ScienceoftheTotalEnvironment424(2012)316–321 ContentslistsavailableatSciVerseScienceDirect Science of the Total Environment journal homepage: www.elsevier.com/locate/scitotenv Factors influencing blood mercury levels of inhabitants living near fishing areas☆,☆☆ Ching-Chang Lee b,c, Jung-Wei Chang b, Hsin-Yi Huang b, Hsiu-Ling Chen a,⁎ aInstituteofOccupationalSafetyandHazardPrevention,HungKuangUniversity,Taichung,Taiwan bDepartmentofEnvironmentalandOccupationalHealth,MedicalCollege,NationalChengKungUniversity,Tainan,Taiwan cEnvironmentalTraceToxicSubstancesResearchCenter,MedicalCollege,NationalChengKungUniversity,Tainan,Taiwan a r t i c l e i n f o a b s t r a c t Articlehistory: Methylmercury(MeHg),awell-knownneuro-toxicant,isusuallyemittedbyindustrialandotherman-made Received3November2011 activities;itisingestedwithseafoodandshellfish,andaccumulatesinthehumanbody.Theaimofthisstudy Receivedinrevisedform3January2012 wastocomparethedifferencesinbloodlevelsoftotalmercury(T-Hg)andMeHginresidentsof4coastal Accepted23January2012 sites and 4 inland sites around Taiwan. Meanwhile, the potential question is warranted to find out the Availableonline22March2012 association between dietary intake and MeHg accumulation. We found that coastal residents had significantlyhighermeanbloodT-Hglevels(mean:16.1μg/L,range:0.9–184.9μg/L)thaninlandresidents Keywords: (mean: 11.8μg/L, range:0.8–146.6μg/L). Thesame was for blood MeHg levels: coastal residents (mean: Totalmercury Methylmercury 16.5μg/L,range:0.9–184.9μg/L),inlandresidents(mean:11.8μg/L,range:2.1–133.4μg/L).Theseelevated Blood levels were positively associated with seafood and shellfish consumption. However, the nature of their Coastalandinlandinhabitants residentialareamayalsobeanimportantfactor,becausethehighestT-HgandMeHglevelswerefoundin Fishconsumption residentsofarelativelynon-industrializedarea.Toprotectvulnerablepopulation—especiallychildrenand Industrialpollution pregnantwomen—itisimportanttoknowwhetherlocallycaughtorraisedandconsumedfishhasanysource ofHgandMeHgpollution. ©2012ElsevierB.V.Allrightsreserved. 1.Introduction comefrommainlandChina(Fangetal.,2009).Therefore,bothlocal industrialemissionsandoverseassourcesofHgpollutionaresignifi- Mercury (Hg) occurs naturally and because of human activities. cantcontributorstoTaiwan'senvironmentalHgcontamination. OneprimarychemicalformofHgismethylmercury(MeHg),awell- ThemeanbloodHgconcentrationinCambodianswas5.2–58μg/L, known neurotoxin. Approximately 300,000 personal computers are lowerthanthoseinHg-contaminatedorhighfish-intakeregions,but disposed of every year in Taiwan. The Hg contained in these higherthanthoseinnon-contaminatedregions(Agusaetal.,2007). computersmaycontaminatetheenvironmentiftheyarenotproperly HgaccumulationwasestimatedbasedontheHgcontentinfishand disposedof(Leeetal.,2000).Moreattentionshouldbepaidtohow on the daily fish consumption by women of childbearing age and thecurrentcomputerrecyclingsysteminTaiwancontributestoHg pregnant women because Hg might be transferred to the fetus via pollutionofthelocalenvironment. cord blood or to the newborn via breastfeeding (Bjönberg et al., There is considerable Hg pollution in northern Taiwan; this is 2005). For example, Hg levels decrease during lactation, which is primarily anthropogenic contamination, and re-emission may exist probablyattributabletoitsbeingexcretedinmother'smilk(Vahter because of Hg contamination in soil surfaces (Kuo et al., 2006). In etal.,2000).InTaiwan,21.6%–24.3%and45.6%–57.4%oftheestimat- southern Taiwan, a cross-sectional study (Chang et al., 2008) eddailyHgdosesinthosewhoconsumetypicalandlargequantities reportedthatelevatedbloodtotal-mercury(T-Hg)andMeHglevels ofseafood,basedontheMonteCarlosimulation(Chienetal.,2007), in 240 adults living near a deserted chloralkali plant had polluted exceedtheUSEPA'sreferencedose(0.1μg/kg/day).However,inother the environment with a substantial amount of Hg 20years before. cases,extremelyhighHgaccumulationinspecificpopulationscannot Both studies showed that Hg contamination has occasionally beexplainedbyfishconsumption,whichindicatesthatsomeother occurred in Taiwan. The atmospheric Hg detectable in Taiwan may source of Hg contamination exists (Agusa et al., 2005). Meanwhile, in addition to the fact that fish consumption might be the major ☆ Interestdeclaration:Allauthorsdeclarethattheyhavenocompetinginterests. source, age and racial/ethnic differences were also noted as factors ☆☆ Ethicalconsideration:ThestudyprotocolwasapprovedbytheHumanExperi- affectinglevelofHgcontamination(Caldwelletal.,2009). mentandEthicsCommitteeofNationalChengKungUniversityMedicalCenter.The AtmosphericHgsamplinginurban,suburban,rural,andindustrial participantsprovidedwritteninformedconsent. areashasshownthatthehighestlevelwas30ng/m3inurbansites, ⁎ Correspondingauthorat:InstituteofOccupationalSafetyandHazardPrevention, upto22ng/m3inruralsites,upto24ng/m3inindustrialsites,and Hung Kuang University, 34 Chung Chie Road, Sha Lu, Taichung 433, Taiwan. Tel.: up to 90ng/m3 in suburban sites in Taiwan (Kuo et al., 2006). In +886426318652x4010;fax:+886426319175. E-mailaddress:[email protected](H.-L.Chen). addition,thereisconsiderableatmosphericHginspecialareas,such 0048-9697/$–seefrontmatter©2012ElsevierB.V.Allrightsreserved. doi:10.1016/j.scitotenv.2012.01.049 C.-C.Leeetal./ScienceoftheTotalEnvironment424(2012)316–321 317 asminingareas(Fangetal.,2009),andlocalHgsourcesneedtobe 2.4.MeasuringqualitycontrolandqualityassuranceforT-HgandMeHg investigated. TheprimarypublichealthconcernisrelatedtoMeHgexposure. Eachanalyticalrunconsistedofamethodblank,aqualitycontrol, MeHg ingested and bio-accumulated with seafood, shellfish, and andsixunknownsamplesforqualityassuranceandqualitycontrol. freshwater fish have not been systematically investigated, even Dataqualitywascontrolledandassuredbyspikingknownamounts though fish and other marine foods are popular and frequently ofT-HgandMeHgintobloodsamplesbeforeanalyzingtheblood.A eaten in Taiwan. Therefore, to identify regional Hg contamination reference material, Standard Reference Materials 966 Toxic Metals levels,weinvestigatedthebloodHgandMeHglevelsinpeopleliving inBovineBlood(SRM966)(NationalInstituteofStandardsTechnol- in4coastalsitesand4inlandsitesaroundTaiwan.Wehaveincluded ogy, NIST) was used for quality assurance of T-Hg; the measured information about fish consumption and general dietary habits concentration met the certified values (29.7–33.1μg/L).The method to evaluate the association between dietary intake and MeHg detection limits of T-Hg and MeHg were 0.09 and 0.144μg/L, accumulation. respectively. 2.Materialsandmethods 2.5.Interviewer-administeredquestionnaire 2.1.Participantselection Each participant was asked to fill out a questionnaire about personal characteristics (gender, age, height, weight, occupational We chose eight locations around Taiwan to measure the blood history, neighborhood geography, pregnancy history, etc.), lifestyle T-HgandMeHglevelsinresidents:TaipeiCounty(north),Changhua (alcohol consumption and smoking habit), and dietary intake for County (west central), Kaohsiung City (south), and Yilan County the previous year based on a semi-quantitative food-frequency (east). In each location, one coastal and one inland townor village questionnaire.Fishandotherseafoodwerethemajoritemsthatwe wereselected.Theinclusioncriteriaforstudyparticipantswerethat selected for assessing the association between blood MeHg levels they were between 18 and 65years old and that they had lived in andconsumptionquantity.Thefishitemwasgroupedaslarge-sized the selected area for a minimum of 5years. Each study participant remoteseafish,small-sizedremoteseafish,small-sizedoffshoresea provided 20mL of venous blood after signing an informed consent fish,fish-farmfish,freshwaterfish,shrimp,shellfish,oysters,andoc- form, which, along with the study protocol, had been approved by topus.Theintakefrequenciesonthequestionnairewere:3times/day, the Human Experiment and Ethics Committee of National Cheng 1–2times/day,4–6times/week,1–3times/week,1–3times/month, KungUniversityMedicalCenter.Theparticipantswereaskedtofast 1–11times/year,andnever.Consumedquantitiespermealforeach overnight before blood sampling. Blood samples were drawn into food type were then estimated. Quantitative data for intake of fish chemically clean tubes containing anticoagulants, and part of the andotherseafoodwerecalculatedbasedonbowls(200g)foreach serum samples was obtained after the blood had been centrifuged forbiochemicalanalysis.Bloodsampleswerestoredat−20°Cuntil food items. The questionnaires were administered by our trained interviewersaccordingtostandardoperatingprocedures. T-Hg and MeHg analysis. First, we recruited 565 participants for T-Hg analysis, and the following, 249 of those participants were selectedforMeHganalysisbasedontheyeatmorefishandseafood thanotherpeople. Table1 Demographiccharacteristicsofthestudysubjects. 2.2.BloodT-Hganalysis Coastalsites Inlandsites P-value N= 262 303 T-Hg was analyzed with fully-automatic heat vaporization Sexa mercury-measuring equipment (MA-2000; Nippon Instruments Men 127(48.5%) 150(49.5%) 0.866 Corporation, Tokyo, Japan) using a method that complied with US Women 136(51.3%) 153(50.5%) EPA 7473 and American Society For Testing and Materials (ASTM) Ageb 43.4(17.0–69.0) 43.9(18.0–74.0) 0.749 D6722-01.HeatvaporizationliberatesHg,whichiscollectedasgold BMIb 24.7(16.0–48.3) 24.6(16.4–40.9) 0.821 Bodylipid amalgamandthenmeasured.Afterthegoldamalgamisheated,Hg Menb 23.6(8.3–34.5) 24.2(9.8–35.0) 0.344 atomsemitted,andtheirintensityisdetectedusingcoldvaporatomic Womenb 31.9(21.2–63.2) 31.4(17.1–43.9) 0.599 fluorescencespectrometry(CVAFS)atawavelengthof253.7nm.To Occupationc limitinterference,thevaporwasdehumidifiedusingagaswash. Agriculture 14(5.4%) 19(6.3%) b.0001⁎ Fishery 14(5.4%) 1(0.3%) Livestockbreeding 4(1.5%) 0(0%) 2.3.BloodMeHganalysis Bluecollar 12(4.6%) 17(5.6%) Business 8(3.1%) 23(7.6%) Service 38(14.6%) 69(22.5%) The blood sample analysis procedures used in this study were Publicaffairs 75(28.7%) 38(12.5%) modifiedfromthosereportedbyVázquezetal.(1999).First,2.5mL Others 74(28.4%) 112(36.9%) blood was placed in a Teflon-lined tube and then toluene (15mL) Residentperiodb 29.8(0.25–69) 28.9(0.33–75) 0.585 wasaddedformicrowavedigestion.Themicrowaveextractionwas Smokingstatusc Smoker 77(29.7%) 79(26.1%) 0.373 done at 100°C with 100% power (Microwave Accelerated Reaction Passivesmokers 170(65.1%) 183(60.0%) 0.258 System[MARS];CEMCorp.,Matthews,NC).Aftertheextractionhad Smokingyear(year)a 18.8 20.9 0.116 beencompletedandthesupernatantcooledtoroomtemperature,it Alcoholusagec was cleaned using 3mL of a 1% aqueous cysteine acetate solution. Drinker 52(20.2%) 75(24.8%) 0.225 Finally, 1mL of the toluene extract dried over anhydrous sodium Drinkingperiod 19.6 21.7 0.249 Drinkingquality 2.0 1.9 0.613 sulfate was analyzed using a gas chromatograph (6890; Hewlett- PackardCompany,PaloAlto,CA)equippedwithanelectroncapture Note:Inparenthesesarerangesorpercentages. a TestedbyFisher'sExactTest. detector and an Ulbon HR-thermon-Hg capillary column (15m b TestedbyWilcoxonRankSumsTest. long,0.53mm internal diameter)(ShinwaChemical IndustriesLtd., c TestbyChiSquareTest. Kyoto,Japan). ⁎ P-valueb0.05. 318 C.-C.Leeetal./ScienceoftheTotalEnvironment424(2012)316–321 160 2.6.Statisticalanalysis mL)140 MeHg level=1.304+0.786*T-Hg level; r2 = 0.956; T-HgandMeHgconcentrationsarereportedasμg/L.JMP(version5.0; n (ng/120 p<0.0001, dotted line were 95% confident interval SwAeSreInsutsietudtef,oCrarsyta,NtisCt)icaanldaSntaaltyisstisic.aT(hveerpsiaornti7ci.p1;anSttastSwoeftr,eIndc.i,vTiduelsda,iOnKto) atio100 coastalandinlandresidentgroups.Fisher'sexacttestoraχ2testwas ntr used to comparethe demographic data between the two groups, and ce 80 theWilcoxonSigned-RanktestandKruskalWallistestwereusedtocom- n o paretheT-HgandMeHglevelsbetweenparticipantslivingindifferent d c 60 areas.Inaddition,afteranadjustmentforageandotherfactors,simple o blo 40 andmultivariateregressionanalyseswereusedtoexaminetheassocia- g tionbetweenbloodMeHglevelandtotalseafoodandfishconsumption. H e 20 M 0 3.Results 0 20 40 60 80 100 120 140 160 180 200 T-Hg blood concentration (ng/mL) 3.1.Demographiccharacteristicsofsubjects Fig. 1. The association between total blood mercury (T-Hg) and methylmercury (MeHg) concentrations. MeHg level=1.304+0.786; *T-Hg level; r2=0.956; The gender ratios, age, BMI, body lipid levels, duration of resi- pb0.0001,dottedlinesarethe95%confidenceinterval. dence, smoking status, and alcohol intake of the inhabitants were not statistically different between coastal and inland sites (Pb0.05, Table1).Thereweremorefishermenincoastalsites(5.4%)thanin inlandsites(0.3%). CN T-Hg: 10.2 ng/mL MeHg: 8.8 ng/mL RN T-Hg: 7.9 ng/mL CE MeHg: 6.7 ng/mL T-Hg: 26.1ng/mL MeHg: 25.1 ng/mL RE T-Hg: 18.7ng/mL RC MeHg: 18.2ng/mL T-Hg:8.0ng/mL MeHg:7.3ng/mL CC T-Hg:6.9ng/mL MeHg:6.1ng/mL RS T-Hg:12.3ng/mL MeHg:12.8 ng/mL CS T-Hg:21.7ng/mL MeHg:22.0ng/mL Fig.2.T-HgandMeHgbloodconcentrationsinTaiwanese. C.-C.Leeetal./ScienceoftheTotalEnvironment424(2012)316–321 319 Table2 DifferenceofbloodT-HgandMeHglevelsamongtheinhabitantlivingnearcoastalandinlandsites. Areas Total North Center South East P-value Coastalsites T-Hg(μg/L) N=262 N=70 N=59 N=59 N=68 b.0001⁎,a 16.2±17.6 10.2±5.1 6.9±3.7 21.7±26.7 26.1±17.4 (0.9–184.9) (0.9–30.8) (1.8–16.3) (2.5–184.9) (5.0–91.1) Inlandsites T-Hg(μg/L) N=303 N=71 N=84 N=68 N=80 b.0001⁎,a 11.8±12.1 7.9±4.3 8.0±3.9 12.3±18.0 18.7±13.1 (0.8–146.6) (0.8–20.2) (2.0–18.3) (2.7–146.6) (1.1–73.4) P-value b0.001* 0.003* 0.105 b0.001* 0.004* Coastalsites MeHg(μg/L) N=111 N=28 N=22 N=25 N=36 b.0001⁎,a 16.5±18.1 8.8±3.4 6.1±3.5 22.0±26.7 25.1±16.6 (2.3–137.8) (3.7–16.4) (2.3–14.9) (3.1–137.8) (5.5–60.6) Inlandsites MeHg(μg/L) N=138 N=33 N=31 N=31 N=43 b.0001⁎,a 11.8±12.1 6.7±3.1 7.3±3.5 12.8±23.0 18.2±13.4 (2.1–133.4) (2.1–14.8) (2.4–16.2) (2.1–133.4) (3.1–66.1) ⁎ ⁎ ⁎ ⁎ P-value 0.010 0.018 0.194 0.028 0.036 Note:thedatameantmean±standarddeviationandinparenthesesarerangesorpercentages. a TestbyKruskal–WallisTestamonginhabitantlivingindifferentareas. ⁎ P-valueb0.05. 3.2.Serumconcentrationsoftheparticipants 3.3.Hgexposureandfoodintake BloodT-HgandMeHglevelsweresignificantlycorrelatedinour 3.3.1.Sourceoffoodanddietaryintake participants (Fig. 1). Mean blood T-Hg levels (coastal site mean: Lessthan1%oftheinhabitantswerevegetariansin coastalsites 16.1μg/L, range: 0.9–184.9μg/L versus inland site mean: 11.8μg/L, and b3.3% in inland sites (Table 4). In coastal sites, 90.1% of the range:0.8–146.6μg/L)andMeHglevels(coastalsitemean:16.5μg/L, participantsreportedthatthefishtheyatewaspurchasedinmarkets, range: 0.9–184.9μg/L versus inland site mean: 11.8μg/L, range: 29.4%fromcatchingfish,and8.4%ofthefishwascultivated,aswellas 2.1–133.4μg/L) were significantly higher in coastal sites (Table 2). 96.7%,6.0%and0.7%,respectively,ininlandsites.Coastalresidentsate Geographically,bloodT-HgandMeHglevelsweresignificantlyhigher small-sizedoffshoreseafish,shrimp,oyster,andoctopussignificantly in eastern and southern sites thanin the northern and central sites. morefrequentlythandidinlandresidents(Table5). The blood Hg levels were further grouped into fishermen and non-fishermen(Table3).FishermenhadsignificantlyhigherT-Hgand 3.3.2.AssociationbetweenseafoodintakeandbloodMeHg MeHglevelsthandidnon-fishermenineasternandsouthernTaiwan, SignificantlypositivecorrelationswerefoundbetweenMeHgand butnotinnorthernandcentralTaiwan.InTaiwan,Hgaccumulation age,intakeoflarge-sizedremoteseafish,small-sizedremoteseafish, in52.9%ofTaiwan'swomenofchildbearingageexceedstheUSEPA shrimp, crab, and octopus, respectively (Pb0.05, Table 6). Multiple referencedose(Chienetal.,2010).Inthepresentstudy,theaverage linear regressions also showed positive associations for fish intake, bloodT-Hglevelinourparticipants(13.8μg/L)wassignificantlyhigher age,andwheretheparticipantslived. than blood T-Hg levels in 40 women sensitive to amalgam fillings Inthepresentstudy,bloodT-HgandMeHglevelswerehigherin (median: 2.35μg/L) and in 43 non-sensitive controls (median: residents of eastern and southern Taiwan than of northern and 2.40μg/L) (Zimmer et al., 2002), than in 2369 Koreans 18years old central Taiwan, and higher in fishermen than in non-fishermen. In andolder(mean:3.80μg/L)(Sonetal.,2009),andthantheindirectly Sweden,theintakedoseof4μgMeHg/kgbodyweight/dayestimated exposed residents of a gold-mining area (Cortes-Maramba et al., fromfishintakerecordscorrespondedtobloodHglevelshigherthan 2006).Anotherstudy(ZhangandWong,2007)showedthatmainland 300ng/g(Skerfving,1974).About30yearsaftertheoutbreakofMin- Chinesemenwhoatefishformorethan4mealsperweektendedto amatadisease,T-Hglevelsintheredbloodcellsofmaleresidentsof havemoreHgintheirhair(ZhangandWong,2007).Overall,industrial the coastal area near Minamata City, especially in fisherman, were pollutionandfishconsumptionappeartobethetwolargestsourcesof still significantly higher than those in male residents of the inland anthropogenicHgaccumulationinhumans. area (Sakamoto et al., 1991). A cross-sectional study in Spain Table3 DifferenceofbloodT-HgandMeHglevelsamongfishermanandnon-fishermenlivingaroundTaiwan. Groups North Center South East Total Fisherman T-Hg(μg/L) N=2 N=25 N=24 N=23 N=74 8.9 7.0±3.6 27.4±35.7 33.6±21.4 21.9±26.0 (4.6–13.2) (1.9–16.7) (3.4–184.9) (10.3–91.1) (1.9–184.9) Non-fishermen T-Hg(μg/L) N=141 N=103 N=95 N=125 N=464 9.1±4.9 8.05±4.0 14.2±18.6 20.0±13.3 12.8±12.3 (0.8–30.8) (1.8–18.3) (2.5–146.6) (1.1–73.4) (0.8–146.6) P-value – 0.327 b0.001⁎ 0.002⁎ b0.001⁎ Fisherman MeHg(μg/L) N=8 N=8 N=11 N=27 5.4±3.0 33.2±43.8 36.6±19.4 26.4±29.3 – (2.3–11.5) (3.3–137.8) (10.1–60.6) (2.3–137.8) Non-fishermen MeHg(μg/L) N=59 N=39 N=45 N=68 N=211 7.7±3.4 7.3±3.7 14.7±20.9 18.9±13.1 12.7±13.3 (2.1–16.4) (2.3–16.2) (2.1–133.4) (3.1–66.1) (2.1–133.4) P-value – 0.246 0.096⁎ 0.01⁎ 0.027⁎ Note:thedatameantmean±standarddeviationandinparenthesesarerangesorpercentages. –:Datanotavailable. ⁎ P-valueb0.05. 320 C.-C.Leeetal./ScienceoftheTotalEnvironment424(2012)316–321 Table4 Table6 Dietarysourceanddietaryhabitsbetweentheinhabitantlivingnearcoastalandinland Simpleandmultiplelinearregressionanalysisofend-points. sites. Models r R2 P-value Source Coastalsites Inlandsites P-value LogMeHgversusage 0.335 b0.001* (N=262) (N=303) LogMeHgversusLoglarge-sizedremoteseafish 0.326 b0.001* Foodtype LogMeHgversusLogsmall-sizedremoteseafish 0.205 0.002* Vegetarian 2(0.8%) 10(3.3%) 0.043⁎ LogMeHgversusLogcultivatedfish 0.114 0.112 Carnivorous 260(99.2%) 293(96.7%) LogMeHgversusfreshwaterfish −0.085 0.215 Sourceoffish LogMeHgversusLogshrimp 0.220 0.001* Cultivated 22(8.4%) 2(0.7%) b.0001⁎ LogMeHgversusLogcrab 0.273 b0.001* Fishing 77(29.4%) 18(6.0%) b.0001⁎ LogMeHgversusLogshellfish 0.115 0.114 Purchased 236(90.1%) 289(96.7%) 0.002⁎ LogMeHgversusLogoyster −0.054 0.454 Unknown 16(6.1%) 20(6.7%) 0.864 LogMeHgversusLogoctopus 0.181 0.007* Sourceofotherseafood LogMeHgversusfishintakeandage 0.280 b0.001* Cultivated 16(6.1%) 0(0%) --- LogMeHgversusfishintake,ageandwhether 0.294 b0.001* Fishing 41(16.7%) 1(0.3%) b.0001⁎ livingincoastalorinlandareas Purchased 238(90.8%) 279(93.3%) 0.345 LogMeHgversusfishintake,ageandlocations 0.447 b0.001* unknown 7(2.7%) 14(4.7%) 0.267 ofwheretheylivedinTaiwan Note:thedatameantnumberofstudysubjectsandinparenthesesarepercentages, Note:Thefoodintakequantity(gram)wasusedforeachmodel. TestbyFisher'sExactTest ⁎ P-valueb0.05. ⁎ P-valueb0.05. (Passos et al., 2007) reportedthattheaveragebloodT-Hglevelwas terrestrialbiota,suchasfungi,plants,earthworms,snails,crabs,in- 38.6±21.7μg/L, and the average MeHglevel was33.6±19.4μg/L in sects, amphibians, lizards, snakes, and bats, in southern Taiwan, studyparticipantswhoate7.4fishmealsperweek,morefishmeals which indicated significant industrial pollution of the environment. thaneatenbytheTaiwaneseinthepresentstudy(3.88meals);their However, it is surprising that the highest T-Hg and MeHg levels bloodT-HgandMeHglevelswerealsohigherthanthoseinourstudy. werefoundineasternTaiwan,whichistheleastindustrializedpor- In contrast, the average blood MeHg level (median 1.7μg/L; range tionoftheisland.Ananalysisofheavymetalsinthefluegasfrommu- 0.30–14μg/L)in 127 Swedish women of childbearing agewhoatea nicipalsolidwasteincineratorsinTaiwan(Yuanetal.,2005)found greatdealofvarioustypesoffish(about4meals/week)was(median that the removal efficiency of the air pollution control devices for 9.2μg/L;range2.1–137.8μg/L)lowerthaninourparticipantswhoate Pb,Cd,Zn,Cu,andCrwashigherthan90%,but thatformercuryit fishalmostasfrequently.Theabovedatapointoutthatdespitesimilar was significantly lower because Hg appeared mainly in the gas levelsoffishconsumptionbydifferentgroupsofpeople,bloodT-Hgor phase. Others have reported significant anthropogenic Hg emission MeHglevelsareinfluencedbylocalpollutionsources(Fig.2). insouthandeastAsiafromthedevelopmentofelectricalandelec- ChenandChen(2006)reportedthatthehighestHglevelswerein tronicmanufacturingindustries(Wongetal.,2006),smeltingfacili- marinefish,especiallyintuna,andtheninshellfishandfreshwater ties (Cortes-Maramba et al., 2006; Fu et al., 2009), and mining fish in Taiwan. Elevated T-Hg levels in the cord blood of newborns activitiesandwaste-disposalsites(Horvatetal.,2003).Taiwanwas havebeenassociatedwithmaternalfishintake,particularlyoflarge, the major producer of large-sized liquid-crystal display television oilyfishspecies(Ramóetal.,2008).Therefore,thequestionnairein- panels (LCD-TV), accounting for 34.7% of the worldwide market terviewhasbeensetthatallfishwasgroupedintolarge-sizedremote (Tseng et al., 2007; Wang et al., 2007). This suggested that some seafish,small-sizedremoteseafish,small-sizedoffshoreseafish,cul- localareasmightbecontaminatedwithHgbecauseoflocalmining tivatedfishandothers.Wealsofoundthatlarge-sizedremoteseafish operations or the disposal of personal computers, among other wasasignificantcontributortoHgaccumulationinTaiwanese. things. In addition, Hg contamination is more widespread because aircontaminatedwithHgvaporistransportedacrossnationalbound- 3.4.Areapollution ariestoneighboringcountriesandbeyond.Hgintakethroughfood, particularlyriceandfish,wasthemostimportantrouteofHgexpo- Our findings suggest that the remarkably high blood T-Hg and sure,however,themostriskislocatedinthevicinityofsmeltingfacil- MeHglevelsinTaiwanmightbeattributabletothenumberofweekly ities,miningactivitiesandclosetothewastedisposalsitesforgeneral fishmealseatenbyTaiwaneseorhighMeHgcontaminationinfishof population(Horvatetal.,2003).Astudy(PalhetaandTaylor,1995) Taiwan,especiallyineasternandsouthernTaiwan,whereresidents that compared T-Hg and inorganic Hg levels between unpolluted had significantly higher T-Hg levels than in central and northern areasandHg-pollutedgoldminingareasintheAmazonregionofBrazil Taiwan. Hsu et al. (2006) reported very high Hg levels found in showedthattheenvironmentalHgwastransferredtofishandanimals usedforfoodand,subsequently,intothepeoplewhoconsumedthem. Table5 Intakefrequencyofseafoodbetweentheinhabitantlivingnearcoastalandinlandsites 4.Conclusions (time/month). SignificantlyhigherT-HgandMeHglevelswerefoundinresidentsof Types Coastalsites Inlandsites P-value (N=262) (N=303) Taiwan's coastal sites than inland sites. The elevatedT-Hg andMeHg levels appeared to be related to eating large-sized remote sea fish, Large-sizedremoteseafish 3.77±8.4 3.09±6.5 0.950 Small-sizedremoteseafish 3.42±6.4 3.26±6.6 0.771 small-sized remote sea fish, shrimp, crab, and octopus. Of the four Small-sizedoffshoreseafish 5.06±11.8 2.62±5.4 b0.001⁎ areas that we investigated, the highest T-Hg and MeHg levels were Cultivatedfish 1.67±2.9 1.66±2.8 0.935 foundintheleastindustrializedarea,Yilan,ineasternTaiwan,andthe Freshwaterfish 3.06±5.6 3.58±6.1 0.014⁎⁎ next highest were in the highly industrialized area of Kaohsiung, in Shrimp 2.71±5.2 2.52±6.7 0.015 Shellfish 3.25±4.0 3.65±7.7 b0.001⁎ southernTaiwan.Toprotectourcitizensfromaccumulatingtoomuch Oyster 2.76±6.9 1.62±5.4 b0.001⁎ HgandMeHgintheirbloodbecauseofthefoodtheyeat,itisnecessary Octopus 3.06±6.3 2.11±5.5 0.023⁎ toexaminetheprimarylocalsourcesofseafoodinparticular,especially forsensitivepopulationslikechildrenandpregnantwomen.Webelieve Note:thedatameantmean±standardizedeviation,TestbyWilcoxonRankSumsTest. ⁎ P-valueb0.05. thatinvestigationsofthelocalsourcesofHgpollutionarejustified. 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