JournalofEnvironmentalSciences2010221218331331839Distributionofpolybro - PDF document

1 JournalofEnvironmentalSciences2010,22(12
JournalofEnvironmentalSciences2010,22(12)1833…1839DistributionofpolybrominateddiphenylethersanddecabromodiphenylethaneinsurfacesedimentsfromFuheRiverandBaiyangdianLake,NorthChinaGuochengHu,ZhenchengXu,JiayinDai NineteensurfacesedimentsamplescollectedfromBaiyangdianLakeanditsin”owingriver(FuheRiver)inNorthChinawereanalyzedforpolybrominateddiphenylethers(PBDEs)anddecabromodiphenylethane(DBDPE).TheconcentrationsofPBDEsandDBDPEinsedimentsrangedfrom5.5to300.7nggdryweight(dw)and1.1to68.2nggdw,respectively.Theirlevelsinsedimentsin IntroductionPolybrominateddiphenylethers(PBDEs)are”ameretardantsthatarewidelyusedinplastics,paints,electronics,textiles,foam,andrubber.Asaresult,theypresentinmanycommercialandhouseholdproducts,suchascomputers,televisions,furniture,carpetsandtoys(Haleetal.,2002,Chenetal.,2009).ThreecommercialPBDE *Correspondingauthor.E-mail:xumq@ioz.ac.cn Inviewsoftheirbioaccumulationpotential,environ-mentalpersistence,andpotentialhumanandwildlifetoxicities,PBDEsareincludedamongstsixenvironmen-tallyhazardoussubstancesintheEuropeanUnion(EU)issuedDirective2002ECregardingtherestricteduseofcertainhazardoussubstancesinelectricalandelectronicequipment(RoHS).Thetechnicalpenta-BDEandocta-BDEproductswerebannedin2004bytheEUaswellasbysomestatesoftheUnitedStates(Renner,2004). GuochengHuetal.Vol.22 DBDPEwasintroducedasanalternativetodeca-BDEintheearly1990s(Kierkegaardetal.,2004).Withincreasingregulationandphasing-outofproductionofthecommer-cialusageofPBDEs,itisexpectedthattheproductionandusageofDBDPEwillbepredominantinthecomingfuture(Ricklundetal.,2008).ToxicologicalstudiesshowedthatoraltoxicityofDBDPEinratswaslow,duetopoorbioavailability,largemolecularweightandlogetal.,2002).IthasbeenreportedthepresenceofDBDPEintheenvironment.DBDPEhasbeendetectedinairneartheGreatLakes(VenierandHites,2008),sedimentsfromsewagetreatmentplant(Kierkegaardetal.,2004;Ricklundetal.,2008),andhousedustfromUSA(Stapletonetal.,2008).DBDPEhasalsobeenfoundinbenthic“sh(Lawetal.,2006),waterbird(Luoetal.,2009),terrestrialmammal(Huetal.,2008)andtreebarkfromNorthAmerican(ZhuandHites,2006).However,thepotentialsourcesandenvironmentalbehaviorsofDBDPEwerenotclear.Itisgenerallyacceptedthatsedimentsconstituteasinkforhydrophobiccompoundsinaquaticenvironment.Thecontaminationofsedimentsmayposeanunacceptablerisktoaquaticorganisms,wildlifeandhumans(Eljarratetal.,2004).Thestudyofsedimentsisanimportantstepinmappingpossiblepollutionsourcesandexposurepathwaysthatmakespollutantsbioavailabletosediment-dwellingorganisms.PBDEsandDBDPE,sharingsimilarstructures,willveryquicklybindtoorganicrichsuspendedparticlesinthewatercolumnandaretransportedtothebottomsediments.Sedimentationwillplayimportantrolesintheprocessofcontaminantstransport.BaiyangdianLakeisthelargestnaturalfreshwaterbodyintheNorthChinaPlain.Thelakeconsistsofmorethan100smallandshallowlakeslinkedtoeachotherbythousandsditcheswithsurfaceareaof366kmandacatchmentof31,200m.FuheRiverisamajorin”owingriverofBaiyangdianLakewith63kmlength,”owingthroughBaodingCity.BaiyangdianLakereceivesnutrientinputsfromFuheRiver.BoththeBaiyangdianLakeandFuheRiverarestronglyin”uencedbyhumanactivities.Inaddition,BaiyangdianLakeislikelytoplayanimportantroleintheSouth-to-NorthWaterDivisionProjectunderconstructionbecauseofitsgeographiclocation.Previ-ousstudiesshowedpersistentorganicpollutants(POPs)suchasorganochlorinepesticide(OCPs),polychlorinatedbiphenyls(PCBs)andpolycyclicaromatichydrocarbon(PAHs)weredetectedinthesediments(DouandZhao,1998;Huetal.,2010).However,therehavebeenfewstudiesofthedistributionanddepositionofPBDEsandDBDPEinthesedimentsfromBaiyangdianLakeandFuheRiver.Inthepresentstudy,BaiyangdianLake,aheavilyindust

2 rializedplainareawithextensivelyanthropo
rializedplainareawithextensivelyanthropogenicactivities,wasselectedforthe“rsttimetostudytheenvironmentalPBDEsandDBDPEcontamination.ThestudydetectedPBDEsandDBDPElevelsandassessedtheirspatialdistributioninthesurfacesedimentsfromBaiyangdianLakeandFuheRiver.Inaddition,thestudyprimarilydiscussedtheemissionsourcesofPBDEsandDBDPEintheregionsofBaiyangdianLake.1Materialandmethods1.1SamplecollectionandmaterialNineteensurfacesampleswerecollected,ofwhichsevenfromBaiyangdianLakeandtwelvefromFuheRiver,inAugust2007andMarch2008,usingastainlesssteelgrabsampler(Fig.1).Thetop5-cmlayerofsedimentswasscoopedintosolvent-rinsedaluminumcontainersus-ingaprecleanedstainlesssteelscoop.Allsamplesweretransportedonicetothelaboratory,andwerestoredat…20°Cuntilfurtheranalysis.PBDEsstandardmixtures,containingBDE28,47,66,85,99,100,138,153,154,183,197,203,196,205,206,207,208,and209,wereobtainedfromAccuStan-dard(USA).C-PCB141andC-PCB208wereobtainedfromCambridgeIsotopeLaboratoriesInc.(USA).DB-DPEand2,2,4,4,5-pentachlorodiphenylether(CDE99)wereobtainedfromWellingtonLaboratories(Canada).AllsolventsandreagentsusedintheextractionandcleanupprocedureswereARgradeandallorganicsolventswerere-distilledusingglasssystem.Neutralsilicagel(80…100mesh)wasextractedwithamixtureofdichloromethaneandmethanol(1:1,)for72hrusingaSoxhletextractor.Upondryingunderroomtemperature,silicagelwasbakedat180°Cfor12hr.Sodiumsulfatewasbakedat450°Candstoredinsealedcontainers.1.2SampleextractionandcleanupSedimentsampleswerefreeze-dried,ground,andho-mogenizedbysievingthroughastainlesssteel80mesh(0.2mm)sieveandstoredinglasscontainersat…20°Cuntilextraction.TheextractionprocedurewassimilartothatdescribedforthedeterminationofPBDEsinsediment Fig.1Mapofstudyareaandsamplingsites.S1…S12fromFuheRiver,S13-S19fromBaiyangdianLake. No.12Distributionofpolybrominateddiphenylethersanddecabromodiphenylethaneinsurfacesediments (Maietal.,2005).AfterspikewithC-PCB141andCDE99,sampleswereextractedwithamixtureofacetoneandhexane(1:1,)for48hrwithaSoxhletextractor.Activatedcoppergranuleswereaddedtotheextraction”asksduringtheextractiontoremoveelementalsulfur.Concentratedextractswerecleanedona10mmi.d.silicacolumnpackedwithneutralsilica(8cm,3%deactivated),44%sulfuricacidsilica(8cm),andanhydroussodiumsulfate(1cm).Thecolumnwaselutedwith30mLhexane:dichloromethane(1:1,).BDE118andBDE128wereaddedasinternalstandardforanalysis.1.3InstrumentalanalysisSampleanalysiswasperformedwithaShimadzuModel2010gaschromatograph(GC)coupledwithaModelQP2010massspectrometer(MS)(Shimadzu,Japan)usingnegativechemicalionization(NCI)intheselectedionmonitoring(SIM)mode.ADB-XLBcapillarycolumn(300.25mmm)wasusedfortheseparationoftri-tohepta-BDEcongeners(BDE28,47,66,85,99,100,138,153,154,and183).Forocta-todeca-BDEcongeners(BDE196,197,203,205,206,207,208,and209)andDBDPE,aDE-5HTcapillarycolumn(15m0.25mmm)wasused.DetailsoftheGCtemperatureprogramandmonitoredionsweregivenelsewhere(Maietal.,2005;Huetal.,2008).Splitlessinjectionof1Lofsamplewasconductedwithanautosampler.Methanewasusedasachemicalionizationmoderatinggasatanionsourcepressureof2.4Paandheliumasthecarriergasata”owrateof1mLmin.Theionsourceandinterfacetemperaturesweresetto200and280°C,respectively.Quanti“cationwasperformedusinganinternalcalibrationmethod(“vetonineconcentrationlevels).1.4Qualitycontrolqualityassurance(QCInstrumentalqualitycontrol(QC)includedregularin-jectionofsolventblanksandstandardsolutions.Therelativepercentdierencewerelessthan20%foralltargetsanalyses.Formethodsqualityassurance(QA),threeproceduralblanks,triplicatespikedblanks,andtrip-licatespikedmatriceswereanalyzed.OnlytracelevelsofBDE47andBDE99weredetectedinblanksandthemeanconc

3 entrationsweresubtractedfromthoseinsampl
entrationsweresubtractedfromthoseinsamples.Therecoveriesof11PBDEcongeners(BDE28,47,66,85,100,99,154,153,138,183,and209)rangedfrom65.7%to82.0%and67.4%to79.7%inspikedblanksandmatrixspikedsamples,respectively.ThemeanrecoveriesofDBDPEinspikedblanksandmatrixeswere87.6%and103.6%,respectively.Thesurrogatestandardrecoveriesin19sampleswere83.2%…103.8%forC-PCB141,86.1%…109.0%forCDE99,and54.6%…117.4%forThelimitofdetection(LOD),de“nedasasignalratio(SN)of3,rangedfrom0.1to2.2pggdryweight(dw)forPBDEsand2.9to4.4pggdwforDBDPE,respectively.1.5DataanalysisForsampleswithconcentrationbelowLOD,zerowasusedforthecalculations.Alllevelsarepresentedasadryweightbasis.BDE66,85,138,and196werenotdetectedinallthesedimentsamples.PBDEsisde“nedasthesumofthe14mostfrequentlydetectedcongeners(BDE28,47,99,100,153,154,183,197,203,205,206,207,208,and209).ThedierencesofcontaminantsinsedimentsbetweenBaiyangdianLakeandFuheRiverwereanalyzedusingTwo-SampleKolmogorov-Smirnov-Test.Principalcomponentanalysis(PCA)wasconductedtoassessthecompositionsofPBDEcongeners.PCAwithvarimaxrotationwasperformedusingSPSS11.5software(SPSS,USA).Thelevelofsigni“cancewassetatthroughoutthisstudy.2Resultsanddiscussion2.1ConcentrationConcentrationsofPBDEsandDBDPEinthesurfacesedimentsamplesaregiveninTable1.PBDE1isde“nedasthesumoftri-tohepta-BDEs,includingBDE28,47,99,100,153,154,and183.Theconcentrationsofocta-BDE,nona-BDE,anddeca-BDEinsedimentsofFuheRiverwereintherangeof0.13…6.39,0.27…2.92,5.07…34.9,and11.8…292.7nggdw,respectively.TheconcentrationsofPBDE1,octa-BDE,nona-BDE,anddeca-BDEinsedimentsofBaiyangdianLakewereintherangeof0.05…5.03,0.44…0.75,2.10…4.19,and4.35…19.3nggdw,respectively.ThelevelsofPBDEsinFuheRiverweresigni“cantlyhigherthanthoseinBaiyangdianLake(0.05).PBDEsandDBDPEinFuheRiverandBaiyangdianLakewerelikelyoriginatedfromacombi-nationofpointandnon-pointsourcesandatmosphericdeposition.Largeamountsofindustrialactivities(suchasdismantlingelectronicproducts,cablesandwires,re“neryoils,andchemicalplants)werelikelyresponsibleforthehighconcentrationsofPBDEsandDBDPEinsedimentsinFuheRiver.TheprimitiveelectronicwastesrecyclingactivitieswereobservedalongtheFuheRiver.AmongTable1PBDEsandDBDPEconcentrationsinsedimentsfromFuheRiverandBaiyangdianLakein2008 Concentration(nggdw) FuheRiverBaiyangdianLake 0.00…0.34(0.09)0.00…0.07(0.01)0.03…1.58(0.58)0.01…0.78(0.13)0.02…1.92(0.60)0.01…2.68(0.39)0.01…0.23(0.07)0.002…0.58(0.09)0.02…1.03(0.27)0.01…0.47(0.08)0.01…0.94(0.18)0.002…0.41(0.06)0.04…1.82(0.54)0.01…0.04(0.02)Sumtri-tohepta-BDE0.13…6.39(2.33)0.05…5.03(0.78)0.07…1.57(0.31)0.17…0.23(0.19)0.11…1.13(0.34)0.14…0.19(0.16)0.10…0.26(0.20)0.14…0.38(0.22)Sumocta-BDE0.27…2.92(0.86)0.44…0.75(0.57)1.43…14.6(4.51)0.91…1.95(1.34)2.69…17.1(5.57)0.85…1.75(1.24)0.82…5.07(2.17)0.30…0.48(0.37)Sumnona-BDE5.07…34.9(12.3)2.10…4.19(2.95)11.8…292.7(102.6)4.35…19.3(10.4)16.1…68.2(31.3)1.10…5.29(2.78) Meanvalueispresentedinparenthesis. GuochengHuetal.Vol.22 thesedimentsamplesfromBaiyangdianLake,thehighestconcentrationofPBDE1(5.03ngg)wasobservedatS15(Wangjiazhai),whichpossiblyrelatedtothelargeamountofanthropogenicactivities(Fig.2).Thiswasnotsurprising,becauseWangjiazhaiwassurroundedbythesmallerlakeswithtourismblooming.AmongPBDEscongeners,BDE209wasthemostpre-dominant.TheaverageconcentrationsofBDE209were1…2ordersmagnitudehigherthanthoseofPBDE1insedimentsfromFuheRiverandBaiyangdianLake.The“ndingswereconsistentwithpreviousreportedresults,whichindicatedthatBD

4 E209wasthedominantcompo-nentofPBDEsdetec
E209wasthedominantcompo-nentofPBDEsdetectedinthesedimentsfromPearlRiverDelta,SouthChina(Maietal.,2005;Zhangetal.,2009). Fig.2DistributionofPBDE1,BDE209,andDBDPEinsurfacesedimentsfromFuheRiverandBaiyangdianLake.ThehighestconcentrationoftotalPBDEsinsedimentwasfoundatS2,BaodingCity(307.2nggdw),whichisalarg-erindustrialcitycomprisingautomobile,textile,buildingmaterials,electronicproductsmanufacturingfactories.ThelowerconcentrationsofPBDEsinsedimentswerefoundinBaiyangdianLake,rangingfrom7.4to23.7nggdw,whichpossiblyrelatedtobefarfromindustrialandurbanactivities.DBDPEwasfoundinallthesedimentsamples.TheconcentrationsofDBDPEinsedimentsrangedfrom16.1…68.2nggdwforFuheRiverand1.1…5.3nggdwforBaiyangdianLake.ThelevelsofDBDPEinFuheRiv-erweresigni“cantlyhigherthanthoseofBaiyangdianLake(0.05).ItcanbeconcludedthatDBDPEwasbeingusedandemittedinNorthChina.Generally,theBDE209ratiocanbeusedtoassesstherelativeusageofthetwobrominated”ameretardants(BFRs).Inthisstudy,theratioofDBDPEBDE209wasbelow1formostsedimentsamples,exceptforS1andS12.AlthoughDBDPEwasmarkedasreplacementfordeca-BDE,deca-BDE(BDE209)stillwasthemajorbrominatedcompoundsinBaiyangdianLakeregions.ThecorrelationanalysisbetweenDBDPEandBDE209wasconductedforallthesamples(Fig.3).Signi“cantcorrelationbetweenDBDPEandBDE209wasfoundinthepresentstudy(TheresultsindicatedthattheemissionsourcesofDBDPEweresimilartodeca-BDE.DBDPE,asanalternativeofBDE209,wasusedinapplicationssimilartodeca-BDE.These“ndingswereconsistentwiththoseforsedimentsamplesfromSouthChina(Zhangetal.,2009).2.2GeographicalcomparisonsPBDEsarepredominantlyincorporatedintoplasticpolymersinelectroniccomponents(Bayenetal.,2003)andthepresenceofPBDEsinotherlocationsaroundtheworldaregenerallythoughttobederivedfromdischargesofwastesassociatedwiththeproductionordismantlingofelectronicequipment(Shietal.,2009).PBDEshavebeenmeasuredinriver,lake,marinesedimentsfromdiregionsoftheworld(Table2).TheconcentrationsofPBDEsinthepresentstudywerecomparedwiththose Fig.3RegressionanalysesbetweentheconcentrationsofDBDPEandBDE209insedimentsfromFuheRiverandBaiyangdianLake. No.12Distributionofpolybrominateddiphenylethersanddecabromodiphenylethaneinsurfacesediments Table2PBDEsandDBDPEconcentrations(nggdw)insedimentsfromdierentregionsworldwide Concentration(nggdw) Tri-tohepta-BDE Qingdaonearshore,ChinaYangetal.,2003PearlRiver,SouthChinaMaietal.,2005DongjiangRiver,SouthChinaMaietal.,2005MichiganLake,USASongetal.,2005Spanishcoast,SpainEljarratetal.,2005YangtzeRiverDelta,ChinaShenetal.,2006GreifenseeLake,SwitzerlandKohleretal.,2008BohaiSea,NorthChinaWangetal.,2009WesternScheldt,NetherlandsKierkegaardetal.,2004Sewagesludge,CanadaMcCrindleetal.,2004Sewagesludge,GermanyRicklundetal.,2008PearRiverDelta,SouthChinaZhangetal.,2009E-wastearea,SouthChinaShietal.,2009FuheRiver,NorthChinaPresentstudyBaiyangdianLake,NorthChinaPresentstudy …Žnotavailable.reportedforseveralotherregions.PBDE1concentra-tionsinsedimentsmeasuredinthepresentstudywerecomparabletothosereportedforMichiganLake(Songetal.,2005),GreifenseeLake(Kohleretal.,2008),Spanishcoast(Eljarratetal.,2005),BohaiSea(Wangetal.,2009),Qingdaonearshore(Yangetal.,2003),andYangtzeRiverDelta(Shenetal.,2006),however,lowerthanthoseofPearlRiverandDongjiangRiver(Maietal.,2005).Theconcentrationsofocta-BDE,nona-BDE,anddeca-BDEinsedimentsfromFuheRiverandBaiyangdianLakewerehigherthanthosefromGreifenseeLake(Kohleretal.,2008).TheconcentrationsofBDE209insedimentsfromFuheRiverandBaiyangdianLakewerelowerthanthosefromPearlRiverandDongjiangRiver(Maietal.,2005).ThehighconcentrationofPBDEsinthePearlRiverDeltamaybeduetotheintensivemanufacturingofelectronicproductsinthoseareas.Fewpublicationsareavaila

5 blefortheconcentrationsofDBDPEinsurfaces
blefortheconcentrationsofDBDPEinsurfacesediments.TheconcentrationsofDBDPEinsedimentfromFuheRiverandBaiyangdianLakewerecomparabletothoseofsedimentfromWesternScheldt(Kierkegaardetal.,2004),sewagesludgefromCanadian(McCrindleetal.,2004),however,lowerthanthoseofsedimentsfromPearRiverDelta(Zhangetal.,2009),e-wasteareaofSouthernChina(Shietal.,2009),andsewagesludgefromGermany(Ricklundetal.,2008).HighconcentrationsinsedimentsfromChinaandsewagesludgefromGermanymaybeattributedtotherapiddevelopmentofelectronicandautomobileindustry.ThePearRiverDeltawasoneofthelargermanufactureregionsofelectronicproducts.2.3PBDEcongenerspatternandPCAThecompositionalpatternofsedimentsfromFuheRiverwassimilartothatofBaiyangdianLake.BDE209wasthemostpredominantamongallthePBDEcongenersinthestudyarea(Fig.4).ThecontributionsofBDE209tothetotalPBDEsrangedfrom85.7%to97.3%insedimentsfromFuheRiver,and79.4%to92.1%inBaiyangdianLakewiththeexceptionofonesample(S15),inwhich,PBDEshadarelativelylowabundanceofBDE209(35.6%).The Fig.4PBDEscompositionspatterninsedimentsfromFuheRiverandBaiyangdianLake.“ndingsagreewiththefactthatdeca-BDEmixtureaccountformostofthetotalBFRsproductioninNorthChina,whichwassimilartothereportsintheotherregionsofChi-na(Maietal.,2005).Thetotalcontributionsofocta-BDEandnona-BDEtothetotalPBDEswere1.3%and3.9%forFuheRiver,and4.9%and9.6%forBaiyangdianLake,respectively.Theregressionanalysisbetweendeca-BDEandthesumofocta-BDEandnona-BDEwasconductedforallthesamples.Signi“cantcorrelationwasfoundinthepresentstudy(0.05).Theresultsindicatedthatdeca-BDEmixturepossiblycouldbetheoriginalsourcefortheocta-BDEandnona-BDEinthestudyarea.Thecompositionalpatternforlowbrominated”ameretardantsisillustratedinFig.5.Amongthelowbromi-natedcongeners(PBDE1),BDE47andBDE99were GuochengHuetal.Vol.22 thepredominantcompounds.ThetotalcontributionsofBDE47andBDE99tothePBDE1rangedfrom24.4%to64.9%(averagevalue,52.1%),and33.5%to68.9%(averagevalue,44.1%)insedimentsfromFuheRiverandBaiyangdianLake,respectively.BDE47andBDE99werethemajorcongenersinthetechnicalpenta-BDEmixture,comprised87%ofPBDE(LaGuardiaetal.,2006).ThecompositionalpatternsofFuheRiverandBaiyangdianLakeweresimilartothecompositionsofmajorpenta-BDEcommercialmixtures(LaGuardiaetal.,2006).Clearly,penta-BDEcommercialmixturewasanothermajorfor-mulausedinBaiyangdianLakeregioninadditiontothetechnicaldeca-BDEmixture.Althoughtheusageofpenta-BDEandocta-BDEwasociallybannedin2006inChina,the“ndingsindicatedthatFuheRiverandBaiyangdianLakewerepossiblysubjectedtothecontaminationofpenta-BDEmixtureinthepastyears.Principalcomponentanalysis(PCA)wasusedtofurtherexaminethepotentialsourcesofPBDEsinsedimentsfromFuheRiverandBaiyangdianLake(Fig.6).ThePCAclassi“edthePBDEcongenersintotwodistinctclusters,clusterI(lowbrominatedcongeners)andclusterII(highbrominatedcongeners),accountingfor58.2%and Fig.5penta-BDEspatternsinsedimentsfromFuheRiverandBaiyang-dianLakecomparedwiththoseofBromkal70-5DEandDE-71technicalmixture.Dataofcommercialformulationsweredrawnfromtheliterature:Bromkal70-5DEandDE-71from(LaGuardiaetal.,2006). Fig.6Principlecomponentanalysis(PCA)scoreplotforsedimentssamplesfromFuheRiverandBaiyangdianLake.22.5%ofvariationinPBDEconcentrations,respectively.ItwasnoticeablethatPBDEcongenersweredistributedtoerentprincipalcomponentsaccordingtothemolecularweightsorbrominenumbersofsubstitution.TheseresultsindicatedthatthePBDEcongenerpro“lesinsedimentsampleshavebeensubjecttocomplexenvironmentalpro-cesses,andthedierentphysical-chemicalpropertiesofthecongenersmaydictatethedistributionofPBDEsinthepresentstudy.3ConclusionsThisstudy“rstprovidedthelevelsofPBDEsandDB-DPEinthesedimentsfromFuheRiverandBaiyangdianLake,NorthChina.PBDEsandDB

6 DPEweredetectedinallthesedimentsamples,s
DPEweredetectedinallthesedimentsamples,showingtheirubiquityinthesedimentsinthestudyarea.ThehighcontaminationofPBDEsandDBDPEfoundinsedimentsamplesfromFuheRivercouldbeattributedtothehighindustrialimpactofthisarea.Thelevelsofthecontaminantsappeartobecomparabletothelevelsatcontaminatedsitesworldwide.ThecongenerpatternsofPBDEsinsedimentsfromFuheRiverandBaiyangdianLakeweresimilar,whichindicat-edthatBDE209wasthemostpredominantamongthecongeners.ThestudiesfordegradationofBDE209arerequiredtodeterminetheoriginofthecontamination.ThecompositionalpatternsindicatedthatthemajorsourcesofPBDEsandDBDPEwereprobablywastesdischargesfromBaodingCity,HebeiProvince.Furtherstudyinvolvinglargenumbersamplesareneededtocomprehensivelyin-vestigatethecontaminationoforganohalogencompoundsinFuheRiverandBaiyangdianLake,NorthChina.AcknowledgmentsThisworkwassupportedbytheNationalBasicRe-searchProgram(973)ofChina(No.2006CB403306)andtheNationalNaturalScienceFoundationofChina(No.30870311).WegratefullythankDr.FengchaoLifromHebeiUniversityforhisassistancein“eldsamplingandDr.ShejunChenfromGuangzhouInstituteofGeochem-istry,ChineseAcademicScienceforhishelpinrevisingthemanuscript.ReferencesBayenS,ThomasGO,LeeHK,ObbardJP,2003.Oc-currenceofpolychlorinatedbiphenylsandpolybrominateddiphenylethersingreenmussels(Pernaviridis)fromSinga-pore,SoutheastAsia.EnvironmentalToxicologyChemistry22(10):2432…2437.BSEF(BromineScienceandEnvironmentalForum),2003.Majorbromintaed”ameretardantsvolumeestimates.www.bsefsite.com vol2001doc(accessedChenSJ,MaYJ,WangJ,ChenD,LuoXJ,MaiBX,2009.Brominated”ameretardantsinchildrenstoys:con-centration,composition,andchildrensexposureandriskEnvironmentalScienceTechnology,43(11):DarnerudPO,2008.Brominated”ameretardantsaspossible No.12Distributionofpolybrominateddiphenylethersanddecabromodiphenylethaneinsurfacesediments endocrinedisrupters.InternationalJournalofAndrology31(2):152…160.DouW,ZhaoZX,1998.ContaminationofDDTandBHCinwater,sediments,and“sh(Carassiusauratus)musclefromBaiyangdianLake.ActaScientiaeCircumstantiae,18(3):EljarratE,DeLaCA,RalduaD,DuranC,BarceloD,2004.Occurrenceandbioavailabilityofpolybrominateddiphenylethersandhexabromocyclododecaneinsedimentand“shfromtheCincaRiver,atributaryoftheEbroRiver(Spain).EnvironmentalScienceTechnology,38(9):2603…2608.EljarratE,DeLaCA,RalduaD,DuranC,BarceloD,2005.Brominated”ameretardantsinAlburnusalburnusfromCincaRiverBasin(Spain).EnvironmentalPollution133(3):501…508.HaleRC,LaGuardiaMJ,HarveyE,GaylorMO,MainorTM,2006.Brominated”ameretardantconcentrationsandtrendsinabioticmedia.Chemosphere,64(2):181…186.HaleRC,LaGuardiaMJ,HarveyE,MainorTM,2002.Potentialroleof“reretardant-treatedpolyurethanefoamasasourceofbrominateddiphenyletherstotheUSenvironment.Chemosphere,46(5):729…735.HardyML,MargitichD,AckermanL,SmithRL,2002.Thesub-chronicoraltoxicityofethane,1,2-bis(pentabromophenyl)(Saytex8010)inrats.InternationalJournalofToxicology21(3):165…170.HitesRA,2004.Polybrominateddiphenylethersintheenvi-ronmentandinpeople:Ameta-analysisofconcentrations.EnvironmentalScienceTechnology,38(4):945…956.HuGC,LuoXJ,DaiJY,ZhangXL,WuH,ZhangCLetal.,2008.Brominated”ameretardants,polychlorinatedbiphenyls,andorganochlorinepesticidesincaptivegiantpanda(Ailuropodamelanoleuca)andredpanda(fulgens)fromChina.EnvironmentalScienceTechnology42(13):4704…4709.HuGC,LuoXJ,LiFC,DaiJY,GuoJY,ChenSJetal.,2010.OrganochlorinecompoundsandpolycyclicaromatichydrocarbonsinsurfacesedimentfromBaiyangdianLake,NorthChina:Concentrations,sourcespro“lesandpotentialJournalofEnvironmentalSciences,22(2):176…183.KierkegaardA,BjorklundJ,FridenU,2004.Identi“c

7 ationofthe”ameretardantdeca-bromodi
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