杭州市PM_(2.5)中PAHs和PAEs气固分布特征及其安全风险研究
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摘要
为了解杭州市PM_(2.5)中多环芳烃(PAHs)、邻苯二甲酸酯(PAEs)的气固分布特征,于2016年12月—2017年5月在杭州市主城区同步采集PM_(2.5)与气相样品。经气相色谱-质谱法分析可知:气相中总PAHs的月平均质量浓度大于PM_(2.5)中的数值,PAHs的相分布特征是气相占优型;气相中总PAEs的月平均质量浓度略小于PM_(2.5)中的数值,PAEs的相分布特征是固相占优型。据分析结果计算PAHs和PAEs单体分子的气-固分配系数(K_p),结果表明:单体分子量越大,其K_p值越高,越容易分布在固相颗粒物中。此外,大气环境中总PAHs和PAEs的质量浓度变化规律为冬季大于春季,且冬季PAHs和PAEs的气相质量浓度亦大于春季。根据大气环境中PAHs和PAEs的安全风险评价可知:气相中PAHs的毒性当量浓度远大于PM_(2.5)中PAHs的毒性当量浓度,PAEs致癌风险的模型估算结果表明大气环境中PAEs不具有致癌风险。
In order to understand the gas-solid distribution characteristics of polycyclic aromatic hydrocarbons(PAHs) and phthalates(PAEs) in PM_(2.5) of Hangzhou city, the PM_(2.5)and ambient air samples were synchronously collected in this study from December 2016 to May 2017 in main urban area of Hangzhou. Analysis of the samples was performed by the GC-MS method. It was found that the monthly average mass concentration of PAHs in ambient air was higher than that in PM_(2.5), suggesting that the phase distribution of PAHs was dominated in gas phase; while the monthly average mass concentration of PAEs in ambient air was slightly lower than that in PM_(2.5), suggesting that the phase distribution of PAEs was dominated in solid phase. The gas-solid distribution coefficients(K_p) of PAHs and PAEs were evaluated. The results suggested K_p values were higher for PAHs and PAEs with higher molecular weight, which were more likely to be distributed in the solid phase. Furthermore, it was found that the mass concentrations of both total atmospheric and gaseous PAHs or PAEs in winter were higher than that in spring. Safety risk assessment of atmospheric PAHs and PAEs showed that the toxic equivalent concentration of PAHs in the gas phase was much higher than that in PM_(2.5). Carcinogenic risk assessment of PAEs by a model indicated that the atmospheric PAEs had no carcinogenic risk.
In order to understand the gas-solid distribution characteristics of polycyclic aromatic hydrocarbons(PAHs) and phthalates(PAEs) in PM_(2.5) of Hangzhou city, the PM_(2.5)and ambient air samples were synchronously collected in this study from December 2016 to May 2017 in main urban area of Hangzhou. Analysis of the samples was performed by the GC-MS method. It was found that the monthly average mass concentration of PAHs in ambient air was higher than that in PM_(2.5), suggesting that the phase distribution of PAHs was dominated in gas phase; while the monthly average mass concentration of PAEs in ambient air was slightly lower than that in PM_(2.5), suggesting that the phase distribution of PAEs was dominated in solid phase. The gas-solid distribution coefficients(K_p) of PAHs and PAEs were evaluated. The results suggested K_p values were higher for PAHs and PAEs with higher molecular weight, which were more likely to be distributed in the solid phase. Furthermore, it was found that the mass concentrations of both total atmospheric and gaseous PAHs or PAEs in winter were higher than that in spring. Safety risk assessment of atmospheric PAHs and PAEs showed that the toxic equivalent concentration of PAHs in the gas phase was much higher than that in PM_(2.5). Carcinogenic risk assessment of PAEs by a model indicated that the atmospheric PAEs had no carcinogenic risk.
引文
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[35] KJELLSTROM T,ROSENSTOCK L.The role of environmental and occupational hazards in the adult health transition[J].World health statistics quarterly,1990,43(3):188-196.
[2] OFFENBERJ J H,BAKER J E.The influence of aerosol size and organic carbon content on gas/particle partitioning of polycyclic aromatic hydrocarbons (PAHs)[J].Atmospheric environment,2002,36(7):1205-1220.
[3] PANKOW J F.A consideration of the role of gas/particulate partitioning in the deposition of nicotine and other tobacco smoke compounds in the respiratory track[J].Chemical research in toxicology,2001,14:1465-1481.
[4] 任培芳.北黄海沿岸大气中多环芳烃沉降特征及气固分配研究[D].吉林:长春理工大学,2012.
[5] 王军良,梅益柔,潘军,等.钱塘江齐溪水库表层沉积物中多环芳烃的分布研究[J].浙江工业大学学报,2015,43(5):547-551.
[6] WANG Z,NA G S,MA X D et al.Occurrence and gas/particle partitioning of PAHs in the atmosphere from the North Pacific to the Arctic Ocean[J].Atmospheric environment,2013,77(6):640-646.
[7] PARK S S,KIM Y J,KANG C H,et al.Atmospheric polycyclic aromatic hydrocarbons in Seoul,Korea[J].Atmospheric environment,2002,36:2917-2924.
[8] 邱乐泉,王子超,陈阳,等.一株DEP降解菌的筛选及其休止细胞的降解特性[J].浙江工业大学学报,2013,41(2):178-182.
[9] 米立杰,唐建辉.黄海海洋大气中邻苯二甲酸酯类塑化剂的测定与分析[J].华北科技学院学报,2016,13(5):106-110.
[10] GE R S,CHEN G R,TANRIKUT C,et al.Phthalate ester toxicity in Leydig cells:developmental timing and dosage considerations[J].Reproductive toxicology,2007,23(3):366-373.
[11] HERREROS M A,GONZALEZ-BULNES A.Toxicokinetics of di (2-ethylhexyl) phthalate (DEHP) and its effects on luteal function in sheep[J].Reproductive biology,2013,13(1):66-74.
[12] LI X J,JIANG L,CHEN L,et al.Neurotoxicity of dibutyl phthalate in brain development following perinatal exposure:a study in rats[J].Environmental toxicology & pharmacology,2013,36(2):392-402.
[13] WANG P,WANG S L,FAN C Q.Atmospheric distribution of particulate and gas phase phthalic esters (PAEs) in a Metropolitan city,Nanjing,East China[J].Chemosphere,2008,72(10):1567-1572.
[14] 陈金媛,徐圣辰.杭州市PM2.5中PAEs污染现状与特征分析[J].浙江工业大学学报,2015,43(6):600-606.
[15] TERZI E,SAMARA C.Gas-particle partitioning of polycyclic aromatic hydrocarbons in urban,adjacent coastal,and continental background sites of western Greece[J].Environmental science and technology,2004,38(19):4973-4978.
[16] 王夫美,陈丽,焦姣,等.冬季天津家庭室内空气颗粒物中邻苯二甲酸酯污染研究[J].环境科学,2012,33(5):1446-1450.
[17] 王肖红.大气颗粒物PM2.5中15种邻苯二甲酸酯类检测方法的研究[D].北京:中国疾病预防控制中心环境所,2015.
[18] 曾凡刚.大气中邻苯二甲酸酯类环境激素的定性定量研究[J].中央民族大学学报,2003,12(2):151-153.
[19] 沈婷.室内空气和降尘中邻苯二甲酸酯的分析研究[D].北京:北京工业大学,2009.
[20] 顾爱军,刘佳澍,罗世鹏,等.常州市大气PM2.5中PAHs污染特征及来源解析[J].环境科学,2017,38(8):3110-3118.
[21] 刘效峰,彭林,白慧玲,等.焦化厂区环境空气中多环芳烃的气固分布特征[J].江苏大学学报,2013,34(2):228-233.
[22] 王晟升.杭州湾地区典型城市大气中多环芳烃和PM2.5的污染特征研究[D].杭州:浙江工商大学,2016.
[23] 黄永庆,杨运云,牟德海,等.大流量PUF采样-气相色谱质谱联用测定广州市大气中多环芳烃[J].分析测试学报,2007,26(1):90-96.
[24] 朱振宇,姬亚芹,赵静波,等.天津市大气PM10与降尘中邻苯二甲酸酯的污染特征及相关性分析[J].环境污染与防治,2015,37(12):24-28.
[25] 刘碧莲,吴水平,杨冰玉.大气中多环芳烃气/粒分配的不确定性分析[J].环境科学,2011,32(9):2794-2799.
[26] 朱青青,张宪,董姝君.大气中持久性有机污染物在气相和颗粒相中的分配特征研究进展[J].环境化学,2014,33(10):1629-1636.
[27] 肖燕.南昌市空气环境中多环芳烃(PAHs)的相分配研究[D].南昌:南昌大学,2012.
[28] 王晓丹,杨杰,严浩.兰州市西固区大气降尘中邻苯二甲酸酯分布特征及来源分析[J].地球与环境,2012,40(3):336-341.
[29] ALESSANDRA C,MASSIMO D B,TANIA M,et al.Gas-particle concentration and distribution of n-alkanes and polycyclic aromatic hydrocarbons in the atmosphere of Prato (Italy)[J].Chemosphere,2007,68:472-478.
[30] NISBET I C,LAGOY P K.Toxic equivalency factors (Tefs) for polycyclic aromatic hydrocarbons (PAHs)[J].Regulatory toxicology and pharmacology,1992,16(3):290-300.
[31] 裴小强.室内空气中邻苯二甲酸酯的污染特征及健康风险[D].杭州:浙江大学,2013.
[32] 秦晓雷,章涛,孙红文.中国室内和室外灰尘中邻苯二甲酸酯的分布和健康风险评价[J].生态毒理学报,2016,11(2):231-237.
[33] PEI X Q,SONG M,GUO M,et al.Concentration and risk assessment of phthalates present in indoor air from newly decorated apartments[J].Atmospheric environment,2013,68(1):17-23.
[34] 王雪晴.典型交通微环境空气中15种邻苯二甲酸酯的污染特征及健康风险[D].杭州:浙江大学,2015.
[35] KJELLSTROM T,ROSENSTOCK L.The role of environmental and occupational hazards in the adult health transition[J].World health statistics quarterly,1990,43(3):188-196.