Influence of atmospheric in-cloud aqueous-phase chemistry on the global simulation of SO<sub>2</sub> in CESM2
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Published:2021-11-02
Issue:21
Volume:21
Page:16093-16120
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ISSN:1680-7324
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Container-title:Atmospheric Chemistry and Physics
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language:en
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Short-container-title:Atmos. Chem. Phys.
Author:
Ge Wendong, Liu Junfeng, Yi Kan, Xu Jiayu, Zhang Yizhou, Hu Xiurong, Ma Jianmin, Wang XuejunORCID, Wan Yi, Hu Jianying, Zhang Zhaobin, Wang Xilong, Tao Shu
Abstract
Abstract. Sulfur dioxide (SO2) is a major atmospheric pollutant and precursor of sulfate aerosols, which influences air quality, cloud microphysics, and climate. Therefore, better understanding the conversion of SO2 to sulfate is essential to simulate and predict sulfur compounds more accurately. This study evaluates the effects of in-cloud aqueous-phase chemistry on SO2 oxidation in the Community Earth System Model version 2 (CESM2). We replaced the default parameterized SO2 aqueous-phase reactions with detailed HOx, Fe, N, and carbonate chemistry in cloud droplets and performed a global simulation for 2014–2015. Compared with the observations, the results incorporating detailed cloud aqueous-phase chemistry greatly reduced SO2 overestimation. This overestimation was reduced by 0.1–10 ppbv (parts per billion by volume) in most of Europe, North America, and Asia and more than 10 ppbv in parts of China. The biases in annual simulated SO2 mixing ratios decreased by 46 %, 41 %, and 22 % in Europe, the USA, and China, respectively. Fe chemistry and HOx chemistry contributed more to SO2 oxidation than N chemistry. Higher concentrations of soluble Fe and higher pH values could further enhance the oxidation capacity. This study emphasizes the importance of detailed in-cloud aqueous-phase chemistry for the oxidation of SO2. These mechanisms can improve SO2 simulation in CESM2 and deepen understanding of SO2 oxidation and sulfate formation.
Funder
National Natural Science Foundation of China
Publisher
Copernicus GmbH
Subject
Atmospheric Science
Reference213 articles.
1. Acid Deposition Monitoring Network in East Asia: Data Report, Acid Deposition Monitoring Network in East Asia [data set], available at: https://monitoring.eanet.asia/document/public/index, last access: 2 November 2020. 2. Adams, G. E. and Boag, J. W.:
Spectroscopic studies of reactions of the OH radical,
P. Chem. Soc. London,
1, 112–118, 1964. 3. Alexander, B., Park, R. J., Jacob, D. J., and Gong, S.:
Transition metal-catalyzed oxidation of atmospheric sulfur: Global implications for the sulfur budget,
J. Geophys. Res.,
114, D02309, https://doi.org/10.1029/2008jd010486, 2009. 4. Amels, P., Elias, H., Götz, U., Steinges, U., and Wannowius, K. J.:
Kinetic investigation of the stability of peroxonitric acid and of its reaction with sulfur(IV) in aqueous solution,
in: Heterogeneous and Liquid Phase Processes,
edited by: Warneck, P.,
Transport and Chemical Transformation in Pollutants in the Troposphere,
Springer, Berlin, 77–88, 1996. 5. Au Yang, D., Bardoux, G., Assayag, N., Laskar, C., Widory, D., and Cartigny, P.:
Atmospheric SO2 oxidation by NO2 plays no role in the mass independent sulfur isotope fractionation of urban aerosols,
Atmos. Environ.,
193, 109–117, https://doi.org/10.1016/j.atmosenv.2018.09.007, 2018.
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