不同季节人为氯排放对二次气溶胶影响的数值模拟

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摘要利用WRF-CMAQ模式对比有无人为氯排放的模拟试验,定量分析了不同季节人为氯排放对二次无机气溶胶和二次有机气溶胶的影响.结果表明,人为氯排放对硫酸盐的影响较小,而硝酸盐对人为氯排放较为敏感,Cl^-颗粒物与HNO₃、N₂O₅、NO₃和NO₂均可发生反应生成硝酸盐,同时NH₃也会转化为铵盐.人为氯排放使冬、春、夏、秋季硝酸盐月均浓度分别最高增加9.8 μg/m³(34.3%)、1.5μg/m³(11.4%)、1.3μg/m³(9.1%)和2.6μg/m³(10.3%),铵盐月均浓度分别最高增加3.0μg/m³(30.7%)、0.6μg/m³(10.3%)、0.5μg/m³(6.5%)和1.1μg/m³(8.0%),冬季影响最大,夏季影响最小.人为氯排放增强了Cl原子和OH自由基对VOCs的降解作用,不同种类的SOA浓度略有上升,人为氯排放对SOA浓度影响最大约为6%.二次无机气溶胶和二次有机气溶胶的增加导致了颗粒物总量的增加,人为氯排放使冬、春、夏、秋季PM₁₀月均浓度分别最高增加14.0μg/m³(18.3%)、2.5μg/m³(3.0%)、1.9μg/m³(2.8%)和4.5μg/m³(4.3%),PM_2.5月均浓度分别最高增加15.0μg/m³(24.4%)、2.1μg/m³(3.5%)、1.2μg/m³(3.2%)和3.9μg/m³(4.4%).人为氯排放的季节性影响从大到小分别为冬、秋、春、夏季,内陆的影响比沿海大.

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关键词 ：氯化氢, 氯气, 二次气溶胶, 公共多尺度空气质量模式(CMAQ), PM_2.5

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 PM_2.5 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.

Key words： HCl Cl₂ secondary aerosol CMAQ PM_2.5

收稿日期: 2022-01-10

PACS:

X513

基金资助:国家自然科学基金资助项目(42105097,42075181);国家重点研发计划(2019YFC0214605);广东省科技计划项目(科技创新平台类)(2019B121201002);广东省基础与应用基础研究重大项目(2020B0301030004)

通讯作者: 刘一鸣,助理教授,liuym88@mail.sysu.edu.cn E-mail: liuym88@mail.sysu.edu.cn

作者简介: 刘一鸣(1993-),男,广东广州人,助理教授,博士,主要从事空气污染数值模拟研究.发表文章40余篇.

引用本文:

刘一鸣, 周慧娴, 李思婷, 沈傲, 樊琦. 不同季节人为氯排放对二次气溶胶影响的数值模拟[J]. 中国环境科学, 2022, 42(9): 4059-4072. 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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http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2022/V42/I9/4059

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