarding the use of antibiotics in aqua-culture are multiple, including the contamination of indigenous, non-target organisms and the induction of drug resistance in microbial andother wild populations (Grigorakis and Rigos, 2011; Samuelsen et al.,2014).

3.2.1.2. Parasiticides. Several antiparasitic agents are routinely used fordelousing farmed fish, including pyrethroids such as cypermethrinand deltamethrin, organophosphates such as azamethiphos, as wellas benzamide and avermectins such as flubenzurons and emamectinbenzoate. The compounds are either dissolved in water and used forbath treatment or administered orally via the feed (Olsvik et al.,2014; Samuelsen et al., 2014). Following the treatment period,these therapeutants are released into themarine environment eitherdispersed throughout the water column or in particulate form viauneaten feed, fecal material and in soluble form in urine. Thereforeboth water column and seabed potentially receive inputs of activeingredients and metabolite from such treatments (Telfer et al.,2006). Studies under laboratory conditions suggest that negative im-pacts from anti-louse treatments, if they occur, are minor and will berestricted in spatial and temporal scales. However, field data are lim-ited (Haya et al., 2005; Burridge et al., 2010).

3.2.1.3. Anesthetics. Anesthetic are used in aquaculture to assist immobi-lization of brood animals during egg and milt stripping and to sedateand calm animals during transportation. They are used infrequentlyand in low doses, thus limiting potential for environmental damage(Burridge et al., 2010). However, there is a paucity of information re-garding their tolerance and associated behavioral responses by fish(Readman et al., 2013). Most common anesthetic agents include benzo-caine, quinaldine and tricainemethane sulphonate (MS-222) (GESAMP,1997; Costello et al., 2001).

3.2.1.4. Disinfectants. Disinfectants are widely used in aquaculturethroughout the world to maintain hygiene throughout the production


cycle and, sometimes, to treat disease (GESAMP, 1997). Formalin andiodophors are the most common disinfectants in European aquaculture(Costello et al., 2001). However, there are very few data available re-garding the presence and effects of disinfectants in themarine environ-ment and there appears to be no regulations regarding their use(Burridge et al., 2010).

3.2.2. Food additives and contaminantsThe addition of additives to fish and crustacean feeds represents a

non-intrusive method by which a variety of absorbable compoundsmay be delivered to cultured stock. Food additives include artificialand natural pigments, such as astaxanthin and canthaxanthin, vaccines,antioxidants such as butylated hydroxytoluene and ethoxyquin, andimmunostimulants such as vitamins C and E. These compounds are un-likely to cause any effects in the environment and are generally recog-nized as safe (GESAMP, 1997; Fisheries and Oceans Canada, 2003).

It is well accepted that the main source of metal pollution in sedi-ments under fish cages are fish food formulations which are supple-mented with various metals to fulfill complete mineral requirementsof farmed fish (Grigorakis and Rigos, 2011; Simpson et al., 2013). Themetals in feed mainly include copper, zinc, iron, manganese, and otherslike cobalt, arsenic,magnesium and selenium (CIESM, 2007; Burridge etal., 2010).

Farmed fish diet is also a potential source of other contaminantssuch as polychlorinated dibenzodioxins (PCDDs), polychlorinateddibenzofurans (PCDFs), polychlorinated biphenyls (PCBs), PAHs,hexachlorobenzenes (HCBs), polybrominated diphenyl ethers(PBDEs), and organochlorine pesticides like DDT resulting from theconsumption of feed (Grigorakis and Rigos, 2011). Several studieshave showed higher concentrations of these toxic substances infarmed than wild fish (Cole et al., 2009). This may result in the redis-tribution of contaminants in the surrounding marine environment.For example, the sediments collected close to Scottish marine fishfarms have been found to be slightly contaminated by PCBs, but atlevels unlikely to give rise to unacceptable biological effects(OSPAR, 2009a; Russell et al., 2011).

3.2.3. Antifouling biocidesAquaculture in general, and the fish farming industry in particular,

suffers significantly from the effects of biofouling. Applying a biocidalcoating on the submerged structures and net-cages is still commonlyused in aquaculture. With the elimination of TBT, anti-fouling paintshave been mostly based on copper, usually in the form of copperoxide. Hence, the sediment close to the fish farms have been found toexhibit high copper levels, often higher than the recommended sedi-ment quality guidelines (Willemsen, 2005; Simpson et al., 2013). Theextensive use of anti-fouling biocides is also considered a potentialsource of metal accumulation in cultured fish, which have been associ-ated to lethal or sub-lethal effects and the immediate immune defensemechanism of the exposed fish (Nikolaou et al., 2014).

Other antifouling compounds widely used in aquaculture includechorothalonil, copper pyrithione (CuPT), dichlofuanid, sea-nine 211, di-uron, irgarol-1051, TCMS pyridine, zinc pyrithione (ZnPT), and zineb(Guardiola et al., 2012).

3.3. Offshore activities

3.3.1. Offshore oil and gas exploration and productionThe highest risks of chemical contamination due to offshore activi-

ties are generally related to the oil and gas industry. Rock cuttingsfrom drilling (drill cuttings) and formation water brought up with thehydrocarbons (produced water) are considered the largest sources ofcontaminants entering the sea from regular offshore oil and gas opera-tions (Bakke et al., 2013). There is limited monitoring of quantitiesand consequent inputs tomarine ecosystems, and consequently a great-er transparency with regard to the chemicals used as well as a better

knowledge of the possible environmental impact of offshore effluentshas beenpointed out as a priority (Roose et al., 2011). This becomes par-ticularly relevant considering that the European oil and gas industry isshifting to deeper regions of the ocean, where even less is knownabout effects on the species that inhabit them andwhere proper regula-tory frameworks to minimize damage to the environment can be morecomplicated (Science for Environment Policy, 2012).

3.3.1.1. Drilling waste. The drilling of wells generates significant quanti-ties of wastes. This waste is made up of drilling fluids and the cuttingsgenerated during drilling. Drilling fluids (drilling muds) are used to liftformation cuttings to the surface, control subsurface pressures, lubricatedrill strings, bottom hole cleaning and cooling, and maintenance andstability of uncased sections of the borehole (Holdway, 2002; Breueret al., 2004). Drill cuttings are particles of crushed rock produced bythe grinding action of the drill bit as it penetrates the earth (Neff, 2005).

The major components of drill muds are a base fluid (water, oil, oranother organic fluid, such as esters, ethers, or olefins) and a weightingmaterial, often barite (bariumsulfate). Various additives are also used toimprove the technical performance of the mud, and their use varies be-tweendrilling operations and in the course of the drilling. The chemicalsused as additives include viscosifiers, biocides, corrosion inhibitors,shale inhibitors, emulsifiers, lubricants, wetting agents, surfactants, de-tergents, salts and organic polymers, and are mostly classified asPLONOR (substances considered to pose little or no risk to the environ-ment) by OSPAR (Neff, 2005; Bakke et al., 2013). While N1000 productsare available for formulating drilling fluids, the total number of ingredi-ents in most drilling fluids is in the range of 8–12 (Holdway, 2002). Inaddition, several metals are present in most water-based drillingmuds, being arsenic, barium, chromium, cadmium, copper, iron, lead,mercury, nickel, and zinc the metals of greatest concern, taking into ac-count their potential toxicity and/or abundance in drillingfluids (ARPEL,1999; Neff, 2005).

Drill cuttings contain, besides formation solids, small amounts of liq-uid and solid drilling mud components. The amounts of drilling fluidsolids that remain attached to cuttings vary depending on the grainsize of the crushed rock from the strata being drilled. Cuttings producedduring drilling with water-based drilling muds may contain smallamounts of petroleum hydrocarbons (Neff, 2005). Moreover, the pres-ence of radionuclides in both liquid and solid wastes generated duringoil and gas production is well known.With respect to drill cuttings, im-portant radionuclides are 226Ra, 228Ra, and others that form from theirdecay, e.g. 210Pb (Breuer et al., 2004).

In practice, operational discharges today only take place from dril-ling using water-based drilling muds, since the discharges of oil-basedmuds and synthetic muds were gradually phased out from mid-1990sfor environmental reasons (Neff, 2005; Bakke et al., 2013). Even thoughthe environmentalmonitoring has not found effects of water-based cut-tings on benthic fauna at a distance of N250m from the drilling installa-tions, and that the effect mechanism is mainly physical stress, it is stilluncertainwhether the discharges can have undesirable chemical effectsover a prolonged period (Research Council of Norway, 2012; Bakke etal., 2013).

Drill cutting accumulations (cuttings piles) represent another anthro-pogenic perturbation on the seabed. Before regulations, extensive dis-charges of oil-based cuttings resulted in large waste deposits ofpolluted drilling cuttings beneath and around the platforms, causingwidespread sediment contamination and effects on the benthos. Sincethe discharges no longer contain oil, the recovery of local sedimentfauna has been substantial and nowadays it is rare to find effects onfauna N500 m from the piles (Research Council of Norway, 2012;Bakke et al., 2013). However, the old, polluted cuttings piles still exist.For example, in the North Sea, 79 large (N5000 m3) and 66 small(b5000 m3) cutting piles have been identified and their total hydrocar-bon concentration has been measured in the range of 10,000 to600,000 mg/kg (Bakke et al., 2013). Hydrocarbons within the cuttings


piles seem to remain relatively unchangedwith time. Other constituentssuch as heavymetals are also likely to remainwithin the cuttings pile un-less physical disturbance from platform activities, storms, or trawlingprovoke the dispersion of material and enhance the leakage of contami-nants (Breuer et al., 2004). Moreover, biodegradation and other diage-netic processes in the piles over the years might have produced otherpotentially toxic compounds such as complex esters and organic acidswhich until recently could not be identified analytically. Therefore,older cuttings piles might represent a source of episodic and continuouscontamination in the marine environment (Bakke et al., 2013).

3.3.1.2. Producedwater. Producedwatermeanswater which is producedin oil and/or gas production operations and is a combination of forma-tion water, condensation water and re-produced injection water; italso includes water used for desalting oil. Produced water representsthe largest waste stream generated in the offshore production activities,in both volume and quantity of pollutants. As an example, in the OSPARmaritime area, producedwater has been found to represent N90% of thetotal amount of oil discharged to the sea from offshore oil and gas activ-ities (OSPAR, 2014a).

The composition of produced waters may vary significantly fromwell to well and over time in individual wells (Roose et al., 2011). Thiswide variation does not help itself to the establishment of routinemon-itoring and region specific studies might be needed to address the envi-ronmental risks from its discharge (Neff et al., 2011). OSPAR provides alist of the naturally occurring substances usually being analyzed to char-acterize produced water samples along with their established PNECs(Agreement 2014–05). Typical compounds include PAHs and other dis-solved hydrocarbons (e.g. benzene, toluene, ethylbenzene, and xylene),alkylphenols, heavy metals (e.g. barium, chromium, lead, and nickel),organic acids (e.g. formic and acetic acid), and radioactive isotopessuch as 226Ra and 228Ra. In addition, large numbers of specialty additives(treatment chemicals), such as scale (mostly based on phosphonates,phosphate esters or acrylic acid copolymers) and corrosion inhibitors(generally complex mixtures of amides, amines, amine salts,imadazolines, and quaternary ammonium salts), biocides, antifoams,and flocculants are also regularly discharged from produced waters(ARPEL, 1999; Meier et al., 2010; Neff et al., 2011). For reasons of com-mercial confidentiality, the specific chemicals and quantities containedin oilfield products are not generally made public and only the legallyrequired health and safety data are normally specified onmaterial safe-ty data sheets (McCormack et al., 2001).

Most of these chemicals are usually present at very low concentra-tions and, upon discharge to the sea, the level of contamination can bereduced due to natural dispersion, volatilization and biodegradationprocesses. Consequently, any large-scale negative biological effects ofproduced water at offshore installations are likely to be minor, withthe possible exception of bioaccumulation in shellfish (Neff et al.,2011; Lourenço et al., 2015). Nonetheless, there is still need for a betterunderstanding of the producedwater's constituents, environmental fateand potential effects, particularly chronic, low-level exposure to the dif-ferent chemicals (Neff et al., 2011; Bakke et al., 2013). Due to the sheervolume discharged, producedwater is still considered amajor source ofmarine pollution and there is considerable concern over its ocean dis-posal (Meier et al., 2010; Brooks et al., 2011).

3.3.1.3. Accidental spills. Accidental spills from offshore installations in-clude well blowouts, acute or slow releases from subsea equipmentand pipelines, structural failure or damage of production or pumpingplatforms, and platform-tanker loading activities. Oil pollution from oiland gas installations, especially well blowouts, can differ substantiallyfrom ship-sourced oil spills, principally due to the potentially largerquantity and prolonged release of fresh oil (EMSA, 2013b). As saidabove, chemical dispersants can be used as a response to an oil spill. Dis-persant usage has been an issue of renewed interest for the Europeannational administrations in recent years, in particular following the

explosion of the Deepwater Horizon oil platform in the Gulf of Mexicoin 2010, where emergency responders applied extensive amounts ofthe chemical dispersants Corexit 9500A and Corexit 9527A (Grahamet al., 2016).

Furthermore, the effects of more frequent small spills are not to beunderestimated. In the OSPAR area, in addition to planned discharges,1205 tonnes of chemicals were accidentally spilled in 2012. The major-ity of the chemicals spilled were on the OSPAR PLONOR list (84%) orwere chemicals not containing candidates for substitution (12%), andof the 455 spills in 2012, over 80% were b1 tonne (OSPAR, 2014a).

3.3.1.4. Decommissioning of disused installations. Once oil or gas fieldsreach the end of their operating life, the issue of decommissioning(essentially a reclamation process) arises. The offshore oil and gas in-dustry is facing the prospect of de-commissioning thousands of installa-tions in the coming decades. In some parts of the world the issue isalready pressing, particularly in the OSPAR region decommissioning isexpected to peak during 2010–2020 (OSPAR, 2010a). There seems tobe a fine line between decommissioning and dumping (Hamzah,2003). Nowadays, there are many different regulatory frameworksaround the world relevant for decommissioning operations, but thereis no clear consensus on what best practices should be (Testa, 2014;Techera and Chandler, 2015).

A proper decommissioning policy must consider the environmentalhazards of the process. All removal options will result in ecosystem dis-turbance and subsequent localized impacts, including release of con-taminants from re-suspended sediments or from the drill cuttingspiles accumulated on the seabed (Schroeder and Love, 2004; OGP,2012). If the installation is to be retained in situ, it could also result ina source of marine pollution since any structures left over will eventual-ly corrode and leach contaminants such as PCBs, residual oil, heavymetals and other toxic substances (Lakhal et al., 2009; Adedayo,2011). When it is not possible to remove the lower parts of a platform,for example concrete substructures and the footings of the largeststeel installations, the parts left in place may form artificial reefs(OSPAR, 2010a). However, this action has also repercussions. A typicallarge steel installation is composed of 90% steel, 2% aluminum and0.3% copper. When the structure ultimately deteriorates, the surround-ing environment will be exposed to chemicals like iron, lead, cadmiumand mercury (Adedayo, 2011).

3.3.2. Other offshore installationsPotential risks due to the operation of subsea cables or pipelines cer-

tainly exist, but mainly linked to the mobilization of contaminants heldwithin the sediment when the seabed is disturbed and therefore onlyexpected for heavily contaminated areas. Release of contaminantsfrom the cable itself can only occur if cables are not removed after termi-nation of service and iffluid-filled cables are used (Meißner et al., 2006).Major concerns related to offshore structures for renewable energy gen-eration (wind, wave and tidal energy devices) are the increase of noiselevels and risks of collisions, while pollution by chemicals might be aproblem due to the increased vessel traffic and potential spills or fromseabed sediments disturbance (Bailey et al., 2014). There is also risk ofpollution during routine operation and maintenance activities, includ-ing leaching of chemicals from antifouling paints and accidental spillsof hydraulic fluid or lubricant oil from operational devices (Bonar etal., 2015). Organic ormetal pollutants associatedwith the infrastructureused for electrical signals, and metals associated with sacrificial anodesmight be also released into surrounding marine waters. Therefore, thecontaminants potentially discharged from marine renewable energydevices includemetals such as aluminum, copper, and zinc, booster bio-cides such as diuron and irgarol, hydrocarbons such as BTEX and PAHs(e.g. naphthalene), and also chemicals used as dielectric fluids such assilicone fluids (e.g. polydimethylsiloxane, PDMS), mineral oils (e.g.naphthenic oil), biodiesel, natural vegetable oils (e.g. soybean, canola,corn, and sunflower oil), and synthetic esters (e.g. MIDEL 7131),


coolants such as ethylene and propylene glycols, and electrolytes suchas sulfuric acid (Bejarano et al., 2013; California State LandsCommission, 2013; Copping et al., 2015).

3.4. Seabed mining

Seabedmining is concernedwith the retrieval ofminerals occupyingthe ocean floor. Commercial scale seabed mining operations are up tonow limited to shallow water, mainly to the extraction of aggregates(sand and gravel) for the construction industry and nourishing beaches,and other material such as tin, phosphates, iron ore and diamonds.Commercial scale mining activities in deeper water (i.e. beyond 500 mwater depth) has never been conducted. However, the rapid expansionin the capabilities of underwater technology aswell as concerns over se-curity of supply of raw materials for industry have encouraged miningcompanies to consider what the sea can provide. The number of con-tracts granted to explore minerals on the seabed has increased greatlyin latest years and commercial exploitation is planned to begin in thenear future (Jaeckel, 2015). By 2020, deep seabed mining could provide5% of the world's minerals, including cobalt, copper and zinc and thiscould rise to 10% by 2030 (EC, 2012).

Seabed mining has, therefore, the potential for new mineral re-sources, but also raises serious environmental concerns. The deep seahosts a unique and rich biodiversity, which has been suggested to playsignificant roles in the ocean processes. The environmental conse-quences of mining in this hostile and vulnerable environment may beconcealed and difficult to monitor (Clark and Smith, 2013; Sarkar etal., 2013). In addition to the destruction of habitats and other directphysical impacts, marine organisms near the miner can be exposed tocontaminant plumes generated by the physical activity of the miningmachine, the movement of the unconsolidated sediment drape, andthe dewatering process. The spatial distribution of the plumes will de-pend on themining activity and the strength of surface and bottom cur-rents, so there is the potential for toxicity over widespread geographicalareas (Coffey, 2008; Clark and Smith, 2013). Along with normal opera-tions, the accidental hydraulic fluid leaks, fuel spills during transfers atthe site of the production support vehicles, ore spills during transfer tobarges and bulk ore carriers, and accidental collisions may also resultin the release of chemicals into the marine environment (Hunter andTaylor, 2014).

Research about chemical impacts and toxicity resulting fromdeep sea mining is very limited, so it is difficult to predict what ef-fects will occur and how significant they will be (Zhou, 2007). Oneof the primary concerns is related to the release of metals (e.g. zinc,copper, cadmium, and mercury), which could lead to toxic effectson pelagic biota, including bioaccumulation through the food chain,and affect the surrounding seafloor habitats (Boschen et al., 2013;Ramirez-Llodra et al., 2015). In fact, it has been said that mining activi-ties can introduce heavy metals in the deep sea in concentrations ex-ceeding 4000 times the limits considered to be safe (Coffey, 2008).Other chemicals are often used during ore processing to aid in concen-trating the ore and therefore, can be emitted into the aquatic environ-ment. Process chemicals include flotation agents such as xanthatesalts and Lilaflot (a mixture of 60–80% N-(3-(tridecyloxy)propyl)-1,3-propane diamine and 20–40% N-(3-(tridecyloxy)propyl)-1,3-propanediamine acetate), and flocculants such as polyacrylamide. These sub-stances are toxic to aquatic organisms but, in general, very little isknown about their effects on marine wildlife (Olsvik et al., 2015;Ramirez-Llodra et al., 2015). This kind of information is essential to de-velop sustainable guidelines and regulations for managing deep seamining activities (Hunter and Taylor, 2014). Deep sea mining is not di-rectly addressed in EU law, hence theMSFD can constitute an importantmechanism for regulating the environmental aspects associated withthis activity (EC, 2014). The regulations governing deep sea mining ac-tivities depend on whether they take place inside or outside the juris-dictional waters of a sovereign state. When operating within the

Exclusive Eco-nomic Zone (EEZ) (up to 200 nautical miles from the ter-ritorial sea baseline) of a certain country, mining activities are subject tothe country's internal legislation. However, when deep sea mining op-erations occur in the international seabed (the “Area”which is the sea-bed and ocean floor and subsoil thereof beyond the limits of nationaljurisdiction), the rules of the 1982 United Nations Convention on theLaw of the Sea (UNCLOS) apply. Compliancewith these rules is checkedby the International SeabedAuthority (ISA), an intergovernmental bodyestablished under UNCLOS.

3.5. Dredging of sediment and dumping at sea

Dredging and dumping are regulated human activities that con-tribute to the input of sea-sourced substances. Estuarine and coastalmarine sediments are frequently contaminated with a suite of metalsand organic compounds from both historical and current inputs. Re-suspension of bottom sediments by dredging processes has beenproven to cause large scale increases in water column contaminantlevels, which has been linked to community-level and sub-lethal re-sponses in exposed populations of invertebrates and fish (Hedge etal., 2009; Katsiaras et al., 2015). Despite the potential environmentalhazards, dredging is essential tomaintain ports and harbors and nav-igational access, and so dredging operations have increased in sever-al countries worldwide (Wasserman et al., 2013).

Ocean dumping is defined as “any deliberate disposal of wastes orother matter from vessels, aircraft, platforms or other man-madestructures at sea”. Dumping, therefore, is always intentional, anddoes not include accidental discharges or operational discharges,which are regulated under MARPOL (Frank, 2007). Much of the ma-terial removed during dredging activities requires disposal at seaand may also harm the marine environment (Parnell et al., 2008).EU legislation does not deal specifically with dredged material, al-though a number of EU Directives (namely theWaste Framework Di-rective, Natura 2000 areas under the Birds and Habitat Directives, theWFD, and the MSFD) have an impact on the management of dredgedmaterial, either direct or indirectly. Today, the deliberate disposal ofdredged sediments into the ocean is essentially regulated by theConvention on the Prevention of Marine Pollution by Dumping ofWastes and Other Matter 1972 (London Convention) and its 1996Protocol (London Protocol).

Guidelines for the management of dredged material in Europe areprovided on a regional level by RSCs. These guidelines include theneed for the chemical characterization of the dredged material inorder to provide decision points that determine whether sedimentscan be disposed of at sea. The chemicals recommended to be consideredare trace metals and metalloids (arsenic, cadmium, chromium, copper,lead, mercury, nickel, and zinc), PCBs, PAHs, and organotin compounds.Other substances that may also require analysis, based upon local infor-mation of sources of contamination or historic inputs, include otherchlorobiphenyls, organochlorine pesticides, organophosphorus pesti-cides, triphenyl tin (TPhT), other anti‐fouling agents, petroleum hydro-carbons, PCDDs/PCDFs, and phthalates (OSPAR Agreement 2014-06).

Although properly managed dredged material seems to representvirtually all material dumped into the ocean today (OSPAR, 2009b), al-ready-dumped toxic material, as well as some permitted, unregulatedor illegal dumping activities, can still represent a substantial environ-mental hazard (Frank, 2007).

3.5.1. Emissions from historical dumping sitesDumping of the most toxic materials is banned by the London Con-

vention but in the past all types of wastes were ocean dumped, includ-ing contaminated dredged material, industrial wastes and sewagesludge. Although there are no complete records of the volumes andtypes of materials disposed in marine waters prior to 1972, someareaswith decades of uncontrolled dumping becamedemonstrably pol-luted with high concentrations of PAHs, acid chemical wastes (e.g.


titanium dioxide waste), heavy metals, and organic chemical wastes(Vethaak and Van Der Meer, 1991; Leipe et al., 2013; Liehr et al., 2013).

Radioactivewastes,munitions and chemicalweaponswere also rou-tinely dumped into the sea worldwide previously and until the prohibi-tion with the London Convention (OSPAR, 2010b, 2010c).

3.5.1.1. Radioactive wastes. A first global inventory of radioactive wastedisposal at sea was issued in 1991 by the International Atomic EnergyAgency (IAEA) and subsequently updated in 1999 and 2015. This reportprovides data on the date and location of the disposal operations aswellas the type, number and weight or volume of the disposed containers.Yet, the information is heterogeneous due to the different ways inwhich the countries had kept their records and, unfortunately, detailedinformation on radionuclide composition of the waste is generally lack-ing (IAEA, 1999, 2015).

In the OSPARhigh seas areas of theNorth-East Atlantic, it is assumedthat approximately 98% of the disposed radioactive waste consisted ofbeta and gamma emitters, mainly tritium (3H) and others such as 90Sr,134Cs, 137Cs, 55Fe, 58Co, 60Co, and 14C. The rest 2% were alpha-emittersand consisted principally of plutonium and americium isotopes(OSPAR, 2014b). In the Baltic Sea region, several dumpings of radioac-tive waste have been officially confirmed, but there is no further infor-mation available on radionuclide composition (HELCOM, 2003). Thereis no official record and no environmental evidence of radioactivewaste dumping into the Black Sea (IAEA, 1999). In the Mediterranean,detailed information on historical dumping of radioactive waste is diffi-cult to access or absent (Coll et al., 2012).

The impact of this radioactive contamination on themarine environ-ment and humans is still unclear. The scientific research conducted dur-ing and for some years after cessation of the dumping operationsshowed that calculated doses to man were negligible, although robustconclusions about environmental impacts could not be drawn due tothe lack of baseline data on the benthic biology (HELCOM, 2003;OSPAR, 2014b). A recent study has reported deviations from expected238Pu/239, 240Pu activity ratios and 240Pu/239Pu atom ratios in sedimentsamples from the Kara Sea, suggesting the possibility of leakages of ra-dioactive material from dumping containers into the environment(Gwynn et al., 2016). At present, dumping grounds are not routinelysubject to radiological assessment, although the need for such regularmonitoring is under discussion (OSPAR, 2014b).

3.5.1.2. Munitions and chemical weapons. Chemical weapons and con-ventional munitions were commonly dumped in European watersafter World Wars I and II, principally in the Baltic Sea (Roose et al.,2011; Bełdowski et al., 2016). Large amounts were also dumped in theOSPAR Maritime Area (OSPAR, 2010c) and in the Mediterranean Sea,particularly in the Southern Adriatic, which was also more recently af-fected by the Balkans War (Frank, 2007). Warfare agents constitute,therefore, a class of legacy contaminants, but inmany cases, accurate in-formation on the quantities, locations and current condition of thedumpsites is unavailable (Benn et al., 2010).

Chemicals originating from warfare materials can eventually leakinto the sea and spread from the sites of disposal over more distantareas. Leakage of toxic compounds from the corroded munitions hasbeen recently suggested in dumpsites of the Baltic (Missiaen et al.,2010; Baršienė et al., 2014) and Adriatic Sea (Amato et al., 2006; DellaTorre et al., 2013), and there are predictions that corrosion will lead tomaximal leakage periods in the middle of the 21st century (Roose etal., 2011). Furthermore, the increasing demand for marine activitiessuch as offshore wind farms and pipelines as well as changes in fishingpractices raise new issues since these activities could also alter undis-turbed munitions.

About 70 different chemicals have been used or stockpiled aswarfareagents in the 20th century (CHEMSEA, 2013). A comprehensive list doesnot exist, as the composition of material in many dumping incidents isunknown (Beddington and Kinloch, 2005). Conventional munitions are

believed to represent the main proportion of the dumped material andthey consist primarily of nitroaromatics explosives, such as TNT (2,4,6-trinitrotoluene) and DNT (2,4-dinitrotoluene), and nitramines explo-sives, such as RDX (hexahydro-1,3,5-trinitro-1,3,5-triazine). Besides theexplosive material, conventional ammunition consists almost complete-ly of metals, mainly copper, iron, nickel, tungsten, tin, lead, aluminumand zinc, and also contains propellants, plasticizers, and stabilizers,such as the nitrate esters nitroglycerin and nitrocellulose (Liebezeit,2002; Lotufo et al., 2013; Smith et al., 2013). Large numbers of incendiarymunitions (e.g. containing white phosphorus) are known to have beenalso frequently disposed of at sea. Contamination by white phosphorusstemming from incendiary devices has been reported in many coastalareas around the world, including the OSPAR maritime area, the Balticand the Mediterranean Seas (Amato et al., 2006; OSPAR, 2010c;HELCOM, 2013a).

Regarding chemical weapons, the main compounds known orsuspected to have been dumped into the sea are blistering agents,most-ly sulfurmustard gas (yperite) and arsenic-containing compounds suchas adamsite (diphenylaminechloroarsine), Clark I (diphenylarsine chlo-ride), Clark II (diphenylarsine cyanide) and arsine oil (a technical mix-ture of Clark I (35%), phenyldichloroarsine (50%), trichloroarsine (5%),and triphenylarsine (5%)). Other compounds considerably dumped in-clude nerve agent organophosphates (e.g. Tabun), choking agents (e.g.phosgene), and lachrymatory agents (e.g. α-chloroacetophenone)(Sanderson et al., 2012; HELCOM, 2013a; Baršienė et al., 2014). Manyof these weapons contain hazardous additives, such as aromatic andchlorinated solvents (e.g., benzene, chlorobenzene, tetrachlorometh-ane) (HELCOM, 2013a). Despite this, little is still known about their per-sistence, bioaccumulation and adverse effects on humans and biota(OSPAR, 2009c; Sanderson et al., 2012). Table S3 compiles data on con-centrations and toxicity of main warfare agents thought to be dumpedat sea at one time or another.

3.6. Other sea-based activities

Other activities can be included as potential sea-based sources ofcontamination. Several accidents at sea resulting in actual or potentialrelease of radioactivematerials have been reported (IAEA, 2015). Artifi-cial radionuclides can also be introduced into the marine environmentby under-water testing of nuclear weapons (Benn et al., 2010).

Furthermore, potentially polluting shipwrecks, both recent and relic,can represent a hazard for themarine environment (Alcaro et al., 2007).Between 2.5 and 20.4 million metric tons of oil have been calculated tobe contained in sunken wrecks worldwide, which might be released asthe shipwrecks deteriorate (Landquist et al., 2013). Deterioration andcorrosion of the aged structures can also lead to the leakage of othertoxic substances, mainly arsenic,metals such as cadmium, copper, chro-mium, lead, mercury, and zinc, and other compounds like PCBs, asbes-tos, biocides, PVC, and radioactive waste (Alcaro et al., 2007; Annibaldiet al., 2011; Sprovieri et al., 2013).

4. Results and conclusions

Table 1 presents the resulting list of contaminants identified fromthe literature as potentially released into the marine environmentfrom sea-based anthropogenic activities. It includes 276 substanceswith their CAS identification number and major sea-based sources: 19metals/metalloids, 10 organometallic compounds, 24 inorganic com-pounds, 204 organic compounds, and 19 radionuclides. The offshoreoil and gas operations contribute to this list with the highest numberof substances, followed by shipping and mariculture activities (Fig. 1).Moreover, although most substances have been linked to only onesea-based activity, there are cases in which they are associated withmore than one source, thus increasing their potential risks.

However, it is necessary to bear in mind that this manuscript is notintended to be a risk assessment. While all substances in the list are

Table 1List ofmain chemical substances entering themarine environment from sea-based sources and their consideration under relevant legislative/regulatory frameworks andRSCs in Europeanmarine waters.

(continued on next page)


Table 1 (continued)


Fig. 1. Percentage of the total number of identified substances linked to each sea-basedsource.


likely to be introduced into the marine environment, this does not im-plicitly mean that all of them have to be regarded as being very hazard-ous or discharged at levels of concern. The degree of concern must beevaluated in terms of a combination of factors, mainly the temporaland spatial scales over which the compound can be found togetherwith their toxicity and adverse effects onmarine organisms. Yet, this lit-erature review has evidenced either a lack of information on many ofthese crucial aspects or the difficulty to get access to it (as seen in TablesS1, S2, and S3).

The environmental safety information for many chemicals in usetoday is seldom available, in particular for those used in the aquacultureand offshore industries. Even when data are accessible, the same prod-uct can be marketed under different names and the active ingredientsmay not be registered. This makes it exceedingly hard to keep uniformrecords, to perform large-scale comparisons and to assess the potentialeffects on the aquatic environment. Furthermore, quantitative data onpatterns of use and release of chemicals are also very difficult to obtain.For many substances, only the fact of use is typically documented, espe-cially in the case of warfarematerial, which is usually steeped in secrecyand confidentiality.With the increased use of the sea and its resources, aregularly updated inventory of the types and quantities of chemicals re-leased is essential to understand the relative influence of each humanactivity and how they accumulate and interact to impact the marineecosystems.

What can be learnt from this experience is that, despite the growingattention to the risk linked to the emission of harmful substances intothe sea, and the fact that monitoring activities are likely conducted ata regular pace, much of the generated information is still hard to access,not systematically analyzed, and, hardly ever, the object of re-analysis toproduce a synthetic view. This illustrates the commendable effortsmade by the scientific community to convey important messages tothe structures devoted to environmental monitoring and protection aswell as that the contributions are generally related to episodic and iso-lated efforts. Thus, improving information gathering and exchange toensure that it is as useful and accessible as possible is equally importantthan improving the observational strategies and the quality of the data.

Clearly, this is not meant to be seen as a closed and definite list ofmarine-relevant contaminants but as a consolidated starting pointwhen approaching the management of chemical pollution from coastalto open sea environments. For this purpose, the Table 1 also provides anoverview of environmental policy instruments and frameworks in placeto oversee and regulate these substances within the EU. Hence, it can beseen that several WFD substances are not tackled under any RSC pro-gramme and vice versa. Furthermore, only four WFD PS (PAHs, cadmi-um, mercury, and lead) are also prioritized in the four Europeanmarine regions, while other substances are shared by the differentframeworks but in a varying way. Therefore, it can be ascertained thatthe level of harmonization across Europe with regard to the contami-nants selected bydifferent regional frameworks is rather low. Neverthe-less, as seen in Table 1, there are a number of other European orinternational legislations and regulations as well as recommendations,agreements and programmes at national or regional level, which direct-ly or indirectly deal with most substances or group of substances. It is

important, though, to notice that nearly one-third of the identifiedchemicals appears not to be considered under any framework in place.

In summary, this review contributes to the challenging endeavor ofgathering and integrating information already accessible onmarine-rel-evant contaminants. On one hand, it can help decide where to prioritizeefforts in order to access and mobilize additional data. On the otherhand, by bringing up the existing legal and regulatory landscape, itcan help understandwhich substances are currently covered at Europe-an and/or regional level and which substances might require furthercontrol and/or monitoring actions. This compilation should providesupport for setting-up of approaches to marine pollution monitoring,including hotspots screening.

Supplementary data to this article can be found online at http://dx.doi.org/10.1016/j.marpolbul.2016.06.091.

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