lead cadmium on health

8/6/2019 Lead Cadmium on Health

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GLOBALENVIRONMENTMONITORINGSYSTEM

EXPOSUREMONITORING OF LEAD AND CADMIUMAn internationalpilot studywithin theWHOruNEP HumanExposureAssessmentocation(HEAL) Programme

Technical eporteditedbyMarie Vahter

Instituteof EnvironmentMedicineKarolinska nstutet rStockholm, wedenStuart Slorach

SwedishNationalFoodAdministrationUppsala,Sweden

ENVIRONMENTPR,OGRAMMEG}

#*touu-h8U-I 3 ",ljii{ $ggfo,,ont*

WOR,LD IEALTH ORGANISATIONUNEP


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TABLB OF CONTENTSSUMMARY1 INTRODUCTION1.1 UNEPAM{O {EAL projecubackground ndobjectivesL.2 Healtheffectsandenvironmentalexposurc o leadandcadmiumL.2.1 Healtheffectsof leadandcadmium1.2.2 Totalexposureo leadandcadmium1.2.3 Exposureo airborneeadandcadmiumI.2.4 Exposureo leadandcadmiumvia thediet2 MATERIALS AND METHODS2.1 Selection f subjects2.2 Questionnaires2.3 Samplecollection2.4 Analyticalprocedures2.5 Quatityassurance2.5.L Preanalyticalualitycontrol2.5.2 Analyticalperformance valuation2.5.3 Qualitycontnol anrples3 RESULTS3.1 Analytical raining3.2 Monitoringof exposureo leadandcadmium3.2.L Qualitycontrol3.2.2 Leadandcadmium n blood3.2.3 Exposureo airborne,leadndcadmium3.2.4 Exposureo leadandcadniiumvia the diet3.2.5 Eliminationof teadandcadmium n faeces3.2.6 Conribution of inhaledand ngestedeadandcadmium o the totalexposure4 DISCUSSION4.1 Methods or exposuremonitoringof leadandcadmium4.1.1 Studydesignandsample ollection4.1.2 Analysisof leadandcadmium4.L.3 Qualitycontrol4.2 Routesand evelsof exposure4.3 ConclusionsREFERENCES

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Annex A.Annex B.

Annex C.AnnexD.Annex E.

General nformation aboutthe HEAL sitesGuidelines for samplingprocedures or blood,faeces,airborneparticles andduplicate dietsAnalytical proceduresReferenceanalyses lResultsof QC-analyses,rainingphase

LIST OF FIGURES

Figure1: Lead n bloodQCsamples nalysed tnationalinstitutes ogetherwith themonitoringsamples'Acceptancenterval ndicatedby broken ines

Figure2: Cadmiumn bloodQC samples nalysed tnationalinstitutes ogetherwith themonitoringsamples.Acceptancenterval ndicatedby broken inesFigure 3: I-ead n air filter QQsamples nalysedatnationalinstitutes ogetherwith themonitoring samples.Acceptancenterval ndicatedby broken inesFigure4: Cadmiumn air filter QC samples nalysedatnational nstitutes ogetlrcrwith themonitoringsamples.Acceptancentenraf ndicatedby b,rokeninesFigure5: Lead andcadmiumn dustQC samples nalysed tnational nstitutesogetherwith themonitoringsamples.Acceptancenterval ndicatedby bnokeninesFigure6: l-eadin diet QC samples nalysedatnationalinstitutes ogetherwith themonitoringsamples.Acceptancenterval ndicatedby broken inesFigure7: Cadmiumn dietQC samples nalysed tnational'nstitutestogetherwith themonitoringsamples.

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Figure 9: Cadmium in faecesQC samplesanalysedatnational institutes together with the monitoringsamples.Acceptance nterval indicated by bnoken inesExample of day-to-day variations in the dietaryintakesof lead and cadmium by a subject duringone week in Sweden

Figure10:

Figure 11: Daily absorptionof leadesrimated rom theamounts n air, duplicate diets and faecesFigure 12: Daily absorptionof cadmium estimated rorn theamounts n air, duplicate diets and faecesFigure 13: Concentrationsof lead in blood in relatio:r to theaverage otal daily absorptionof lead estimated romthe amountson air filters and in faeces.Each datapointrepresentsthe averagedaily absorption by one womanFigure 14: Concentrationsof cadmium in blood in relation tothe averagetotal daily absorption of cadmium estimated

from the amountson air filters and in faeces,Each datapolnt represents he averagedaily absorptionby one woman

LIST OF TABLES

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Table1:

Table2:

Table3:

Table4:Table5: Concentrations f cadmium n blood

Concentrations f lead n theb'reathing oneair(personalmonitoring)Concentrationsf cadmium n the breathing oneair (personalmonitoring)

Samplingscheme or exposuremonitoringof leadandcadmiumMAD intervalsused or theevaluationof analyticalperformancen thepilot HEAL lead/cadmium rudyNumberof QC samples nd he concentration angesfor thevariousQC sanrplesn the I{EAL studyConcentrationsf lead n blood

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Table6:

Table7: 29


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Table 8: Estimated daily absorptionof lead following. inhalation of lead-containingparticles

Table9:

Table10:

Table 11:

29Estimated daily absorption of cadmium followinginhalation of cadmium-containingparticlesLead in the daily duplicate diets, including beverages,collected by the I{EAL study gloups

Cadmium in the daily duplicate diets, including beverages,collectedby the HEAL study groups 31

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Table 12: Average daily elimination of lead via faecesTable 13: Average daily elimination of cadmium via faecesTable 14: Comparisonof the averagedaily dietary intake of lead(basedon the duplicate diet analysis) and the average

daily faecal eliminationTable 15: Comparisonof the averagedaily dietary intake ofcadmium (basedon the duplicate diet analysis)andthe averagedaily faecal eliminationTable 16: A cornparisonof the concentrationsof lead in blood(ug PbA) with thosereported in non-smoking womenin previous studies carried out at the various TIEAL sites.

Arithmetic meanvalues tS.D. N= number of subjectsTable 17: A comparisonof the concentrationsof cadmium inblood (ug Cd/l) with thosereported n non-smokingwomen in previous studiescarried out at the variousHEAL sites.Arithmetic rneanvalues tS.D. N= numberof subjects 4L

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PREFACEHuman exposureto a pollutant occurs when a personcomes in contact with thatpollutant through the air they breathe, he water and food they consumeor through skin

absorption.Knowing the degreeof exposures necessaryo study he effectsonhealthandto devise appropriate control strategies.In recent years new techniques have beendeveloped directly to monitor such exposures,assess hem accurately and evaluatecontributions from the individual sources.An increasingnumber of countries areusingthis technology in a multidisciplinary approachto multi-media human exposureandassessment.

To assistthe further development andapplication of the technique crurently beingapplied n severalcountries, heWHO and UNEP through theGEMS are co-operating na coordinated effort - Human Exposure Assessment -ocation Studies (tIEALs). Thisprogamme aims to improveexposuremonitoring andassessnrentnternationally leadingto better protection of human health. Direct measurementsof human exposure usingestablished methodology, coupled with human activity patterns and social and culturalconditions provide the basic data enabling exposures in a given population to bedetermined.Accurate risk assessment tudiescan then be undertakenand cost effectivestrategiesdeveloped f required to further protect humanhealth.

For each study in the I{EAL programme,one of the panicipating instirutions in aparticular countT/ is designatedas aTechnical Co-ordinating Centre(TCC). The Centreis responsible for monitoring protocols, design and implementation of quality controlprograrnmesand other technicalsupport o helpparticipants mplement theproject. Eachcountry has, however, a major responsibility for conducting their own study.

In the pilot phase seven countries were involved: Brazil, China, India, Japan,Sweden,U.S.A. andYugoslavia, and threegroupsof chemicalsweremonitored by someof them, namely the heavymetals ead andcadmium,the organicchemicalshexachloro-benzene(HCB) and dichlorodiphenyltrichloroethane(DDT) and the gaseoussubstancenitrogen dioxide. The substanceswere chosenfor they may pose health risks and theparticipants were interested n determiningexposure o suchsubstances.Reportsof the threepilot phasestudiesarepublishedseparately.This reportpresents

the results from the monitoring of lead and cadmium co-ordinatedby a TCC in Swedenasdescribed n the section Institutions and Investigators.Laboratories in China, Japan,Sweden andYugoslavia completed heproject, while Brazil, India and U.S.A. participa-ted in part of the analytical training programme


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INSTITUTIONS AND INVESTIGATORSThe IEAL PilotProjectonExposureMonitoringof Lead pb)andCadmium Cd)was coordinatedby a Technicalco-ordinating ceitre GCC) in sweden in closecollaborationwith thenetworkof nationalnstitutionsparticipatingn theproject.TheTCCwasorganized sacommitteewith representativesf the nstituteof Environmen-tal M9dicineand heDepartment f EnvironmenhlHygieneat theKarolinska nstitute(Drlars Friberg,chairman,M ScMarikaBergluna,apiorteur,Dr MarievahrerandMrBirgerLind), thENationalFoodAdministrationor StuartslorachandMr LarsJorhem),theNationalBoardof Healthandwelfare(DrHakanwahren), heNationalEnvironmen-tal ProtectionBoard,andthe Depanmentof EnvironmentalMedicineandInfectiousDisease ontrol, stockholmcounty council, KarolinskaHospital (Dr carl FredrikdeRon).

TheIIEAL pilot Pb/Cdproject ncludedananalyrical rainingprograrnme ndanexposuremonitoring study. Initially, China, Japan,Sweden,uie ano yugoslaviaparticipatedn theproject,Brazil and ndia oinedata arcrstage. hina,Japan, wedenandYugoslavia ompletedhepilot project.Brazil, ndiaanduSA participatedn partoftheanalytical rainingprcgramme nly.The ollowingnationalnstitutionspanicipatedin theproject:BRAZIL: Minisuryof Health,NationalDivisionof HumanEcologyandEnvironmentalHealth,Brasilia;oswardocruz Foundation,Rio deJaneiro; tatesecretariat f HealthandEnvironmenLRio Grandedo Sul;EnvironmentDivision,portoAlegrePrincipal nvestigators: r NestordacostaBorbaandLuiz AugustocassanhaGalvaoResponsiblemlyst:Dr MariaLuciaKoslowskiRodriguesGHINA: Instituteof EnvironmentalHearthMonitoring,BeijingPrincipal nvestigatqrg: r ZhengxingquanandDr zhuangLiResponsiblenalysrs:Mr cia stritin "n'au, Gao luiINDIA: National nstituteof occupationalHealth,Ahmedabad; ir euality MonitoringandResearch"aboratory,Bombay&incipal invesdgators: r s.K. Kashyap,Dr D.J.parikh andDr s.R. KamathResponsiblenalysLr: r c.B. Pandya,i, N.G.sathawara ndMr G.M.shah or NIOH;Mr J'M' Deshpandeor Air QualityMonitoringandResearch aboratory

JAPAN: Instituteof publicHealth,Tokyo;Yokohama ity Instituteof public Hearth, okohamaPrincipat nv,cstigatg:Dr MasahikoFujitaResnonsiblenalyst:Dr TaroKawamuraSWEDEN:Karolinskanstitutet,nstituteof EnvironmentalMedicineandDcpartmentofEnvironmentalHygiene,S ockholm;NationalFoodAdministration,UppsalaPrinciBalnvestigator$: r Marievarrter,Dr sruartslorachandM sc uarita BerglundResponsiblenalysts:Mr BirgerLind andMr Larsrorhem


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usA: u.s. Environmental rotection gency,washingtonD.c.Principal nvestigator:Dr MichaelDellarcoResponsiblenalyst:Dr DavidMcNelis,EnvironmentalResearch enter,UniversityofNevadaYUGOSLAVIA: Institute or MedicalResearch ndOccupational ealth, ZagrebPrincipal nvestigator:Dr Marko Satic'Responsiblenalysts:Dr MajaBlanuXa ndDr Spomenka eli5manUNEP/UTHO ECRETARIATMr GuntisOzolins,WHO,GenevaDr Henkde Koning,WHO, GenevaDr MichaelGwynne,UNEp, Nairobi


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SIJMMARYAn internationalntegratedhumanexposuremonitoring study or lead(Pb)and

cadmium fr), involving thesamplingof duplicatediets,airborneparticles,bloodandfaeces,was mplemented.he irstphase f theprojectconsisted f ananalytical ainingphase,which wascompleted y participatingnstitutionsn China, apan,Sweden ndYugoslavia.nstitutionsn Brazil, ndiaand heUSApanicipatednpanof thisphaseThesecondphase,which consistedof a pilot cxposuremonitoringstudyfor Pb and Cdincludinganextensive ualitycontrol QC)component, asperformedn China,Japan,Sweden ndYugoslavia.Theexperience ainedn theQCprofaurme shows hatgoodanalyticalperfor-manceor one ype of mediums noguarantee f goodanalytical esultswith other ypes

ofmedia.Furthermorc,heQCsamplesaveocoverherange f concentrationsxpectedto be found in the monitoringsamples.Although major analyticalproblemswereencountered,speciallywith thc duplicatedict andair filters, the analyticalperformanceimprovcdduring tre rainingphase.Exposuremonitoringof Pb andCdwascarriedout duringFebruary May, 1988onsmallgroups f non-smoking ome ,23-53 ears f age,at ourIIEAL sites:Beijing(12subjects), okohama3subjects), tockholm15subjects) ndTagreb17subjects).Airbornepanicles TSP,personal ampler)andduplicatediets were collectedby each

subjectduring7 consecutive ays.Faeceswerecollectedduring 4-7 daysand bloodsamples t the end of the monitoringperiod(day 8). Foodconsumptionecordsandactivity diarieswerekept during the whole samplingperiod.Determinations f theconcentrationsf PbandCd n thecollected amples erecarriedout by theparticipatinginstitution n each ounfiry. orvalidationof the esults, xternalQCsamplesair filters,dust,diets, aeces ndblood)wereanalysedogetherwith thecollected amples nd heresultswereevaluated y the echnical oordinating entren Sweden.Evaluationof the otalexposureo Pb andCd wasbased n theconcentrationsnblood.Theaverage loodPb evelwas73ugfi in Beijing,29 ugt in Stockholm, 1 ug/l

in Yokoharna nd50ug/l n Zagreb. hecorrespondingigures or Cd n bloodwere0.6,0.3, 1.6and0.7ugn.ThePbdata rom Beijing,whencompared ithpreviousesults romsimilarstudies, ouldbeconsideredo ndicate ncreasedxposure, hile thoserom theother FIEAL sites ndicatea decreasen Pb exposure.The Cd data are n reasonableagteement ith earlierdata rcm these ities.Theresultsndicate hat hediet s an mportantouteof exposureo PbandCd.In general, irborneCd contributed nly afewpercent f thc otalexposure, trd irbornePb5- 1%on Beijing,Stockholm ndYokohama.n Zagrebthe ptake f lead rom airwas

about wice hat romthediet.Highcontent f Pb andCd n faecesndicated thersourcesof oralexposurehan hedict.Therewereargeday-to-day nd nter-individual ariationsin Pb/Cdntake,ndicatinghatcertain oodstuffs anhaveaprofoundcffect onthe otalexposureo Pb/Cd.Theaverage ietary ead ntakeat hedifferent mAL sitesvaried romapproximately to 1 7oof theProvisional olerableWeekly ntake PTWI)proposed yanFAOIfrIIIO ExpertGroup.Thecorrespondingadmiumntake anged rom about12to 33Vo f thePTWI. On agroupbasis,hecontentof PbandCd n faeceswas ound o


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reflect the dietary intake, except in 7.agreb,where the content of Pb and Cd in faecesexceeded he content n the collected duplicatediets for most women.This pilot study was one of the first to be developedand mplementedaspart ofthe HEAL project The experiencegainedshows that, although costly and complicated,it is possible o makecomparable lreasurements n an nternational scale. t waspossibleto identify a number of problems in the collection and analysis of different types ofexposuremonitoring samples,as well as to identify the major routesof exposure.Suchinforrnation is valuable for the design of a full-scale study on a representative sampleofthe general population.


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r01. INTRODUCTIONl-.1. UNEP/WHOHEAL project: backgroundand objectives

The UNEPAMFIO umanExposureAssessment-ocation([{EAL) projectwasdeveloped spartof theWHOHeatth-Related onitoringhogramme,whichwassrarredin 1973 ndoriginallycomprisedrbanairmonitoring, rrct qoalitymonitoringand oodcontaminationmonitoring.These hreemonitoringprojerti for* par:tof the GlobalEnvironmentMonitoringSystemGEMS).Between1970and 1980several eportsshowing hat data from outdoorairmonitoringstations o notreflect he otalhuman xposure ppearede.g.yocom, 197l;Ott andMage,L97S; ugas,1976;Cortese ndSpengler, iA>. h D71a Governmenr

Designated xpenGroup ecommendedhatmoreattentionshouldbegivento humanexposure ssessmentWHO 1977).Two ilotprojectsweredcveloped, nedealingwithhealth-relatedir pollutionmonitoring wHo, lg82o,b, c; wHo, 1gg5)and heotherwith biologicalmonitoringof lead,cadmiumandcenainorganochlorine ompounds(Vahter,1982;FribergandVatrter,1983;Slorach ndVaz,1983;BruauxandSvarten-8retr,1985).n 198 a consultationn health-relatcdonitoringWHO,198 reviewedtheongoingactivitiesandconcludedhatsource-orientedonitoringwasnotprovidingadequatenformationoestimate uman xposurend hat herewasaneedodevelop nJagreeon acceptablemethodologyo determine xposureo environmental ollurants.Therefore,ongoingexposure-oriented onitoringactivitieswithin the UNEP/UrHOHumanExposureAssessment-ocation [IEAL) froject were nitiated(WHO, lggh;wHo 1983).Themainobjectives f theFIEALprojectare tINEp MHO,19g5):-to improve, ield test,harmoni e anddemonstrate ethodsfor the ntegratedmonitoringandassessmentf humanexposureo environmental ollutants;-to promote heassessnrentf humanexposuresopollutantsasa basis or thedevelopment f environmentalontrolstrategiesfor theprotecrion f publichealth;-to provideanoverviewof existingexposurcsf selected opula-tions o pollutants nd, f possible,o observe endsn this regard;-to improvenationalcapabilitiesor environmentalmonitoringandhumanexposure ssessment,articularlyn thedevelopingountries.Initially'exposureoPb,Cd,DDT,HCBandNO,has een rudied.echnical oor-dinatingCentres TCCs)havebeenappointedor nf,riou, typesof pollutants uNEp/WHO,1986a). or he imebeing, even ountries repanicipatingn theFIEALproject:Brazil,china, India,Japan, weden, sA andyugosiavia.For many commonlyoccurtingenvironmental ollutants here s only a smalldifferencebetween normal" exposureevelsand he *porurc levelat which the flrst


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signsof adverse ealtheffectsoccur.Therefore,t is important o bc able o detectsmalldifferences n exposurcbetrveendifferent populationsor groupsof subjects,otrsmallchangesnexposurewithin apopulationover ime. This requiressensitivemethodsor thedetectionof systematicerron in the analytical results.The analyucalquality controlprogrammehat hasbeen ecommendedy UNEpAMHO 1986b)andFriberg(19gg) sbasedonthe methodsdevelopedn theLJNEPAMI{O rojecton biologrcalmonitoringofleadandcadmium Vatrter,1982;FribergandVatrter,1983)and nvolves heanalysis fsetsof 4=6quality control (QC) samplesandthe evaluationof theresultsusing inearregression nalysis.Themainobjectiveof thepilot TIEALPb/Cdstudywas o developand estmethodsfor monitoringof exposureo eadandcadmium.Thedesignof thepilor studywasdecidedat a meetingn Stockholmn October,1986 VahterandSlorach,1986),with represen-

tativesof theparticipatingnstirudons.t includedafirst phase f analyticalraininganda secondphaseof exposuremonitoringstudies.Monitoring studieson exposureo leadandcadmiumwerecarriedout in Beijing, Stockholm,Yokohama,andZ.agreb. hortdescriptionsof the IEAL sitesaregiven tt A*r* A. Basicily, themonitoring nvolvedmeasurementsf theexposureo leadandcarrmium ia air anddict during oneweek na smallgroupof wornenateachHEAL site.In order to assure he reliability and comparabilityof the monitoring dara,anextensivequality assurancercgrammewas mplemented.t included he samplingandsamplehandling (preanalyticalquality control), as well as the analytical procedures(analytical quality control).

1.2. Heattheffectsand environmentalexpqture to leadand cadmium1.2.1. Heattheffectsof leadand cadmiurn

Inorganicead nayaffecthcmesynthesis, ryttuocytesurvival, henervous ystem,thekidneys,and eproduction for reviewseee.g.Skerfoing,1988).Leadexposurc asalso beenassociatedwith cardiovasculareffects and cancer.An early effect of leadexposunc,he disnubancesn hemesynthesis, s seenat blood lead levels of about100ug[, but hasnotbeen hownobedetrimentalo health see .g.MushakandCroceni,1988;Skerfuing,1988).Thecriticalorgans thenervous ystem, speciallyhe etalandthe developingbnain.Recentstudiessuggesthat neurobehavioural efects n the firstyearsof life mayresultfrom fetal exposurcat maternalor cordblood ead evelsas owas100ug/l (Bellingeret al, L987;Davis& Svendsgaard,987;Dietrichet al, 1987).The critical effect of long-tenn ow level cxposure o cadmium s kidney cortexdamage, iving rise ourinaryexcretionof low rnolecularweightproteins forreview see

e.g.Fribcrgetal, 1986a).t hasbeen alculatedhatan average aily intakeof about200ugCdwill result n anaverageenalcortexconcentration f about bo mgCd/kg(Fribergetal, 1986b).n suchapopulation bout }%of the ndividualswouldhaveexceededheircritical concentrations ndcanbe expectedo develop enaltubulardamage.


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t21.2.2.Total exposureo leadand cadmiurn

Both lcadandcadmiummaybefound n ambientair,dust, ood,drinkingwater,tobacco mokeand n theworkingenvironment.Therefore, iologicalmonitorings thebestmeansof estimating otal humanexposure nd herisk for adverse ealtheffects(Lauwerys, 983;Nordberg tal., 9g5;Friberg,19g5;Clarkson tal.,19gg).Availableinformationon themetabolism f leadandcadmiumndicateshat t is possibleo rclatetheconcentrationsn blood o theexposru Skerfving, ggg; NordbergandNordbrg,1988)' n order o identifythemain*o*rm and outesofexposure,ntcgrated xpos'remonitoring s needed.

1.2.3.Exposure o airborne eadand cadmiumTheconcentration f leadn airmayvary rom esshan0. 1ngpb/m3inremoteareasto over 10ugPb/m3nearpoint sources FacheaiandGeiss, gg2; Elias, lgg5; tINEp/wHo, 1988)' n areaswith heavymotor raffic (urbanareas) ir ead evels rom0.13ugPb/rn3o 5'3 ug Pb/m3havebeen cportcd. n Tokyo andEuropeancities the averageconcentration f cadmium n air normallyvariesbetweenO.OOZnd0.05 ug Cd/m3(Friberget al, 1986a).Airborne ead s oftenassociated ith smallparticlesfCfraniUerfaint al, l97g;Chamberlain, 985).For example,n [.ondon60voof the airborne eadwasfound nparticlesess han0.3umandonly lva above0 um(Chamberlaintal, 1973). n1a,grebthemassmediandiameterofparticlescontainingeadwas ound o be0.3um,while ina leadsmelterarca t was2-f um (Fugas, g77t. This shows hat the sizedistributiondepends n theoriginof the eadpaniJtes.t hasbecnshown hat arge ead-containingparticles rom motorvehicles xhaust ettlen the mmediate icinity of theroad,whilesmall particlesare transponedmuch further (vominen, l9s3). studieson the sizedistributionpatternof cadmium anicles n nual, suburban ndurbanareas aveshownthat40-65%of thepaniclesatsmallerhan2um(I.eeral, 196g; g71;Dornetal, Lg7).

Air is inhaledbothvia themouthand henose,evenduring ow physicalactivity(camnerandBakke,1980).For particlesarger hanabout um thedepositions moreefficient n thenosc han n themouthand hroat.Forparticlcsbetweerrg.gland 5 um,inhaledvia themouth, he ractiondepositcdn thealveolar ractmayrange rom 10 offi%o rask Groupon LungDynami"s, tgoo;EPA, 19s6).For particles nhaledvia thenose he ractiondepositedn thealveolar ractmayrange rom 10 o zavo.Mostof themetalsdepositedn the alveolarpartof the ung .ir prJuablyabsorbed ooneror later(Lrrndborg tal, 1985;Nielsen tal, 19s8).Thus, t canbeestimatedhat lo-606oofheinhaled eadandcadmiumassociated ith smallparticles s absorbed. hemajorityofpanicles arger hanabout10um aredepositedn thetracheobnonchial,eadandneckregions, learedandswallowedand huscontributen a minorway to ingested ompo-nents.

1.2.4.Exposure o leadand cadmiumvia the dietTheamounts f leadandcadmiumngested ill dependmainlyon he evelsof these


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metals n staple oods, such as cerealproducts, ruit andvegetables,darryproducts,meatand ish. However, the ntakescan be markedly elevatedby the consumption of relativelysmall amounts of certain foodstuffs which contain high levels of these metals. Forexample, the lead levels in foods packed n lead-solderedcansareoften five to ten timeshigher than those n the corresponding resh or frozen foods (Jorhemand Slorach,1979;Slorachand Jorhem, 1982)and wine usuallycontainshigher ead evels (50-100ugn) thanother beverages Jorhemet al, 1988).In areaswith soft and/or acid water the use of leadin plumbing systemsmay result in very high lead evels in drinking water (Moore, 1985;Sherlockand Quinn, 1986).Relatively high levels of cadmium havebeen ound in someshellfish and in liver and kidney (Jorhemer al, 1984).

The absorptionof ingested ead and cadmium in adults s normally relatively low- in the order of lAVo or lead andSVoor cadmium (Rosen,1985;Friberg et al, 1986a).However, the absorption s influenced by thepresenceof various nutritional factors, nteralia other metals (for review seeBruaux and Svartengren,1985;Nordberg et al, 1935).Fufihermore, the absorption of dietary lead in infants is much higher than in adults(Alexander et al, t97 4).

2. MATERIALS AND METHODS2.1. Selectionof subjects

The main objective of the pilot study was to testexposuremonitoring methodolo-gieson small groupsof women at eachHEAL site.By selectingwomen employed at theparticipating institutions the identification and evaluation of problems involved in theextensivesampling was facilitated. It was recornmended o select 10-15women at eachI{EAL site, and that the women should be betw een 25 and 50 years of age and non-smokers,since smoking may be a significant source of exposure to cadmium (Vahter,1982; Elinder, 1985).For various reasons t was not possibleto follow the recommen-dationscompletely in all the participatingcountries. A descriptionof the subjectsstudiedat the various HEAL sites s given below.Beijing: 12non-smokingwomen,33-48 yearsof age,working at Beijing Antiepi-demiology and SanitaryStation (urban area).All of the women lived in urban areas, 10of them near the work place (about 10 minutes walk).Stockholm:15non-smokingwomen,27-46yearsof age,working at the KarolinskaInstitute (urbanarea).Two of thewomen lived in centralStockholm,one n an urbanareaoutside central Stockholm, nine in suburbanareasand three n rural areas.Yokohama: 3 non-smokingwomen, M-47 yearsof age,housewivesof staff of the

Yokohama Institute of Pubtic Health, living in Yokohama City (urban area). Bloodsampleswere collected from 9 additional non-smoking women, 24-54 years of age,working for the Yokohama City Institute of Public Health, living in Yokohama City(urban area).Zagreb:17 non-smokingwomen, 23-53yearsof age,working at the Institute forMedical Researchand OccupationalHealth, Zagreb.Sevenof thewomen lived in urban,


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2.2. QuestionnairesEach participantcompleteda questionnaire oncerningpersonaldataand different

life-style actors.Daily activity and ood records VahterandSlorach,1986)werekeptduring the entiresamplingperiod.

2,3. SamplecollectionThe samplecolle.ctionschernes sumrn;lrize.dn table 1. Dstaitre.dui.delinesor thesampling procedures Annex B) were preparedby the TCC and distributedto theparticipating nstitutions.

Table 1. Samplingscherneor exp$surmonitoringof lead and cadmium.

Sampling 1a 2 Daysof sarnpling34567 9

BloodAirDietbFaeces"

a)b)c)

Half of the studygroup shouldstart heir samplingperiod on a Monday,and the otherson a ThursdayDuplicatesof food andbeverages,ncluding drinking waterFaeces orrespondingo the food and beveragesngested

Blood samples 10-20ml) werecollected n themorningafter the astday of the estperiod (day 8), using evacuatedblood collecting tubes (Venoject VT-100H, TerumoCorp., Tokyo, containing heparin), provided by the TCC. In Stockhclm blood wascollectedalso on day I . In Zagrebblood was sampledusing Safety-Monovettebloodcollecting ubes Sarstedt,Numbrecht,with colourless aps), ontaining 1.5mg \EDTA/ml. The blood sampleswere storeddeep-frozen rior to analysis.Total suspended anicles TSP) n thebreathingzoneof eachsubjectwere sampledduring a periodof 7 consecutive ays,using ow-volume personalair samplers Beijing:DupontmodelP2500A,Stockholm:T 13350Casella ersonal amplingpumpAFC 123,

Zagreb:Casella,Model T 13050 with a flow rateof approximately2 litres/minute.Thesampling period was 24 hours per filter. The filter holders, equipped with 37 mmmembrane ilters of 0.45 um pore size(Millipore HAWP 03700,providedby theTCC),werekept asclose o the breathingzoneaspossible.Most of the time at homeand n theoffice the pumps were connected to the mains to recharge the baneries. In Zagrebmembrane ilters of 0.8 umporesizewereused n order o obtain ahigh enough low rate.Determinationof lead n samples ollectedsimultaneouslywith 0.45 um and0.8 um pore


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size filters showed no significant difference in collection efficiency over 24 hours. InYokohama air was sampled 24-h samples)usingstationary ow volume samplers TokyoDylec Co. low noise type; air flow 20 litres/minute), equippedwith 55 mm quartz fibrefilters (Pallflex 2500 QAST). The sampleswere collectedat a heightof 1.5 m above hefloor in the living room during the whole test period of 7 consecutivedays.

The dietary intake of tead and cadmium was determined using the duplicate tliettechnique. Duplicate portions of all foods and beverages, ncluding drinking water,consumedduring each}4-hperiod of the sevenday studywere collected n acid-washedplastic containers. The only items not collected were special medicines. Each 24-hduplicate diet was thoroughly homogenized and stored deep frozen prior to analysis.Separatecollection of drinking water and beveragesprepared from tap water was notperformed. However, earlier studies have shown ttrat the concentrations of lead andcadmium in drinking water at the IIEAL sitesstudiedwere low.

Due to thelow gastrointestinalabsorptionof leadandcadmium most of the ngestedlead and cadmium will be recovered n the faeces.The lead and cadmium contents offaeceswere determined o validate the duplicatediet procedure.Faecescorresponding othe food intake during the 4 first days (in Stockholm 7 days) of the food sampling werecollected. In Stockholm and Zagteb a coloured marker (Carmine red) was ingested toindicate the startand the end of the faecescollection period. In Beijing andYokohama,the faecescollection started48 hoursafter the startof the food collection. The faeceswascollected in specially designedplastic bags,which were provided by the TCC.

2.4. Analytical proceduresThe laboratoriescould useany analytical procedure,as ong as heresultsobtainedwere acceptableaccording o thequality assurance rogramme.The methodsused or thedetermination of lead and cadmium in the collected samplesand the quality controlsamplesaresummarized n this section.The proceduresused n the different countriesaredescribed n detail in Annex C.In most laboratories ead and cadmium in blood were determined using graphitefurnace atomic absorption spectrophotomerry (GFAAS) with background correction(BC) after nitric acid deproteinizationor wet digestion. One aboratory used heDelves'cup flame AAS techniquewith BC and one laboratory usedan afirmonium pyrrolidinedithiocarbamate/methylisobutylketone (APDCMIBK) extraction method followed byflame AAS. The latter methd was not sensitive enough for the determination ofcadmium. Calibration solutions werepreparedby the addition of known amountsof leadand cadmium to bovine or humanblood.

. For the determination of lead and cadmium in air filters and dust most of thelaboratories used GFAAS and BC after acid digestion of the sampleswith nitric andperchloric acids. n one nstitute the slottedtubeatomtrap (STAT) flame AAS systemandBC was used, n order to obtain a high enough sensitivity.The diet samples were homogenized and treated by wet digestion (nitric and


18/83

16

quartzwere usedand he ash wasdissolved n nitric acid. All laboratoriesusedCFAASwith the BC system n operation.However, for cadmium, one of the laboratoriesusedflame AAS with BC.

The faecessampleswere treated n about the same way as the diet samples,butglazeAporcelain crucibles were used for the dry ashing. Three of the participatinglaboratoriesused lame AAS with BC for the metaldeterminationsand wo usedGFAASwith BC.

2.5. Quality assuranceIn order to ensurethe reliability and comparability of the monitoring data, anextensive quality assurance rograrnmewas implemented. t coveredthe sampling andsample handling (preanalytical quality control), as well as the analytical procedures(analyticalquality control). Quality control (QC) samples or each matrix involved wereanalysedbothduring the raining phase seesection3.1.)and ogetherwith the monitoringsamples seesection3.2.1.).

2.5.1. Preanalytical quality controlA crucialpoint in the monitoringprojectwas o ensure orrectsampling, .e. hat hecollected air particles,food and aeces eally representedhewhole sampling period, andto avoid contamination of the samples.The TCC prepareddetailed guidelines for thesamplingprocedures AnnexB), which weredistributed o theparticipating nstitutions.The sampling proceduresand the risk for contaminationwere also discussedwith thepanicipating women prior to commencing he sampling.As mentioned n section2.3.,lead and cadmium in faeceswere used or validation of the duplicate diet collection.In order to avoid contamination, all containers and other equipment used forsamplingandstoragewerechecked or leadandcadmiumcontentbeforesampling.Someof the samplingequipment, .e. membrane ilters, evacuatedblood collection tubesandplastic bags for faecessampling, was distributed by the TCC after control of the metalcontent n a suitablenumberof samplesof each )?e of equipment.

2.5.2. Analytical performance evaluationIn order to guardagainstsystematicanalyticalerrors n the rangeof concen6ationslikely to occur, the regressioninesof reportedversus tnJe" values or a set of externalQC sampleswereevaluated Vahter, l98Z; UNEP fHO, 1986b;Friberg, 19gg).A eCsetconsistedof 1-2 nternal quality control (IQC) samples, he metal concentrations fwhich wereknown to the aboratories, nd3-6externalqualitycontrol (EQC)samples,hemetal concentrationsof which were not known to the laboratories.The Maximum At-lowable Deviation (MAD) of the empiric regression ine from the ideal line y =


19/83

t7

Table2. MAD intervalsusedor theevaluationof analyticalpedormancen thepilotH EAL leadlcadrniwnstudy.Typeof sample MAD-interval

BloodCd (udt)Pb (ue/)Spikedair filtersCd (ng/filter)Pb (ugffilter)DustCd (ue/e)Pb ue/e)DietsCd (udkg, dry weight)Pb (ue/kg,dry weight)FaecesCd (ug,/g, ry weight)Pb (ue/g,dry weight)

y=xt(0.05x+0.2)y=x{0.05x+10)

y=xt(0.1x+10)y=xt(O.1x+1)

y=x+(O.1x+0.2)y=xt(0.1x+5)

Y=xt(0.1x+25)y=xt(0.lx+25)

y=xt(O.1x+0.5)y=xt(0.1x+l)

Sinee heregression ine, basedon the resultsof a setof QC sarnples, asa samplingerror (the operating error) the decision on acceptanceor rejection of the regression inewas basedon statisticalcriteria. A total power of X)Vowas employed,which means hattheprobability of acceptingan unsatisfactoryperformance the rue regression ine fallingoutside the lvlAD-interval) was not more than lO Vo.Thus, for acceptance he empiricalregression ineshad o fall not only insidethe MAD-interval, but also nside anacceptanceinterval (AI), which is narrowerthan heMAD-interval. The distanceberween he MAD-lines andthe acceptanceines is 1.645 imes the operatingerror, dg;calculatedaccordingto the formula: '

4= o?owheren = number of observationsd = difference betweenx-value and x-rneand ,= standarddeviation of x-values6 ,h = elror of method or residual deviation (estimated rom previous analyses)

( :&\+,*-3l


20/83


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19

esdmationdid not influence the final referencevalue to any significant extent.The dust,diet and aecesQC sampleswerenot spiked and hereferencevalueshadto be establishedfor eachQC sampleby analysesatanumberof reference aboratories.Severalsubsamplefrom eachQC samplewereanalysedat theTCC in order to checkthepreparationprocessand the homogeneity of the samples and to provide the laboratories with tentativereferencevalues.Details on the reference analyses or lead and cadmium in blood, airfilters, dust, diets and faeces aregiven in Annex D.

The concentrationsof lead andcadmium n theQC sampleswerechosenso hat theywould correspond o the range of concentrationsexpected o be found in the collectedsamples table3).

T,abile . Nttrrrberof QC sanples and the concentrationrangesor thevariohr QC sarnplesin the HEAL stttdy.Typeofsample NumberofQC samplesperQC set

Concentrationrange

Blood: '

Spikedair filters:.'.

Dust

Diets

Faeces

4

0.3- 5.2ug Cdll28 - 366 ug Pb/l4 - I13 ng Cd/filter1- 30 ugPb/filter2 - 8.5 ug Cd/g4L - 7M ug Pb/g28 - 909ug Cdlkg,dry weight35 - 457ug Pb/kg,dry weight

0.4 - 6 ug Cd/g,dry weight0.4- 13ugPb/g,dry weight

3-4

4


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20

3. RESULTS3.1. Analytical training

The first two yearsof the project wene ocusedon analytical methodsandtrainingin the chemical analyses.The analysesof the coliected monitoring sampleswere notstarteduntil satisfactoryperformancewas achieved n the training ptrur". The traininginvolved the analysisof severalQC sampleswi& assistancerom technical consulrantsfrom theTCC. Some nstituteswercprovided with instnrmentsparepafis andsomeotheritems of laboratory equipmenrAnalytical performanceevaluationwascarriedout on severaloccasionsduring thetraining phase.The aboratories eceivedsetsof EQC samples 4 setsof bloodqC samptesand 3 setsof the other QC samples)and the results wire evaluated at the TCC. Theevaluationwas reportedback to the laboratories n the form of the regression ine, basedon thereponedvaluesversus hereferencevalues,with theacceptancenterval indicated.In addition, the referencevalues,the calculatedslopeand the intercept of the regressionline and theempirical residualdeviation werereportedto the laboratories.The resultsofQC-analyse of the training phasearcpresentedn detail in Annex E. A summary s givenbelow.Severalof thepanicipating instituteshad ong experienceof theanalysisof leadandcadmium in blood andproduced n generalsatisfaCtoryesulrs.The analyiis or cad.miumin blood causedmore problems than the analysisof lead. In eC 1 only three of eightlaboratoriesproducedsatisfactory esults or cadmium,while five of theeight abomtoriesproducedsatisfactory esults or lead.Essentiallyall resultsof eC 3-4 (f; participatinglaboratories)were satisfactory.The participating institutions had less experience in the determination of lowconcentrationsof lead and cadmium in air filters and there was an obvious need foranalytical training. In QC I four of eight panicipating institurions producedsatisfactoryresults for lead andfour of six for cadmium.Therewas ittle improvement during eC 1-3.In QC I for dust,which consistedof NBS SRM 1648with high concenrrarionsflead and cadmium' seve"n f the nine participating laboratories produced satisfactoryresults (the certified value tl}Vo) for lead and four for cadmiu-. In eC 2 and 3, whichconsistedof housedust with low concentrations f lead and cadmium (normal for thegeneral environment), two of three panicipating laboratories produced satisfactoryresults.The resultsof QC 1 or dietsrevealed he nece sityof funher training. Threeof thefive laboratoriesproducedsatisfactoryresults. n QC 3the results rom on" of the ourpar-ticipating laboratories were not quite satisfactory.There was, however, even for thatlaboratoryagreat mprovement n resultsafterQC 1.Thecomplexmatricesof thesampleand herelatively low concentrationsof leadandcadmium n ih, ,u*ples areprobably thereasons or the analytical difficulties.


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2T

In the analysisof faeces he matrix problems areabout the sameasthose or diets,but the concentrationsof lead and cadmium are normally higher. In QC 1 threeof fourpar:ticipating aboratoriesproduced satisfactory esults or leadandcadmium. Analyticalimprovementsduring the training phasecouldbe seen.n QC 3essentiallyall resultsweresatisfactory.

3.2. Monitoring of exposure to lead and cadmium3.2.L. Quality control

The results of the QC analysescarried out togetherwith the analyses of themonitoring samplesare shown in figures 1-9. In general the QC results were in goodagreementwith the referencevalues,and t can be assumed hat the systematicerrors

ofG *onitoring data do not exceedthe limits indicated by the MAD criteria applied.

The institutes in Yugoslavia and Swedenanalysed12 blood QC samples ogetherwith theblood monitoring samples,while the nstitutes n China andJapananalysed6 QCsamplesonly. All the regrcssion lines for lead in blood were within the acceptanceinterval, except he regression ine in theYokohama analyses,which was slightly outside(above) the acceptancenterval in the low concentrationrange (figtrre 1). The averageerror of themethod or theacceptedeadQCresultswas5 2ug Pb/I.For c admium n blood(figure 2), the regression ine in the Beijing study was slightly outside (below) theacceptancenterval in the low concentration ange,while the other regression ines werewithin the acceprance nterval. The averageerror of the method for the accepted QCcadmiumresultswas0.09ug Cd/l.

The institure in Swedenanalysedall the 12QC air filten and he 8 dustQC samplestogetherwith theair monitoring samples.The institutes n ChinaandYugoslavia analysedg 0C air filters only. All thereporredQC resultsmet theMAD criteria used(figures 3-5).The institure in Japandid not analyseany QC samples ogether with the air monitoringsamples, so the u".orury of the air monitoring results cannot be properly evaluated-However, basedon the good resultsobtainedduring the training phase t seemsprobablethat the air monitoring results are accurate. n genefal, the errors of the methd for theacceptedQC resultswere improved compared o thetraining phase.The errorswere0.55ug Pb/filter, 4.1 ng Cd/filter 4.9 ug Pb/gdustand0.25 ug Cd/g dust.


24/83

,\ 3(X,;o-sr*T3b 100t5o

.^ 3(X);o-sr*3t3b 10o.9I.85o

^ 3(Xl5o-S.*TIb l ( n.g5o

^ 5OO>-s2oottEb r0o3Jo

!C'stoEIboE

u'oln'o1r'o12,0l

S'st5Eb3-9

5.04.05,02.O1,00.00.0 1.0

Rcfcrcncc

QC5+6 Sweden

22

QC5 Jopon

Rcfqurccwlucs (n UA,

Figure I. Lead inblood QC sarnplesana$sed at natiorwlinstirutes togetherwith themonitoringsamples.Acceptan-ce interyat indica-ted by broken lines.

Figure 2. Cadrniuntin blood QC samp-les analysed at na-tional institutestogether with the

a 5.0

3n'o

E 3'0E 2,0b i.o.85 o.o

^ 5.0p: 4.0sg 3'09 2.0b r.o

2.4 5.0 4.0 5.0vofncc (H eAA,

QC5+6 Swsdcn QC5+6 Yugoslorio

QC5+6 Yugoelovio


25/83

9roq.t 21!P$ r EooE'2-gogoEo

'soEq.f. 24S.,,, t ,i ' ,g'Io

rso;P roo3IE5et!o

rsolc5'$ rooootEsoFIPo3o

$ rsoS)3,rooI3Eoobgo

Rcfcrrncc volucr (ng

23

Figure 3. Lead inair fiIter QC samp-les arwlysed at na-tional institutestogether with themonitoring sunples.Acceptance nterttalindicatedby brokenlines.

Figure4.Cadrniuntin air frlter QCsamplesanalysedatnational institutestogether with themonitoring santples.Accepnrrce ntentalindicated by broken

9toq.&24s,,ooE,,g6!o

0 6 1 2 l E 2 4

Rcfcrunccvolucc (ng Alr4fltcr)

QC4+5 Swcden


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24

jd{E()s!o=gboEIJ

4+5 Swedon

2.40.0

Figure S. I-eadandcdrniwn in dusteCsamplesanalysedatnational irwtitutestogether with themoninrtng sarnples.Acceptancenterryalindicatedby brokenlines.

All theregressioninesfor leadandcadmium n rhe7 diet ec samples, xcept hene or lead rom the nstirute,inYugoslavia,-wereaccepted ccording o theMAD criteriased figures6 and 7)' The Yugosliviun *sr"ssion line for leadwasoutside(below) thecceptancenterval in the high concenffutiln range,but the resurtswere better han theesultsof the threeQc roundsor the trainingphase.The error of the methodwas 17 ugb/kg and l3 ug Cd&g for the ur"rpr*J aa anatyses.The regressionines basedon theanalysisof faecesec samples g samples) romhe institutes n china, swede-nand Yugosiaviawere acceptedaccord.ingo the MADriteria used figures8 and9). Trre nstittite n Japananalysed4 faecesec samples nly.heresults or leadwereaccepted ut the efession line for cadmiumwasslightly outsideabove) he acceptancenterval in the higrrJoncenradon range.The averageerrorsof theethodoratt heacceptedeC resutrsirr d;ffi;;*i f",*ht ando.osugCd/gdryeight.

Rcfsruncsvofucr (14 pb/g d.v,) Rafaranc*vcfucs *q Ca/g a.w.)


27/83

25

$ +oogh.*so 200gE3 , 1 0 0!o

a: 100ttJhr*so 200o=Eb 1 @oEEoJ

45 4oog) soosg 200I9 , 1 0 0.9EIo

4: 4000J) sooso 200o:'33 1003B!o

4: 750$ too(,$ +soI toogE'*go

Figure 6. Lead indiet QC samplesarutysedat rwtionalinstitutes togetherwith themonitoringsamples.Acceptan-ce interval indica'tedbybrokenlines

FigureT. Cadmiwnin diet QC samplesarutysedat nartonalinstitutes togetherwiththe monttoringsamples.Acceptan-ce interttal indica'tedby broken ines .

QC 4+5 JoPon

Rcfcrunocvolucr (Pg eU/kg a.w.)Rderunocvolucr (rrg Pbr/k dJ.)

Rcfcrunccwlucr (trg Pbr/kgd.w.) Rcforrnocvolucr (Pg Pb/kg d;u.)

QC4+5 Chinq

Rcfcrcnccvolucr (Pg Cd/tg C.w.)

750600450500150

0

-?!E!(,sttEboEoD5

750600450500150

0

+I!o--(,st.3IboEI3

Rcfcrunccvoluce (14 H/Tg d.Y,)

Rcfcturcc wlrrcc (Pg C


28/83

QC4+5 Chino

Rcfcrcnc. vofucc Q4 Pb/g d.y.)

26

-? 1 6!Ol

i E 1 2so 6o5Et'. 1oEEoJ

3rt{f , rzso B3Eb 4go

-: 1 6orF*so BgEb 1.9eEo

3rt- oF ',sg8Ib 4IgEoJFigure 8. Lead infaecesQC samptesanatysed natiorwlinstitutes togetherwith themonitoringsamples. cceptan-ce ifierval indica-tedbybroken ines.

Figure 9. CadmiwninfaecesQC samp-les analysed atnational institutestogether with themonitoring samples.Acceptance ntertal

? e.o$ n.us

3 r.o{E 4.ss

QC4+5 Chino

QC 4+5 Sweden

33t!(JsgIb.g5

3 r.oE 4.ss

Rcfcr.cnoc ufucr (14 Pb/g d,v.)

Rcfcrrnoc vuluq (14 Pb/g d,v,)

QC4+5 Yugoslovio

Rcfcrrncc ofuca (tn eb/g a,r.,)

Rsfcrrncc wfucr (14 A/g d,y,)


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27

3.2.2.Leadand cadmium n blmdTheconcentrations f leadandcadmiumn theblood samples f thewomenat thevariousHEAL sitesaregiven n tables4 and5.

Table4. Concentrations f lead n blood

TMALsite Number ofsubjects ugPbIMedian

BeijingStockholmYokohamaZagreb

1215t2t7

732y3L50

208.3

L2L7

69283247

48 - t2415- 413- 6025- 101

a) Meanof results rom days1(30ugfl)andg (29 uel)

Table5. Concentratioru f cadmiumn blood

IIEALsite Numberofsubjects ug Cd/tS.D. Median Range


T215T2t7

0.60.3.1.64.7

0.280.160.634.25

0.50.31.50.8

0.2 1.00.1 0.80.8 2.90.2 1.1

a) Mean of results from days 1 (0.3 ugn) and g (0.3 ue/t)

There was no significant difference in the blood lead and blood cadmium concen-trations betweendaysone and eight in the swedish srudy.


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28

3.2.3. Exposure to airborne lead and cadmiumThe concentrations of lead and cadrrrium in thc inhaled air were calculated by

dividing the amountsof lead andcadmium on the filters used n thepersonal air monitorsby the rotal volume (mt) of air filtered during the%l hotu sarrpling perid. There werelarge variations in the concentrationsof lead andcadmium in breathing zone air both be-tweenHEAL sitesandbetweensubjectsat oneandthe sameHEAL site (tables6 and7).There were also large day-to-day variations in the air metal concentrations-

In yokohama, the air monitoring wascaried out using stationary samplen, placedin the living rooms of the 3 subjects.The particles wre collected on quartz fib're filtersinstead of the membrane filtcrs provided by the TCC. The average indoor air con-centrarionof leadwas 19ngPb/m3and herangewas 19-20ng Pb/m3.The averagendgorair concentrationof cadmium was 1.9 ng Cdlm3and the

rangewas 0.9-2-5 ngcd/m3.

Table 6. Concentratiors of lead in the breathing zoneair (persorul ntanitorinil- :

rMALsite Number ofsubjects Mean'ng Pb/m3

Range RangeMedian weeklY dailYaveragesb averages"s.D.

BeijingStockholmZagreb

20t4

t215t7

116d&

4L2 195

11866

400

77 r53 21-3 842-94 15-169140-840 0-2530

a) Mean of the weekly averageair concentrations for all subjectsb) Rangeof the weekly averageair concentrationsamongsubjectsc) Range of all daily averageair concentrationsmeasuredd) Six of the subjectswere monitored for 4 days only


31/83


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30

Table 9. Estimateddaily absorptionof cadmiuntollowing inlntation of cadmiuntcontaining articles.

HEALsite Number ofsubjects ng fr absorbed/24S.D. Medianean' Rangeb

BeijingStockholmYokohama"Zagteb

t2153

L7

7.95.2

12.529.2

2.81 .1

15.4

7.25.2

22.4

5.0,.14.03 .3 '7 .26.0,- '16.511.1=64.2

a) Mean of the averagedaily absorptionfor all subjectsb) Rangeof the averagedaily absorptionfor all subjectsc) Stationarysamplerswere used

3.2.4. Exposure o leadand cadmiumvia the diet, I . . . . .The averagecontentsof lead and cadmium in the duplicate diets cotlected'byrtheI{EAL studygroupsaregiven n tables10and 11.Duplicatediet datawer rnissing or twcsubjectsn Beij ing. .:: , , ' : : , : : i i :' ' : , , : : ; , ; , . . ' ,,, , ,

Table 10.Lead in the daily duplicate diets including beverages collectedby'the,HEALsmdygroups.

HEALsite Numberof subj. ug Pb n dailydietsS.D. Median Rangeb Range"'


10153

L7

46263T15

187.9

7.2

4l26

15

29-9\3-44

26-346.t-37

L2-1744.4-13012-ffi2.r-99


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TableIr' cadmiurn n thedaityduplicatediets,ncludingbeverages,ollectedby theEAL studygroups.

IIEALsite Numberof subj. Mean" ug Cd n dailydietsMedian Rangeb Range".D.BeijingStockholmYokohamaZagreb

20 2.98.5

1015

7.1 7.18 .1.1.5

1.4

3.87

5.4-8.9 3.0-125.7 r4 1.8_5617-22 8_33

8.0 3.s- 9 r.5_37a) Mean of averagecd in daily diets (basedon T daily diets) of all subjectsb.)l*ge of averagecd in daily diets of all subjectsc) Rangefor all daily duplicate diets

Assuming that Lovoof the ingested ead is absorbed n the gastrointestinalftacr, itanbeestimatedhaton average.6, 2.6,3. il-l"J .il thedaily ngestedeadwasbsorbed y the women n Beijing, stockholm,yokoiaml *d ngJi,respectively.Assumin a Svogastro-intestinala'usorptionr cadmium, t can be estimatedhat onverage '35' 0'43' 1'0and 0'42ugof thedaily ingested admiumwasabsorbed y theomen n Beijing,stockholm,yokohamu*d z^lgra,respectively.It is obvious rom tables10and11 hat herewere arge nter-individualandday-o-davvariationsn the ntakesof leadd;;d-il. ;;; 10showsexamples f the31l.jl;1avvariadonsn the ntakesf leadandcadmi;*;;*tt,i ,iro, periodn

Figare 10. Examp-le of day-to-dayvariations in thedietary intakes of


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3.2.5. Elimination of leadand cadmium n faecrcs :Theaverage ailyeliminationof leadandcadmium ia faecesn thevariousHEAI

studygroupss given n tables12and13.Tabte12.Averagedaily elimirntionof leadviafaeces.HEALsite Number ofsubjects ug Pb eliminatedS.D. Medianean' Range


10153

t7

42b23"304y

159.45.9

23 50

432L

L7-&10-4023-348.s-112

a) Mean of the averagedaily elimination of all subjectsb) Four daysper subject.Coloured marker not usedc) Sevendaysper subjectd) Four daysper subject

Table 13. Averagedaily elimination of cadrniwnviafaeces.

FIEALsite

Number ofsubjects Mean'

ug fr eliminatedS.D. Median Range

BeijingStockholmYokohama

Zagreb

10153

L7

7.s8.4"

33b15d

2.32.0

116.7

7.58.7

15

2.3-t05.5-r226-46s.0-25

a) Mean of the averagedaily elimination of all subjectsb) Four daysper subject.Coloured marker not usedc) Mean of sevendaysper subjectd) Four daysper subject


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33

Some of the first faeces sanrplescollected contained much more lead and/orcadmium than the correspondingfrst duplicate diets. In the Chineseand the fapanesestudiescoloured markers were not used. Therefore, the high pb and/or Cd content in thefirst faeces samples may indicate that the faeces collected during days 3-6 did notcorrospond to the diets of the four first days of the sampling period. In the other studygroups' the carmine marker may havebeen mixed in the stomachwith food ingested priorto the start of the duplicate diet collection. The Swedish monitoring periods stafied at3 p.m., at which time also thc carmine marker was ingested.Ttrus,-a high lcad and/orcadmium content of the food and/or beverages ngested earlier that day could very wellhave influenced the first coloured faeces sample. Therefore, the firsi coloured iuo6sampleswhich greatly exceeded he correspondingfirst duplicate diet with respect rocontentof lead and cadmium were excludedA comparison of the average daily dietary content of lead and cadmium and theaveragedaily faecal elimination is shown in tables 14 and 15. In the study groups inBeijing and StockholmaboutW%o f thedaily ingestcdleadandalmostall of the ngisredcadmium were recovered in the faeces. n Beijing and Yokohama coloured markeri werenot used n the faecescollection (4daysper subject),which may explain the relatively highstandarddeviations in the aecal elimination, expressedasapercentageof thedaily intake,aswell as he high faecalelimination of cadmium in theJapanrr" rtuJy. In the sruiy grou;inZagreb the average aecalelimination of leadwas nrore thanthree times higher than thiaverageead contentof theduplicatediets. The faecalelimination of cadmium was abouttwice the averagecadmium contentof the duplicatediets. '

Table 14- Comparisonof theaveragedaily dietary intakeof lead (basedon theduplicatediet analysls)and the averagedaity faecal elimination.

HEALsite Numberof subjects Dailyintake,ug PbDaily faecalelimination,Voof intake

ug Pb Mean S.D. RangeBeijingStockholmYokohamaZagreb

49. 42'.26b

1015

93 29

4y

23b

346 17030

65- 5065-t2664-106118-738

182T

9187

L734,15"

a) Meanof four days or eachsubject.Colouncdmarkernot usedn the faeces ollec-tionb) Meanof seven ayspersubjectc) Meanof four daysper subject


36/83


37/83

35

Beij ing Stoc|dlolm Zagreb

Figre 11.Daihy b-sorption of lead esti-mated from the(mlountsnair,dup-Iicate diets andfae-ces.

Figure 12.Daily ab-sorptionof cadnthanestimatedfrom thearnountsn air, dup-licate dietsandfae-ces.

ElElFaecesmDiet-Fl i r

@lFaesDiet0.00 Bei ine Stocldrolm Zaereb

tr3Hir


38/83

36

There was no significant correlation between the concentrations of lcad andcadmium in blood and the estimated total daily absorbedamountsof lead and cadmium(frgures 13and 14).The absorbedamountsof leadand cadmiumwere estimated rom theamounts of the metals in breathing zone air and in faeces"200

1 0090893o 60:soCL(rr 30i-

20

i* l *r

3 4 5obsorbed pg Pb/doy

x Beijinga Stockholmr Zogreb

AaA A

4t

obsorbedx Beijinga Stockholm

A6 r f Ja l Figure 73.Concen-trations of lead inblood n relationtothe (Nerage totaldaily absorptionoflead,esfurutedfromtlrc anwuntson air

filtersardinfaeces.Each data pointrepresentshe ave-rage daily absorp-tion byonewornan.

Figun 14. Concen-trationsofcadrntunin blood n relationto the6)erage otaldaily absorptionofcadmiwn,estimatedfromtfu arnountsnair fiIters and infaeces. Each datapoint representshe(Nerage daily ab-soirption by onewomfln.

.Itoo-o\EC)c'lc

1000800600400

ng Cd/doy


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4. DISCUSSION4.1. Methods for exposure monitoring of readand cadmium4.1.1. Study design and sample cottection

The aim of the present study was to test and demonstratemethods for integratedexposuremonitoring of lead and cadmiurn. The monitoring involved the collection ofduplicate diets, airborne particles (personalsampler), blood and faecesduring a studyperid of a week. At most HEAL sites the greatestproblems were encountered n thecollection of airbome particles. Most commercially available personal air monitoringequipment sdesigned or measruements f occupationalexposwewith samplingperiodsof abouteight hoursat the most.Therefore, thepump bauerieshadto berechargedevery6-8 hours' As a consequencethepumpshad o beconnected o themainsmostof the timewhenthesubjectswereat homeor sitting in their offices. Thenoiseof theoperatingpumpsalsogaverise to somecomplaintsandsomeof the subjectscpuld not keepthe pump nearthe bed at night, in somecasesnot even in the beoroom.Attempts to insulate the pumpsin order to decreasehe noisewere not complctely successful.

Normally, dietary exposure o pollutants is estimatedby analysingduplicate dietsor "market baskets", or from the concentations in individual foodstuffs and fbodconsumption data. The latter requires information on concenffations of pollutants inessentiallyall foodstuffs. The greatday-to-dayvariation in thedietary intake of leadandcadmiumfound in this study ndicates hata ew foodstuffs (probablynorstaple oods)cancontribute a large part of the total intake of lead andcadmium. It hasbeenreportedthat,in theUSA, more than500foodsmust beanalysed o cover90Vobyweight of thetotal diet,andalmost 1000 oods to cover95vo(Pennington,1983).Furthermore, hedietary intakecalculated from the concentrations n individual foodstuffs and food consumptiondatamay not take into account the differences in concentrationsof pollutants in differentsamplesof one and the same oodstuff.

The duplicate diet method will most likely grve a better estimate of the dietaryintake, especiallyat the ndividual level. However, in duplicatediet studies here s ariskthat the subjectsmay declease heir food intake andchange heir food consumptionpat-terns' In countries like China where, especially at home, *a is usually not servedasacompletedish on individual plates,as n the westerncountries, hecollection of duplicatediets may be more difficult.In Beijing and Stockholm aboutX)Voof the lead ingesteddaily and essentiallyallof the ingestedcadmium wererecovered n the faeces.Assuming u iovogastrointestinalabsorptionof leadand|%oabsorptionof cadmium, hedata ndicatetrrat heauplicatedietsreally reflected the diets consumed.The situation in Yokohama is difficult to evaluatesinceonly threewomenparticipated n themonitoring andcolouredmarkerswerenot usedfor the identification of the faeces hat corresponded o the collected food. rnZagreb theaveragedaily faecal elimination of lead and cadmium far exceeded he averagemetalcontentof thedaily duplicatediets.The reason or this discrepancyhasnot been ully elu-cidated' A review of the collection of food and beveragesdid not indicate incompleteduplicate diet collection asa major reason.Also, the concentrationsof leadandcadmiumin the duplicate diets were confirmed by analysesof someduplicate diet samplesat the


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TCC. Basedon the air measurements f lead andcadmium t can be estimated hat onlyabut 5-t0Voof thefaecalleadandlessthan Toofthefaecalcadmiummayhaveorigr-natedfrom particles which hadbecn nhaled and thencleared rom the respiratory tract.Therefore t seemsikely thattherewasa significantperoral exposureo leadandcadmiumfrom other sources han the diet, e.g. dust.Sincethe possibility of peroralexposureother thanthe dict can neverbe ruled out,the use of faecal lead and cadmium nrcasunementor validation of the duplicate dietcollection is limited. The large day-to-day variation in the dietary intake of lead andcadmium and the large variation in the rate of elimination of the metals also makevalidation ditficult. Even with the useof coloured markersthe faecescollected did notalways correspondexactly to the food ingestedduring the samplingperiod.On agroup basis, aecal eadandcadmiummay be usedas an ndicator of the total

intakeof leadand cadmium.Faeces ollection is considerablycheaper&fld,probably, lessinconvenientfor the subjects nvolved than the duplicatediet collection, unless herearecultural reasonsspeakingagainstfaecescollection. Furthermore,faecescollection willnot influence the food consumption pattern to the same extent as the duplicate dietcollection. However, therea^re ifferences n defaecationhabitsbetween ndividuals andoften betweendays n oneand he same ndividual. For somesubjects,defaecationbecamemore irregular thannormal during the monitoring perid, especiallyduring the first days.Therefore, the longer the faecessampling period, the better the estimate of the dailyamounts ngested.

An evaluationof thequestionnairesand ecordsused n thisstudyhasnotbeenperformed"Evaluation of themonitoring data n relation to the nformation collected n the food anddaily activity recordswill be madeat a national level.After completion of the samplecollection, theparticipating women were intervie-wed about the problems encountered,as well as the positive aspects of the samplecollection procedure. The importance of motivating the subjects participating in themonitoring, i.e. giving detailed nformation about heaim anddesignof theproject beforethe startof thesample ollection,wasconfirmed.The participants lsopointedoutthat hepossibilities hey had to discussany problems nvolved in the sampling,as well asorherexperiences, .g. comments rom other passengers n the bus/train/subway,made thesamplecollection less nconvenient.Our impression s that the women participated n theproject with greatenthusiasmand ntercst. In Stockholmand Tagreb he local televisionservicecovered he monitoring projects,which obviously encouragedheparticipantstoa grcat extent.

4.L.2.Analysis of lead and cadmiumTheexternalQC programmesduring the training phaseshowed heneed or carefulchoice of analytical echniquesas well asanalytical raining.Severalof theparticipating

institutions improved their analyticalperformanceconsiderablyduring the 3-4QCroundsof the training phase.Even institutionswith previousexperience n the type of analysesinvolved discoveredproblemsthat had to be solvedbefore the analysesof the collectedsamplescould start.


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Most problerns were encountered n the analysis of diets, due to their complexmatrix and the low levels of lead and cadmium. Also the analysis of air filten wascomplicateddue to the the small amountsof metals collectedduring the Z4h samplingperiods with the useof low volume samplers.4.1.3. Quality control

The method used or the analyticalperformanceevaluation gives the upper limitsfor the systematicerrors n themonitoringbutu.The maximum allowable deviationof theregression inesof reportedversus eferencevaluesof the QC sampless oftendeterminedby thesensitivityandaccuracyof theanalyticalmethod.Forexample, theexperience romthe QC activities in the HEAL pilot project shows that for lead in blood (ug pb/l) ex-perienced aboratoriescanmeet heMAD criteria y = x t (0.05x + r )), which go**trmthat a reportedmean blood lead value of, for example, 50 ug pb7l . ith gOVofrobabilitylies between37.5and62.5ug PbA.For cadmium in Lrooo (ug Cd/l) well experiencedandequipped aboratoriesmer the MAD criteria y = xt (0.05x i A.D,which guarantees hata reportedmeanblood cadmiumvalueof, for example,0.5 ug Cd/, with iOEoprobabilitylies between0.28 and}J}ug Cd/.The regressionmethd may also give valuable nformation on the typeof error. Forexample, a regression ine parallel to the ideal line {}.,= x) indicates an absoluteerrorcausedby e'9. a falseblank valueor inadequatebackgroundcorrection.A slopedeviating

from 1'0 indicatesaconstant elative "ooidu, to e.g., ncorrect standardsor errors n theconcentrationsof the standards.The experience rom the analyticalquality control programmewithin the UNEp/TVHO HEAL project shows that good analytical rrf;ance for a pollutanr in onernedium,e'8' lead n blood, s no guaranteeor goodperformancewith othermedia.Thus,it is important thatquality control sampleshavea matrix similar to thatof the monitoringsamples'Funhermore, the QC samplesshouldcover therangeof concentrationsexpectedto be found in themonitoring samples.Good analyticalperformanceat oneconcentrationis no guarantee or good performanceat higher or lowir ron""ntrations. Resultson oneor a few reference samples are not sufficient for the evaluation of the analyticalperformance' This was clearly demonstrated n the analysisof cadmium in air filters.

4"2. Routes and levelsof exposureAlthough thesmallnumberofsubjects tudieddoes ot allow a completeevaluationof the exposureto lead and cadmium in the generalpopulation at eachI{EAL site, theresultsof themonitoring studiesmay give afairly goodestimateof the exposuresituation.There s no reason o believethatthe selectedwomendiffer to any significant extent fromthe generalpopulation with regard to their exposure o lead and cadmium. Furthermore,acomparisonof theblood evelsof leadandcadmiumwith those ound n previousstudiesongroupsmore epresentativeor thegeneral opulation n theFIEAL areas tables16and17) ndicates hat thetotal exposureamong he selectedwomenwas similar to thatof thegeneral population. The average concentration of lead in blood of the women instockholm was considerably lower (about 507o) han that found in the UNEp/TrHo


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Biological Monitoring Project (Vatrter, lg82). However, this probably reflects a truedecrease n the general population's exposure to lead. Legislativ, *iurur"s taken inSweden n 1981.owered the muimum permitted level of lead in petrol from 0.4 to 0.15g/1,and n 1987unleadedperol was intnoduced.At presentabout3y7oof thepetrol usedis unleaded.Funhennore, food canswith lead-solderedsideseamshaveto a greatextentbeen replacedby canswith welded side seamsor two-piececans, .e. canswithout sideseams JorhemandSlorach, 1987).Already in 1984, he blood leadconcentrations n thesubjectswho participated n theUNEP/TIHO Biological Monitoring project had decrea-sedby 30Vo@linder et al, 1984).

The results on lead in blood in Beijing indicate an increasedexposure to leadbenveen 1981 and 1988, which may be related to the inceased ronsu*ption of petrolthere.Table 76- A comparison of the concentrations of tead in blood (ug Pbft) with thosereported n rwn'smoking women npreviow studiescanied out at thevariousHEAL sites.Arithrnetic meanvalues t ;.D. N= nrntber of subjects.

TIEAL1988

Nationalstudies

UNEPAMTIO1991-921

Beijing

Stockholm

Yokohama

Tagteb

73t20(N=12)29tL5(N=15)3L+12(N=12)50117(N=17)

&+t9(N=110)42!313(N=18)

59t19(N=118)$tZS(N=45)55t184(N=77)81t33(N=84)

l)Vahter,19822) Zheng,unpublished ata3) Elinderet al, 19844) Tokyo


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Table77. Acomparisonoftheconcentratiorsofcadmiuminblood(uSCdll)withthosereported in rwn-smokingwomen npreviow studies arried out at thevariousHEAL sitesAritlvnetic meanvalues+sD. N= numberof subjects.

IIEAL1988 Nationalstudies I.'NEP/VffiO1991-921Beijing

Stockholm

Yokohama

Zagreb

0.6to.zg(N=12)0.310.16(N=15)1.6t0.01(N=12)0.7!0.25(N=17)

0.610.32(N=110) 0.9r0.54(N=118)0.3!0.19(N=45)1.3t0.6tt(N=77)0.5$.3s(N=84)

1)Vahter, 98Z2) 7-heng t al, 19883) Tokyo

The total exposure o cadmiumdid not seem o havechangedsignificantly during thelast few yearsat most of the HEAL sitesstudied.The blood cadmium levels were aboutthe sameasthosereported in theUNEP/TfHO Biological Msnitoring project on lead andcadmium (Vatrter, 1982).However, in Beijing therer"r-, to havebeena decreasen theexposure o cadmium during the last ten years.This may bedue to theprohibition on theuseof cadmium asa stabilizer andcolour pigmcnrIt is obvious from the results that airborne cadmium conributes only one or a fewpercent of the total exposureof the generalpopulation at all the I{EAL sitesstudied.Forlead the contribution from air was somewhathigher, 5-1SVo, nBeding, Stockholm andYokohama, but still low compared o the arnountabsorbed rom the diet. In Ta,geb theconcentrationsof airborne lead were considerablyhigher than at the other HEAL sites,which is in agreementwith the airborne ead evels found both in the presentstudyand nprevious environmental air monitoring projects (uNEp/\lftIo, r9-gg).The estimaredpulmonary uptake of lead was almost twicc the uptake of dietary lead, estimated fromresultsof theduplicate diet analysis.However, it was only abouthalf of the total amountof lead ingested,estimated rom the analysesof faeces.The averagetotal dietary intake of lead at the different IIEAL sitesvaried from ap-proximately 4to LlVoof the Provisional TolerableWeekly Intake (PTWD proposedby an


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FAO/WHO Expert Group (WHO, L972).The correspondingcadmium valuesobservedranged from about 12 to 33% of the PTWI (WHO, 1989),The average ndividuat leadintake varied from about I to Ztvo of the PTWI, and the average n&vidual cadmiumintakevaried from about6 to 37% of thePTWI. For all theIIEAL sitesexceptZagrebthediet was found to be the major sourceof exposure to lead and cadmium.For many of the women studied, there was a greatday-to-day variation in the dietaryintake of lead and cadmium. One daily diet could contribute more than SyVoof the totalweekly intake of lead and cadmium. Identification of the food items responsible or thehigh peaks n the dietary intake of lead and cadmiummay help to desreasehe exposuresubstantially.Therewas no apparentcorrelation between heblood levels of leadandcadmiumand

the estimatedaverageabsorbedamountsof the metals.For cadmium, for example,therewasa tenfold difference n bloodcadmium evelsbetweenndividuals with about hesameestimatedaveragedaily uptake.Theremay be several easons or this. The study peridwas only a week, with large day-to-day variations in exposure,while the blood concen-tration of lead and especiallythatof cadmium reflect the exposureover severalmonths.Plasmacadmium is probably more relatedto recentexposure,but the concentrationsareoften below thedetection imit. Furthermore, here-uy U"greatvariations n gastrointes-tinal absorptiondependingon the type of metal compound ngested, hecompositionandamountof food ingested,nutritional status,especially ow iron stores.The chemicalformof themetalcompound ngestedmay also nfluence the blood concentrations. t hasbeenreported hatoysterfishermenwith high cadmium ntakefrom protein-boundcadmium nthe'oystershave ower bloodcadmium evelsthanexpected Sharmaet al, 19g3).

4.3 ConclusionsA pilot study, of the presentdesign and carried out on a small number of selected.subjects,may identify themain problems n the collection and analysisof different typesof exposuremonitoring samples,as well as the major routes of exposgreto lead and

cadmium.Such nformation is important for thedesignof a ull-scale studyon ar"pr"r"n-tative sampleof the generalpopulation.Furth"r-orl, the experiencegaineOshowsthat,althoughcostly and complicated, t is possibleto makecomplrable measurements n aninternationalscale.The experience rom the analyticalquality control programmeof the project showsthatit is important that QC sampleshavea matrix similar to that of the monitoring samples,that the QC samplesshouldcover the rangeof concentrationsexpected o be found, andthat one or a few referencesamplesarenot sufficient for the evaluationof the analvticalperformance.


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5. REtrERENCESAlexanderF\V, ClaytonBE andDelvesH'T(1974)Mineraland race-metal

balancesn children eceivingnonnalandsynthetic iets.Q J Med,NewSeries3:89-111.Andrds, Mdtivier H, I-anfenoisG, BoyerM, NoliH D andMasseR (19g7)Beryllium metalsolubility in the ung.Comparison f metalandhot-pressedformsby u vivo andb vitro dissolution ioassays. umanToxicol 6:2j3-240.

BellingerD, Irviton A, WaternauxC, Needleman andRabinowitzM (19g7)Longitudinalanalyses,ofrenatalandpostnataleadexposure ndearlycognitivedevelopment. EngJ Med 36:1037-1043.BruauxP andSvar:tengren (1985)Assessmentf humanexposureo lead:Comparisonbetweenelgium,Malta,MexicoandSweden.Reportpreparedfor UNEPAWIO by NationalSwedishnstituteof EnvironmentalMedicineandDepartment f EnvironmenmlHygiene,,Karolinskanstitute,Stockholnr" ndInstituteof HygieneandEpidemiology,Ministry of Health,Brussels.Camner ndBakke 1980)Noseor mouthbreathing? nvironRes Zl:394-39g.Chamberlain C (1985)Predictionof response f blood ead o airborneand

dietary ead rom volunteerexperiments ith lead sotopes. roc.Roy.Soc.London,B 224: l4g-Ig}.Chamberlain C, HeardMI, Little P,NewtonD, V/ellsAC andWiffen RD (1973)Investigationsnto lead rom motorvehicles.Environmental ndMedicalScien-cesDivision,AERE-R 9199,Harwell.ClarksonT'W,FribergL, NordbergGFandSagerPR (1988)BiologicalMonitoring,of Toxic Metals.plenumpress,Newyork.

CorteseAD andSpengler D (1976)Ability of fixedmonitoringstarionsorepresent ersonal arbonmonoxideexposure. A PollutControlAssoc26:1144.Dierich K, Krafft K, BornscheinR, HammondP,BergerO, Succopp andBier M(1987)Low-level fetal eadexposure ffecton nenrobehavioralevelopmentnearly nfancy.pediatrics80: 7ZL-30DornCR,Pierce O,PhillipsPEandChaseGR (1976)Airbornepb, Cd,Zn andCuconcentration y particlesizeneara Pb smelter.AtrnosEnviron L0:443-446.EliasRw (1985)Leadexposuresn thehumanenvironment.n: DietaryandEnvironmental-ead:HumanHealthEffects,Topics n environmental ealth,vol. 7. K Mahaffey Ed),Elsevier,Amsterdam.


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JorhemL, MattssonP andSlorachS(1984)Lead,cadmium, inc andcertainothermetalsn foodson theSwedishmarket.VArFfi a36:Suppl.3.JorhemL andSlorachS (1937)Lead,chromium, in, iron andcadmiumn foodsin welded ans.FoodAdditandcontam4: 309.316.JorhemLandSlorachS (1938)Thedesignanduseof qualitycontrolsamplesnacollaborative tudyof tracemetalsn dailydiets.FieseniusZ Anal Chem332:738-740.Jorhem , MattssonP andSlorachS (1988) rad in tablewineson theSwedishmarket.FoodAddit andContam5: &5_&9.LauwerysRR-(f83) Guidelinesor BiologicatMonitoring. n: IndustriaLChemicalExposure.R R Lauwerys ed),BiomedicalRrblications,Davis,California,u.s.A.LeeRE,PattersonRK andWagman (1968)Panicle-sizedistributionof metalcomponentsn urbanair.Environsci Technolz:Zgg_z9f'.Lind B, VahterM, Rahnster andBjdrsU (1988)Qualitycontrolsamplesor thedetermination f leadandcadmiumn blood, aeces,t Rlt"rsanddust.Fresenius AnalChem3i2:741_743.LundborgM, EklundA, Lind B andCamnerP (1935)Dissolutionof metalsbyhumanandrabbit alveolarmacrophages. r J Ind Med 42:642-&s. ,MooreM (1985) nfluenceof acidrainuponwaterplumbosolvency. nvironHealthPerspectives3: IZL-L26. -MushakP andCtocettiAF (1988)TheNatureandExtentof Irad poisoninginChildren n theUnitedStates:A Report o Congress, gency.forToxicSubstancesndDiseaseRegisury, .S. Deparmentof HealthandHumanServices,Atlanta,Georgra,U.S.A.

fnha*L^ielsenA, NybergK andCannner (19s8) ntraphagosomalH in alveolar ,macrophagesfter phagocytosis!g vivo and g Utrg of fluorescein-labelledyeastparticles.ExpLung Res14: Lg7 207NordbergGF,KjellstrdmT andNordbergM (1985)KineticsandMetabolism.n:CadmiumandHealth:A ToxicologicalAppraisal,Vol. I. L Friberg,C-GElinder,T Kjellstriim, G F Nordberg Eds).cRC hrrr, BocaRaton,Frorida,u.s.A.NordbergGF andNordbergM (1988)BiologicalMsnitoringof Cadmium.n:BiologicalMonitoringof Toxic Metals.T W Clarkson, Friberg,G F Nordbrg,P R Sager Eds).plenumhess, New york.PenningtonAT (1983)Revisionof theTotalDiet Study ood ist anddiets.Journalof rhe AmericanDietic Associationg2: 166-17i.


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VoorinenA (1983)Emissionof Ladby HighwayTraffic: LeadFixationandSpeciation, r,oceedingsf InternationalConferenceTleavyMetals n theEn-vironment",Heidelberg,1 159-162.WHO (1972)SixteenthReportof theJointFAO MIIO ExpertCommittee nFoodAdditives.TechnicalReportSeries505,V/orld HealthOrganizarion, eneva,Switzerland.WHO (L977)Reportof theMeetingof aGovernment xpertGrouponHealtfi-relatedMonitoring,WHO internal eportCEpn7.6,WorldHealthOrganizarion,Geneva,Switzerland.WHO (1981)Consultation n Health-related nvironmentalMonitoring,Geneva,22-24April 1981,WHO Int Doc No EFp/gL.LZ,WorldHealthOrganizarion,Geneva,Switzerland.WHO (1982a)Estimatinghumanexposureo air pollutants,WHO Offsetpublica-tion No. 69,world Healthorganization,Geneva,Switzerland.WHO (1982b)Humanexposureo carbonmonoxideandsuspendedarriculatematter nh,greb, Yugoslavia.EFPtgZ.33,WorldHealthOrganiz.tiorr,Geneva,Switzerland.

WHO (1982c)Humanexposureo SQ, NO, andsuspendedarticulatemaner nToronto,Canada. Fp/82.38,Worla HeatttrOrganization,Geneva,Switzer_land.WHO (1982d)Reportof ameetingof Government-designatedxperts n health-relatedmonitoring,Geneva, -lzMarch lg82.EFP/82.28,Woild HealthOrga-nization,Geneva,Switzerland.WHO (1983)Assessmentf humanexposureo environmental ollutants.EFp/83.52,world Healthorganization,Geneva, witzerland.WHO (1935)Humanexposureo carbonmonoxideandsuspendedarticulatemattern Beijing,People'sRepublic f china.pEp/gs.l1,world Healthorga-nization,Geneva, witzerland.WHO (1989)Thirty-thirdReportof the oint FAO/UfHOExpertCommittee nFoodAdditives.TechnicalReportSerie 776,WorldHealthOrganizarion,Ge-neva,Switzerland.ZhengXQet al (1988)Studyon BloodCadmium evelof Non-occuparionalExposurePopulationn China.Presentedn InternationalSymposium n En-vironmental ife Elements ndHealth,Beijing,china.Abs.p 90.YocomJE,ClinkWL andCoteWA (L971) ndoor/Outdoorir quality elationships.J Air PollutConrol AssocZL: Z5l-ZSg.


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ANNEXA. GENERAL NFORMATIONABOUTTHE HEAL SITESBEUING

Beijing,capitalof thePeople'sRepublicof China, s locatedon thenorth-westernedgeof thenorthChinaplain,betrveen115.25 nd I 17.30east-longrrude,9.2g-41.05north-latitude,with atotalareaof 16,800 m2.The otalpopulations g,7g6,001andthepopulationof theurbanareass 2,399,000.Theclimateof Berjing sof the emperate-conrinentalype.Spring April andMay)andautumn SeptemberndOctober)are athershort,whilewinter (NovemberoMarch)is rather ong.Theaverage nnual emperatures l!-lz"C, the owestaveragemonthlytemperatures -4 to -5'c in January. heaverage nnual rccipitations around650mm.Theground s coveredwith snow or about + oay, p", y"rr.Theoccupational istributio-nn percent f the otalnumber mployeds: technicalpersonnel 4'5,publicservices 0.4, rade5.5,agricultureZ}.S,indusurynd ansport19^0 ndothers .1.Chinahas ompletereedom r*hgion. Theresnospicial estrictionin foodhabits or theoverwhel*ittgmajorityof thepopularionn Beijin!, tne nhabitantslive primarily on commerciallyproauted *0. The-maincaloric intake s via cerealproductsThereareabout193,200 ars n Beijing,corresDondingo about20 carsper 1000inhabitants.Cycling s themainmeansoi t *rponution for the nhabitants.Recently,transportwith buses,rolleybuses,nderground nd ailwaytrains,aswell as rucks,hasbeen unher developedIn Chinameasuresavebeen aken o limit theemissions f leadandcadmiumotheenvironment. eadaddedopetrol s restrictedobelowI s/kg.Theres ead-free ilateach etrolstation. heconsumptionf lead-free etrol nnei;in! comprises boutgavoof the otalconsumption. heuseof cadmiumand eadasstabilizers ndcolourpigmcntsisprohibited'Although eadprpeand ead-solderedinscanbesignificant ources f leadexposure,t is notaproblem n China. *ad-pipes le veryrare,andmost oodcansarenot eadsoldered. esides,heannual onsomption f ,.nnrd foods s nothigh.Wine sanother ource f lead,but he eadcontentof all thewineontheBeijingmarketsbelowthehygienicstandard f food.Theaverage nnual onsumption f alloholic beveragesnBeijing,calculatedrom he otalsales,i zt.s litresp"rp"rron,of wh ch6Tvois eerand6.57os low alcoholdrinks.

STOCKHOLMThe surveywascarriedout in stockholm, he capitalof sweden.stockholm slocated t59"north-latitudend18'east-longituden hecoast f theBalticSea. he otalpopulation f stockholm,ncludingsuburbt,r t ,462,00awith 70,000n thecenrral rca.About20voof the nhabitantsn Stockholm reof foreignorigin.The otalpopulation fSwedens 8.4miltion(19g7).


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temperatureeached26.8'C in August, hehottestmonthof theyear.The owestmonthlymeanwas 5'6'C in January.The annualprecipitation n 1987amounted o 1 Z1gmm andthe annualmeanhumidity 68 percent.The period from mid-June to mid-Iuty is the rainyseason'n AugustandSeptemberYokohama s visitedoccasionallyby rainstormscausedby typhoons.Theannualmeanwind velocity in 1987was3.7 metresper second.Usually,north winds prevail in winter and southwestor southwest-by-southwinds in the otherseasons.

According to the Origin-DestinationSurvey (1985), passengercars are 10.70million x km/day and tnrcks,7 42 million x km/day. th"r, are about0.91 million cars nthe city, corresponding o 3 carsper 10 nhabitants. n addition, there s a well developedpublic transportationsystemwith buses,subwaysandrailways for cornmercial ransport.Yokohama is situated n the largest ittoral industri*. belt of Japanand is a majorindustrial centre. ndustry in Yokohama representsone of the principie industrial struc-tures of the counbry'consisting as it doesof u wide spectrum of industries such as oilrefining, transportequipmenq foodstuffs, appliancesand generalmachinery.To check heairpollution situation hecity operates16 ull-time monitoring stationsand eight automobile exhaustmonitoring stations.The latter, also maintained on a full-time basis,are ocatedalongmain roads.Fuel consumption evels andpollutant concen-trations at 4Dlarge ndustrial factoriesare measuredautomatically. Monitoring dataarecentrally recordedby telemetersattheAirPollution SurveillanceCenter.Guidelineshavebeen established to control emission levels of sulfur oxides and nitrogen oxides. Atpresent' sulfur dioxide emissions are kept at the level of the municipal-environmentalstandard 0'04 ppm per day on the average.However, the volume of nitrogen dioxides,which forms oxidantsandcauses hotoctremicator white smog, emainsata considerablyhigh level' In Japan he addition of lead to petrol has been banned since LgTSand hedischargeof cadmium into theenvironmenthasbeenstrictly prohibited by the BasicLawfor Environmental Pollution Contnol.As for water pollution, toxic substancessuch ascyanide andcadmium areno longerdetected n the indusrial waste iquids, thanksto rheregulatory and supervisory measures akenby the municipality and oiher authorities.

ZAGREBThe FIEAL pilot phasestudy has been carried out in Z-agreb,he capital of theRepublicof Croatia. t is situatedat 15'59'easternongitudeand 45'49'northern latitude,between the south-westslopesof the 1035m high pft UrOrrednica and the,vukomerichills, on both banksof the sava river, Lzz-160m above sea evel.Zagrebhasa moderatecontinental climate. Measuredover a thirty-year period theaveragemonthly temperature asbeenzl.3"Cin July and0.5"C n lanuary. The averageannualprecipitation is 903mm. Thereareon theaverage !46rainy,28 snowy and59cleardays and 1800hours of sunshineper year.Greater Zf;geb covers an areaof 1709km2,of which 859 km2 s agricultural landand594km2iscoveredbywoods.Ithasapopulationofoverg00,000,aboutT}Voofwhomlive in theurban zeaarea 139kmt). ropuiadon densityvaries rom 45,000 nhabitantsperknz in the inner city to a two digrt number in suburbanparts.


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Out of 410,000 employed persons 35Vo are in industry and crafts, ll.S%o inconstruction,6.5Von transport,l5.5%on tradeand ourism,20.5Voneducation,science,health care and administration and 0.6% in agriculttue.About 70Voof the employed do not live in the cornmunity in which they work andthey have to cornmute to the workplace. Most people travel by tram, the rest by bus orprivate car.In 1986 here were about216,000 motorvehicles, X)Voof which areprivatelyowned. Of the total 175,000are personalcars, 1,154buses,23,0m tmcks and specialvehicles and 2400 motorcycles. There arc,247 ramcars and 473city buses ransponingdaily on the average630,000 and380,000passengersespectively. nrushhours the rafficdensity in narrow streets n the city centremay reach more than 10,000carsper hour.Theleadcontent of petrol is 0.6 gll.l-ead-free petrol is available(but s usedmostly by foreigntourists).Zagreb nhabitantsconsumemostly (in descendingorder) milk and dairy products,vegetables,bread and cereals, nrit and meat. As far as alcoholic drinks are concerned,they prefer wine (averageconsumption 17.5Uyearby a householdmember).The main sourcesof lead are food and beverages, ollowed by car exhaustsandcigarette smoking. The latter is a major source of cadmium. High lead intake mayexceptionallyoccurby drinking homemadebrandy distilled from solderedcopperkettlesor through theuseof lead glazedpottery for storingfood. Watercoming from public watersupplies contains on the average1.3 ug Pb and that from individual wells from 4 to

11 ug Pb/I. The concentrationof lead inhgreb ah varies on the average rom 10 ug/m3at the busy crossings o 0.5 ug/m' in the generalatmosphere.The lead content of cigarettes varies depending on the quality class from 1.1 to2.t ug/cigarette and that of smoke condensate rom 0.10 to 0.15 ug/cigarette. Thecadmium content of the same brands of cigarettes varies much less: from 2.5 to 2.6ug/cigarette and that of smoke condensate rom O.22 o 0.27 ug/cigarette (IviEic' et al,1985). Flowever,the exposure o cadmium through smoking canresult on average n a 5-6 fold increase in the blood cadmium levels of the adult general population in Zagreb(TeliSmanet al, 1986).

ReferencesIvidic', N., Tomic',L. andSimeon,V. (1985)Cadmium nd ead n cigarettes ndin smoke ondensate.rh. hig. rada oksikol ,36: 157 l6y'.Teli5manS,Azaric'J andPrpic'-Majic'D (1936)Cadmiumn bloodasan ndicatorofintegrated xposureo cadmiumn the rubanpopulation.Bull Environ Contam


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ANNEX B. GUTDELTNESFOR SAMPLTNG PROCEDURESFOR BLOOD,FAECES,AIRBORNE PARTICLES AND DUPLICATE DIETS

UNEPflIHO GlobalEnvironmentMonitoring ProgrammeHUMAN E)(POSUREASSESSMENT OCATION

TIEAL PROJECT

CADMIUM AI{D LEADEXPOSUREMONITORING

GUIDELINE S FORSAMPLING PROCEDURES

ANDS AMPLE TIANDLING AND S TORAGE

Technical Coordinating Centrefor MetalsStockholm - Sweden

January,1988HEAL TCC Sweden


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BLOOD SAMPLINGThe concentrationsof cadmiumand ead n blood are nonnally very low. Therefore

it is extremely important that contamination of the samplesbe avoided. The followingrecommendationsconcernmainly measureso be taken n order to avoid such contami-nation.Laboratories and personnel

Tobacco smokeoftencontains cadmium in amounts hat may seriously contamina-te the blood samples.Therefore, t is anabsolute equirement hat thesampling, reatmentand analysis of blood samplesarecarriedout in aroom wheresmoking is prohibited.Allpersonnelhandling the blood samplesshould be non-smokers. f this is not possible,smoking personnel should wear a clean laboratory coat and cover their hair duringsampling and handlingof blood samples.

Protective gloves of Pb/Cd-free material should always be used when handlingblood samples.See separateecommendations Handling of potentially contagioushumanbiologi-cal material.

Procedures and equipmentAccording to the Pb/Cd protocol blood sampling should be carried out on themorning after the ast day of the testperiod. If possible,blood should also be taken on themorning of the first day of the testperiod.It is recornmended to collect the blood samples not earlier than 2 hours afterbreakfastBefore the blood sample s taken, the skin should be carefully washed and thencleaned with disposablenapkins containing metal-free disinfectant (70Vo ethanol orisopropyl alcohol is

lead cadmium on health

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