Modeling of Ecological Risks Related to SeaDumped Chem - PDF document

EnvironmentalHazardsofSea-DumpedChemicalWeaponsHANSSANDERSONPATRIKFAUSERMARIANNETHOMSENUniversityofAarhus,DenmarkPAULAVANNINENMARTINSODERSTROMFinnishInstitutefortheVeriÞcationoftheChemicalWeaponsConvention,HelsinkiYURISAVINILDUSKHALIKOVStateInstituteÒResearchandProductionAssociationÔTyphoonÕÓ,Obninsk,RussianFederationANUHIRVONENSUSANIIRANENFinnishEnvironmentInstitute,HelsinkiTINEMISSIAENUniversityofGhent,BelgiumALEXANDERGRESSPAVELBORODINUniversityofBonn,GermanyNADEZDAMEDVEDEVAYULIAPOLYAKSt.PetersburgScientiÞcResearchCenterforEcologicalSafety,RussianFederationVADIMPAKAVICTORZHURBASShirshovInstituteofOceanology-AtlanticBranch,Moscow,RussianFederationPASCALFELLERG-Tec,Belgium Doesthepost-WWIIburialatseaofchemicalweaponsstillposeahumanandenvironmentalrisk?BrewerandNakayama(2008)()pleadedforcompleteinformationconcerningthewhereaboutsofthousandsoftonnesofchemicalweaponsdisposedintheoceanstartingin1946.Currently,however,thereappearstobetheinvertedpolicyof“don’task,don’ttell”onthisissue.Scientistshavenotaskedfortheinformationaboutthedumpingandtheresponsibleagenciesfeelnopressuretoprovidetheinfor-mation.Togetherwiththedistastefulnatureofthesubjectmatterthishasledtoalackofawarenessoftheissue(Chemicalwarfareagents(CWA)representenvironmentallegacycontaminantsasproductionandsubsequentdumpingofCWAtypicallyoccurreddecadesago.DespitebeinglegacycontaminantsitisnotonlythelocationandamountsofoceandumpedCWAthatisunknownduetotheirstatusasillicit coefcients,moleculardiffusivities,andNOECs.Site-specicparametersareareaofdumpsite,currentandverticaldepthofbottomlayer,totalwaterdepth,sedimentaccumulationrate,porosity,andorganiccarboncontentinsediment(Weassumeturbulentmixingofbulkwater,advectivetransportofCWAs,andcontinuousreleaseofCWAsfromburiedshellinthesedimenttobottomboundarylayerwaterover60years.Furthermore,thebulkwaterisdividedintotwostrata:anupperlayer(5070mbelowsurface)primarilyconsistingofbrackishwaterowinginfromthenorthernandeasternpartsoftheBalticSeatowardtheNorthSea,andabottomlayer(20mabovesedimentsurface)originatingfromtheNorthSea.ItisassumedthatallthedumpedCWAsaredispersedinboththeprimaryandthesecondarydumpsite.InthissituationthetotalmixtureTUimmediatelyabovethesedimentsurface,calculatedasasumofTUforallCWAs,is0.62.TriphenylarsineistheCWAwiththehighestriskproleat0.2TU,followedbyadamsiteat0.17,ClarkIat0.086,andyperiteat0.083TU.Thisassessmentdoesnotincludeanassessmentfactor,whichistypicallyintherange5forassessmentsbasedonspeciessensitivitydistributions.Hence,therelativelowmarginofsafetybetweenexposureandeffectconcentrationswouldsuggestthatfurtheras-sessmentsarewarranted(Temporal2DEcopathwithEcosimcontaminanttracing(Ecotracer)modelswithadvectionelds()wereemployedtodescribethepotentialCWAbiomagnicationanddispersalwithintheBalticSeafoodwebdescribedby27functionalgroupsfromprimaryproducerstotoppredatorsandtrophicowsbetweenthem.ThepotentialCWAdispersalwasdescribedwitha2Dmap(1111kmgridsize)thattakesintoaccounthabitatpreferencesofdifferentspecies,aswellasincorporatingsurfaceadvectionelds.ThemostimportantBalticcommercialshwereincluded:cod(Gadusmorhuaherring(Clupeaharengus),andsprat(SprattussprattusThecontaminantconcentrationineachfunctionalgroupasafunctionoftimeandspacewascalculatedfromdirectcontaminantuptakefromtheenvironmentanduptakefromfoodaswellascontaminantlossesbydecayofthecon-taminant,metabolism,predation,othermortality,andshery).InitiallycalculatedenvironmentalCWAconcentrationswereintroducedintothemodel()andthesimulationlengthwas60y.Thebasisfortheparametrizationofthefood-webmodelliesinthefollowingtwosimplemass-balanceequa-tions(eqs1and2):LipophilicandpersistentadamsitewasmostlikelytobiomagnifyoutoftheCWAsstudied.Codwastheshwithhighestmodeledendconcentrationofadamsite.Themod-eledbiomagnication(0.613ppmbioconcentrationfactor(BCF)175)andspatialdispersal(uptocentralBalticProper)ofadamsiteincodwasclearlyhigherinthecaseofthetotalmixingofthewatercolumnthaninthestraticationscenario().Inthemorelikelyscenario,oflimitedmixingduetostratication,adamsiteconcentrationsincodandherringwerepredictedtobe0.485mg/kg(BCF39)and0.167mg/kg(BCF14),respectively,andthespatialdispersalofadamsitewaslimitedtotheSouthernBalticProper.Pelagic-onlyfeedingspratdidnotcontainanyCWAinthisscenario.TheonlyotherCWAstheoreticallytobiomagnifyintoppredatorcodwereClarkIandtriphenylarsine,butthemodelresultsdidnotsupportthis.Allmaximumconcentrationswerereachedwithin2yearsaftercontaminantexposure().ItwasconcludedbasedonEUTGDmethodsthattheindirecthumanhealthriskfromconsumingshmusclewouldbenegligible().SeetheSupportingInformation(SI)formoredata.2.GeophysicalSurveyoftheLocationandCharacter-isticsofObjectsinSediment.Theinitialhistoricalsurveyprovidedaframeworkforthesubsequentexperimentalanalysisofalocationclosertothedumpedmunitions,includingestablishmentofhotspotsforfurtherchemicalinvestigation.DetailedseismicandmagneticmeasurementswerecarriedoutattheBornholmdumpsitetoobtaininformationonthepreciselocationanddistributionofthedumpedweapons(includingtheburialdepth),toobtaininformationonthesedimentaryenvironment,andtoguidesamplingathotspots().Duringthesurveysdifferentacousticsources(boomer,sparker,parametricechosounder)weredeployedsimultaneouslyandcombinedwithmagneticmeasurements.Intotalthreelargeseismicgridswererecordedintheprimarydumpsiteareainadditiontotwosmallanddenseseismic-magneticgridsinthedumpsite(Figure1).Fourshipwrecks()wereidentiedintheprimarydumpsitearea.Thewrecksare2050mlongand510mwidewithaheightabovetheseaoorof1).Alargenumberofburiedobjectswereobservedinthetwoseismic-magneticgrids.TheseobjectsareinterpretedtobeindicationsofCWA.Thesizeoftheobjectsvariesbetween1and5m(exceptionallyupto10m).Allobjectsareburied2mbelowtheseaoor.ThelowsedimentationratesintheBornholmBasincanprobablynotaccountforthisburialdepthsomostlikelythesedimentcoverislargelyduetotheobjectssinkingintothesoftmuddysediments.Thedifferenceinobjectdensity(460objects/kminthenortherngrid,and60objects/inthesouthernpartofthedumpsite)indicatesthattheirdistributionisveryheterogeneous(Figure2).Thedifferenceinobjectdensitybetweenthetwosurveyedareasisstriking.Thismaypartlybeexplainedbythelocation.Indeed,gridSM2islocatedinthecenteroftheprimarydumpsitewhichwastheprimedumpingtarget,whereasgridSM1islocatedclosertotheboundaryoftheprimarydumpsite.Evenso,theresultssuggestthatthedistribution TABLE1ConfirmedDumpedChemicalWarfareAgentsEastofBornholm(2,5,16compounddumped(tons)Logwatersol.(mg/L)vaporpressure(mmHG)molecularweightchloroacetophenone(CAP)5151.9316350.0436154.60sulfurmustardgas(yperite)70272.416050.217159.0714284.050.42ClarkI711.54.5231.8101.55.970.0894.9610173.066390.113222.93101.51.6122919.91181.28ZyklonB0.6995,00030827.0314052.644006.46112.56Riotcontrolagent.Blisteringagent.Organoarsenicblisteringagent.Arsineoilconstitutents-organoarsenicblisteringagent.Bloodagent. othermortalitybiomassaccumulationstandingbiomassunassimilatedfood(2) VOL.xxx,NO.xx,XXXX/ENVIRONMENTALSCIENCE&TECHNOLOGY ofwarmaterialintheBornholmBasinismostlikelyveryheterogeneous,withlocallyhighobjectconcentrations.ThetotalamountofwarmaterialdumpedintheBornholmBasinamountstoover560,000objects,mainlyinvolvingartilleryshellsandaircraftbombs.Ifweassumethat50%ofthedumpedwarmaterialislocatedwithintheprimarydumpsitearea(aconservativeestimate),weobtainameanobjectdensityofroughly3000objects/km.Thisisalmostfourtimeshigherthanthehighestobjectdensitymeasuredintheseismic-magneticgrids.Thissuggeststhatalargenumberofobjects,mostlikelyshellsandmines,wereprobablynotdetectedwhiletheseobjectsmakeupasubstantialpartofthedumpedmaterial.Thelatterisprobablyaresultoftheirsmallsize(averagelength3040cm)andmass(magnetizable10kg)ascomparedtothetrack-linespacing(10m).Furthermore,anadvancedstateofcorrosionlikelyreducesthedetectabilityoftheobjects(3.SamplingandChemicalAnalysisofWaterandThesamplingforchemicalanalysisofCWAswasconductedtocoverasmuchaspossibleoftheprimarydumpsitenearthewrecks,andinthesecondarydumpsite(Figure3).Inadditiontosamplingpointswithinthedumpsites,vetransectsreaching30kmfromtheprimarydumpsitewereThetransects(TR17)allstartedfromthesouthernpartoftheprimarydumpsiteandsamplingwasmadewithapproximateintervalsof50m,100m,500m,1km,5km,10km,20km,and30km.Thesamplesweretakenwitha¨bottomcorer.Thiswasperformedover6daysat63samplingpointsduringFebruary2008.Fifty-ninesedimentsamplesand61near-bottomwatersamples(0.2mabovetheseaoor)from63samplingpointswerecollected.ThesampleswerefrozenandshippedtoVERIFINinHelsinki,Finland,forchemicalanalysisoftracesofCWAandtheirmajordegradationproducts.Sedimentandnear-bottomwatersamplesattheBorn-holmdumpsitewereanalyzedforthepresenceofCWAsandtheirprimarydegradationandoxidationproducts,usingtherecommendedoperatingproceduresforaqueousandsoilsamples().TheselectedtargetCWAincludedsulfurmustard(yperite),ClarkI,adamsite,andAsoilconstituents.TheanalysisofthesampleswascarriedoutusinggaschromatographymassspectrometryMS)andliquidchromatographytandemmassspec-trometry(LCNointactCWAwasfound,exceptonestablecomponentinAsoil,triphenylarsine,inthesediment.Severaldegradationproductsofyperite,ClarkI,adamsite,andAsoilcomponentsweredetectedinthe56sedimentsamples.Inmanysamples, FIGURE2.Verticalmagneticgradientmapsofthetwoseismic-magneticgridsSM1andSM2.Greenandredindicatepositivemagneticanomalies,purpleandblueindicatenegativeanomalies(unitnT/m).WhereasthenortherngridSM2ismarkedbythepresenceofnumerousanomalies(over440),thesoutherngridSM1showsonlyrelativelyfewanomalies(justover40).ThetwolargeanomaliesobservedingridSM1arerelatedtoshipwrecks. FIGURE3.Samplingpoints. ENVIRONMENTALSCIENCE&TECHNOLOGY/VOL.xxx,NO.xx,XXXX somedegradationproductswerenotpresentabovethelowestconcentrationlimit,butmostsamplescontainedatleastonedegradationproductthatwasquantiable.ThehighestdetectedamountsofthemeasuredCWA-relatedchemicalsinthesedimentwerebetween0.7and81250g/kgdependingupontheproximitytothehotspotsasidentiedinthegeophysicalsurvey(Figure2).Anoxidationproductofadamsitedetectedinthesedimentwas20kmawayfromthehotspotintheprimarydumpsitealongthetransect2(TR2)at1.2g/kg(dw)towardtheislandChristiansø.OnlyfourporewaterportionsofthesedimentsamplescontainedoxidationproductsoforganoarsenicCWA.NoCWA-relatedchemicalswerefoundinthenear-bottomwatersamples.ElevatedconcentrationsofAs(45mg/kg)werefoundin9samplesofbottomsedimentsintheprimarydumpsitearea(morefrequentlyintheupper05cmlayer).ThehighestAsconcentration(210mg/kg)registeredinthepeliticmudwasfoundnearthehotspotsintheprimarydumpsite(seeSIformoreinformation).4.MicrobialCommunity.Duetothefrequenthypoxicconditionsnearthebottomofthedumpsite()andtheoftensoftsediment()itislesslikelythatthereisasignicantmacrozoobenthiccommunitynearthehotspots;hence,theinitialecologicalassessmentendpointchosenwasthemicrobialcommunity.Moreover,toassesstheriskrelatingtodumpedCWAs,itisnecessarytoevaluatetheabilityoftheecosystemitselfforself-puricationofcontaminatedwaterandsedimentsmediatedbymicrobes.TheanalysisofthemicrobialcommunitywasalsousedasanindicatorofCWApresence,assomespeciesofmicrobesaretoleranttomustardgashydrolysisproducts(MGHP)(primarilythiodiglycol)andusetheseastheirsolesourceofcarbonandenergy(Yperitecanrapidlypenetratecells,andisabletoalkylateDNA,RNA,andproteinsaffectingavarietyofcellfunctions,includingalteringproteinsthathavebeencodedbyalkylatedRNAandstructurallyalteringcellmembranes().Somemicrobesarehoweverasmentionedresistanttothesetoxicmechanisms,theseorganismsoxidize,andcleaveCSbondsintheMGHP.Thehydrolysisproductsofmustardgashaveawidespectrumoftoxicactiononothermicrobiota(ThesamplestakenattheBornholmdumpsiteyieldeduptocells/mLforthetotalamountofmicrobiota,upto6.5mg/Lforbacterialbiomass,andupto4.9fortheamountofheterotrophicmicroorganisms.Atseveralstationsweobservedsignicantamountsofbacterialculturestoleranttomustardgasproducts(bothchlorinatedandnonchlorinated)inthenear-bottomwater.Thetolerantmicroorganismswerefoundatabout40%ofstationsinthedumpsitearea.OutsideofthedumpsitetheconcentrationofMGHPtolerantmicroorganismsinnear-bottomwaterwasonlybetween0%and3%(Thenear-bottomwaterheterotrophicmicroorganismcommunityinthedumpsitecomprisedupto58%micro-organismstoleranttomustardgashydrolysisproductsrepresentedbymicroorganismsof,andothergenera,withdominating.Theprimarydumpsitedemonstratedfurthermarkedreduceddiversityofmicrobiotatypicallyrepresentedby,and.Thespeciesdiversityofthemicrobialpopulationatthedumpsitewasreducedcomparedtoreferencesites,mostprobablybecauseofanincreaseinthenumberofyperite-tolerantmicroorganisms,thusindicatingthepresenceandeffectofdumpedCWAinthedumpsiteandnearthewrecks.Parallellaboratorystudies,moreover,conrmedthatMHGP-tolerantmicrobescanmineralizeMGHPevenatlowtemperatures(7C)andthuscontributetoself-puricationofthedumpsite().Theseresultssuggestthatthetimescaleofthethreatfromdumpedchemicalmunitionsundersimilarlowoxygenconditionsislimitedto100years;probablycloserto50y,bywhichtimethereleasedCWAswillhavebeensignicantlyhydrolyzedandmineralized(seeSIformoreinformation).5.HistoricalReviewandInterviews.HELCOMhasprovidedasoundbaselineofinformationontheamountsofCWAdumpedintheBalticSea.Thesedataweresupple-mentedbyareviewofthenewspaperarticlesrelatedtoCWAfromthelargestdailynewspaper(Social-DemokratenBorn-holm)ontheislandofBornholmfortheperiod1947to1992.ThemainresultofthereviewwastheconsistencybetweentheHELCOMreportsandthenewsclippingsfortheperiod.Moreover,dumpedmunitionswererevealedtohavedriftedtotheshoresofBornholm,i.e.,notallthedumpedmunitionsremaininthedesignateddumpsite.Theoutcomeoftheinterviewswithlocalexpertsandstakeholderswereprinci-pallyasfollows.MostshermenfromBornholmhavehadencounterswithdumpedmunitions;some200shermenhaveovertheyearssustainedinjuriesrequiringmedicalassistanceasaresult.ThemunitionscaughtnowadaysarecompletelycorrodedandtheCWAappearsassolidbrittlelumps.TheintervieweescannotascribeimpactsontheshstockstothepresenceofdumpedCWA.Itwasconcluded,basedontheconservativedesk-basedriskassessment,thatriskstowardtheshcommunitycouldnotberuledoutandthatasite-specicassessmentwaswar-ranted.ThegeophysicalsurveydetectedburiedobjectsandwrecksintheprimarydumpsiteandidentiedthesetobepotentialhotspotsforCWA.SeveralCWAdegradationproductswerefoundinthesedimentsamplesnearthewrecksandneartheburiedmagneticobjects(56outof59samples).Fourporewatersamplesoutof59samplescontainedorganoarsenicCWAdegradationproducts.Noneofthenear-bottomwatersamplescontainedCWAsortheirdegradationproducts.AnalysisofthemicrobialcommunitiesindicatedpresenceofCWAdegradationproducts,thatthecommunitieswereaffected,andthatthemicrobescandegradeMGHP.Thehistoricalandlocalexpertanalysissuggeststhatthemajorityofdumpedmunitionscaughtforthepast20yhavebeencorrodedandempty.TherearestillsignicantuncertaintiesregardingCWArisksintheBalticSea,specicallyduetothesizeofthedisposalsite,theratiobetweenintactburiedmunitionsandemptyshells,andthestatisticalpowerlimitationsinrelationtothesampling.Thusmoresamplesareneeded.Moregenerallythereareuncertaintiesregardingthelocation,types,andamountsofCWAdumpedglobally().Thesendingsindicatethatthereisaclearneedforthefollowing:furtherdevelopmentofthechemicalanalyticalmethods;up-to-dateecotoxicologicalandphysicochemicaldata;bettersite-specicknowledgeaboutthematerialsfateandtransportpropertiesindeepseaenvironments(improvedenvironmentalecotoxicologicalindicatorsspecicforCWA(ThemarineenvironmentisprotectedagainstdumpingofCWAviainternationalmaritimeconventions:theLondonConvention(marinedumpingofwaste),theBaselConvention(controllingmovement/tradeof[hazardous]wasteacrossinternationalboundaries,andCWA’sregulationbytheChemicalWeaponsConventionmandatingthesafedestruc-tionofallCWAby2012.Thereare,however,asmentionedaboveremainingpolicyissuesregardingassessmentofthehumanandenvironmentalrisksposedbydumpedCWA,notonlyscienticallybutalsowhomaybeheldaccountable VOL.xxx,NO.xx,XXXX/ENVIRONMENTALSCIENCE&TECHNOLOGY andwhatshouldbedoneaboutthemunitions;ultimately,thisisasite-specicquestion. 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