Numerical simulation of impacts of anthropogenic chlorine emissions on secondary aerosols in different seasons
LIU Yi-ming1,2,3, ZHOU Hui-xian1,2,3, LI Si-ting1,2,3, SHEN Ao1,2,3, FAN Qi1,2,3
1. Guangdong Province Key Laboratory for Climate Change and Natural Disaster Studies, School of Atmospheric Sciences, Sun Yat-sen University, Guangzhou 510275, China; 2. Southern Marine Science and Engineering Guangdong Laboratory (Zhuhai), Zhuhai 519082, China; 3. Field Scientific Observation and Research Station of Climate Environment and Air Quality Change in the Pearl River Estuary, Guangzhou 510275, China
Abstract：Chlorine-containing species released from anthropogenic sources can participate in atmospheric chemical reactions and have an important impact on the formation of secondary aerosols. However, there are few studies on its contribution to the concentration of secondary aerosols in eastern China. In this study, we quantified effects of anthropogenic chlorine emissions on secondary inorganic and organic aerosols in different seasons using the WRF-CMAQ model. The results show that anthropogenic chlorine emissions had much stronger effect on nitrates than on sulfates. Particulate Cl- could react with HNO3, N2O5, NO3 and NO2 to form nitrates, and NH3 could be converted to ammonium. In winter, spring, summer and autumn, the anthropogenic chlorine emissions elevated both the monthly mean nitrate concentrations by up to 9.8μg/m3 (34.3%), 1.5μg/m3(11.4%), 1.3μg/m3(9.1%), and 2.6μg/m3(10.3%), respectively, and the monthly mean ammonium concentrations by up to 3.0μg/m3 (30.7%), 0.6μg/m3 (10.3%), 0.5μg/m3 (6.5%), and 1.1μg/m3 (8.0%), respectively. This impact was the most significant in winter, while the least in summer. Anthropogenic chlorine emissions have enhanced the degradation of VOCs by Cl atoms and OH radicals. The concentrations of different types of SOA have increased slightly, and the increase in SOA concentration was up to about 6%. The increase in secondary inorganic aerosols and secondary organic aerosols has led to an increase in the total amount of particulate matter. In winter, spring, summer and autumn, the anthropogenic chlorine emissions increased the monthly mean PM10 concentrations by up to 14.0μg/m3(18.3%), 2.5μg/m3(3.0%), 1.9μg/m3(2.8%), and 4.5μg/m3(4.3%), respectively, and also elevated the monthly mean PM2.5 concentrations by up to 15.0μg/m3(24.4%), 2.1μg/m3(3.5%), 1.2μg/m3(3.2%), and 3.9μg/m3(4.4%), respectively. Such impacts from large to small were winter, autumn, spring and summer and greater in the inland areas than in the coastal areas.
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LIU Yi-ming, ZHOU Hui-xian, LI Si-ting, SHEN Ao, FAN Qi. Numerical simulation of impacts of anthropogenic chlorine emissions on secondary aerosols in different seasons. CHINA ENVIRONMENTAL SCIENCECE, 2022, 42(9): 4059-4072.
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