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ROCA a Spatial and Temporal Patterns in Concentrations of Perfluorinated Compounds in Bald Eagle Nestlings in the Upper Midwestern United States `WilliamT. Route;*" Robin E. Russell, Andrew B. Lindstro$m Mark J. Strynar,* and Rebecca L. Key" WiUsSc.onNsatiino5n4a8l0P6,akUnSeervdicS,eGeesst Lake Ioventryand Maritoring Network, Ste D, 2800 Lake Shoe Drive Est, And, US. Geological Sarey, National Wile Hlth CenG0t06Sechrrod,er Rod, Mis, Wisconsin 53711, United Sstes aUtniotnedalSisEtxeprosure Reseach Laboratory, US. Evironment Protection Agency, Research Triangle Park, North Carlin 2711, SportingInformation A`BwiSdTesRprAeCadTu:sP,ecpefrusoirsitnenscieeidn_cthheemiecnivlisro(nmPeFnC,st)endreenocyftcooanccceummuldauteetinoatnihmealr [Fass- FE= balosocd,palnadnsrforvoimn2ge6v1ibdeundceoefagtleonesst.linBgestiwneens 2s0t0u6dyaanrdea2s01r1owmetchoelulepcpteedr =e2X Midwest UnitedSatea s.Samples wre esdforlevlsof16diffePFCs.| = e esmupmerosftraelnds1f6orPthCesye an(aSlPyFtCe.sW).eoPuenrdfuloeroeocstuncisguhli1o7n5at7e0ng(/PmFlO.Sf)oratnhde && -- p7% enduonhrIoC(bFdErDSn)erweacrptnheemeLoesvsiabsuonfidSuPnElaCr,aobEeOsnS,mwaskdinFgeDoSp &(0, Foae `verehighesetinn mreun aCndodtusetwres,v moderfieooencaokemSueperriaorr, indn =[)ERT| i (iPnFSOFAC)naontdrseenvdeinnatnwaloytaels,tinecl;udainngdiPnFcrOeSa,sePsFDinSt,waondapnetrfeuso,rWooecaarngooscahadt = rr PsDhSo,u b3elcnogncsihdienreeddfPorECtweiehspomtaenltiaanl bforhrighasbiconixcumultion andfoxy u INTRODUCTION Jie FIC spo pli rvs Perorinsted compounds (PE0 C) haveoebeean,iniwordlwiede "rPolutes oifn heusmtiamnatienxgpodssubreutionsIn" paorngalte,rmtitneen]dsspeacnds Tropes pin oh wt dof ing hem cl 20 te id cle (lg), wih ei nToFnesvttieckyocfompirnogpsain cnocoakdwianreganhedfporooddupctiaoncofapgtwyiamtoeersganf,odr Co6ohta0mintthieont.r"ophicEoagoldeswperbo,vsideeseexvceelrlenttsiesnuteisn(ele,obxloPoFdCs Streiinghreipnegllnftosafmo,rtaenxdtpeso,adndeinftohremmaatnuifoanc.tTurheofirlubrreicpaontrst,s P`ietnhegrss,acnedepgigc) thatsacrelrefloartimvoenliytoeraisyngtoloocabltaoinllo7nand oa 1f9t6h0esirapenrdesne1n9co7e0i0nn5 hwuibmyhanthibnldiocoadtiwo7nesr0eo0pfubst lgniisihceada nitntchoelioamntee 3G0a6rH3ee1necttoeatcflo'nn*terasetmviiinngeawnbetddssfeocvuearngadelisnvsattruihdeiidesyoafrunodnmgess1teSimkadttiecdatotheo2om1fe7 bponteeyrstuo ds3o0frd(paPuFooOrAo)ocitnnpccautlofansstnen di(tPeodFO3)cwaidned cThoebaodctawgialriamnn2ge6idkamcnroosfsahmeonsietsotiofnNgsnoehAmericabt sidenagtehosftdrelttiavielnyslocwscdosnedritneg nbdepssttyotroensyar,cahenrscbeogadn iclilinngdhianbtihte tleos,1950s and196s cdounetatmoiniatnidosnc.rminant tSoeexspreessecosnceinrnobeystahpealtaotnedl1y970spolseeaddwiongkteosnt?udiPeFsCosntshee CPhoapunlea)tivoanss ibnacnrneeasdedi tafhteerUSD.DiTn (1d9i7c2halnordodCiaphneandyaitirnich1lo9r8o onocbuimttehsinrpsectrrt.eenhcdee, gataebseofasnedmcaunmyusltioanistsinholen Theywereremofvomethde US.LitofEndangeraend aSnid cc,csrogolntorhsu,maanndhmaenahgersinacorditnhgcccohriled fnbenheaevdioro?f RRoevckeevdd::|MMarych, 22000414 Ex2h4i0b5it PiEnfCormation on the spuial patterns snd tempers fends in APucbpliuebded:: JMoanye250,,22001144 S rr vv s ACS Publications R BESeSSp EEIuASERL wen tory 0s105en8. ect 90,58 2405.0001 Environmental Science & Technology ce| | Re J ps creute Hpwrs acon EEN s98yAartosot ears478) 988 oesEomuseunrsee5r55) 06Lg ac rtsao ne 2 9O8F L Mesu mrrospr3m.ig eeciei3ne8. ean UP ---- Tspherceisets,enehdowWeivdeirfeduien 2to007it.s" vCloncnrcaebmiltryemstionspefrosrtotnhits pthroamneae<ro1m0remdlobflopodlcnelt.o A2 spoelryperhopsylsenpeipveitalvfaosaunsesd .to pbloolodlspl.asmTanotfhibsasltdudciyglweenresetploirntgsonfroPmECthecounpcepnetrraMtiidownessti,n Grelmaosvepipcehtetemsicwaleerepdruevsiso.uslAy bsamkpedleato6f50syriFng(e3s,43neCe)dletso tOeumrporoabljecttrievnedss woefre16to.PFeCvalauantaeetsheinsphiastrepgaitotnemasnd4nfdo Lvaabcourtsationreys,, Maanpdlevwalasodw,eMeNtensdtedv by the efe3Mofd EPnEvCs.onPmleanstmla uggs implicoaftexipoosunrest humans and wide, asahmoprletsrywere kept frozen, snl delivered to an analytical BW MATERIALS fAt,NDMMEaTHOeDS we weAe 0ne0atyingos u(o1rn-o4l)gdwetoehsaandmlpel.edAfsrionmglescshameplsetwualsecshotsheeny a a i ond fom cach nestfo anys in his say (brary in 2006, "Apo Lands National Lakeshre (API); Wisconsin's Lake andomly thea). The remining samples were archived `SScuepneircioRroSiomuvtyh(eS1h(owS0rAeSaCA(NLyR)S;)SS,t)h;etthMehsesTiuopsrppteeprioStNta.tiCCorrnooawilexRNNiavoetorimoananaldl ~~ 02Tehne (W=i2s0consCi)nfoSratfueturLeabaonraaltysoersy. of Hygiene (WSLH) in Madison, W1wasthe primary analytical iboratony. To measure Rovio ves (MISS); ads portion ofPol 3 a4nofdhe miboratory varity we conduced bind studies with the hMisgishippailyRoTvoem(cPaocohkye3st&h4e)n(Fiionrge s1).weFvreomomtitod mMianye URSe:seaErncvhionTmrenngtlael PPaokt,eiNonCAgaendncyth(eUS3EMPA)Enlvabcoormatmoernytiln wneeeskisngosld,anwde. dbiromubgehdt ttohoecmcutpoiedthenesrtso,uhnadndfcoarpsoamplitngh,e Neslings wee wigheds ged banded sumpled, and placed 3iLnadbnorddaitdoenroytpkiennwonMwsptdulhneeaewwlooanocradett,oiofnlMorNefyss.ual,mtEspalrcehodmlneobstotrhliaenoglsr.ayborwaotorrkieeds binvuesticingatkthoermsesitn. Athle muepspsenremMeindtswewesret:soNnesslitngwiatgeotwhaesr perLfaobromraantcoeryl.iquiPdroccherodmuarteosg.rapEhsychtanldboermatmoarys sspeedctrhiogmh toexrwmaisnededtebymitnheedlbenyPgtCh Rofbtrhed<igghetnhetpicriamamryafusther andyatiaonndsgroafdieunpt cttoio1n6.chPrEomCa,togirnacplhuyditnog mtehsesrfeolcloonwicnegn: wWientgo+okst<e1d,1 m1L0.omfL.blopoydpfroompykthneebrycihnigse,vanode f2n0esgtnaiongges ~~ p(ePrFfSlu)o,ropbeurtlaunoorioedeaccaiodic(PcFdBA)(,PFDpAe)r,flpaeorrfobuuotraondcosdiefconnoaltee Sneerile.1T0hmei.bvoadcoasnaemrp.leWiwtahsinim1m2edbiaotfelcyoltlrctainosne,resadmptloes3 h3ecpan(cPsFfDoOnAa),tep(ePdFfHuEoSr)e,depceafnacosrloonhaetpetan(PcFcDaSi),d (pPeFrHupoAr)o, ere cntriged st 1200 rpm for 10-12 min to spate perloorohexanci acd (PFHAA), peduorohexanesalonste ase 1 en e9 e 2405.0002 Environmental Science & Technology wn (acPiFdHX(SP)F,ONp)e,rupoerlounoornooacntinccsaacldfon(sPtFeNA()FOpSe)d,laopreouocotraontoiec buctsti<mt8e0s%wewreeeabaobvoeveoforbelboewlozwereo,ro",weaankd" e"vniodeenvciedeinfc5e"70o%f tpreardleucoarncoitcid3edcon(iPcFaTcEiDdA(),PFpDedAu)r,opaenndtapneroliscoraocudnd(ePcFaPnRo)i,c cdehtaenrgmeinifed<t7o0b%e wiehreeraibnocvreeasoirngboerlodwezcer.eAainsf>ia7nn0al%gyteofwtahse Sweerde (mPeFaDsuAr)a.bleThuesin1g6 satnaalnydtaersd wWebeorsseolrecytedp.robceecdauursees tahnedy posterior estimates wre above or below ser, spectively. belEiaecvhedBtboorbaetoprreysesnetdinsltihgehlreygidoinf.erent procdures and bad W RESULTS AND DISCUSSION Sample Collection. From2006 though 2011 we called dIniffofrcmeantiolnim(iSt1s) TofaequSaInTt)i.fiAcaltlihonee(bLOoGr)atr(isesehaSduppproervtiionugs b(lToaobldepl1).asTmshefrnoummb26e1robfalsdamsapglesnfoer saclhiinanrgeaisxvasrteuddyyaeraeralsy experience with PRC analyses and used mati spikes ofknown +1"1 temberofimple or achasvariedyey clounctenetractxitoenisctitoon fafscesncya.ccRuersauclytsafnrdomsusrcohgaitbeorssptiokrSyS a1r0t TEaglae1N.ebDwilsinrlgbsutSeiaomnplAecdroasnsdStAundysAyresasfoarnPdEYCeaArsnafloyrtBead knownonlyto the study author ee LbOy`SQttawtoiinsotir5ca9mlo%Arneaolflyatsbheoersia.rtosrTaiwmeepsllveaseo, lfaetvnehdlest1ha6ebsoP evewetrE hweeerruesC rdedestpefecos crtteiadvl.el AsTlSy are 20s06" e2007 20508" 2000% 2s010 v2011 owwus 1555 6 4 0 0 iow eanrdysseisn.ciFuodeudr ianntyhesEP(PEFCDS,butPFwHeprA,oPmFiFtReAd,farnodm fPFhPAe) ~~ LUSSKNN 31 48 70 90 Bun5 ow aThnesyesfobuerccaoumsteebtuhetyedw<r1e%deotfetchteedtoitnal<P2F5C%obfurdtheen samples, PMSoSses 0nono0 1s oomm oo4m o2w ow in WPeFCtsimuastiengd trheegrsepsatiioanl dainsalrybsoitsioinn a3ndBatyeemspioarnalacthaingces "iAk=PAIpo S BandosxNatorsloLwikshoosw, LS8S= Lakwe Soupewrior vfuaemse,wpootrenktTMita2ol adcicfofuenntcfeos vdaruieabitliotyaignelbaornadtosreixc,s,amnidsifnogr SSoutAh=SCohwUNsSSto.CCrNoirx=Nap,tpieorna5l.ScCeonikc RNaetinonaa,l SMIeSnS =RMivierwsayi, macecaosuunrteemdentfsor tthhaet owbesreervbeedloPwFC4 llbevoerlastorfyr'osm LtOhQe,hrWees sborstorie by formulating log ransomed PEC levels (1) NSaamt4pilsooenasnltn KshaetbMraoidne sdbbyRyiebBcshreoitaRrd tipsivtoepunor.rAsrTew1aao3nPwdnao2dyl.sTTb3ihhn&dse4bwo=woarpayotbteiironyndasnabolfpsboeosolssayl3l fmourlticvaacrhiatiendinvoidmuaall ndeiststb(u)tio3nn.d. 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Aflrlosmam3p0le0s6 woeurganhdys0e0d8bywtehree prnidmyarsycdBbobrytotrnye, LfOroGm twhee bbboournsdoeryd:the upper imi of 1 by the lowest LOQ. baybotrhaeteoileasbo(r1at=ori1e1s4)(,1a=nd39s)a.mples from 2009 were ansyred tePrEm3Cletviemlesfwelre,m3odtemlebdyasp.afceulnetc,oatfnaifsepoacttnofcaorleaeti8o%n,. 12EanalfytefoswfeeLaabclourltatteosdrycoanneldatNieosntcionegfcAegnet.sF(oCrOc)acbhetowfetehne awnaslhfigthlyofccogmleeltteadge,wiatnhdaagef3x0dwesfencottofinlclaubdoerda)t.oryPri(owresigohrt bpaeitrweedenbboarlatrtkhrcese, tLhaeboirnattroarcilaesss canodrclntotn coccfoiscfiiecniten(tIsCCo)f nthoenincfstoirmmaatievse ofnorcmoavlaridtiesticbouetiiocnen#ts ~weNr(e00b0a0se1d).onTo3 vcoanrcseinotnrat(iConVs) w(eTrae.blereSp2)r.odTuhcoeteanad.naceonssisftoeunntd bientwiegehn aucsceodunttheforcosmpaltaitaledcoraeultaotreigornesbseitveweemnodeealg,lectaecmntoormiaesl wien bluabrodreant,oriaensd, tPheEyO,SsloanngdwiPtEhDthSesmuamdeofupll>1960P%ECof,htheexaPfFeCr nWeiarnesBtUGupTMSstWreeamconasnidderdeodwanlsl tLriekaemSunpeesrtisor onnessf,ivaensd, th3e P<3R6.CT,hehaldesCOsbsonadnadntIaCnsalyt5e0s.8v0arainedd mwoitrheinwiadbeolrytwoirtyh CCVCs `"wneeiigghhebdoresr.wiThhesptaitmielbwyeiegrhttsoorfyofneec;twalal sotfhoernmeusltawt3eerde3 7a1n5d5,ICTChersaengirnegsfsromar~e0.s1i2mi1l0e0t9o.7 oatnhdeeC_Visneodfbo1r2s.t3ortyo craannddoomm lvafrtia,blaenNd z)thwehperreecijsison ptahreammeetaene 1l/0o. Woef ttahne aconmapaersisofnosundwhaet eextlraregmeelydifllocwenccoesncehnatveratbieeonn,s fHouondw.erfo,r havbeur chaiinnsEfvorry0100000 vcalauteiionntsheancdhicnsarwdaesdustehde f0itest2i5m0a0t0e wmhsilteCsCosmeinlaaubrorsattoryy (m6e8s%s)rewmeentasbodvief0er8e0d iinndicmaatginnigthudte,, pWoestesrieorcdsisciobnuvteirognesnocfe twhienegstthiemaGteedlmpaanraRmuebtienr cstoaetfisitciicnatnsd. theWyetrfeonudneddsitnrotnhgeesvaimdeencdiere(ctthieon9.5% CI did not include eto) oRfhFaitt vanaallyssiswionngcsltiivmeartyes"fcroodmat"heWieeacrocnhidcoatledmo3deGloogdannessts teshttimeavteedlcoofeftfihceieentafnoryasgewfeoer PafEfNctAedwabny e11s7 i(95a%geCIth=e echsedcuksosn omfodoeblsesrevnesditiPviFtOyS(v=alue0s31f)r.om all iborstories 3 3 i1n0d2i-c1t3n5g)ananindcrfeoarsePwiFthUgewsfor1t2h3se(9tw5o% aCnIaly=tes10w0hi-l1e2t7h)e int"eTrhvealBsay(eCs1i)an3frtarmueewoprrkobaallloiweesd uosf0chianntgeerprient ltehveelcsreodfibalne c3oedffeiccliiennet fwoirthPFaBgAewiins0th7i7s (an9a5ly%teC.1 =Ot0h6e0r-1P0EC0s) isndpipceaatriendg n29y0e%.oWfethceonpocsltuedreidorthcestrimwaatses"swterornegsebovveiordofbeeclhonawngcsee"reoi,f udniafffercetnecde lbiykel3y66i,nclTuhdee thmecbhiaoancicsummsulaitnivvoelvpedroinpaegreortfecilaaetceshd "moderte vince of chinge" if 380% but <90% of the yt, sxposure time, and the development of excretory ws acorns i eet 1 2405.0003 Environmental Science & Technology Po] TNaebileog2.sExtimated Geometric Mesn and Range (ng/mL) in Concentsions of 2 PFC n Blood Plan of Bd Egle ie TRE == omTdeig) CTno Gy" = Fe FIonse Wo 0 wwm un beGoaiy mmOnGw Drea meessam)o emsae wedoamD Die ime o@i@e mmpm wews mw0w mew uw mei ww WWoorn Tow mDbsauGGau7nDD lUaRGgGeme mskpnD Ammdnoedmimispw SpOG(wDw ebwDD anleeeGawGnRnMBneO 5ss8suG0io%d6aw0bn TTIhohn AlOMnn0nean0 esrewameme hNiDpo ALMA@GAeEQMASwwD Lemuebndbo emmdanonaenwnn eSined00nQunuoD TTWoiinnsn ilLmnelGuooanssup)o IoinMwGUGoabQewsaowd 0Iavndd0OooQtqaam MLAmaODGPnRQUEMD0O L0ia8mG4G0xoQNaIm0Nd 069I7n0G(0e02nd nwwDoo tsTy nnsorrmmoadod:ned0EfoeEamCnneeedos onfolqHuu PwCbyarbertbewrdododsowmi dpeann(d0QisbNohheosudGoarh(or0tQeaADnfoksm4o00m<edsuor1fehbey vo sv do EGGS ote i we etd fo ty ss ==r [S=irevoas oSuener 0 2270 a Z ~~ Meow = 57S No 7 3 St a acesn Nur ea 8 STmocorn N, ae jTeesnorno z eerrarmarsa] aFHATgeNA2:T. TGDHodaaStt.meCsDacapomniocnieoeAnsrwptoffPEiCgs tfcn obbamlmexies onfcMtSCcigsGC,5ot20F0i-cl30M11tsVdoaTsoPtsoCdFpberdoMt.friSo ymFerser1eMnossbdryftdhee gllicnonanPdErC elvclsduien th0enreovlingsexw.eling, We found m0 mPtRCmCeonnc(enGtMr)atoifoZns PandvFaSCpiagtehtPtatPtoelne. 3T.h6e3 (cOo41 anLg)/,mLA)PIlSow(5e52d nbgy/mLS),ACnNd(L6E4SSng(/1m9L),ngM/mILS)S, (w6i07h nhge/ nlogw/emstl)so(nTcielneat2o).nsTahci cpaitoemn ohfehivgheermTUPFSCAcCon(c1e6n3 nrvoioenmennctl wmiantceonse"s hIcn 2hesntfowiudned. ae3smnagts ooff nPeEseCMiinnnMcisnpnoclii/ott.iP,alf,nMPNECthsinweinemfooruendrtdhsigrhssoef hee 2405.0004 EH meen I Environmental Science & Technology Fic| sRaeteBSai,mlNaC, e10cPRfoCunidn 3surhfiacgehevrilteesofnthce CkanpeoeFeaorx NcoargtehnAsimnigsraors tha thse decades fe being banned in hpaevcetsehdowtohirgsher1lwvlbaofrPeECss nndairfanbEovsek dAcuh,sctueeds intPraatltsern(snofBayIensdiainv.idusaaltisAinsa.lytthees.e Tahre a9n5d%logcoruesdisteo giTornse aeseven sourcesof PEin Chis region' but most sTaednydosnesco(nfTiadelncSe13t):eNvon)tholvsesd,spfef.or gael nPeFCspatdtneranls neotdablceeicrtohcehe3mMicClotMguoeriGnraoivoen c(iCtFy)(tPogmsik2e, Ap)ewahciceh m3nodrweas(tThaebmlea2t)a(b1u)ndPaRnOtSwPEaCf(ouGnMd. 7s7l.s83a0m0enge/smtLi)nign Snrieng lmaotte for pro(daSctOioPn woiflF0O0S1anSd OoFh PFhCe. 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PhCiBghs lv(plaslychlboratd Pe 170N0eangadPROScmaLl.btHedood opxami arsefperroetneccetivveeof 2(TfRoYe) IoVf rGhepcartiong sbiad .shWeaf5ouannd GaAlTecornecsnprecatiiovnes fobsexbxeland n1d1ivTdRaVl minianllgosf wurredNgyheas,of h8ow(e5r1e%)l8acMsIfSoSt asnodme3 C0a2g]e p(r3o5d%u)dstttLySnAoCNu.r WStedyf.ouWndendoufniottsmoefsPaRO.Spoonrbnddl smcdeipoacslogl, phyogos eho ellos the 2h3eT%hMoefsstpehcepontsodtamalonbsdutlrodsewbneu.rndSPatntCPFrFwoanCRsDwhiaivsgehSsePsE(tDSin,Pna3cscionuogn5ts,iMnssIgiSonSrg f3nrdm LLSikAeCKS,uGrMo=(8A0P-S26a5ndngL/35m5L,) Gmoode=rat1e57in-1e7s5tinnggs) mSLA)CN;anG d lo=w3M es9t5)on(hTealap3)prThSet.iCgrhePFRDoSrldavnwealsfosu(n0d piothte anmbPaFsDtudiyn scsos ansopotrentiallhyasainamnp.i.ewFsautds th ft ee 0 2405.0005 Environmental Sci&Teecnhnocloegy oL2iu1k"neflEoeuivnedalnPdoEobiwDnct8o9Sn%mLooefktkweeSiodhptrrPoiuRotOrSf.rbokmbttrhoheutbG.rieHagtoLwgahekoersstatnhidne Nona Hkh and Nutrtiorsl Baminaton Study, which bPtieEsatCnsnsuaalBlriyee,predPsoeeDnsSta.ntoitvteeinnscdalmuptdloee PboFefDSSm0.o0"r0sGpievtoeopnlxethaaactnrdolsosnpgrteohrencehUaSi1.n0 beiaoWaeec csufmoruunlldatiRdoOn,hRwecaoanrcgseuetuatidhaotn it s shoul to be d c be considered in omparatively low aSuvpaaloradndudtyheavhisghTsseeve2l). wTeoree lnowneeselilngns fbomshoelsLaakree eilikhnelecydueeTsteowisnPEaiOnAv'aLsiikleo,w SbiTooFpaOcecArumilnaegtsietoinnngcpsreompfeyorutni5desa" dahuniedghttThose. lTieinvgcehlosettitnhgaamnLoinkPgeFSO23SupaienpresuwsrfhaecmeeesSwasoteetrds ionaf.stfhroeucnGdrewPaatFteOrLAatkT-ehbsee, hCaocrowfatheir awat.s sftruodmy spsriecmptieadtotntn3d9.% 9o%tfh wPasFOfAoimn rruittaa,, ncootnincgeithtaetdWPWFTOPA,umpan10y 3w0hiochdahretlooafteidkoen Ftoru aBymocngom1p3aPnF,Csmeesdtieadn isnonsceuntcatiwoantseooffPtFhOeAuppwears MmiLsO)s,tishsPieEppUminajARoir(ves3r3n.9e01s75inmcga/dmeLd),PEPDEANA(G(M11=5-8S4195-1ng2/6mLn)g,/ o12ndTceeDmtpaoairoanl(s3Tr1<e53n78d.7s0.m5gvn/elrb. h:e iAlytarhsstuPdyCwrewfooutnfdosunodnig c5i0d%e1n0t1o0f0%d)e,cmiodineErPiCdSenncde oofsdneciyor(trwoobnaabll3sy (iombeabi(iyr>ab3b0%i10 3<030%%1)0,OnoNevidaenndceoofdcehasngoefcinehvee Tinavtoofmchtansge S(p1r1o0ba,biTliutbye134 dHeoiwnes=,03hnedehteenpdescwtreed rt ior srs say ara (Table S18). Fo ample, he rpraoblabiulityy tahaetsPEcHxpeSpdePcolliened fr4owm h20e0t6d0e2n0c11ewoafsde5i9n2e% InTatbelreal3. (ECx1pe)ctfeord R13atPiECofAChnaangte aFnoduntdhei5n5T%adCrEeadgilbele Nestings ia p le atdis oF rmss Essie) nms a = Po smeibemi 2B0s seaembeus m on o mon 11129 wn dui 0) puirl| o=e 72 = a5 . hiFeneneisi)(nYa scd as] ebithffoo ys (Ho OV) ooff Tiotge ienhot fpieptn.of bend tts bo Pp re] Jmwaoosidlnaecksiwngast(pMsrItobrSaoSbniglaintodytL=SP$oA3o%kC)s.N3Co(n&vrebr3saebl(yir,yoebv=aibd8iel3nyc%e fo=of P93F5%O%)S), weak APS and LSS (rab5% b076i8), nd cing iaPtnFdUOSfShAhaCvsNelob(nepgreonbtahdbeiolciMutIymSoeSfn.tdeesdcelibcnyet=otoh47e5r%st)h.ienSiMwmaiitlseaor,pdspeecidliimneRensetsei,n eSbesNt,Ewetedhnio2o0mo0d4anwideb2n0w1i2lal.foPTFmhOeiSsecdperctolodiuncceoisnoraneninlPi3kFe0lO0yS.thaeNnrodensuielhtheorf wPEiCsefon nmadnyroyeuarn. dThsicoisntdamuinfaotitonh, ehxtienntgofffoomalPsECo tpchoenrtaUoiSndi.nguopcfrlsoitdamuidcitteisdooninanlmmoauunnnditcaipoaflmelatntdfiilPlscF, CanHadECbt.haep.croondetuicnntuineodn cthoeentsaipnqueeusseiwnhfeoorofedFtwheeCr.e bFayorerTnnaeomdpkilnnego,wcnannalm0ti1ek1em,.athviveeenns*.aaMhovresdoovenrtg,o cZvPdEeCnseionfa dneectliinnesg,(w3e.70fonugnd/mtLh)e HTiogthfs cloncoenatworatrieonndooff lSoenegdeirng{woanlltihteMhiedghedtcvapee rwehsicihnwpearihoidg)hecromnpdarfeded10 AhensprioMrN)30. yes (unpublished USGS. seamen a W90e%T)oufrnordfPeomEroPNdnEAenNdatAeaPsinoddsePn3EceD8coAf1adlaeoncdldiiUnfefseSrAe(dCrKaom,toannogryasvti=udde3yn0acr%ecso1.0f ndevieidnuetnece ao1MfIASdPSeIiSsnnd(epL.rSoSbP,aFbQDirlAbaowfbisimlcet<isyn.1g0%=i)n$a5l0nl)d.oadSnyicameiof s(wperpotbaalyoUfScACaNsw$h5e0)e. 1 showed eudence of creme etWeiideeutian isoensgiisdenfcoem lhlattPdFTaSrDsA (andrPoFbDeAf rthesmtsn 9c0a%peTherptewesd3.a5itooofPcEhTaenDgAe dwihr >s,tantd on erg, csofts comin were more than dling Jtevaoek]ryoDfykeFanrolw(olTaeadbdligneea3)sc.htTiohnwegs,he ehtwooswPoEewCstaemnadrdeeeuipwn<0.sl5o%urosgf atnhdea neTsn ferxnctrnned8ty yar sly docu, sstenive coownttam1i6nadtififornenotf PaEaCcamoadso.rsBaoftthgehgenerstMiindgvessetrvbedy a ffo rbsbistsattateoffinldoinas ocfoomtahemrisntohnt,PaFnCd loewd ruhse Sao tnenmsan nd oindue ssainiwnagen .eDvyee esnnmodfes loingpfreois iend ta iSonrcteerasdeancdinalfloowaecdhuosf1to3 PstCarsedheipdronbanb.anWcshiof eweFsxTooumsghngattdhmamneyeoPtFforCocodmtiurnededaedusricdng tihi sny etht rASiSpOCeIAnTErD CoONTnENT bd sop mongMee, 0 We providCerpfaoutrontasblersowni.th Bbc, information oonmnidlgagebsorataonrdy o20ppToibeatcesoarle va5lolfcher a hs Incrnt sp---------------- 2405.0006 Environmental Science & Technology ice| B AUTHOR INFORMATION Corresponding Author pin"h(A1er2ti2Hc0o1aln,sd561N;o(r9Mt)ih,d7aA5cth-n,2i50c.mRaiancshma,aKnC,Ke1,994M-;200R9e,vpehro, o N"oPtheosne: 715 652 0631 cat 21. Email: bil outc@psgov. oAfngeeclriso:riKniteecdiccholmep,oPunMdasrcinhahliNryei n andbdMl.eBeocpmo, ead1n on dais ot opipengng finaTaniintrest ePretuporo2c0t08n,an1t1e6c(5o)n,a6m51i-m6t57d.. dking water. son. Heh B ACKNOWLEDGMENTS S1h5de Oybae1n;T,a0n.g1a, m$e5Gutlsouf,oA;Ytami, Ns Pema funding was provided by the US, National Park 0d rpc in human bing on th Bic Cot? Emin. Sc. SSeorinedGresptrLoaknes fInovmenttorey aMndiMnonsitorPinog oNentworCkowimth (T1eh9elKe20n0a6 4K,i 7F43o-7a51m,) C3 owen eM, fae XJ W`AgeancycethFeouGnrdeaattioLnakeAspRoersttioornatoifonthiIsniwtioatrikve,waasndcothneduDocntaeladds oJorne,eluGdeo).es and.Pheraarnreosct.neEnisulfonate i4n fhTeeantidng 3wa0t0e1r pSitruonfatChoeopUeSraEtPiAvenRdssArgcehnandTeDecvehlnopomen(t 3Ag7rs0em7sn.t Y(o1,5)obeadw1easvdinDoerVoiefr,pK.lcro sgh s+ Blaobso,ratUorSyEPaAn,lyacnsd, tahned 3GM. MCiollrepro,ratPriaoinrieprToavaindded InBdiinadn M(1a6)GrecbhbeinWpkhnA. ELnuec.hIRr3J;0He0be6r(t,3,).E,5+7W-36d1 , D.V.C:. Cino'mimnudnictoyntipbrootvoindse.d saTmhpeleWirsecsounssinandStaftedLaabiosratnocrey, 5of~~Tcuucbaotynyyercoomfmtiemtpsolindbnrigngingupceassfoosm tmheloLsatrcconnadn HWey.gietnheankwasJ. cCoammepabceildl SaspitcheerprnimdaryG.amRyteicmlahboforrsortye.e G(r1e) LHaokel]oF,erKosE.MoJroka3n0a1,15A(K12)B,e3r36,6-A3;57L2indberg Ps niemsbliinngg,snnddhmanadnlyinngoatfionraelsipanrsk,sMe.rviMcaertsetalflffaonrdhvaonlduinntegerosf| DDreetg,neU. aTkeompnorcaglgstr(eFndasloefppoenaet)ed197s4f-i2c0t0a7n.tsEinn iSw.edSsch ome whats eulechn nd logics. we appears Teal 200.4 (11), 0534088 cFonrsteruoctniv.e cVommientes onn drafts oef lthois d manuscre ipt by B.ThLea (g15t) nGaraetttM. Gns WeatsCono, nWseAnRtohonEy, RaG. Bld sagge hoeme COffince ofSRcessaEcmhvaonndmDeemvllopPmoenntethoa aregvoienwyedthoioSo emS to19) merRseOnidnTnethesthd ocgWAilltehmloweHr 4e8 staFteos roorgs h3e0Li0st3o5f indmmapeprsovaedr ifofrrdspucbplticitvieon.purApnoyseuseonolfy tarnadd,doprnoodtcitm,pl0y ((13500))Baowreromgano, Wh. W. Regltonofbod ce prdacisty nthe endorsemebnyt the US: Government DGirsocrLtiokne,s MTiach:igaannSctsnUgnivnedr,tEotvcLoigniilngprMol,ac1h,99PAD. W REFERENCES eset N(e2y1)erBM,oWw,nP,oWAs;tBSsp.,JDSiAisdkGay)i..,G.PAysSociiticonks b,eMt.weCe5n ram. No oo 583 perp tehmaun Pgornocdyfnocns iinpaoldeofteesdibbdocslnrdanddcorroic obs on et eiMea p2ro)duDctyi.eEeC.nK.; MTeyielr,.M.ChWens. R2a00s3m,u2s2n,(2), 3731-W3a76r.e, DK. Recored eARtZ26w2e000e.F UhSo.sEnCion onSmenoal RPmosoctSnounesAAgMenciy: i1198a3,2S)SE rts,a tCoroneddIptemtidinesg 2tsndofOasyskfeoeSlspie dy aobftSsnyDC loke du.FGuNorIuAdE |SaSrhNoneal d(2a) Beou1 tFsd.ORnotm199F.5C;5o(g3)r,e6,7-40N1y Kor S. An Da oman COo aparo, Wh US. EPA Dobe No iimptos,ipmtenet cphercdoenstrinincig}nineikh 9(9) DDuepontportMcNetstiinnggwiwihth336M MayMy 30. US EPA Adminsaive Si520b0o8r16T(3e), y198 evading rl he deci of aARiC0 l7 iae i ha sr stl sess B(2n6).GemPhainn,.AT;rCeorkSo..LSoteonn, F1S78,,R53a,i,0-D4B1.5.Byesondta an th bah ict of perc sb od (Pi ROR). iFdoenecse i (27)Lin2n,0DoddJTChheonmAaaxndisHatllSCRpC:iogcaRat,oDn,WFlB, 2U0G05S3 H5)hPoew,spG.eB;20C0ob,,17. (D8), C1o1o0p0e-r1,10K5..R. Prboruacamoic aid SKaayCsompmuotca2l0n0g,1f0ame(4v)o,rk3:25-s3o37nt cus, nd ten. (FFON) a cmergng dkingwatermconetaeines, Aci res of p(28)pBegb, J iYnoprkaJ; iMoilln,.A.AnBny.soitnSitm.agMeetrhst1o9st0i,o1n3,i1h Per)tuGruodnopn,icBl. (BPyFC)Wop, oQrseDiunmacs,heA.s Ks;oKiannnsan,wiKh S(39) Parmer, Ms Best, Ny Cows, Kj Vines, K. CODA SimpSirSd response (10) Hows, Ms inition. De Sika, Fain. Sc. A O; Moi, Teel 011, 45 D. C. Gy Letcher, (19), RJ. 20C0(o36n0v,)erLg(eo1nnc,eg7-nd1ie1a.gcnMoks.isPsanSd.iohup,C.utKaipilsof,Gor.MEsOCHo.ppRinJNeAwss Me1e)onRrnanonkdf,peStAftyaoKTorihnrnndelad 2cnA0s0o,Vm4a5np(a9o),,uw9Bun6sn2dP-7db9or7t3sAnRoiep,aBls JD:GUoEHrhdOo)M.LS.sLDeakne,g5s 5EbLreb,arDA.JsLEiinldosonMr,A.,.B RFeisgheerny,, W. K; Suma, M. J Soba, Wy. An ebro ty of MACouTncsroeuni,nGg. eAvselVoifkilonngg,haGns Gpberriscohre,oc.ubWoonBoacdhs, D(P3FDCaAsS,) p20e0c8s,o1n0i7ae(2d),l1y52-c1o9m,pound cl in human plana. vn. Rex wn arr i Tet 13 2405.0007 Envonmental sence & Technology mm flwSi=hippRc A,ESe St, Ot VTl.t TBrg,Ae TeaoSvto SeA eve.a1 dSae .TevCitl2li a Te Fo No Kolo 5 SoTss lm i Se Ba] Te war Deeh ISTor OaLoInN pKooslulgtii,onY;byYmauglutcihpil,e Kp;erMlausourniangtse,d Sc. omSppaotuianldlsy dientatihleedTosukryvoeyBaoyn hous me ri sin Fo honk Ri(v5e0r)s,NUeSwAs.teEdnJ,viLro.n.JPoonlels.,20P.0D8;,Co1a5d6y,(3K);, G1i2e2s7-y1,23J.P2. .Avian tonicity PT pNaekriafyoSeaormaadk ,tedSp. cFo;o mpo hLoiunnddsstrooimnb hS,SfaoAlbt.h fBr.oe mTGTeMooigonrnaeplshoi5tcSaaslhMidkiessttL abnudtiorkncgss.of TTr(5e3 1n)dnsKian KSet;xpWooosEnur,ge,H tLYoNJpoalylfuLo.roT)alKkyulkFlBcehenmiiadckZal,;s,CinaltaheiAtUMS,.. aBdtoemosphrseS ric mSeeaho suoretrmesnt tLs.LESnJviJroFn. D.Scli.rTyeDchnoly.3 20A000, #4S2 B(11E), o) S RCS C. Toe PERn yCseWp onS0ehoi lae niAsOtSpAel ner ceir,d serLvieopwt rwitl5coTme paaelionsn5n. rom the Upper Misisippi River Enron, I. 2008,34 (7), 932-3, 27d sources. |. Great LakesRe 30103,6 (2), 277-254, sobs Ban Sh RY Be(i3g6)e,MMo;nsSotna,,B.J;AD;eSloile,m.,ML;iHoiff,RiPv;erHPooral,2M;teMrcsceantn,yPosf a(3s4)sfe3,e Tn aFssocKiiaetnesd, pDolLluWtieobnferro Ry I3WiPEkCnprAoduRcPtiOon mpiatPRfGn AE Vivo.hrs Misi sr 208 NOTE ADDED AFTER ISSUE PUBLICATION i EupTdate;nmMisnCesooa D tsmPoSlle outka ioenbCon ntrn oPl Agnencye ,PSa to. rPanue l,, MDNa,io2e0s1s3.Cr o"oTyhisepa0pehr wasdpubplisheodfJune S,es2014, Ihnthte verssionbputblished e a in ep 1.0 Bl e5 trlay) e I eS eee Bs aoos n a tnmmwee ao Comaol, Stig Ta i emnno ftaaonn s eoeei,nn Lm FiEnEodR.s by rra ene,A . Foiintis,Zidte, mdd rraie H,aaens Rot wstT MEoot.n beRaslm, aee KeasLrpei t n n Br oveti . 6nis ni3l0 einnmt a ps ooa n oKnpeJhen Sl ee eSon ielesao of pont EE a a nheatthonsas eR is es ots wo snsprsm-------------- 2405.0008