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南京夏季大气臭氧光化学特征与敏感性分析
引用本文:罗丽彤,章炎麟,林煜棋,Ahsan Mozaffar,曹梦瑶. 南京夏季大气臭氧光化学特征与敏感性分析[J]. 环境科学, 2024, 45(3): 1382-1391
作者姓名:罗丽彤  章炎麟  林煜棋  Ahsan Mozaffar  曹梦瑶
作者单位:南京信息工程大学应用气象学院, 南京 210044;南京信息工程大学教育部气候与环境变化国际合作联合实验室, 大气环境中心, 南京 210044
基金项目:国家自然科学基金项目(42192512,41977305,42150410379)
摘    要:对流层臭氧(O3)主要由氮氧化物(NOx)和挥发性有机物(VOCs)经过一系列光化学反应生成,反应过程呈现复杂的非线性关系.为深入了解O3的光化学特征及生成机制,利用2018年夏季大气O3与VOCs的观测数据,结合大气零维框架模拟模型F0AM-MCM,研究O3超标日和非O3超标日的O3光化学特征之间的差异性.观测结果表明,O3超标日期间φ(O3)和φ(TVOCs)的平均值分别为47.8×10-9和49.0×10-9,为非O3超标日期间O3(26×10-9)和TVOCs(30×10-9)体积分数的1.8倍和1.6倍.使用F0AM模型,借助EKMA曲线和RIR分析等识别O3敏感性,发现南京市O3超标日和非O3超标日O3的形成均主要受VOCs和NOx的协同控制.F0AM-MCM模拟结果表明,在O3超标日,·OH和HO2的日平均混合比分别是非O3超标日的1.3倍和1.8倍,表明O3超标日期间具有更强的大气氧化能力,且·OH和HO2的形成和损失速率也有明显的增加,表明自由基循环的增强.此外,O3超标日的O3生成速率明显高于非O3超标日,从而导致了O3超标日的O3净生成速率明显高于非O3超标日.以上发现提高了对南京夏季O3超标日大气O3光化学特征的认识.

关 键 词:臭氧(O3)  挥发性有机物(VOCs)  臭氧敏感性  F0AM模型  生成机制
收稿时间:2023-03-25
修稿时间:2023-05-18

Analysis of Photochemical Characteristics and Sensitivity of Atmospheric Ozone in Nanjing in Summer
LUO Li-tong,ZHANG Yan-lin,LIN Yu-qi,Ahsan Mozaffar,CAO Meng-yao. Analysis of Photochemical Characteristics and Sensitivity of Atmospheric Ozone in Nanjing in Summer[J]. Chinese Journal of Environmental Science, 2024, 45(3): 1382-1391
Authors:LUO Li-tong  ZHANG Yan-lin  LIN Yu-qi  Ahsan Mozaffar  CAO Meng-yao
Affiliation:School of Applied Meteorology, Nanjing University of Information Science & Technology, Nanjing 210044, China;Atmospheric Environment Center, Joint Laboratory for International Cooperation on Climate and Environmental Change Ministry of Education (ILCEC), Nanjing University of Information Science & Technology, Nanjing 210044, China
Abstract:Tropospheric ozone (O3) is mainly produced through a series of photochemical reactions of nitrogen oxides (NOx) and volatile organic compounds (VOCs). The reaction process presents complex non-linear relationships. In this work, datasets of atmospheric ozone and volatile organic compounds (VOCs) observed during the summer of 2018 in Nanjing were used. Combining with the framework for 0-D atmospheric model-master chemical mechanism (F0AM-MCM), the characteristics of photochemical reactions for ozone (O3) formation in Nanjing during the O3 episode days and non-episode days were investigated. The results showed that φ(O3) and φ(TVOCs) in the O3 episode days were 47.8×10-9 and 49.0×10-9, respectively, exceeding those in the non-episode days by factors of 1.8 and 1.6. Furthermore, F0AM, the empirical kinetic modeling approach (EKMA), and relative incremental reactivity (RIR) were utilized for the calculation of ozone chemical sensitivity. It was found that O3 formation in Nanjing was attributed to both VOCs and NOx limitation. In addition, the modeled ·OH and HO2 concentrations in the O3 episode days were 1.3 and 1.8 times higher than those in the non-episode days. The higher formation and loss rates of ·OH and HO2 were also found during O3 episode days. These findings reflected that the enhancements of atmospheric oxidation capacity resulted in increased production rates of O3, providing an explanation for the enhancements of O3 concentrations in Nanjing during the O3 episode days. The findings also improved the understanding of the O3 photochemical characteristics over Nanjing in the summer during the O3 episode days.
Keywords:ozone(O3)  volatile organic compounds(VOCs)  ozone sensitivity  F0AM  formation mechanisms
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