天津市大气中多环芳烃衍生物污染特征和来源

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摘要为探究天津市大气中多环芳烃衍生物污染特征与来源，使用石英纤维滤膜（QFFs）和聚氨酯泡沫（PUFs）采集环境空气样品，并使用气相色谱-质谱法测定其浓度．结果表明，天津市大气中Σ₁₈NPAHs在秋季和冬季平均浓度分别为840，894pg/m³，Σ₅OPAHs在秋季和冬季平均浓度分别为8.08，9.36ng/m³，表现为冬季略大于秋季.大气中9N-ANT、2N-NAP、1N-NAP、2+3N-FLT、BZO和9-FO为主要的多环芳烃衍生物.PM_2.5中多环芳烃衍生物的浓度冬季大于秋季，在气相中则为秋季大于冬季.从昼夜差异来看，PM_2.5中，多环芳烃衍生物浓度的夜昼比在大部分采样天数都大于1，在秋季的气相和PM_2.5中，昼间二次形成的NPAHs较冬季高.基于特征比值法进行来源初析，发现天津秋冬季大气PM_2.5中NPAHs主要以一次排放为主，同时二次生成对NPAHs也有一定贡献，大气PM_2.5中NPAHs二次生成方式以与OH·催化反应生成为主．气粒分配特征表现为：多数化合物在冬季PM_2.5占比较秋季高，同时气相中多环芳烃衍生物占比秋季较冬季呈上升趋势.

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	高玉宗
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	王冰冰
	杨夏微

关键词 ：硝基多环芳烃(NPAHs), 氧基多环芳烃(OPAHs), 大气污染特征, 来源分析, 气粒分配

Abstract：To investigate the pollution characteristics and sources of PAH derivatives in the atmosphere of Tianjin, ambient air samples were collected by using quartz fiber filer membranes (QFFs) and polyurethane foam (PUFs), and the concentrations of PAH derivatives were measured by gas chromatography-mass spectrometry (GC-MS). The results showed that the average concentrations of ∑₁₈NPAHs in autumn and winter were 840, 894pg/m³, respectively, and the average concentrations of ∑₅OPAHs in autumn and winter were 8.08, 9.36ng/m³, respectively, which were slightly higher in winter than in autumn. In the atmosphere, 9N-ANT, 2N-NAP, 1N-NAP, 2+3N-FLT, BZO and 9-FO were the main PAH derivatives. The concentrations of PAH derivatives in PM_2.5 were greater in winter than in autumn, while in the gas phase, they were greater in autumn than in winter. From the perspective of diurnal difference, the night-day ratios of PAH derivatives in PM_2.5 were greater than 1 in most sampling days, and the secondary formation of NPAHs in the daytime in the gas phase and PM_2.5 was higher in autumn than in winter. Based on the characteristic ratio method, the preliminary source analysis showed that primary emission was the main source of NPAHs in PM_2.5 in autumn and winter, and secondary generation also contributed to NPAHs. The secondary generation of NPAHs in PM_2.5 was mainly generated by catalytic reaction with OH. The characteristics of gas particle distribution are as follows:most compounds occupied a higher proportion of PM_2.5 in winter than in autumn, while the proportion of SPAHs in the gas phase were higher in autumn than in winter.

Key words： nitrated polycyclic aromatic hydrocarbons (NPAHs) oxy-polycyclic aromatic hydrocarbons (OPAHs) atmospheric pollution characteristics source apportionment gas-particle distribution

收稿日期: 2022-07-25

PACS:	X132
	X513

基金资助:天津市科技计划项目（21JCYBJC00200）

通讯作者: 姬亚芹,jiyaqin@nankai.edu.cn E-mail: jiyaqin@nankai.edu.cn

作者简介: 高玉宗(1998-),男,山西大同人,南开大学硕士研究生,主要从事环境空气污染防治技术与理论研究.

引用本文:

高玉宗, 姬亚芹, 杨益, 王淼, 肖扬, 王冰冰, 杨夏微. 天津市大气中多环芳烃衍生物污染特征和来源[J]. 中国环境科学, 2023, 43(3): 1026-1034. GAO Yu-zong, JI Ya-qin, YANG Yi, WANG Miao, XIAO Yang, WANG Bing-bing, YANG Xia-wei. Pollution characteristics and sources of polycyclic aromatic hydrocarbon derivatives in the atmosphere of Tianjin. CHINA ENVIRONMENTAL SCIENCECE, 2023, 43(3): 1026-1034.

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[1]	Keyte I J, Harrison R M, Lammel G. Chemical reactivity and long-range transport potential of polycyclic aromatic hydrocarbons-a review[J]. Chemical Society Reviews, 2013,42(24):9333-9391.
[2]	马涛,孔继婕,韩孟书,等.环境中硝基多环芳烃的污染现状及其毒性效应研究进展[J]. 环境化学, 2020,39(9):2430-2440. Ma T, Kong J J, Han M S, et al. Review on the pollution status and toxicity effects of nitrated polycyclic aromatic hydrocarbons in the environment[J]. Environmental Chemistry, 2020,39(9):2430-2440.
[3]	Wei S, Bo H, Liu M, et al. Characterization of PM2.5-bound nitrated and oxygenated PAHs in two industrial sites of South China[J]. Atmospheric Research, 2012,109-110:76-83.
[4]	Durant J L, Busby W F, Lafleur A L, et al. Human cell mutagenicity of oxygenated, nitrated and unsubstituted polycyclic aromatic hydrocarbons associated with urban aerosols[J]. Mutation Research, 1996,371(3/4):123.
[5]	Talcott R, Wei E. Airborne Mutagens Bioassayed in Salmonella typhimurium2[J]. J. Natl. Cancer Inst., 1977,58:449-451.
[6]	Jäger J. Detection and characterization of nitro derivatives of some polycylic aromatic hydrocarbons by fluorescence quenching after thin-layer chromatography:application to air pollution analysis[J]. Journal of Chromatography A, 1978,152(2):575-578.
[7]	Schuetzle D, Lee S C, Prater T J, et al. The identification of polynuclear aromatic hydrocarbon (PAH) derivatives in mutagenic fractions of diesel particulate extracts[J]. Int. J. Environ. Anal. Chem., 1981,9(2):93-144.
[8]	Walgraeve C, Demeestere K, Dewulf J, et al. Oxygenated polycyclic aromatic hydrocarbons in atmospheric particulate matter:Molecular characterization and occurrence[J]. Atmospheric Environment, 2010, 44(15):1831-1846.
[9]	张玉洁,云洋.环境中的氧化多环芳烃综述[J]. 环境化学, 2021, 40(1):150-163. Zhang Y J, Yun Y. Oxygenated polycyclic aromatic hydrocarbons in the environment:A review[J]. Environmental Chemistry, 2021,40(1):150-163
[10]	Huang W, Huang B, Bi X H, et al. Emission of PAHs, NPAHs and OPAHs from residential honeycomb coal briquette combustion[J]. Energy & Fuels, 2015,28(1):636-642.
[11]	Titaley I A, Chlebowski A, Truong L, et al. Identification and toxicological evaluation of unsubstituted PAHs and novel PAH derivatives in pavement sealcoat products[J]. Environmental Science & Technology Lett, 2016,3(6):234-242.
[12]	Webb P J, Hamilton J F, Lewis A C, et al. Formation of oxygenated-polycyclic aromatic compounds in aerosol from the photo-oxidation of otolualdehyde[J]. Polycyclic Aromatic Compounds, 2006,26(4):237-252.
[13]	Akimoto Y, Aoki T, Nito S, et al. Oxygenated polycyclic aromatic hydrocarbons from MSW incinerator fly ash[J]. Chemosphere, 1997,34(2):263-273.
[14]	李宏宇,李沛祺,黄娟,等.兰州市大气OPAHs污染特征及潜在来源分析[J]. 中国环境科学, 2022,42(8):3561-3571. Li H Y, Li P Q, Huang J, et al. Pollution characteristics and potential pollution source regions of atmospheric OPAHs in Lanzhou.[J]. China Environmental Science, 2022,42(8):3561-3571.
[15]	Hayakawa K. Environmental behaviors and toxicities of polycyclic aromatic hydrocarbons and nitropolycyclic aromatic hydrocarbons[J]. Chemical & Pharmaceutical Bulletin, 2016,47(2):83-94.
[16]	Andersson B E, Henrysson T. Accumulation and degradation of dead-end metabolites during treatment of soil contaminated with polycyclic aromatic hydrocarbons with five strains of white-rot fungi[J]. Applied Microbiology and Biotechnology, 1996,46(5/6):647-652.
[17]	韩德明,叶磊,张承中,等.西安城区大气中多氯联苯的气粒分配研究[J]. 中国环境科学, 2014,34(10):2466-2471. Han D M, Ye L, Zhang C Z, et al. Gas-particle partitioning of polychlorinated biphenyls in air of Xi'an City[J]. China Environmental Science, 2014,34(10):2466-2471.
[18]	Alves C A, Vicente A M, Custódio D, et al. Polycyclic aromatic hydrocarbons and their derivatives (nitro-PAHs, oxygenated PAHs, and azaarenes) in PM2.5 from Southern European cities[J]. Science of The Total Environment, 2017,595:494-504.
[19]	Zhao T, Yang L, Huang Q, et al. PM2.5-bound polycyclic aromatic hydrocarbons (PAHs) and nitrated-PAHs (NPAHs) emitted by gasoline vehicles:Characterization and health risk assessment[J]. Science of The Total Environment, 2020,727:138631.
[20]	Lammel G, Kitanovski Z, Kukucka P, et al. Oxygenated and nitrated polycyclic aromatic hydrocarbons in ambient air-levels, phase partitioning, mass size distributions, and inhalation bioaccessibility[J]. Environmental Science & Technology, 2020,54(5):2615.
[21]	Ma L X, Li B, Liu Y P, et al. Characterization, sources and risk assessment of PM2.5-bound polycyclic aromatic hydrocarbons (PAHs) and nitrated PAHs (NPAHs) in Harbin, a cold city in Northern China[J]. Journal of Cleaner Production, 2020,264:121673.
[22]	Benjamin B A M, et al. PM2.5-bound oxygenated PAHs, nitro-PAHs and parent-PAHs from the atmosphere of a Chinese megacity:Seasonal variation, sources and cancer risk assessment.[J]. Science of the Total Environment, 2014,473:77-87.
[23]	Delhomme O, Herckes P, Millet M. Determination of nitro-polycyclic aromatic hydrocarbons in atmospheric aerosols using HPLC fluorescence with a post-column derivatisation technique[J]. Analytical & Bioanalytical Chemistry, 2007,389(6):1953-1959.
[24]	Tomaz S, Shahpoury P, Jaffrezo J L, et al. One-year study of polycyclic aromatic compounds at an urban site in Grenoble (France):Seasonal variations, gas/particle partitioning and cancer risk estimation[J]. Science of the Total Environment, 2016,565:1071-1083.
[25]	Arey J, Zielinska B, Atkinson R, et al. The formation of nitro-PAH from the gas-phase reactions of fluoranthene and pyrene with the OH radical in the presence of NOx[J]. Atmospheric Environment, 1986, 20(12):2339-2345.
[26]	Murahashi T, Kizu R, Kakimoto H, et al. 2-Nitrofluoranthene, 1-, 2-and 4-Nitropyrenes and 6-Nitrochrysene in Diesel-Engine Exhaust and Airborne Particulates[J]. Journal of health science, 1999,45(5):244-250.
[27]	Vione D, Barra S, et al. Polycyclic aromatic hydrocarbons in the atmosphere:monitoring, sources, sinks and fate. II:sinks and fate[J]. Annali Di Chimica, 2004,94(4):257-268.
[28]	Shen G F, Tao S, Wang W, et al.Emission of oxygenated polycyclic aromatic hydrocarbons from indoor solid fuel combustion[J]. Environmental Science & Technology, 2011,45(8):3459-3465.
[29]	Karavalakis G, Boutsika V, Stournas S, et al. Biodiesel emissions profile in modern diesel vehicles. Part 2:Effect of biodiesel origin on carbonyl, PAH, nitro-PAH and oxy-PAH emissions[J]. Science of the total Environment, 2011,409(4):738-747.
[30]	康欣媛,王国文,丁小璘,等.莱州湾大气颗粒相中多环芳烃及其衍生物的赋存特征[J]. 海洋环境科学, 2022,41(1):113-121. Kang X Y, Wang G W, Ding X L, et al. Occurrence of different type polycyclic aromatic hydrocarbon (PAHs) in particle atmosphere of Laizhou Bay[J]. Marine Environmental Science, 2022,41(1):113-121.
[31]	Kalisa E, Nagato E G, Bizuru E, et al. Characterization and risk assessment of atmospheric PM2.5 and PM10 particulate-bound PAHs and NPAHs in Rwanda, Central-East Africa[J]. Environmental Science & Technology, 2018,52(21):12179-12187.
[32]	Alam M S, Keyte I J, Yin J, et al. Diurnal variability of polycyclic aromatic compound (PAC) concentrations:Relationship with meteorological conditions and inferred sources[J]. Atmospheric Environment, 2015,122:427-438.
[33]	Nezikova B, Degrendele C, Bandowe B A M, et al. Three years of atmospheric concentrations of nitrated and oxygenated polycyclic aromatic hydrocarbons and oxygen heterocycles at a central European background site[J]. Chemosphere, 2020,269:128738.
[34]	姜盼.济南春季大气细颗粒物PM2.5中多环芳烃(PAHs)及其衍生物(NPAHs, OPAHs)的污染特征和来源解析[D]. 济南:山东大学, 2018. Jiang P. Characteristics and sources of PM2.5-bound PAHs, NPAHs and OPAHs in Jinan in spring.[D]. Jinan:Shandong University, 2018.
[35]	Ringuet J, Albinet A, Leoz-Garziandia E, et al. Diurnal/nocturnal concentrations and sources of particulate-bound PAHs, OPAHs and NPAHs at traffic and suburban sites in the region of Paris (France)[J]. Science of The Total Environment, 2012,437(1):297-305.
[36]	Wu S P, Yang B Y, Wang X H, et al. Diurnal variation of nitrated polycyclic aromatic hydrocarbons in PM10 at a roadside site in Xiamen, China[J]. Journal of Environmental Sciences, 2012,24(10):1767-1776.
[37]	Hien T T, Thanh LT, Kameda T, et al. Nitro-polycyclic aromatic hydrocarbons and polycyclic aromatic hydrocarbons in particulate matter in an urban area of a tropical region:Ho Chi Minh City, Vietnam[J]. Atmospheric Environment, 2007,41(36):7715-7725.
[38]	Tsapakis M, Stephanou E G. Diurnal cycle of PAHs, Nitro-PAHs, and oxy-PAHs in a high oxidation capacity marine background atmosphere[J]. Environmental Science & Technology, 2007,41(23):8011-8017.
[39]	Albinet A, Leoz-Garziandia E, Budzinski H, et al. Nitrated and oxygenated derivatives of polycyclic aromatic hydrocarbons in the ambient air of two French alpine valleys Part 2:Particle size distribution[J]. Atmospheric Environment, 2008,42(1):55-64.
[40]	Amador-Muñoz O, Villalobos-Pietrini R, Miranda J, et al. Organic compounds of PM2.5 in Mexico Valley:Spatial and temporal patterns, behavior and sources[J]. Science of the Total Environment, 2011, 409(8):1453-1465.
[41]	Bamford H A, Baker J E. Nitro-polycyclic aromatic hydrocarbon concentrations and sources in urban and suburban atmospheres of the Mid-Atlantic region[J]. Atmospheric Environment, 2003,37(15):2077-2091.
[42]	Wang W T, Jariyasopit N, Schrlau J, et al. Concentration and photochemistry of PAHs, NPAHs, and OPAHs and toxicity of PM2.5 during the Beijing Olympic Games[J]. Environmental Science & Technology, 2011,45(16):6887-6895.
[43]	Chuesaard T, Chetiyanukornkul T, Kameda T, et al. Influence of biomass burning on the levels of atmospheric polycyclic aromatic hydrocarbons and their nitro derivatives in Chiang Mai, Thailand[J]. Aerosol and Air Quality Research, 2014,14(4):1247-1257.
[44]	朱青青,张宪,董姝君,等.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. Zhu Q Q, Zhang X, Dong S J, et al. Progress on the gas/particle partitioning of persistent organic pollutants in atmosphere.[J]. Environmental Chemistry, 2014,33(10):1629-1636.
[45]	Harner T, Bidleman T F. Octanol air partition coefficient for describing particle/gas partitioning of aromatic compounds in urban air[J]. Environmental Science & Technology, 1998,32(10):1494-1502.
[46]	Pankow J F. The calculated effects of non-exchangeable material on the gas-particle distributions of organic compounds[J]. Atmospheric Environment, 1988,22:1405-1409.
[47]	He J, Balasubramanian R. A study of gas/particle partitioning of SVOCs in the tropical atmosphere of Southeast Asia[J]. Atmospheric Environment, 2009,43(29):4375-4383.
[48]	Su Y, Lei Y D, Wania F, et al. Regressing gas/particle partitioning data for polycyclic aromatic hydrocarbons[J]. Environmental Science & Technology, 2006,40(11):3558-3564.