济南市夏季环境空气中PBDEs的浓度分布及潜在风险分析
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摘要
为准确评估济南市夏季环境空气中PBDEs (多溴联苯醚)的污染情况,利用气相色谱-负化学离子源-质谱(GC-NCI-MS)方法,对采集到的大气颗粒物滤膜和气相样品进行了分析,得到不同粒径颗粒相和气相PBDEs在济南市夏季环境空气中的质量浓度.结果表明:观测期间,济南市环境空气中TSP (总悬浮颗粒物)、PM10和PM2. 5中的ρ(PBDEs)分别为(224. 1±14. 0)(156. 5±43. 7)(110. 2±27. 4) pg/m3,质量浓度较高的3种PBDEs单体分别为BDE209、BDE99、BDE183;气相中ρ(PBDEs)为(54. 8±13. 2) pg/m3,其中,质量浓度较高的单体分别为BDE209、BDE47、BDE99.通过主因子分析发现,不同粒径颗粒物上吸附的PBDEs特征单体不同,TSP中以五溴联苯醚为主,PM10中以八溴联苯醚和五溴联苯醚为主,PM2. 5中则以五溴联苯醚、八溴联苯醚、十溴联苯醚为主.通过将2种模型的预测值和实测值进行比较发现,稳衡态模型比KOA(辛醇-空气分配系数)模型更好地模拟了PBDEs的气-粒分配情况.在稳衡态模型下,PBDEs在气-粒分配中接近于平衡状态.高溴代PBDEs主要分布于颗粒相中,而低溴代PBDEs的真实情况不同于理论预测结果,BDE99及BDE47在颗粒相的分配比高于50%,说明济南市低溴代PBDEs也容易吸附在颗粒相中.根据计算的PBDEs呼吸暴露水平可知,PM2. 5上PBDEs呼吸暴露量占TSP呼吸暴露量的49. 1%,儿童约是成人的1. 5倍.济南市普通儿童和成人对BDE99最高总摄入量分别为234. 78和169. 57 pg/(kg·d),均低于BDE99最大允许摄入量260 pg/(kg·d).根据US EPA (美国环境保护局)发布的PBDEs健康风险评价方法(EPA/540/R/070/002),利用国内外相关参数分别计算空气吸入致癌风险指数发现,济南市夏季环境空气中PBDEs的致癌风险处于较低水平.研究显示,济南市夏季环境空气中不同粒径颗粒物PBDEs的质量浓度处于较低污染水平,其产生的潜在健康风险也较低.
To evaluate the pollution level of atmospheric PBDEs in summer in Jinan City,the concentrations of PBDEs in various particle sizes and gas phase were obtained using gas chromatography-negative chemical ionization-mass spectrometry( GC-NCI-MS) to analyze particle and PUF membrane samples. The results show that during the monitoring period the average concentrations of PBDEs on TSP,PM10 and PM2. 5 in Jinan City were( 224. 1±14. 0),( 156. 5±43. 7) and( 110. 2±27. 4) pg/m3,respectively; and the top 3 congeners of PBDEs with the highest concentration were BDE209,BDE99 and BDE183. The average concentration of gaseous PBDEs was( 54. 8 ±13. 2) pg/m3; and the top 3 congeners were BDE209,BDE47 and BDE99. A SPSS 22. 0 software was used to conduct the principal factor analysis,indicating that the adsorbed PBDEs on different particle sizes were different: pentabromodiphenyl ether the dominant compound on the TSP, octabromo and decabromodiphenyl ether was mainly associated with the PM10, and pentabromo, octabromo,decabromodiphenyl ether were mainly on the PM2. 5. By comparing the predicted values of the two models with the measured values,it was found that the steady-state model simulation of the air-particle distribution of PBDEs was more reliable than the equilibrium model. Based on the steady model,the PBDEs in Jinan City were near equilibrium state in gas-particle distribution. High-brominated PBDEs were mainly distributed in the particulate form,while the actual concentration of low-brominated PBDEs was different from the model predicted results. For instance,the mass fraction of BDE99 and BDE47 on particles were higher than 50%,indicating that low-brominated PBDEs in Jinan also tended to be adsorbed on the particles. According to the calculations of respiratory exposure levels of PBDEs,the values on PM2. 5 accounted for 49. 1% of TSP respiratory exposure,indicating that the influence on children was approximately 1. 5 times as many as adults. The total intake of BDE99 for children and adults in Jinan City was 234. 78 and 169. 57 pg/( kg·d),respectively,which was lower than the suggested maximum intake of BDE99( 260 pg/( kg·d)). According to the PBDEs health risk assessment method of EPA( EPA/540/R/070/002),it was found that the inhalation cancer risk of PBDEs in summer air in Jinan,calculated using the reported parameters,was very low. The results showed that the mass concentration of PBDEs with different particle sizes in the ambient air of Jinan City in summer was at a lower pollution level,and the potential health risks were also lower.
To evaluate the pollution level of atmospheric PBDEs in summer in Jinan City,the concentrations of PBDEs in various particle sizes and gas phase were obtained using gas chromatography-negative chemical ionization-mass spectrometry( GC-NCI-MS) to analyze particle and PUF membrane samples. The results show that during the monitoring period the average concentrations of PBDEs on TSP,PM10 and PM2. 5 in Jinan City were( 224. 1±14. 0),( 156. 5±43. 7) and( 110. 2±27. 4) pg/m3,respectively; and the top 3 congeners of PBDEs with the highest concentration were BDE209,BDE99 and BDE183. The average concentration of gaseous PBDEs was( 54. 8 ±13. 2) pg/m3; and the top 3 congeners were BDE209,BDE47 and BDE99. A SPSS 22. 0 software was used to conduct the principal factor analysis,indicating that the adsorbed PBDEs on different particle sizes were different: pentabromodiphenyl ether the dominant compound on the TSP, octabromo and decabromodiphenyl ether was mainly associated with the PM10, and pentabromo, octabromo,decabromodiphenyl ether were mainly on the PM2. 5. By comparing the predicted values of the two models with the measured values,it was found that the steady-state model simulation of the air-particle distribution of PBDEs was more reliable than the equilibrium model. Based on the steady model,the PBDEs in Jinan City were near equilibrium state in gas-particle distribution. High-brominated PBDEs were mainly distributed in the particulate form,while the actual concentration of low-brominated PBDEs was different from the model predicted results. For instance,the mass fraction of BDE99 and BDE47 on particles were higher than 50%,indicating that low-brominated PBDEs in Jinan also tended to be adsorbed on the particles. According to the calculations of respiratory exposure levels of PBDEs,the values on PM2. 5 accounted for 49. 1% of TSP respiratory exposure,indicating that the influence on children was approximately 1. 5 times as many as adults. The total intake of BDE99 for children and adults in Jinan City was 234. 78 and 169. 57 pg/( kg·d),respectively,which was lower than the suggested maximum intake of BDE99( 260 pg/( kg·d)). According to the PBDEs health risk assessment method of EPA( EPA/540/R/070/002),it was found that the inhalation cancer risk of PBDEs in summer air in Jinan,calculated using the reported parameters,was very low. The results showed that the mass concentration of PBDEs with different particle sizes in the ambient air of Jinan City in summer was at a lower pollution level,and the potential health risks were also lower.
引文
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[22] LI Yifan,MA Wei Li,YANG Meng. Rediction of gas/particle partitioning polybrominated diphenyl ethers(PBDEs)in global air:a theoretic study.Atmospheric Chemistry and Physics,2015,15(7):1669-1681.
[23]赵洪霞.溴代阻燃剂的化学表征及氧化降解的基础研究[D].大连:中国科学院大连化学物理研究所,2006:84-105.
[24]吴辉.典型地区环境介质中卤代化合物的水平及人群摄入状况的初步研究[D].北京:中央民族大学,2014:35-40.
[25] PANKOW J F.An absorption model of gas/particle partitioning of organic compounds in the atmosphere[J]. Atmospheric Environment,1994,28(10):185-188.
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[28] HAKK H,LETCHER R J.Metabolism in the toxicokinetics and fate of brominated flame retardants:a review[J]. Environment International,2003,29(6):801-828.
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[2] ELJARRAT E,CAL A,RALDUA D,et al. Occurrence and bioavailability of polybrominated diphenyl ethers and hexabromocyclododecane in sediment and fish from the Cinca River,a tributary of the Ebro River(Spain)[J]. Environmental Science&Technology,2004,38(5):2603-2608.
[3] VENIER M,HITES R A.Atmospheric deposition of PBDEs to the Great Lakes featuring a Monte Carlo analysis of errors[J].Environmental Science&Technology,2008,42(24):9058-9064.
[4] GOUIN T,HARNER T. Modelling the environmental fate of the polybrominated diphenyl ethers[J]. Environment International,2003,108(4):717-724.
[5]张烃,陈社军,李楠,等.台州水系表层沉积物典型POPs污染现状及生态风险[J].环境科学研究,2014,27(12):1540-1548.ZHANG Ting,CHEN Shejun,LI Nan,et al. Occurrence and ecological risks of typical POPs in surface sediments from the Taizhou river system[J]. Research of Environmental Sciences,2014,27(12):1540-1548.
[6] JURADO E,JAWARD F M,LOHMANN R,et al.Atmospheric dry deposition of persistent organic pollutants to the Atlantic and inferences for the global oceans[J]. Environmental Science&Technology,2004,38(21):5505-5513.
[7] JAWARD F M,ZHANG G,NAM J J,et al.Passive air sampling of polychlorinated biphenyls, organochlorine compounds, and polybrominated diphenyl ethers across Asia[J]. Environmental Science&Technology,2005,39(22):8638-8645.
[8]林海涛,李琦路,张干,等.中国8个城市大气多溴联苯醚的污染特征及人体暴露水平[J].环境科学,2016,37(1):10-15.LIN Haitao, LI Qilu, ZHANG Gan, et al. Atmospheric polybrominated diphenyl ethers in eight cities of China pollution characteristics and human exposure[J]. Environmental Science,2016,37(1):10-15.
[9]孟博,刘丽艳,马万里,等.垃圾焚烧发电厂周边土壤多溴联苯醚污染特征及来源解析[J].环境科学研究,2015,28(5):775-781.MENG Bo,LIU Liyan,MA Wanli,et al.Characteristics and possible sources of polybrominated diphenyl ethers in soils in vicinity of municipal solid waste incineration power plants[J]. Research of Environmental Sciences,2015,28(5):775-781.
[10]杨延梅,陶义,唐阵武,等.典型电子废物焚烧区水生生物多溴联苯醚累积特征[J].环境科学研究,2013,26(4):439-445.YANG Yanmei,TAO Yi,TANG Zhenwu,et al. Bioaccumulation of polybrominated diphenyl ethers in aquatic species from the typical e-waste burning site[J]. Research of Environmental Sciences,2013,26(4):439-445.
[11] GOSS K U,RENE P,SCHWARZENBA C H. Gas/solid and gas/liquid partitioning of organic compounds:critical evaluation of the interpretation of equilibrium constants[J]. Environmental Science and Technology,1998,32(25):2025-2032.
[12]杨萌.中国大气中多溴联苯醚的含量组成及气-粒分配[D].大连:大连海事大学,2013:99-101.
[13]金军,吴辉,王英等.典型地区大气中多溴联苯醚和新型溴代阻燃剂的水平及组成分布[J].环境科学,2014,35(4):1230-1237.JIN Jun,WU Hui,WANG Ying,et al.Comparative study of the level and distribution of polybrominated diphenyl ethers and new brominated flame retardants in the atmosphere of typical urban[J].Environmental Science,2014,35(4):1230-1237.
[14]周变红,张承中,蒋君丽,等.西安市大气中多溴联苯醚的季节变化特征及人体暴露评估[J].中国环境科学,2012,32(9):1591-1596.ZHOU Bianhong,ZHANG Chengzhong,JIANG Junli,et al.Seasonal variations and human exposure assessment of polybrominated diphenyl ethers in air of Xi'an[J]. China Environmental Science,2012,32(9):1591-1596.
[15] CINCINELLI A,PIERI F,MARTELLINI T.Atmospheric occurrence and gas-particle partitioning of PBDEs in an industrialised and urban area of Florence,Italy[J]. Aerosol&Air Quality Research,2014,14(4):1121-1130.
[16] HAYAKAWA K, TAKATSUKI H, WATANABE I, et al.Polybrominated diphenyl ethers(PBDEs),polybrominated and dibenzo-p-dioxins/dibenzofurans(PBDD/Fs)monobromopolychlorinated dibenzo-p-dioxins/dibenzofurans(Mo BPXDD/Fs)in the atmosphere and bulk deposition in Kyoto,Japan[J].Chemosphere,2004,57(5):343-356.
[17]孟博.二?英和多溴联苯醚的城市点源污染特征与气-粒分配[D].哈尔滨:哈尔滨工业大学,2016:75-83.
[18] DIE Q,NIE Z Q,LIU F,et al. Seasonal variations in atmospheric concentrations and gas-particle partitioning of PCDD/Fs and dioxinlike PCBs around industrial sites in Shanghai,China[J].Atmospheric Environment,2015,119(5):220-227.
[19] CINCINELLI A,PIERI F,MARTELLINI T.Atmospheric occurrence and gas-particle partitioning of PBDEs in an industrialised and urban area of Florence,Italy[J]. Aerosol&Air Quality Research,2014,14(4):1121-1130.
[20] KIM D,CHOI K,LEE D.Gas-particle partitioning and behavior of dioxin-like PCBs in the urban atmosphere of Gyeonggi-do,South Korea[J].Atmospheric Research,2011,101(1):386-395.
[21] LI Yifan,JIA Hongliang. Prediction of gas/particle partition quotients of polybrominated diphenyl ethers(PBDEs)in north temperate zone air:an empirical approach[J]. Ecotoxicology&Environmental Safety,2014,108(3):65-71.
[22] LI Yifan,MA Wei Li,YANG Meng. Rediction of gas/particle partitioning polybrominated diphenyl ethers(PBDEs)in global air:a theoretic study.Atmospheric Chemistry and Physics,2015,15(7):1669-1681.
[23]赵洪霞.溴代阻燃剂的化学表征及氧化降解的基础研究[D].大连:中国科学院大连化学物理研究所,2006:84-105.
[24]吴辉.典型地区环境介质中卤代化合物的水平及人群摄入状况的初步研究[D].北京:中央民族大学,2014:35-40.
[25] PANKOW J F.An absorption model of gas/particle partitioning of organic compounds in the atmosphere[J]. Atmospheric Environment,1994,28(10):185-188.
[26] NOUWEN J,CORNELIS C,DEFRE R. Health risk assessment of dioxin emissions from municipal waste incinerators:the Neerlandquarter(Wiltijk,Beigium)[J]. Chemosphere,2001,43(6):909-923.
[27]段小丽.暴露参数的研究方法及其在环境健康风险评价中的应用[M].北京:科学出版社,2012:65-71.
[28] HAKK H,LETCHER R J.Metabolism in the toxicokinetics and fate of brominated flame retardants:a review[J]. Environment International,2003,29(6):801-828.
[29] JOHNSON-RESTREPO B,KANNAN K. An assessment of sources and pathways of human exposure to polybrominated diphenyl ethers in the United States[J].Chemosphere,2009,76(4):542-548.
[30] WINTER-SORKINA D,BAKKER M I,WOLTERINK G,et al.Brominated flame retardants:occurrence,dietary intake and risk assessment[J].Environment International,2006,7(5):20-46.
[31] CHEN D,BI X,ZHAO J,et al. Pollution characterization and diurnal variation of PBDEs in the atmosphere of an e-waste dismantling region[J]. Environmental Pollution,2009,157(3):1051-1057.
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