北京市一次重污染天气下大气颗粒物中PCDD/Fs、PCNs、PCBs粒径分布特征及呼吸暴露风险评估
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摘要
本研究于2017年5月4日至7日,采集了北京城区一次重污染天气下4种不同粒径段(>10μm、5—10μm、2.5—5μm、<2.5μm)大气颗粒物样本,并采集了晴朗天气样本作为对照.首先,测定了各粒径段颗粒物中17种2,3,7,8-PCDD/Fs、三氯代至八氯代PCNs及12种dl-PCBs单体的含量,进而对这些化合物的粒径分布特征及呼吸暴露风险进行了分析和评估.结果表明,在本次重污染天气下,北京城区大气颗粒物中PCDD/Fs、PCNs、dl-PCBs浓度依次为8.03、6.68、1.18 pg·m~(-3),明显高于晴朗天气.PCDD/Fs、PCNs、dl-PCBs主要富集于粒径<2.5μm的细颗粒物中,含量分别达到86.5%、47.9%、39.8%.PCNs、dl-PCBs大致呈现出随颗粒物粒径减小,其高氯代同系物相对富集量增加的趋势.通过呼吸暴露风险评估发现,本次重污染天气下大气颗粒物中PCDD/Fs、PCNs、dl-PCBs致癌风险分别为1.1×10~(-5)、1.4×10~(-7)、2.2×10~(-7),总致癌风险是晴朗天气下的33倍.PCDD/Fs对总致癌风险贡献率为96.7%,是需优先控制的持久性有机污染物.
From May 4th to 7th, 2017, atmospheric particulate matter of 4 different sizes(>10 μm, 5—10 μm, 2.5—5 μm, <2.5 μm) were collected in Beijing during a heavy pollution episode and the clear episode sample was collected as contral. The concentrations of 17 species, 2,3,7,8-PCDD/Fs, tri-to octa-chlorinated naphthalene, and 12 dl-PCBs congeners in different particle size fractions were determined, and then size distribution and exposure risk of these compounds were analyzed and evaluated. The results showed that the concentrations of PCDD/Fs, PCNs and dl-PCBs in atmospheric particulate matter were 8.03, 6.68 and 1.18 pg·m~(-3) during the heavy pollution episode in urban area of Beijing, respectively, which were significantly higher than those in the clear episode. PCDD/Fs, PCNs and dl-PCBs were mainly found in fine particles with particle size <2.5 μm, accounting for 86.5%, 47.9% and 39.8% of the total concentrations, respectively. The proportion of high chlorinated PCNs and PCBs homologues in a fraction increased as the particle size decreased. According to the results of the risk assessment, the cancer risks of PCDD/Fs, PCNs and dl-PCBs in atmospheric particulate matter by inhalation were 1.1×10~(-5), 1.4×10~(-7) and 2.2×10~(-7), respectively. They were 33 times higher than that of the clear episode. The contribution rate of PCDD/Fs to total cancer risk was 96.7%, so PCDD/Fs should be controlled as a priority persistent organic pollutant.
From May 4th to 7th, 2017, atmospheric particulate matter of 4 different sizes(>10 μm, 5—10 μm, 2.5—5 μm, <2.5 μm) were collected in Beijing during a heavy pollution episode and the clear episode sample was collected as contral. The concentrations of 17 species, 2,3,7,8-PCDD/Fs, tri-to octa-chlorinated naphthalene, and 12 dl-PCBs congeners in different particle size fractions were determined, and then size distribution and exposure risk of these compounds were analyzed and evaluated. The results showed that the concentrations of PCDD/Fs, PCNs and dl-PCBs in atmospheric particulate matter were 8.03, 6.68 and 1.18 pg·m~(-3) during the heavy pollution episode in urban area of Beijing, respectively, which were significantly higher than those in the clear episode. PCDD/Fs, PCNs and dl-PCBs were mainly found in fine particles with particle size <2.5 μm, accounting for 86.5%, 47.9% and 39.8% of the total concentrations, respectively. The proportion of high chlorinated PCNs and PCBs homologues in a fraction increased as the particle size decreased. According to the results of the risk assessment, the cancer risks of PCDD/Fs, PCNs and dl-PCBs in atmospheric particulate matter by inhalation were 1.1×10~(-5), 1.4×10~(-7) and 2.2×10~(-7), respectively. They were 33 times higher than that of the clear episode. The contribution rate of PCDD/Fs to total cancer risk was 96.7%, so PCDD/Fs should be controlled as a priority persistent organic pollutant.
引文
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[2] 张利飞,任玥,许鹏军,等.气相色谱-三重四极杆质谱测定环境样品中17种二■英[J].中国环境科学,2014,34(4):1052-1058.ZHANG L F,REN Y,XU P J,et al.Triple quadrupole mass spectrometry for the analysis of 17dioxins and furans in environmental samples[J].China Environmental Science,2014,34(4):1052-1058(in Chinese).
[3] 李沐霏,刘劲松,周欣,等.杭州市冬季大气气溶胶PM2.5中二■英和多氯联苯的污染特征[J].色谱,2014,32(9):948-954.LI M F,LIU J S,ZHOU X,et al.Pollution characteristics of polychlorinated dibenzo-p-dioxins,polychlorinated dibenzofurans and polychlorinated biphenyls in PM2.5 of Hangzhou City during winter[J].Chinese Journal of Chromatography,2014,32(9):948-954(in Chinese).
[4] BATTERMAN S,CHERNYAK S,GOUDEN Y,et al.PCBs in air,soil and milk in industrialized and urban areas of KwaZulu-Natal,South Africa[J].Enironmental Pollution,2009,157(2):654-663.
[5] 郭丽,巴特,郑明辉.多氯萘的研究[J].化学进展,2009,21(1):377 -388.GUO L,BA T,ZHENG M H,et al.Study of sources and distribution characteristics of polychlorinated naphthalenes[J].Progress in Chemistry,2009,21(1):377 -388(in Chinese).
[6] BERG M V D,BIRNBAUM L S,DENISON M,et al.The 2005 world health organization revaluation of human and mammalian toxic equivalency factors for dioxins and dioxin-like compounds[J].Toxicological Sciences,2006,93(2):223-241.
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[8] 唐孝炎,张远航,邵敏.大气环境化学(第二版)[M].北京:高等教育出版社,2006.TANG X Y,ZHANG Y H,SHAO M.Atmospheric Environmental Chemistry(Second Edition) [M].BeiJing:Higher Education Press,2006(in Chinese).
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[10] ENGLERT N.Fine particles and human health-a review of epidemiological studies[J].Toxicology Letters,2004,149(1-3):235-242.
[11] PAATERO P,TAPPER U.Positive matrix factorization non-negative factor model with optimal utilization of error estimates of data values[J].Environm Etrics,1994,5(2):111-126.
[12] DEGRENDELE C,OKONSKI K,MELYMUK L,et al.Size specific distribution of the atmospheric particulate PCDD/Fs,dl-PCBs and PAHs on a seasonal scale:Implications for cancer risks from inhalation[J].Atmospheric Environment,2014,98:410-416.
[13] ZHU Q Q,ZHENG M H,LIU G R,et al.Particle size distribution and gas-particle partitioning of polychlorinated biphenyls in the atmosphere in Beijing,China[J].Environ Sci Pollut Res,2017,24:1389-1396.
[14] BI X,SHENG G,PENG P,et al.Size distribution of n-alkanes and polycyclic aromatic hydrocarbons(PAHs) in urban and rural atmospheres of Guangzhou,China[J].Atmos.Environ,2005,39:477-487.
[15] COSOLLA` C,YAHYAOUI A,COLIN P,et al.Partical size distributions of currently used pesticides in a rural atmosphere of France[J].Atmos.Environ,2013,81:32-38.
[16] CAO Z,XU F,COVACI A,et al.Distribution patterns of brominated,chlorinated,and phosphorus flam retardants with particle size in indoor and outdoor dust and implications for human exposure[J].Environmental Science & Technology,2014,48:8839-8846.
[17] NI H,ZENG H.HBCD and TBBPA in particulate phase of indoor air in Shenzhen,China[J].Sci.Total.Environ,2013,458:15-19.
[18] 王占山,李云婷,李倩,等.基于大气超级站观测的2017年5月北京市沙尘天气过程分析[J].中国环境监测,2017,33(5):28-34.WANG Z S,LI Y T,LI Q,et al.Analysis on a dust pollution event in Beijing in May,2017 Based on the observation of an Atmospheric Supersite[J].Environmental Monitoring in China,2017,33(5):28-34(in Chinese).
[19] 徐文帅,张大伟,李云婷,等.北京两次沙尘天气污染过程中PM2.5浓度变化特征[J].气候与环境研究,2016,21(1):78-86.XU W S,ZHANG D W,LI Y T,et al.Variation of PM2.5 concentration during two dust pollution events in Beijing [J].Climatic and Environmental Research,2016,21 (1):78-86(in Chinese).
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[22] LEE S J,CHOI S D,JIN G Z,et al.Assessment of PCDD/F risk after implementation of emission reduction at a MSWI[J].Chemosphere,2007,68(1):856-863.
[23] 张春辉,郭建阳,石顺权,等.贵阳市主干道降尘中的多环芳烃及其健康风险评估[J].生态学杂志,2014,33(10):2810-2816.ZHANG C H,GUO J Y,SHI S Q,et al.Polycyclic aromatic hydrocarbons and their health risk assessment in urban surface dust from main roads of Guiyang,Southwest China[J].Chinese Journal of Ecology,2014,33(10):2810-2816(in Chinese).
[24] 环境保护部.中国人群暴露参数(成人卷)[M].北京:中国环境科学出版社,2013.Ministry of Environmental Protection.Exposure parameters of Chinese population(adult volume) [M].BeiJing:China Environmental Science Press,2013(in Chinese).
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[26] FALANDYSZ J.Chloronaphthalenes as food-chain contaminants:A review[J].Food Additives&Contaminants,2003,20:995-1014.
[27] YANG L L,LIU G R,ZHENG M H,et al.Atmospheric occurrence and health risks of PCDD/Fs,polychlorinated biphenyls,and polychlorinated naphthalenes by air inhalation in metallurgical plants[J].Science of the Total Environment,2017,580:1146-1154.
[28] 王春雷,杨大成,张建清,等.深圳市大气中PCDD /Fs污染水平初步研究[J].中国环境监测,2010,26(6):74-79.WANG C L,YANG D C,ZHANG Q J,et al.Determination of dioxins and furans in atmosphere of Shenzhen,China[J].Environmental Monitoring in China,2010,26(6):74-79(in Chinese).
[29] 王春雷,张建清,杨大成,等.深圳市大气中多氯联苯污染水平[J].环境化学,2010,29(5):892-897.WANG C L,ZHANG J Q,YANG D C,et al.Study on contam ination level of folychlorinted biphenyls in atmosphere of Shenzhen,China[J].Environmental Chemistry,2010,29(5):892-897(in Chinese).
[30] 赵淑惠,矫立萍,孙霞,等.冬春季台湾海峡西北部海域大气颗粒物中多氯联苯污染特征[J].应用海洋学学报,2015,2(34):254-263.ZHAO S H,JIAO L P,SUN X,et al.Characteristics of polychlorinated biphenyls (PCBs) in atmospheric particulate matters in northwestern Taiwan Strait during winter and spring[J].Journal of Applied Oceanography,2015,2(34):254-263(in Chinese).
[31] 李燕.大连市大气中多氯联苯的时空分布与组分特征研究[D].大连:大连海事大学,2009.LI Y.Component characteristics and spatial and temporal distribution in the atmosphere in Dalian[D].Dalian:Dalian Maritime University,2009(in Chinese).
[32] HOGARH J N,SEIKE N,KOBARA Y,et al.Passive air monitoring of PCBs and PCNs across East Asia:A comprehensive congener evaluation for source characterization[J].Chemosphere,2012,86(7):718-726.
[33] ZHU Q Q,ZHANG X,DONG S J,et al.Gas and article size distributions of polychlorinated naphthalenes in the atmosphere of Beijing,China[J].Environmental Pollution,2016,212:128-134.
[34] BARBAS B,TORRE A,SANZ P,et al.Gas/particle partitioning and particle size distribution of PCDD/Fs and PCBs in urban ambient air[J].Science of the Total Environment,2018,624:170-179.
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