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2023 , Vol. 40 >Issue 1: 39 - 49

DOI: https://doi.org/10.7523/j.ucas.2021.0025

环境科学与地理学

北京怀柔夏季大气中的VOCs及其对O3和SOA的生成贡献

  • 周毕安 ,
  • 胡君 ,
  • 奇奕轩 ,
  • 张逦嘉 ,
  • 霍鹏 ,
  • 张元勋 ,
  • 张阳 ,
  • 王淑兰
展开
  • 1. 中国科学院大学资源与环境学院, 北京 101408;
    2. 中环天合(北京)环境科学研究院有限公司, 北京 100085;
    3. 内蒙古鄂尔多斯市气象局, 内蒙古 鄂尔多斯 017010;
    4. 中国标准化研究院资源环境研究分院, 北京 100191;
    5. 中国科学院大学 北京燕山地球关键带国家野外科学观测研究站, 北京 101400;
    6. 中国科学院大学VOCs污染控制材料与技术国家工程实验室, 北京 101400;
    7. 中国环境科学研究院, 北京 100012

收稿日期: 2021-01-25

  修回日期: 2021-03-23

  网络出版日期: 2021-03-23

基金资助

国家重点研发计划(2016YFC0503600)和国家环境保护公益性行业科研专项(201509002)资助

收起

Atmospheric VOCs and their contribution to O3 and SOA formation in summer of Huairou District, Beijing City

  • ZHOU Bi ,
  • HU Jun ,
  • QI Yixuan ,
  • ZHANG Lijia ,
  • HUO Peng ,
  • ZHANG Yuanxun ,
  • ZHANG Yang ,
  • WANG Shulan
Expand
  • 1. College of Resources and Environment, University of Chinese Academy of Sciences, Beijing 101408, China;
    2. ZHTH(Beijing) Environmental Science Research Institute Co. Ltd, Beijing 100085, China;
    3. Ordos Meteorological Bureau, Ordos 017010, Inner Mongolia, China;
    4. Resource and Environmental Branch, China National Institute of Standardization, Beijing 100191, China;
    5. Beijing Yanshan Earth Critical Zone National Research Station, University of Chinese Academy of Sciences, Beijing 101400, China;
    6. National Engineering Laboratory for VOCs Pollution Control Material & Technology, University of Chinese Academy of Sciences, Beijing 101400, China;
    7. Chinese Research Academy of Environmental Sciences, Beijing 100012, China

Received date: 2021-01-25

  Revised date: 2021-03-23

  Online published: 2021-03-23

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摘要

为研究北京郊区挥发性有机物(VOCs)的污染特征、来源以及环境影响，于2016年夏季对北京市怀柔区大气中99种VOCs进行在线监测。结果表明，观测期间VOCs体积分数平均值为20.02×10-9，其中烷烃占比最高为38.48%，其次是含氧挥发性有机物(OVOCs)占比28.28%，卤代烃、芳香烃、烯烃和炔烃及乙腈占比较小。初始VOCs每小时的臭氧生成潜势为157.03μg·m-3，主要贡献来自于OVOCs、烯烃和芳香烃,对二次有机气溶胶生成潜势贡献最大的组分为芳香烃。源解析结果表明VOCs来自背景源和燃烧源、工业源、柴油车排放、汽油车排放、油气挥发、天然源和有机溶剂使用。后向轨迹结果表明，除北京本地源排放外，河北、河南和山东省对北京VOCs污染贡献最大，天津市、辽宁省和内蒙古自治区也有一定贡献。

关键词： 挥发性有机物(VOCs); 臭氧生成潜势(OFP); 二次有机气溶胶生成潜势(SOAFP); 源解析; 后向轨迹; 区域传输

本文引用格式

周毕安 , 胡君 , 奇奕轩 , 张逦嘉 , 霍鹏 , 张元勋 , 张阳 , 王淑兰 . 北京怀柔夏季大气中的VOCs及其对O3和SOA的生成贡献[J]. 中国科学院大学学报, 2023 , 40(1) : 39 -49 . DOI: 10.7523/j.ucas.2021.0025

Abstract

In order to study the pollution characteristics and sources of volatile organic compounds (VOCs) and their environmental impact, 99 VOCs in Huairou District of Beijing were monitored online in summer 2016. During the observation period, the average concentration of VOCs was 20.02×10-9, among which alkanes accounted for the highest proportion of 38.48%, followed by oxygenated volatile organic compounds (OVOCs) (28.28%), halogenated hydrocarbons (12.89%), and halogenated hydrocarbons, aromatic hydrocarbons, olefins and alkynes and acetonitrile for a smaller percentage. The average hourly ozone formation potential of the initial VOCs was 157.03μg·m-3 and the major contributors were OVOCs, while alkenes and aromatics, aromatics were the major contributors to secondary organic aerosol formation potential. Seven sources were identified by the PMF model, including background and combustion sources, industrial sources, diesel vehicle emissions, gasoline vehicle emissions oil and gas volatilization, natural sources, and organic solvent use. The results from backward trajectory show that, in addition to local emissions, Hebei, Henan， and Shandong provinces have major contributions to Beijing VOCs pollution, while Tianjin City, Liaoning Province, and Inner Mongolia Autonomous Region also have some contributions.

Key words： volatile organic compounds(VOCs); ozone formation potential(OFP); secondary organic aerosol formation potential(SOAFP); source apportionment; backward trajectory; regional transmission

参考文献

[1] 江梅, 邹兰, 李晓倩, 等. 我国挥发性有机物定义和控制指标的探讨[J]. 环境科学, 2015, 36(9): 3522-3532.DOI：10.13227/j.hjkx.2015.09.051
[2] Cooper O R, Parrish D D, Stohl A, et al. Increasing springtime ozone mixing ratios in the free troposphere over western North America[J]. Nature, 2010, 463(7279): 344-348.DOI：10.1038/nature08708.
[3] He Z R, Wang X M, Ling Z H, et al. Contributions of different anthropogenic volatile organic compound sources to ozone formation at a receptor site in the Pearl River Delta region and its policy implications[J]. Atmospheric Chemistry and Physics, 2019, 19(13): 8801-8816.DOI：10.5194/acp-19-8801-2019.
[4] 罗达通, 高健, 王淑兰, 等. 北京秋季大气挥发性有机物及相关污染物特征分析[J]. 中国科学院大学学报, 2014, 31(3): 329-336.DOI：10.7523/j.issn.2095-6134.2014.03.006.
[5] Sommariva R, de Gouw J A, Trainer M, et al. Emissions and photochemistry of oxygenated VOCs in urban plumes in the Northeastern United States[J]. Atmospheric Chemistry and Physics, 2011, 11(14): 7081-7096.DOI：10.5194/acp-11-7081-2011.
[6] 桑博, 魏凤霞. 济南市区大气中VOCs的浓度、来源及健康风险评价[J]. 中国科学院大学学报, 2019, 36(2): 169-177.DOI：10.7523/j.issn.2095-6134.2019.02.004.
[7] Song S K, Shon Z H, Kang Y H, et al. Source apportionment of VOCs and their impact on air quality and health in the megacity of Seoul[J]. Environmental Pollution, 2019, 247: 763-774.DOI：10.1016/j.envpol.2019.01.102.
[8] Newman P A, Oman L D, Douglass A R, et al. What would have happened to the ozone layer if chlorofluorocarbons (CFCs) had not been regulated?[J]. Atmospheric Chemistry and Physics, 2009, 9(6): 2113-2128.DOI：10.5194/acp-9-2113-2009.
[9] 高文康, 唐贵谦, 辛金元, 等. 京津冀地区严重光化学污染时段O3的时空分布特征[J]. 环境科学研究, 2016, 29(5): 654-663.DOI：10.13998/j.issn.1001-6929.2016.05.06.
[10] Wang G, Cheng S Y, Wei W, et al. Characteristics and source apportionment of VOCs in the suburban area of Beijing, China[J]. Atmospheric Pollution Research, 2016, 7(4): 711-724.DOI：10.1016/j.apr.2016.03.006.
[11] Liu Y F, Song M D, Liu X G, et al. Characterization and sources of volatile organic compounds (VOCs) and their related changes during ozone pollution days in 2016 in Beijing, China[J]. Environmental Pollution, 2020, 257: 113599.DOI：10.1016/j.envpol.2019.113599.
[12] Li Q Q, Su G J, Li C Q, et al. An investigation into the role of VOCs in SOA and ozone production in Beijing, China[J]. Science of the Total Environment, 2020, 720: 137536.DOI：10.1016/j.scitotenv.2020.137536.
[13] Wang M, Shao M, Chen W, et al. Trends of non-methane hydrocarbons (NMHC) emissions in Beijing during 2002—2013[J]. Atmospheric Chemistry and Physics, 2015, 15(3): 1489-1502.DOI：10.5194/acp-15-1489-2015.
[14] Li B W, Ho S S H, Gong S, et al. Characterization of VOCs and their related atmospheric processes in a central Chinese city during severe ozone pollution periods[J]. Atmospheric Chemistry and Physics, 2019, 19(1): 617-638.DOI：10.5194/acp-19-617-2019.
[15] 胡君, 王淑兰, 吴亚君, 等. 北京怀柔O3污染过程初始VOCs浓度特征及来源分析[J]. 环境科学研究, 2019, 32(5): 766-775.DOI：10.13198/j.issn.1001-6929.2019.03.20.
[16] Shao M, Wang B, Lu S H, et al. Effects of Beijing olympics control measures on reducing reactive hydrocarbon species[J]. Environmental Science & Technology, 2011, 45(2): 514-519.DOI：10.1021/es102357t.
[17] Atkinson R, Arey J. Atmospheric degradation of volatile organic compounds[J]. Chemical Reviews, 2003, 103(12): 4605-4638.DOI：10.1021/cr0206420.
[18] Ait-Helal W, Borbon A, Sauvage S, et al. Volatile and intermediate volatility organic compounds in suburban Paris: variability, origin and importance for SOA formation[J]. Atmospheric Chemistry and Physics, 2014, 14(19): 10439-10464.DOI：10.5194/acp-14-10439-2014.
[19] Han D M, Gao S, Fu Q Y, et al. Do volatile organic compounds (VOCs) emitted from petrochemical industries affect regional PM2.5?[J]. Atmospheric Research, 2018, 209: 123-130.DOI：10.1016/j.atmosres.2018.04.002.
[20] Sun J, Wu F K, Hu B, et al. VOC characteristics, emissions and contributions to SOA formation during hazy episodes[J]. Atmospheric Environment, 2016, 141: 560-570.DOI：10.1016/j.atmosenv.2016.06.060.
[21] Stroud C A, Roberts J M, Goldan P D, et al. Isoprene and its oxidation products, methacrolein and methylvinyl ketone, at an urban forested site during the 1999 Southern Oxidants Study[J]. Journal of Geophysical Research: Atmospheres, 2001, 106(D8): 8035-8046.DOI：10.1029/2000jd900628.
[22] Xie X, Shao M, Liu Y, et al. Estimate of initial isoprene contribution to ozone formation potential in Beijing, China[J]. Atmospheric Environment, 2008, 42(24): 6000-6010.DOI：10.1016/j.atmosenv.2008.03.035.
[23] Liang X M, Sun X B, Xu J T, et al. Improved emissions inventory and VOCs speciation for industrial OFP estimation in China[J]. Science of the Total Environment, 2020, 745: 140838.DOI：10.1016/j.scitotenv.2020.140838.
[24] Johnson D, Utembe S R, Jenkin M E. Simulating the detailed chemical composition of secondary organic aerosol formed on a regional scale during the TORCH 2003 campaign in the southern UK[J]. Atmospheric Chemistry and Physics, 2006, 6(2): 419-431.DOI：10.5194/acp-6-419-2006.
[25] Derwent R G, Jenkin M E, Utembe S R, et al. Secondary organic aerosol formation from a large number of reactive man-made organic compounds[J]. Science of the Total Environment, 2010, 408(16): 3374-3381.DOI：10.1016/j.scitotenv.2010.04.013.
[26] Norris G, Duvall R, Brown S, et al. EPA positive matrix factorization(PMF) 5.0 fundamentals and user guide[R]. US Environmental Protection Agency EPA/600/R-14/108, 2014.
[27] Guo H, Cheng H R, Ling Z H, et al. Which emission sources are responsible for the volatile organic compounds in the atmosphere of Pearl River Delta?[J]. Journal of Hazardous Materials, 2011, 188(1/2/3): 116-124.DOI：10.1016/j.jhazmat.2011.01.081.
[28] Paatero P, Hopke P K. Discarding or downweighting high-noise variables in factor analytic models[J]. Analytica Chimica Acta, 2003, 490(1/2): 277-289.DOI：10.1016/S0003-2670(02)01643-4.
[29] Draxler R R, Hess G D. An overview of the HYSPLIT_4 modeling system of trajectories, dispersion and deposition[J]. Australian Meteorological Magazine, 1998, 47(4): 295-308.
[30] Ashbaugh L L, Malm W C, Sadeh W Z. A residence time probability analysis of sulfur concentrations at grand Canyon National Park[J]. Atmospheric Environment(1967), 1985, 19(8): 1263-1270.DOI：10.1016/0004-6981(85)90256-2.
[31] Polissar A V, Hopke P K, Paatero P, et al. The aerosol at Barrow, Alaska: long-term trends and source locations[J]. Atmospheric Environment, 1999, 33(16): 2441-2458.DOI：10.1016/S1352-2310(98)00423-3.
[32] Hsu Y K, Holsen T M, Hopke P K. Comparison of hybrid receptor models to locate PCB sources in Chicago[J]. Atmospheric Environment, 2003, 37(4): 545-562.DOI：10.1016/S1352-2310(02)00886-5.
[33] Han Y J, Holsen T M, Hopke P K, et al. Comparison between back-trajectory based modeling and Lagrangian backward dispersion modeling for locating sources of reactive gaseous mercury[J]. Environmental Science & Technology, 2005, 39(6): 1715-1723.DOI：10.1021/es0498540.
[34] Hui L R, Liu X G, Tan Q W, et al. VOC characteristics, chemical reactivity and sources in urban Wuhan, central China[J]. Atmospheric Environment, 2020, 224: 117340.DOI：10.1016/j.atmosenv.2020.117340.
[35] Liu B S, Liang D N, Yang J M, et al. Characterization and source apportionment of volatile organic compounds based on 1-year of observational data in Tianjin, China[J]. Environmental Pollution, 2016, 218: 757-769.DOI：10.1016/j.envpol.2016.07.072.
[36] Wu F K, Yu Y, Sun J, et al. Characteristics, source apportionment and reactivity of ambient volatile organic compounds at Dinghu Mountain in Guangdong Province, China[J]. Science of the Total Environment, 2016, 548/549: 347-359.DOI：10.1016/j.scitotenv.2015.11.069.
[37] de Gouw J A, Warneke C, Parrish D D, et al. Emission sources and ocean uptake of acetonitrile (CH3CN) in the atmosphere[J]. Journal of Geophysical Research: Atmospheres, 2003, 108(D11): 4329.DOI：10.1029/2002jd002897.
[38] Hecobian A, Liu Z, Hennigan C J, et al. Comparison of chemical characteristics of 495 biomass burning plumes intercepted by the NASA DC-8 aircraft during the ARCTAS/CARB-2008 field campaign[J]. Atmospheric Chemistry and Physics, 2011, 11(24): 13325-13337.DOI：10.5194/acp-11-13325-2011.
[39] Levine J S. Experimental evaluation of biomass burning emissions: nitrogen and carbon containing compounds[M]//Global biomass burning: atmospheric, climatic, and biospheric implications. Cambridge, Mass.: MIT Press, 1991: 289-304.
[40] Ling Z H, Guo H, Cheng H R, et al. Sources of ambient volatile organic compounds and their contributions to photochemical ozone formation at a site in the Pearl River Delta, southern China[J]. Environmental Pollution, 2011, 159(10): 2310-2319.DOI：10.1016/j.envpol.2011.05.001.
[41] 高璟赟, 肖致美, 徐虹, 等. 2019年天津市挥发性有机物污染特征及来源[J]. 环境科学, 2021, 42(1): 55-64.DOI：10.13227/j.hjkx.202006257.
[42] 刘佳, 翟崇治, 余家燕, 等. 重庆市环境空气中VOCs的空间分布及来源解析[J]. 环境科学与技术, 2018, 41(2): 71-76.DOI：10.19672/j.cnki.1003-6504.2018.02.011.
[43] Zhang F, Shang X N, Chen H, et al. Significant impact of coal combustion on VOCs emissions in winter in a North China rural site[J]. Science of the Total Environment, 2020, 720: 137617.DOI：10.1016/j.scitotenv.2020.137617.
[44] Jobson B T, Berkowitz C M, Kuster W C, et al. Hydrocarbon source signatures in Houston, Texas: influence of the petrochemical industry[J]. Journal of Geophysical Research: Atmospheres, 2004, 109(D24): D24305.DOI：10.1029/2004jd004887.
[45] Xiong Y, Bari M A, Xing Z Y, et al. Ambient volatile organic compounds (VOCs) in two coastal cities in western Canada: spatiotemporal variation, source apportionment, and health risk assessment[J]. Science of the Total Environment, 2020, 706: 135970.DOI：10.1016/j.scitotenv.2019.135970.
[46] Bari M A, Kindzierski W B, Wheeler A J, et al. Source apportionment of indoor and outdoor volatile organic compounds at homes in Edmonton, Canada[J]. Building and Environment, 2015, 90: 114-124.DOI：10.1016/j.buildenv.2015.03.023.
[47] Perry R, Gee I L. Vehicle emissions in relation to fuel composition[J]. Science of the Total Environment, 1995, 169(1/2/3): 149-156.DOI：10.1016/0048-9697(95)04643-F.
[48] Barletta B, Meinardi S, Sherwood Rowland F, et al. Volatile organic compounds in 43 Chinese cities[J]. Atmospheric Environment, 2005, 39(32): 5979-5990.DOI：10.1016/j.atmosenv.2005.06.029.
[49] Tsai W Y, Chan L Y, Blake D R, et al. Vehicular fuel composition and atmospheric emissions in South China: Hong Kong, Macau, Guangzhou, and Zhuhai[J]. Atmospheric Chemistry and Physics, 2006, 6: 3281-3288.DOI：10.5194/acp-6-3281-2006.
[50] Legreid G, Reimann S, Steinbacher M, et al. Measurements of OVOCs and NMHCs in a Swiss highway tunnel for estimation of road transport emissions[J]. Environmental Science & Technology, 2007, 41(20): 7060-7066.DOI：10.1021/es062309+.
[51] Zhang Y L, Wang X M, Zhang Z, et al. Sources of C2-C4 alkenes, the most important ozone nonmethane hydrocarbon precursors in the Pearl River Delta region[J]. Science of the Total Environment, 2015, 502: 236-245.DOI：10.1016/j.scitotenv.2014.09.024.
[52] Starn T K, Shepson P B, Bertman S B, et al. Nighttime isoprene chemistry at an urban-impacted forest site[J]. Journal of Geophysical Research: Atmospheres, 1998, 103(D17): 22437-22447.DOI：10.1029/98jd01201.
[53] Ling Z H, Guo H. Contribution of VOC sources to photochemical ozone formation and its control policy implication in Hong Kong[J]. Environmental Science & Policy, 2014, 38: 180-191.DOI：10.1016/j.envsci.2013.12.004.
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