珠三角电子垃圾拆解区室内环境中多溴联苯醚的人体暴露
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摘要
通过对清远市电子垃圾拆解区11户居民室内积尘和室内空气颗粒物中PBDEs和PBB153赋存量和赋存特征的分析,以及利用环境保护部近年编著的《中国人群暴露参数手册》中的暴露参数对该地区的人群暴露量和暴露特征进行评估.结果表明,研究区域居民室内积尘中PBDEs的含量为646—7862 ng·g~(-1),室内空气颗粒物中含量为477—1579 pg·m-3; PBDEs及其各单体以及PBB153在室内积尘和室内空气颗粒物中的含量之间具有显著的相关性(r=0.629—0.895,P<0.05),其主要来源可能是室外输送;男性成人、女性成人和儿童(9—12岁)对室内环境介质中PBDEs的总暴露量分别为2507±2099、2831±2400、8455±7382 pg·kg~(-1)·d~(-1)bw.对不同暴露途径而言,所有暴露人群经口摄入积尘中上述化合物的日均暴露量占总日均暴露量的比例最高,其次是经呼吸暴露,经皮肤暴露相对较低.对于不同暴露人群而言,儿童经皮肤暴露摄入上述化合物的比例相对最高,而男性成人经呼吸摄入上述化合物的比例相对最高.
Human exposure to PBDEs and PBB153 in indoor dust and in indoor air of 11 households at an e-waste recycling area in Qingyuan City was investigated. Using the exposure parameters in the"Exposure Factors Handbook of Chinese Population"compiled by the Ministry of EnvironmentalProtection,the human exposure dose and its characteristics in this area were assessed. The results showed that the PBDEs levels in indoor dust and indoor air particulate were 647—7862 ng·g~(-1) and477—1579 pg·m-3,respectively. And there was a significant correlation between the levels of PBDEs and PBB153 in indoor dust and indoor air particles( r = 0.629— 0. 895,P < 0. 05). Their main source may be from outdoors. The total exposure to PBDEs in indoor environmental media of male adults,female adults and children( 9—12 years old) were 2507 ± 2099,2838 ± 2400 and8455±7382 pg·kg~(-1)·d~(-1) bw,respectively. For different exposure pathways,dust ingestion for the average daily exposure of these compounds was the highest,followed by inhalation exposure and skin exposure. For different exposed populations,skin exposure to these compounds was the highest for children,while male adults had the highest intake of these compounds by breathing.
Human exposure to PBDEs and PBB153 in indoor dust and in indoor air of 11 households at an e-waste recycling area in Qingyuan City was investigated. Using the exposure parameters in the"Exposure Factors Handbook of Chinese Population"compiled by the Ministry of EnvironmentalProtection,the human exposure dose and its characteristics in this area were assessed. The results showed that the PBDEs levels in indoor dust and indoor air particulate were 647—7862 ng·g~(-1) and477—1579 pg·m-3,respectively. And there was a significant correlation between the levels of PBDEs and PBB153 in indoor dust and indoor air particles( r = 0.629— 0. 895,P < 0. 05). Their main source may be from outdoors. The total exposure to PBDEs in indoor environmental media of male adults,female adults and children( 9—12 years old) were 2507 ± 2099,2838 ± 2400 and8455±7382 pg·kg~(-1)·d~(-1) bw,respectively. For different exposure pathways,dust ingestion for the average daily exposure of these compounds was the highest,followed by inhalation exposure and skin exposure. For different exposed populations,skin exposure to these compounds was the highest for children,while male adults had the highest intake of these compounds by breathing.
引文
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[25]刘洋,冀秀玲,马静,等.上海市典型家庭室内空气中PCBs与PBDEs初步研究[J].环境科学研究,2011,24(5):482-488.LIU Y,JI X L,MA J,et al.Preliminary study of PCBs and PBDEs in indoor air samples collected from typical houses in Shanghai[J].Research of Environmental Sciences,2011,24(5):482-488(in Chinese).
[26]CHEN L G,MAI B X,XU Z C,et al.In-and outdoor sources of polybrominated diphenyl ethers and their human inhalation exposure in Guangzhou,China[J].Atmospheric Environment,2008,42(1):78-86.
[27]WEI W,MANDIN C,BLANCHARD O,et al.Distributions of the particle/gas and dust/gas partition coefficients for seventy-two semivolatile organic compounds in indoor environment[J].Chemosphere,2016,153:212-219.
[28]WILFORD B H,SHOEIB M,HARNER T,et al.Polybrominated Diphenyl Ethers in Indoor Dust in Ottawa,Canada:Implications for Sources and Exposure[J].Environmental Science&Technology,2005,39(18):7027-7035.
[29]FROMME H,KOERNER W,SHAHIN N,et al.Human exposure to polybrominated diphenyl ethers(PBDE),as evidenced by data from a duplicate diet study,indoor air,house dust,and biomonitoring in Germany[J].Environment International,2009,35(8):1125-1135.
[30]ALLEN J G,MCCLEAN M D,STAPLETON H M,et al.Critical factors in assessing exposure to PBDEs via house dust[J].Environment International,2008,34(8):1085-1091.
[31]LABUNSK I,HARRAD S,SANTILLO D,et al.Levels and distribution of polybrominated diphenyl ethers in soil,sediment and dust samples collected from various electronic waste recycling sites within Guiyu town,southern China[J].Environmental Science-Processes&Impacts,2013,15(2):503-511.
[32]LABUNSKA I,HARRAD S,WANG M,et al.Human dietary exposure to PBDEs around E-waste recycling sites in Eastern China[J].Environmental Science&Technology,2014,48(10):5555-5564.
[33]LEUNG A O W,ZHENG J,YU C K,et al.Polybrominated Diphenyl Ethers and Polychlorinated Dibenzo-p-dioxins and Dibenzofurans in Surface Dust at an E-Waste Processing Site in Southeast China[J].Environmental Science&Technology,2011,45(13):5775-5782.
[34]NI K,LU Y,WANG T,et al.A review of human exposure to polybrominated diphenyl ethers(PBDEs)in China[J].International Journal of Hygiene and Environmental Health,2013,216(6):607-623.
[35]XU F,TANG W B,ZHANG W,et al.Levels,distributions and correlations of polybrominated diphenyl ethers in air and dust of household and workplace in Shanghai,China:implication for daily human exposure[J].Environmental Science and Pollution Research,2016,23(4):3229-3238.
[36]ZHU N Z,LIU L Y,MA W L,et al.Polybrominated diphenyl ethers(PBDEs)in the indoor dust in China:levels,spatial distribution and human exposure[J].Ecotoxicology and Environmental Safety,2015,111:1-8.
[37]STAPLETON H M,DODDER N G,OFFENBERG J H,et al.Polybrominated Diphenyl Ethers in House Dust and Clothes Dryer Lint[J].Environmental Science&Technology,2005,39(4):925-931.
[38]ANH H Q,NAM V D,TRI T M,et al.Polybrominated diphenyl ethers in plastic products,indoor dust,sediment and fish from informal ewaste recycling sites in Vietnam:a comprehensive assessment of contamination,accumulation pattern,emissions,and human exposure[J].Environ Geochem Health,2017,39(4):935-954.
[39]FROMME H,KORNER W,SHAHIN N,et al.Human exposure to polybrominated diphenyl ethers(PBDE),as evidenced by data from a duplicate diet study,indoor air,house dust,and biomonitoring in Germany[J].Environment International,2009,35(8):1125-1135.
[40]KEFENI K K,OKONKWO J O,BOTHA B M.Concentrations of polybromobiphenyls and polybromodiphenyl ethers in home dust:Relevance to socio-economic status and human exposure rate[J].Science of the Total Environment,2014,470:1250-1256.
[41]SUGENG E J,DE COCK M,SCHOONMADE L J,et al.Toddler exposure to flame retardant chemicals:Magnitude,health concern and potential risk-or protective factors of exposure:Observational studies summarized in a systematic review[J].Chemosphere,2017,184:820-831.
[42]MALLIARI E KALANTZI O-I.Children's exposure to brominated flame retardants in indoor environments-A review[J].Environment International,2017,108:146-169.
[43]SONG Q B LI J H.A systematic review of the human body burden of e-waste exposure in China[J].Environment International,2014,68:82-93.
[44]BRAMWELL L,GLINIANAIA S V,RANKIN J,et al.Associations between human exposure to polybrominated diphenyl ether flame retardants via diet and indoor dust,and internal dose:A systematic review[J].Environment International,2016,92-93:680-694.
[2]BIRNBAUM L S STASKAL D F.Brominated flame retardants:Cause for concern?[J].Environmental Health Perspectives,2004,112(1):9-17.
[3]WONG F,SUZUKI G,MICHINAKA C,et al.Dioxin-like activities,halogenated flame retardants,organophosphate esters and chlorinated paraffins in dust from Australia,the United Kingdom,Canada,Sweden and China[J].Chemosphere,2017,168:1248-1256.
[4]万斌,郭良宏.多溴联苯醚的环境毒理学研究进展[J].环境化学,2011,30(1):143-152.WAN B and GUO L H.Research progress on the investigation of environmental toxicology of polybrominated diphenyl ethers[J].Environmental Chemistry,2011,30(1):143-152(in Chinese).
[5]HAMMEL S C,HOFFMAN K,LORENZO A M,et al.Associations between flame retardant applications in furniture foam,house dust levels,and residents'serum levels[J].Environment International,2017,107:181-189.
[6]JONES-OTAZO H A,CLARKE J P,DIAMOND M L,et al.Is house dust the missing exposure pathway for PBDEs?An analysis of the urban fate and human exposure to PBDEs[J].Environmental Science&Technology,2005,39(14):5121-5130.
[7]PENG C,TAN H,GUO Y,et al.Emerging and legacy flame retardants in indoor dust from East China[J].Chemosphere,2017,186:635-643.
[8]BETTS K S.Unwelcome Guest:PBDEs in Indoor Dust[J].Environmental Health Perspectives,2008,116(5):202-208.
[9]KADEMOGLOU K,XU F,PADILLA-SANCHEZ J A,et al.Legacy and alternative flame retardants in Norwegian and UK indoor environment:Implications of human exposure via dust ingestion[J].Environment International,2017,102:48-56.
[10]LORBER M.Exposure of Americans to polybrominated diphenyl ethers[J].Journal of Exposure Science and Environmental Epidemiology,2008,18(1):2-19.
[11]LIU K,LI J,YAN S,et al.A review of status of tetrabromobisphenol A(TBBPA)in China[J].Chemosphere,2016,148:8-20.
[12]HE C-T,ZHENG X-B,YAN X,et al.Organic contaminants and heavy metals in indoor dust from e-waste recycling,rural,and urban areas in South China:Spatial characteristics and implications for human exposure[J].Ecotoxicology and Environmental Safety,2017,140:109-115.
[13]张利飞,黄业茹,董亮.多溴联苯醚在中国的污染现状研究进展[J].环境化学,2010,29(5):787-795.ZHANG LF,HUANG Y R,DONG L.Pollution of polybrominated diphenyl ethers in China[J].Environmental Chemistry,2010,29(5):787-795(in Chinese).
[14]WANG J,MA Y J,CHEN S J,et al.Brominated flame retardants in house dust from e-waste recycling and urban areas in South China:Implications on human exposure[J].Environment International,2010,36(6):535-541.
[15]向彩红,罗孝俊,余梅,等.珠江河口水生生物中多溴联苯醚的分布[J].环境科学,2006,27(9):1732-1737.XIANG C H,LUO X J,YU M,et al.Distribution of polybrominated diphenyl ethers in aquatic species from the Pearl River estuary[J].Environmental Science,2006,27(9):1732-1737(in Chinese).
[16]环境保护部,中国人群暴露参数手册(成人卷)[M].北京:中国环境出版社,2013.Ministry of Environmental Protection.Exposure factors handbook of Chinese population,adults[M].Beijing:China Environmental Press,2013(in Chinese).
[17]环境保护部,中国人群暴露参数手册(儿童卷:6-17岁)[M].北京:中国环境出版社,2016.Ministry of Environmental Protection.Exposure factors handbook of Chinese population,children(6-17years)[M].Beijing:China Environmental Press,2016(in Chinese).
[18]U.S.EPA.Exposure Factors Handbook 2011 Edition(Final Report)[M].Washington DC:U.S.Environmental Protection Agency,EPA/600/R-09/052F,2011.
[19]赵秀阁,黄楠,段小丽,等.环境健康风险评价中的皮肤暴露参数[J].环境与健康杂志,2012,29(2):124-126.ZHAO X G,HUANG N,DUAN X L,et al.Dermal exposure factors in environmental health risk assessment[J].Journal of Environment and Health,2012,29(2):124-126(in Chinese).
[20]娄素芳,王欣欣,姜子岸,等.贵屿表层土壤中多溴联苯醚的水平与儿童健康风险[J].上海大学学报(自然科学版),2016,22(2):141-150.LOU S F,WANG X X,JIANG Z A,et al.Levels of polybrominated diphenyl ethers in surface soil of Guiyu and the associated health risk to children[J].Journal of Shanghai University(Natural Science),2016,22(2):141-150(in Chinese).
[21]ZHENG X,XU F,CHEN K,et al.Flame retardants and organochlorines in indoor dust from several e-waste recycling sites in South China:Composition variations and implications for human exposure[J].Environment International,2015,78:1-7.
[22]ZHENG J,LUO X J,YUAN J G,et al.Levels and sources of brominated flame retardants in human hair from urban,e-waste,and rural areas in South China[J].Environmental Pollution,2011,159(12):3706-3713.
[23]JIANG H,LIN Z K,WU Y Y,et al.Daily intake of polybrominated diphenyl ethers via dust and diet from an e-waste recycling area in China[J].Journal Of Hazardous Materials,2014,276:35-42.
[24]SUN J Q,WANG Q W,ZHUANG S L,et al.Occurrence of polybrominated diphenyl ethers in indoor air and dust in Hangzhou,China:Level,role of electric appliances,and human exposure[J].Environmental Pollution,2016,218:942-949.
[25]刘洋,冀秀玲,马静,等.上海市典型家庭室内空气中PCBs与PBDEs初步研究[J].环境科学研究,2011,24(5):482-488.LIU Y,JI X L,MA J,et al.Preliminary study of PCBs and PBDEs in indoor air samples collected from typical houses in Shanghai[J].Research of Environmental Sciences,2011,24(5):482-488(in Chinese).
[26]CHEN L G,MAI B X,XU Z C,et al.In-and outdoor sources of polybrominated diphenyl ethers and their human inhalation exposure in Guangzhou,China[J].Atmospheric Environment,2008,42(1):78-86.
[27]WEI W,MANDIN C,BLANCHARD O,et al.Distributions of the particle/gas and dust/gas partition coefficients for seventy-two semivolatile organic compounds in indoor environment[J].Chemosphere,2016,153:212-219.
[28]WILFORD B H,SHOEIB M,HARNER T,et al.Polybrominated Diphenyl Ethers in Indoor Dust in Ottawa,Canada:Implications for Sources and Exposure[J].Environmental Science&Technology,2005,39(18):7027-7035.
[29]FROMME H,KOERNER W,SHAHIN N,et al.Human exposure to polybrominated diphenyl ethers(PBDE),as evidenced by data from a duplicate diet study,indoor air,house dust,and biomonitoring in Germany[J].Environment International,2009,35(8):1125-1135.
[30]ALLEN J G,MCCLEAN M D,STAPLETON H M,et al.Critical factors in assessing exposure to PBDEs via house dust[J].Environment International,2008,34(8):1085-1091.
[31]LABUNSK I,HARRAD S,SANTILLO D,et al.Levels and distribution of polybrominated diphenyl ethers in soil,sediment and dust samples collected from various electronic waste recycling sites within Guiyu town,southern China[J].Environmental Science-Processes&Impacts,2013,15(2):503-511.
[32]LABUNSKA I,HARRAD S,WANG M,et al.Human dietary exposure to PBDEs around E-waste recycling sites in Eastern China[J].Environmental Science&Technology,2014,48(10):5555-5564.
[33]LEUNG A O W,ZHENG J,YU C K,et al.Polybrominated Diphenyl Ethers and Polychlorinated Dibenzo-p-dioxins and Dibenzofurans in Surface Dust at an E-Waste Processing Site in Southeast China[J].Environmental Science&Technology,2011,45(13):5775-5782.
[34]NI K,LU Y,WANG T,et al.A review of human exposure to polybrominated diphenyl ethers(PBDEs)in China[J].International Journal of Hygiene and Environmental Health,2013,216(6):607-623.
[35]XU F,TANG W B,ZHANG W,et al.Levels,distributions and correlations of polybrominated diphenyl ethers in air and dust of household and workplace in Shanghai,China:implication for daily human exposure[J].Environmental Science and Pollution Research,2016,23(4):3229-3238.
[36]ZHU N Z,LIU L Y,MA W L,et al.Polybrominated diphenyl ethers(PBDEs)in the indoor dust in China:levels,spatial distribution and human exposure[J].Ecotoxicology and Environmental Safety,2015,111:1-8.
[37]STAPLETON H M,DODDER N G,OFFENBERG J H,et al.Polybrominated Diphenyl Ethers in House Dust and Clothes Dryer Lint[J].Environmental Science&Technology,2005,39(4):925-931.
[38]ANH H Q,NAM V D,TRI T M,et al.Polybrominated diphenyl ethers in plastic products,indoor dust,sediment and fish from informal ewaste recycling sites in Vietnam:a comprehensive assessment of contamination,accumulation pattern,emissions,and human exposure[J].Environ Geochem Health,2017,39(4):935-954.
[39]FROMME H,KORNER W,SHAHIN N,et al.Human exposure to polybrominated diphenyl ethers(PBDE),as evidenced by data from a duplicate diet study,indoor air,house dust,and biomonitoring in Germany[J].Environment International,2009,35(8):1125-1135.
[40]KEFENI K K,OKONKWO J O,BOTHA B M.Concentrations of polybromobiphenyls and polybromodiphenyl ethers in home dust:Relevance to socio-economic status and human exposure rate[J].Science of the Total Environment,2014,470:1250-1256.
[41]SUGENG E J,DE COCK M,SCHOONMADE L J,et al.Toddler exposure to flame retardant chemicals:Magnitude,health concern and potential risk-or protective factors of exposure:Observational studies summarized in a systematic review[J].Chemosphere,2017,184:820-831.
[42]MALLIARI E KALANTZI O-I.Children's exposure to brominated flame retardants in indoor environments-A review[J].Environment International,2017,108:146-169.
[43]SONG Q B LI J H.A systematic review of the human body burden of e-waste exposure in China[J].Environment International,2014,68:82-93.
[44]BRAMWELL L,GLINIANAIA S V,RANKIN J,et al.Associations between human exposure to polybrominated diphenyl ether flame retardants via diet and indoor dust,and internal dose:A systematic review[J].Environment International,2016,92-93:680-694.