武汉夏季光化学过程二羰基的污染特征及来源

黄海滨; 成海容; 胡柯; 黄宇; 邓萌杰; 陶卉婷

PDF(1320 KB)

中国环境科学 ›› 2023, Vol. 43 ›› Issue (10) : 5114-5122.

大气污染与控制

武汉夏季光化学过程二羰基的污染特征及来源

黄海滨¹, 成海容¹, 胡柯², 黄宇³, 邓萌杰¹, 陶卉婷¹

作者信息 +

Characteristics and sources of dicarbonyl compounds during summer photochemical pollution episodes in Wuhan

HUANG Hai-bin¹, CHENG Hai-rong¹, HU Ke², HUANG Yu³, DENG Meng-jie¹, TAO Hui-ting¹

Author information +

文章历史 +

摘要

2021年在武汉城区开展了夏季光化学污染过程中大气羰基化合物的离线观测和大气挥发性有机物（VOCs）的在线监测，研究该时期乙二醛和甲基乙二醛的污染特征并利用正交矩阵因子模型（PMF）对其来源进行解析.武汉夏季大气乙二醛和甲基乙二醛的平均浓度分别为（0.42±0.34）×10^-9和（0.69±0.19）×10^-9，两者均呈现“单峰型”日变化规律，在上午10：00达到峰值.PMF共解析出6类源，乙二醛的源贡献为二次生成（A）（70.86%）>溶剂使用源（8.05%）>机动车排放源（8.04%）>燃烧源（6.43%）>工业源（3.38%）>二次生成（B）（3.24%）；甲基乙二醛的主要排放源及贡献率为二次生成（A）（39.10%）>二次生成（B）（31.54%）>机动车排放源（13.26%）>溶剂使用源（8.21%）>燃烧源（5.80%）>工业源（2.09%）.由于强烈的光化学作用，二次生成是乙二醛和甲基乙二醛最主要的来源.光化学污染期与非污染期相比，二次生成（A）对乙二醛和甲基乙二醛的贡献显著增加.研究结果有助于提高对武汉市大气乙二醛和甲基乙二醛的认识，为武汉市政府制定大气污染防治策略提供数据基础和科学依据.

Abstract

Field measurements of atmospheric carbonyl compounds and volatile organic compounds (VOCs) were conducted during the summer photochemical pollution process in Wuhan in 2021. This study focused on the pollution characteristics of glyoxal and methylglyoxal and analyzed their sources using positive matrix factor model (PMF). The average concentrations of glyoxal and methylglyoxal in Wuhan were (0.42±0.34)×10^-9and (0.69±0.19)×10^-9, respectively, and both showed a "unimodal type" diurnal pattern, peaking at 10a.m. Six sources were identified using PMF. The contributions of these sources to glyoxal were in the order of secondary formation (A) (70.86%) > solvent usage (8.05%) > vehicle emission (8.04%) > combustion (6.43%) > industrial emission (3.38%) > secondary formation (B). The contributions of different sources to methylglyoxal were in the order of secondary formation (A) (39.10%) > secondary formation (B) (31.54%) > vehicle emission (13.26%) > solvent usage (8.21%) > combustion (5.80%) > industrial emission (2.09%). Due to the strong photochemical reactions in summer, secondary formation was the most important source of glyoxal and methylglyoxal. Compared with those during the non-episodes, the contribution of secondary formation (A) to glyoxal and methylglyoxal increased significantly during the O₃-polluted photochemical episodes. This study helps to improve the understanding of glyoxal and methylglyoxal in Wuhan, and provides valuable datasets for the government of Wuhan to formulate air pollution prevention and control strategies.

导出引用

黄海滨, 成海容, 胡柯, 黄宇, 邓萌杰, 陶卉婷. 武汉夏季光化学过程二羰基的污染特征及来源[J]. 中国环境科学. 2023, 43(10): 5114-5122

HUANG Hai-bin, CHENG Hai-rong, HU Ke, HUANG Yu, DENG Meng-jie, TAO Hui-ting. Characteristics and sources of dicarbonyl compounds during summer photochemical pollution episodes in Wuhan[J]. China Environmental Science. 2023, 43(10): 5114-5122

中图分类号： X511

参考文献

[1] Wang N, Lyu X, Deng X, et al. Aggravating O₃ pollution due to NO_x emission control in eastern China[J]. Science of the Total Environment, 2019,677:32-744.
[2] Li Q, Gong D, Wang H, et al. Rapid increase in atmospheric glyoxal and methylglyoxal concentrations in Lhasa, Tibetan Plateau:Potential sources and implications[J]. Science of The Total Environment, 2022,824:153782.
[3] 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.
[4] Liu X F, Guo H, Zeng L W, et al. Photochemical ozone pollution in five Chinese megacities in summer 2018[J]. Science of the Total Environment, 2021,801:49603.
[5] Wang J, Zhang Y L, Wu Z F, et al. Ozone episodes during and after the 2018 Chinese National Day holidays in Guangzhou:Implications for the control of precursor VOCs[J]. Journal of Environmental Sciences, 2022,114:322-333.
[6] Zeng P, Lyu X, Guo H, et al. Spatial variation of sources and photochemistry of formaldehyde in Wuhan, Central China[J]. Atmospheric Environment, 2019,214:116826.
[7] Fu T M, Jacob D J, Wittrock F, et al. Global budgets of atmospheric glyoxal and methylglyoxal, and implications for formation of secondary organic aerosols[J]. Journal of Geophysical Research:Atmospheres, 2008,113(D15).
[8] Qian X, Shen H, Chen Z. Characterizing summer and winter carbonyl compounds in Beijing atmosphere[J]. Atmospheric Environment, 2019,214:116845.
[9] Lv S, Gong D, Ding Y, et al. Elevated levels of glyoxal and methylglyoxal at a remote mountain site in southern China:Prompt in-situ formation combined with strong regional transport[J]. Science of the Total Environment, 2019,672:869-882.
[10] Dai W T, Ho S S H, Ho K F, et al. Seasonal and diurnal variations of mono-and di-carbonyls in Xi'an, China[J]. Atmospheric Research, 2012,113:102-112.
[11] Yang X, Xue L, Wang T, et al. Observations and explicit modeling of summertime carbonyl formation in Beijing:Identification of key precursor species and their impact on atmospheric oxidation chemistry[J]. Journal of Geophysical Research-Atmospheres, 2018,123(2):1426-1440.
[12] Qiu X, Wang S, Ying Q, et al. Importance of wintertime anthropogenic glyoxal and methylglyoxal emissions in Beijing and implications for secondary organic aerosol formation in megacities[J]. Environmental Science and Technology, 2020,54(19):11809-11817.
[13] Liu Y, Wang H, Jing S, et al. Characteristics and sources of volatile organic compounds (VOCs) in Shanghai during summer:Implications of regional transport[J]. Atmospheric Environment, 2019,215:116902.
[14] Guo Y, Wang S, Zhu J, et al. Atmospheric formaldehyde, glyoxal and their relations to ozone pollution under low-and high-NO_x regimes in summertime Shanghai, China[J]. Atmospheric Research, 2021,258:105635.
[15] Liu J, Li X, Li D, et al. Observations of glyoxal and methylglyoxal in a suburban area of the Yangtze River Delta, China[J]. Atmospheric Environment, 2020, 238:117727.
[16] Li X, Brauers T, Hofzumahaus A, et al. MAX-DOAS measurements of NO₂, HCHO and CHOCHO at a rural site in Southern China[J]. Atmospheric Chemistry and Physics, 2013,13(4):2133-2151.
[17] Wu Z, Zhang Y, Pei C, et al. Real-world emissions of carbonyls from vehicles in an urban tunnel in south China[J]. Atmospheric Environment, 2021,258:118491.
[18] Chang D, Wang Z, Guo J, et al. Characterization of organic aerosols and their precursors in southern China during a severe haze episode in January 2017[J]. Science of the Total Environment, 2019,691:101-111.
[19] Ho K F, Ho S S H, Huang R J, et al. Spatiotemporal distribution of carbonyl compounds in China[J]. Environmental Pollution, 2015, 197:316-324.
[20] Yang Z, Cheng H R, Wang Z W, et al. Chemical characteristics of atmospheric carbonyl compounds and source identification of formaldehyde in Wuhan, Central China[J]. Atmospheric Research, 2019,228:95-106.
[21] Lui K H, Dai W T, Chan C S, et al. Spatial distributions of airborne di-carbonyls in urban and rural areas in China[J]. Atmospheric Research, 2017,186:1-8.
[22] HJ 683-2014环境空气醛、酮类化合物的测定高效液相色谱法[S]. HJ 683-2014 Ambient air-Determination of aldehyde and ketone compounds-High performance liquid chromatography[S].
[23] US EPA TO-11A:Determination of formaldehyde in ambient air using adsorbent cartridge followed by high performance liquid chromatography (HPLC)[S]. 1999.
[24] Ling Z H, Zhao J, Fan S J, et al. Sources of formaldehyde and their contributions to photochemical O₃ formation at an urban site in the Pearl River Delta, southern China[J]. Chemosphere, 2017,168:1293-1301.
[25] 胡崑,王鸣,王红丽,等.基于PMF和源示踪物比例法的大气羰基化合物来源解析:以南京市观测为例[J]. 环境科学, 2021,42(1):45-54. Hu K, Wang M, Wang H L, et al. Source apportionment of ambient carbonyl compounds based on a PMF and source tracer ratio method:a case based on observations in Nanjing[J]. Environmental Science, 2021,42(1):45-54.
[26] 苏维峰,孔少飞,郑煌,等.武汉市夏季大气挥发性有机物实时组成及来源[J]. 环境科学, 2022,43(6):2966-2978. Su W F, Kong S F, Zheng H, et al. Real-time composition and sources of VOCs in summer in Wuhan[J]. Environmental Science, 2022, 43(6):2966-2978
[27] Ho K F, Ho S S H, Dai W T, et al. Seasonal variations of monocarbonyl and dicarbonyl in urban and sub-urban sites of Xi'an, China[J]. Environmental Monitoring and Assessment, 2014,186(5):2835-2849.
[28] Kawamura K, Okuzawa K, Aggarwal S G, et al. Determination of gaseous and particulate carbonyls (glycolaldehyde, hydroxyacetone, glyoxal, methylglyoxal, nonanal and decanal) in the atmosphere at Mt. Tai[J]. Atmospheric Chemistry and Physics, 2013,13(10):5369-5380.
[29] Schauer J J, Kleeman M J, Cass G R, et al. Measurement of emissions from air pollution sources. 3. C1−C29organic compounds from fireplace combustion of wood[J]. Environmental Science and Technology, 2001,35(9):1716-1728.
[30] Schauer J J, Kleeman M J, Cass G R, et al. Measurement of emissions from air pollution sources. 5. C1−C32 organic compounds from gasoline-powered motor vehicles[J]. Environmental Science and Technology, 2002,36(6):1169-1180.
[31] DiGangi J P, Henry S B, Kammrath A, et al. Observations of glyoxal and formaldehyde as metrics for the anthropogenic impact on rural photochemistry[J]. Atmospheric Chemistry and Physics, 2012,12(20):9529-9543.
[32] Vrekoussis M, Wittrock F, Richter A, et al. GOME-2observations of oxygenated VOCs:what can we learn from the ratio glyoxal to formaldehyde on a global scale?[J]. Atmospheric Chemistry and Physics, 2010,10(21):10145-10160.
[33] Cui J, Sun M, Wang L, et al. Gas-particle partitioning of carbonyls and its influencing factors in the urban atmosphere of Zhengzhou, China[J]. Science of the Total Environment, 2021,751:142027.
[34] 赵锐,黄络萍,张建强,等.成都市典型溶剂源使用行业VOCs排放成分特征[J]. 环境科学学报, 2018,38(3):1147-1154. Zhao R, Huang L P, Zhang J Q, et al. Emissions characteristics of volatile organic compounds (VOCs) from typical industries of solvent use in Chengdu City[J]. Acta Scientiae Circumstantiae, 2018,38(3):1147-1154.
[35] 黄娟,冯艳丽,王新明,等.浙江嘉兴农场大气羰基化合物水平及来源[J]. 中国环境科学, 2009,29(8):795-800. Huang J, Feng Y L, Wang X M, et al. Carbonyl compounds levels and sources in one farm of JiaXing, Zhejiang Province[J]. China Environmental Science, 2009,29(8):795-800.
[36] 张扬,韩士杰,李勤勤,等.低NO_x环境异戊二烯促进甲苯生成甲基丁烯二醛的模拟实验[J]. 中国环境科学, 2022,42(9):4001-4008. Zhang Y, Han S J, Li Q Q, et al. A chamber study on isoprene-promoting the production of toluene-derived methylbutenedial in low NO_x environment[J]. China Environmental Science, 2022,42(9):4001-4008.
[37] Wennberg P O, Bates K H, Crounse J D, et al. Gas-phase reactions of isoprene and its major oxidation products[J]. Chemical Reviews, 2018, 118(7):3337-3390.
[38] Song C, Liu Y, Sun L, et al. Emissions of volatile organic compounds (VOCs) from gasoline-and liquified natural gas (LNG)-fueled vehicles in tunnel studies[J]. Atmospheric Environment, 2020,234:117626.
[39] Zhang Q, Wu L, Fang X, et al. Emission factors of volatile organic compounds (VOCs) based on the detailed vehicle classification in a tunnel study[J]. Science of the Total Environment, 2018,624:878-886.