天津市大气颗粒物中有机标识物粒径分布的季节特征

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Abstract In order to study the distribution characteristics of organic markers in particulate matter with different sizes during the heating and non-heating period, and identify their pollution sources, the Anderson eight-stage sampler was used to collect one-year samples from May 2018 to April 2019. 17 kinds of polycyclic aromatic hydrocarbons(PAHs), 20kinds of n-Alkanes and 7kinds of hopanes in 9particle size segments were analyzed and the main sources of particulate matter were identified by molecular markers and diagnostic ratios. The results showed the 4~5rings PAHs Pyr, BaA, Chr, BbF and BaP showed a three-peak distribution and the rest of the PAHs showed a bimodal distribution during the non-heating period, and 3rings PAHs showed a bimodal distribution and 4~6rings PAHs showed a approximately unimodal distribution during the heating period. The diagnostic ratios of PAHs indicated that vehicle emissions and coal combustion were the main contributors of PAHs during the non-heating period and the coal combustion was the main contributors of PAHs during the heating period. The n-Alkanes showed a stable bimodal size distribution during the heating period and C29 showed a unimodal distribution, C27, C31, C32 and C33 showed approximately a unimodal distribution, with the remaining n-Alkanes in a bimodal distribution during the non-heating period. According to the CPI and C_max, it is found that anthropogenic sources were the main source of n-Alkanes during the non-heating period and the heating period. The concentration of high molecular weight n-Alkanes was better influenced by natural sources during the non-heating period than during the heating period. In addition, n-Alkanes emitted from natural sources were easy to concentrate in coarser particulates, and n-Alkanes from anthropogenic sources were more likely to concentrate in the finer particles. The hopanes had peaks in both coarse and fine particle modes during two seasons. Traffic was proposed as the main emission source of hopanes during the non-heating period, and the hopanes mainly originated from coal combustion during the heating period.

Key words： atmospheric particulate matter organic markers size distribution the heating period

Received: 11 April 2022

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	WANG Xiao-ning
	TIAN Ying-ze
	XUE Qian-qian

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WANG Xiao-ning,TIAN Ying-ze,XUE Qian-qian. Distribution characteristics of organic markers in particulate matter with different sizes during different seasons in Tianjin[J]. CHINA ENVIRONMENTAL SCIENCECE, 2022, 42(11): 4974-4982.

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http://www.zghjkx.com.cn/EN/ OR http://www.zghjkx.com.cn/EN/Y2022/V42/I11/4974

[1]	Li Y G, Huang H X H, Griffith S M, et al. Quantifying the relationship between visibility degradation and PM2.5 constituents at a suburban site in Hong Kong:Differentiating contributions from hydrophilic and hydrophobic organic compounds[J]. Science of the Total Environment, 2017,575:1571-1581.
[2]	Yang L, Zhang H, Zhang X,et al. Exposure to atmospheric particulate matter-bound polycyclic aromatic hydrocarbons and their health effects:A review[J]. Journal of Environmental Research and Public Health, 2021,18(4).
[3]	Bi X, Sheng G, Peng P A,et al. Size distribution of n-alkanes and polycyclic aromatic hydrocarbons (PAHs) in urban and rural atmospheres of Guangzhou, China[J]. Atmospheric Environment, 2005,39(3):477-487.
[4]	Lv Y, Li X, Xu T T,et al. Size distributions of polycyclic aromatic hydrocarbons in urban atmosphere:sorption mechanism and source contributions to respiratory deposition[J]. Atmospheric Chemistry and Physics, 2016,16:2971-2983.
[5]	翟宇虹,黄晓锋,张丽,等.深圳大气气溶胶中水溶性有机物粒径分布特征[J]. 中国环境科学, 2015,35(11):3211-3216. Zhai Y H, Huang X F, Zhang L, et al. Size distribution characteristics of water-soluble organic matter in atmospheric aerosol in Shenzhen, China[J]. China Environmental Science, 2015,35(11):3211-3216.
[6]	刘臻,祁建华,王琳,等.青岛大气气溶胶水溶性无机离子的粒径分布特征[J]. 中国环境科学, 2012,32(8):1422-1432. Liu Z, Qi J H, Wang L, et al. Particle size distribution of water-soluble inorganic ions of atmospheric aerosol in Qingdao[J]. China Environmental Science, 2012,32(8):1422-1432.
[7]	郝娇,葛颖,何书言,等.南京市秋季大气颗粒物中金属元素的粒径分布[J]. 中国环境科学, 2018,38(12):4409-4414. Hao J, Ge Y, He S Y, et al. Size distribution characteristics of metal elements in air particulate matter during autumn in Nanjing[J]. China Environmental Science, 2018,38(12):4409-4414.
[8]	于广河,曹礼明,朱乔,等.深圳大气有机硝酸酯粒径分布特征和来源研究[J]. 中国环境科学, 2022,42(4):1510-1517. Yu G H, Cao L M, Zhu Q, et al. Sizing and source characterization of particulate organic nitrates based on long time-of-flight aerosol mass spectrometer (Long-ToF-AMS)[J]. China Environmental Science, 2022,42(4):1510-1517.
[9]	Kang M J, Fu P Q, Aggarwal S G, et al. Size distributions of n-alkanes, fatty acids and fatty alcohols in springtime aerosols from New Delhi, India[J]. Environmental Pollution, 2016,219:957-966.
[10]	Mirante F, Alves C, Pio C,et al. Organic composition of size segregated atmospheric particulate matter, during summer and winter sampling campaigns at representative sites in Madrid, Spain[J]. Atmospheric Research, 2013,132-133:345-361.
[11]	Offenberg J H, Baker J E. Aerosol size distributions of polycyclic aromatic hydrocarbons in urban and over-water atmospheres[J]. Environmental Science & Technology, 1999,33(19):3324-3331.
[12]	Zhang J D, Liu W J, Xu Y S,et al. Distribution characteristics of and personal exposure with polycyclic aromatic hydrocarbons and particulate matter in indoor and outdoor air of rural households in Northern China[J]. Environmental Pollution, 2019,255:113176.
[13]	Wang G, Kawamura K, Mingjie X I E, et al. Organic molecular compositions and size distributions of Chinese summer and autumn aerosols from Nanjing:Characteristic haze event caused by wheat straw burning[J]. Environmental Science & Technology, 2009,43(17):6493-6499.
[14]	Yu Q, Ding X, He Q,et al. Nationwide increase of polycyclic aromatic hydrocarbons in ultrafine particles during winter over China revealed by size-segregated measurements[J]. Atmospheric Chemistry and Physics, 2020,20:14581-14595.
[15]	Lyu Y, Xu T T, Yang X,et al. Seasonal contributions to size-resolved n-alkanes (C8-C40) in the Shanghai atmosphere from regional anthropogenic activities and terrestrial plant waxes[J]. Science of the Total Environment, 2017,579:1918-1928.
[16]	Xu Q P, Wang J Z, Liu J Q,et al. Particulate size distribution and sources evaluation of n-alkanes during long-term haze episode around Chaohu Lake, eastern[J]. Aerosol and Air Quality Research, 2017, 17(8):1975-1984.
[17]	唐小玲.广州市典型地区气溶胶中烃类化合物的粒径分布特征及极性组分的分子标志物研究[D]. 北京:中国科学院研究生院, 2006. Tang X L. Size distribution of n-alkanes and polycyclic aromatic hydrocarbons and molecular marker in polar portion in aerosol from typical area of Guangzhou[D]. Beijing:Institue of Earth Environment, Chinese Academy of Sciences, 2006.
[18]	许绍锋.北京市大气中有机气溶胶的分子组成、粒径分布及季节性变化[D]. 天津:天津大学, 2019. Xu S F. Molecular composition, size distributions and seasonal variation of urban organic aerosols in Beijing[D]. Tianjin:Tianjin University, 2019.
[19]	Wu S P, Tao S, Liu W X. Particle size distributions of polycyclic aromatic hydrocarbons in rural and urban atmosphere of Tianjin, China[J]. Chemosphere, 2006,62(3):357-367.
[20]	Khalili N R, Scheff P A, Holsen T M. PAH source fingerprints for coke ovens, diesel and gasoline engines, highway tunnels, and wood combustion emissions[J]. Atmospheric Environment, 1995,29(4):533-542.
[21]	Zhang Y X, Dou H, Chang B,et al. Emission of polycyclic aromatic hydrocarbons from indoor straw burning and emission inventory updating in China[J]. Annals of the New York Academy of Sciences, 2008,1140:218-227.
[22]	Kiss G, Varga-Puchony Z, Rohrbacher G,et al. Distribution of polycyclic aromatic hydrocarbons on atmospheric aerosol particles of different sizes[J]. Atmospheric Research, 1998,46(3):253-261.
[23]	Allen J O, Dookeran N M. Measurement of polycyclic aromatic hydrocarbons associated with size-segregated atmospheric aerosols in Massachusetts[J]. Environmental Science & Technology, 1996,30(3):1023-1031.
[24]	Zhang L L, Yang L, Zhou Q Y,et al. Size distribution of particulate polycyclic aromatic hydrocarbons in fresh combustion smoke and ambient air:A review[J]. Journal of Environmental Sciences, 2020, 88:370-384.
[25]	Tian S L, Pan Y P, Wang Y S. Size-resolved source apportionment of particulate matter in urban Beijing during haze and non-haze episodes[J]. Atmospheric Chemistry and Physics, 2016,16:1-19.
[26]	Hien T T, Le T T, Kameda T,et al. Distribution characteristics of polycyclic aromatic hydrocarbons with particle size in urban aerosols at the roadside in Ho Chi Minh City, Vietnam[J]. Atmospheric Environment, 2007,41(8):1575-1586.
[27]	Wang R W, Huang Q, Cai J W,et al. Seasonal variations of atmospheric polycyclic aromatic hydrocarbons (PAHs) surrounding Chaohu Lake, China:Source, partitioning behavior, and lung cancer risk[J]. Atmospheric Pollution Research, 2021,12(5):101056.
[28]	Yu H, Yu J Z. Polycyclic aromatic hydrocarbons in urban atmosphere of Guangzhou, China:Size distribution characteristics and size-resolved gas-particle partitioning[J]. Atmospheric Environment, 2012, 54:194-200.
[29]	Han D M, Fu Q Y, Gao S,et al. Non-polar organic compounds in aerosols in a typical city of Eastern China:Size distribution, gas-particle partitioning andtracer for PM2.5 source apportionment[J]. Atmospheric Chemistry and Physics, 2018:1-27.
[30]	Grimmer G, Jacob J, Naujack K W,et al. Profile of the polycyclic aromatic hydrocarbons from used engine oil-inventory by GCGC/MS-PAH in environmental materials, Part 2[J]. Fresenius' Zeitschrift für analytische Chemie, 1981,309(1):13-19.
[31]	Aceves M, Grimalt J O. Seasonally dependent size distributions of aliphatic and polycyclic aromatic hydrocarbons in urban aerosols from densely populated areas[J]. Environmental Science & Technology, 1993,27(13):2896-2908.
[32]	Lin L, Lee M L, Eatough D J. Review of recent advances in detection of organic markers in fine particulate matter and their use for source apportionment[J]. Journal of the Air & Waste Management Association, 2010,60(1):3-25.
[33]	唐小玲,毕新慧,陈颖军,等.广州市空气颗粒物中烃类物质的粒径分布[J]. 地球化学, 2005,34(5):508-514. Tang X L, Bi X H, Chen Y J, et al. Size distribution of n-alkanes and polycyclic aromatic hydrocarbons (PAHs) in urban aerosol of Guangzhou[J]. Geochemica, 2005,34(5):508-514.
[34]	Simoneit B. Organic matter of the troposphere-V:Application of molecular marker analysis to biogenic emissions into the troposphere for source reconciliations[J]. Journal of Atmospheric Chemistry, 1989,8(3):251-275.
[35]	Wang Z, An Z, Gao S,et al. Size-distributions of n-alkanes, PAHs and hopanes and their sources in the urban, mountain and marine atmospheres over East Asia[J]. Atmospheric Chemistry and Physics, 2009,9(22):8869-8882.
[36]	Hao Z, Hopke P K, Zhou C,et al. Ambient mercury source identification at a New York State urban site:Rochester, NY[J]. Science of the Total Environment, 2018,650:1327-1337.
[37]	范艳兵.天津市大气有机气溶胶的分子组成、季节变化及来源分析[D]. 天津大学, 2019. Fan Y B. Sources, Molecular composition and seasonal variation in organic aerosols in Tianjin City, North China[D]. Tianjin University, 2019.
[38]	Oros D R, Simoneit B R T. Identification and emission rates of molecular tracers in coal smoke particulate matter[J]. Fuel, 2000, 79(5):515-536.
[39]	Huang X F, Chen D L, Lan Z J,et al. Characterization of organic aerosol in fine particles in a mega-city of South China:Molecular composition, seasonal variation, and size distribution[J]. Atmospheric Research, 2012,114(15):28-37.
[40]	Rogge W F, Hildemann L M, Mazurek M A,et al. Sources of fine organic aerosol. 2. Noncatalyst and catalyst-equipped automobiles and heavy-duty diesel trucks[J]. Environmental Science & Technology, 1993,27(4):636-651.
[41]	Phuleria H, Geller M, Fine P,et al. Size-resolved emissions of organic tracers from light-and heavy-duty vehicles measured in a California roadway tunnel[J]. Environmental Science & Technology, 2006, 40(13):4109-4118.