东海大气中C<sub>2</sub>~C<sub>8</sub>非甲烷烃的来源与环境效应

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摘要采用三级低温预浓缩-气相色谱-质谱联用的方法,测定了2021年10月东海大气中16种C₂~C₈烷烃、烯烃和芳香烃等非甲烷烃(NMHCs)的浓度,探究其空间分布特征与来源,并对其环境效应进行评价.结果表明,大气中NMHCs的浓度范围为1.15~18.05×10^-9,平均值为(4.98±4.91)×10^-9,烷烃、烯烃和芳香烃的平均值分别为(2.11±2.02)×10^-9,(1.18±1.04)×10^-9和(1.69±2.51)×10^-9.东海大气不同NMHCs组分的浓度和空间分布存在较大差异,烷烃和芳香烃在整体上表现出近岸高、远海低的分布特征,但烷烃不同站位间的浓度差异更小,而烯烃则呈现出相对均匀的分布特征,其均受到人类活动的显著影响.正交矩阵因子分解模型(PMF)源解析结果表明,船舶排放对东海大气NMHCs的贡献最高,达到(32±30)%,海洋释放源的贡献占比为(28±23)%.芳香烃是调查海域大气中NMHCs的关键活性组分,其对臭氧(O₃)和二次有机气溶胶(SOA)生成的贡献显著大于烷烃和烯烃.

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关键词 ：非甲烷烃, 空间分布, 来源, 环境效应, 东海

Abstract：The concentrations of 16 kinds of C₂~C₈ non-methane hydrocarbons (NMHCs) such as alkanes, alkenes and aromatic hydrocarbons in the atmosphere over the East China Sea during October 2021 were determined with the three-step low-temperature preconcentration system coupled with a gas chromatography-mass detector, which were used to explore their spatial distribution characteristics and sources and further evaluate their environmental effects. The atmospheric mixing ratios of the total NMHCs ranged from 1.15×10^-9 to 18.05×10^-9 with an average of (4.98±4.91)×10^-9, and the average values of alkanes, alkenes and aromatic hydrocarbons were (2.11±2.02)×10^-9, (1.18±1.04)×10^-9 and (1.69±2.51)×10^-9, respectively. The concentrations and spatial distributions of different NMHCs components were quite different. The concentrations of alkanes and aromatic hydrocarbons were higher near the shore and lower away from the shore, but the concentration differences between different stations of alkanes were smaller, while the alkenes showed relatively uniform distribution characteristics, though they were strongly affected by human activities. Source apportionments by positive matrix factorization (PMF) model showed that the ship emissions were the highest contributor for atmospheric NMHCs, which accounted for (32±30)%, and the contribution of marine emission sources was (28±23)%. Aromatic hydrocarbons were the key active components of the atmospheric NMHCs over the East China Sea, and their contributions to the generation of ozone (O₃) and secondary organic aerosol (SOA) were significantly greater than those of alkanes and alkenes.

Key words： non-methane hydrocarbon spatial distribution source environmental effect East China Sea

收稿日期: 2022-11-18

PACS:

X511

基金资助:国家自然科学基金资助项目(41876082;42276042);自然资源部海洋大气化学与全球变化重点实验室开放基金资助课题(GCMAC2007)

通讯作者: 张洪海,教授,honghaizhang@ouc.edu.cn E-mail: honghaizhang@ouc.edu.cn

作者简介: 柳振飞(1997-),男,山东青岛人,中国海洋大学化学化工学院硕士研究生,主要从事海洋非甲烷烃释放及环境效应评价研究.zfliu1010@163.com

引用本文:

柳振飞, 吴英璀, 乔浩, 周立敏, 张洪海. 东海大气中C₂~C₈非甲烷烃的来源与环境效应[J]. 中国环境科学, 2023, 43(7): 3281-3289. LIU Zhen-fei, WU Ying-cui, QIAO Hao, ZHOU Li-min, ZHANG Hong-hai. Sources and environmental effects of C₂~C₈ non-methane hydrocarbons in the atmosphere over the East China Sea. CHINA ENVIRONMENTAL SCIENCECE, 2023, 43(7): 3281-3289.

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http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2023/V43/I7/3281

[1]	Atkinson R. Atmospheric chemistry of VOCs and NOx [J]. Atmospheric Environment, 2000,34(12-14):2063-2101.
[2]	Hallquist M, Wenger J C, Baltensperger U, et al. The formation, properties and impact of secondary organic aerosol: current and emerging issues [J]. Atmospheric Chemistry and Physics, 2009,9(14): 5155-5236.
[3]	Yuan Q, Lai S, Song J, et al. Seasonal cycles of secondary organic aerosol tracers in rural Guangzhou, Southern China: the importance of atmospheric oxidants [J]. Environmental Pollution, 2018,240:884-893.
[4]	Guenther A B, Jiang X, Heald C L, et al. The model of emissions of gases and aerosols from nature version 2.1 (MEGAN2.1): an extended and updated framework for modeling biogenic emissions [J]. Geoscientific Model Development, 2012,5(6):1471-1492.
[5]	Luo G, Yu F. A numerical evaluation of global oceanic emissions of α-pinene and isoprene [J]. Atmospheric Chemistry and Physics, 2010,10(4):2007-2015.
[6]	Colomb A, Yassaa N, Williams J, et al. Screening volatile organic compounds (VOCs) emissions from five marine phytoplankton species by head space gas chromatography/mass spectrometry (HS-GC/MS) [J]. Journal of Environmental Monitoring, 2008,10(3):325-330.
[7]	吴英璀,李建龙,王健,等.春季黄、渤海中异戊二烯的浓度空间分布与海-气通量 [J]. 中国环境科学, 2018,38(3):893-899. Wu Y C, Li J L, Wang J, et al. Spatial distribution and sea-to-air flux of isoprene concentration in the Yellow Sea and the Bohai Sea in spring [J]. China Environmental Science, 2018,38(3):893-899.
[8]	Gilman J B, Lerner B M, Kuster W C, et al. Source signature of volatile organic compounds from oil and natural gas operations in Northeastern Colorado [J]. Environmental Science & Technology, 2013,47(3):1297-1305.
[9]	Helmig D, Muñoz M, Hueber J, et al. Climatology and atmospheric chemistry of the non-methane hydrocarbons ethane and propane over the North Atlantic [J]. Elementa: Science of the Anthropocene, 2015, 3:000054.
[10]	Singh H, Zimmerman P. Atmospheric distribution and sources of nonmethane hydrocarbons [J]. Gaseous pollutants: Characterization and Cycling, 1992,24:177-235.
[11]	Bourtsoukidis E, Ernle L, Crowley J N, et al. Non-methane hydrocarbon (C2-C8) sources and sinks around the Arabian Peninsula [J]. Atmospheric Chemistry and Physics, 2019,19(10):7209-7232.
[12]	Xiao Q, Li M, Liu H, et al. Characteristics of marine shipping emissions at berth: profiles for particulate matter and volatile organic compounds [J]. Atmospheric Chemistry and Physics, 2018,18(13): 9527-9545.
[13]	Li C, Borken-Kleefeld J, Zheng J, et al. Decadal evolution of ship emissions in China from 2004 to 2013 by using an integrated AIS-based approach and projection to 2040 [J]. Atmospheric Chemistry and Physics, 2018,18(8):6075-6093.
[14]	Mallik C, Lal S, Venkataramani S, et al. Variability in ozone and its precursors over the Bay of Bengal during post monsoon: Transport and emission effects [J]. Journal of Geophysical Research: Atmospheres, 2013,118(17):10190-10209.
[15]	Song J, Zhao Y, Zhang Y, et al. Influence of biomass burning on atmospheric aerosols over the western South China Sea: Insights from ions, carbonaceous fractions and stable carbon isotope ratios [J]. Environmental Pollution, 2018,242:1800-1809.
[16]	Song J, Zhao Y, Zhang Y, et al. A case study on the characterization of non-methane hydrocarbons over the South China Sea: Implication of land-sea air exchange [J]. Science of the Total Environment, 2020, 717:134754.
[17]	张浩然,刘敏,王小嫚,等.南昌市2021年春季大气VOCs污染特征和来源分析 [J]. 中国环境科学, 2022,42(3):1040-1047. Zhang H R, Liu M, Wang X M, et al. Characteristics and sources of atmospheric VOCs during spring of 2021in Nanchang [J]. China Environmental Science, 2022,42(3):1040-1047.
[18]	陆嘉晖,吴影,刘慧琳,等.南宁市冬季挥发性有机物特征及其来源分析 [J]. 中国环境科学, 2022,42(8):3616-3625. Lu J H, Wu Y, Liu H L, et al. Characteristics and sources of volatile organic compounds (VOCs) in winter over Nanning of China [J]. China Environmental Science, 2022,42(8):3616-3625.
[19]	Liu C, Mu Y, Zhang C, et al. A comparison investigation of atmospheric NMHCs at two sampling sites of Beijing city and a rural area during summertime [J]. Science of The Total Environment, 2021, 783:146867.
[20]	李思潼,王健,吴英璀,等.长江口及邻近海域大气中C2-C5非甲烷烃来源与环境效应研究 [J]. 中国海洋大学学报(自然科学版), 2021,51(10):71-79. Li S T, Wang J, Wu Y C, et al. Research on sources and environmental effects of C2-C5non-methane hydrocarbons in the atmosphere over the Yangtze River estuary and its adjacent areas [J]. Periodical of Ocean University of China, 2021,51(10):71-79.
[21]	Li J L, Zhai X, Zhang H H, et al. Temporal variations in the distribution and sea-to-air flux of marine isoprene in the East China Sea [J]. Atmospheric Environment, 2018,187:131-143.
[22]	Li J, Zhai X, Ma Z, et al. Spatial distributions and sea-to-air fluxes of non-methane hydrocarbons in the atmosphere and seawater of the Western Pacific Ocean [J]. Science of the Total Environment, 2019, 672:491-501.
[23]	DB37/T 4434-2021 环境空气57种臭氧前体物的测定罐采样/气相色谱-氢火焰离子化检测器/质谱联用法 [S]. DB37/T 4434-2021 Ambient air-Determination of 57kinds of ozone precursor compounds-Collected inspecially-prepared canisters and analyzed by gas chromatography-flame ionization detector/mass spectrometer [S].
[24]	Carter W P L. Development of ozone reactivity scales for volatile organic compounds [J]. Journal of the Air & Waste Management Association, 1994,44(7):881-899.
[25]	Carter W P L. Development of the SAPRC-07chemical mechanism and updated ozone reactivity scales [J]. Atmospheric Environment, 2010,44:5324-5335.
[26]	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.
[27]	张洲.中国大气非甲烷碳氢化合物时空分布特征初步研究 [D]. 广州:中国科学院广州地球化学研究所, 2016. Zhang Z. Spatiotemporal patterns of ambient non-methane hydrocarbons in China [D]. Guangzhou: Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, 2016.
[28]	Blake D R, Chen T Y, Smith T W, et al. Three-dimensional distribution of nonmenthane hydrocarbons and halocarbons over the northwestern Pacific during the 1991Pacific Exploratory Mission (PEM-West A) [J]. Journal of Geophysical Research: Atmospheres, 1996,101(D1):1763-1778.
[29]	Li J L, Zhai X, Wu Y C, et al. Emissions and potential controls of light alkenes from the marginal seas of China [J]. Science of The Total Environment, 2021,758:143655.
[30]	赵其然,李建龙,吴英璀,等.秋季黄渤海C2~C5非甲烷烃海-气通量与大气反应活性 [J]. 中国环境科学, 2019,39(5):1838-1846. Zhao Q R, Li J L, Wu Y C, et al. Sea-air fluxes and atmospheric chemical reactivity of C2~C5non-methane hydrocarbon in the Yellow Sea and the Bohai Sea during autumn [J]. China Environmental Science, 2019,39(5):1838-1846.
[31]	Kato S, Ui T, Uematsu M, et al. Trace gas measurements over the northwest Pacific during the 2002IOC cruise [J]. Geochemistry Geophysics Geosystems, 2007,8:Q06M10.
[32]	Mo Z, Shao M, Lu S, et al. Characterization of non-methane hydrocarbons and their sources in an industrialized coastal city, Yangtze River Delta, China [J]. Science of the Total Environment, 2017,593-594:641-653.
[33]	Liu Y, Shao M, Fu L, et al. Source profiles of volatile organic compounds (VOCs) measured in China: Part I [J]. Atmospheric Environment, 2008,42(25):6247-6260.
[34]	Rappenglück B, Oyola P, Olaeta I, et al. The evolution of photochemical smog in the metropolitan area of Santiago de Chile [J]. Journal of Applied Meteorology, 2000,39(3):275-290.
[35]	Monod A, Barkley C S, Avino P, et al. Monoaromatic compounds in ambient air of various cities: a focus on correlations between the xylenes and ethylbenzene [J]. Atmospheric Environment, 2001,35(1): 135-149.
[36]	管贤贤,齐安安,雷春妮,等.兰州市大气苯系物的化学活性特征与健康风险评价 [J]. 环境科学学报, 2020,40(2):459-468. Guan X X, Qi A A, Lei C N, et al. Chemical activity characteristics and health risk assessment of atmospheric benzene homologues in Lanzhou [J]. Acta Scientiae Circumstantiae, 2020,40(2):459-468.
[37]	Russo R S, Zhou Y, White M L, et al. Multi-year (2004-2008) record of nonmethane hydrocarbons and halocarbons in New England: seasonal variations and regional sources [J]. Atmospheric Chemistry and Physics, 2010,10(10):4909-4929.
[38]	Gentner D R, Harley R A, Miller A M, et al. Diurnal and seasonal variability of gasoline-related volatile organic compound emissions in Riverside, California [J]. Environmental Science & Technology, 2009,43(12):4247-4252.
[39]	Zhu H, Wang H, Jing S, et al. Characteristics and sources of atmospheric volatile organic compounds (VOCs) along the mid-lower Yangtze River in China [J]. Atmospheric Environment, 2018,190:232-240.
[40]	肖龙,王帅,周颖,等.中国典型背景站夏季VOCs污染特征及来源解析 [J]. 中国环境科学, 2021,41(5):2014-2027. Xiao L, Wang S, Zhou Y, et al. The characteristics and source apportionments of VOCs at typical background sites during summer in China [J]. China Environmental Science, 2021,41(5):2014-2027.
[41]	Blake D R, Rowland F S. Urban leakage of liquefied petroleum gas and its impact on Mexico City air quality [J]. Science, 1995,269(5226): 953-956.
[42]	Song J, Zhang Y, Huang Y, et al. Seasonal variations of C1-C4 alkyl nitrates at a coastal site in Hong Kong: Influence of photochemical formation and oceanic emissions [J]. Chemosphere, 2018,194:275-284.