Preprints
https://doi.org/10.5194/acp-2021-406
https://doi.org/10.5194/acp-2021-406

  16 Jun 2021

16 Jun 2021

Review status: a revised version of this preprint was accepted for the journal ACP and is expected to appear here in due course.

Influence of atmospheric in-cloud aqueous-phase chemistry on global simulation of SO2 in CESM2

Wendong Ge1, Junfeng Liu1, Kan Yi2, Jiayu Xu1, Yizhou Zhang1, Xiurong Hu3, Jianmin Ma1, Xuejun Wang1, Yi Wan1, Jianying Hu1, Zhaobin Zhang1, Xilong Wang1, and Shu Tao1 Wendong Ge et al.
  • 1Laboratory for Earth Surface Processes, College of Urban and Environmental Sciences, Peking University, Beijing, 100871, China
  • 2Institute of Science and Technology, China Three Gorges Corporation, Beijing, 100038, China
  • 3College of Economics and Management, Nanjing University of Aeronautics and Astronautics, Nanjing, 211106, China

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 aqueous-phase reactions with detailed HOx-, Fe-, N- and carbonate chemistry and performed a global simulation for 2014–2015. Compared with the observations, the results incorporating detailed aqueous-phase chemistry greatly reduced SO2 overestimation. This overestimation was reduced by 0.1–10 ppbv in most of Europe, North America and Asia and more than 10 ppbv in parts of China. The biases in annual simulated SO2 concentrations decreased by 46 %, 41 %, and 22 % in Europe, the United States 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 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.

Wendong Ge et al.

Status: closed

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on acp-2021-406, boundary conditions and constraints?', Anonymous Referee #1, 06 Jul 2021
  • RC2: 'Comment on acp-2021-406', Anonymous Referee #2, 07 Aug 2021

Status: closed

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on acp-2021-406, boundary conditions and constraints?', Anonymous Referee #1, 06 Jul 2021
  • RC2: 'Comment on acp-2021-406', Anonymous Referee #2, 07 Aug 2021

Wendong Ge et al.

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Short summary
Compared with the observations, the results incorporating detailed aqueous-phase chemistry greatly reduced SO2 overestimation. The biases in annual simulated SO2 concentrations decreased by 46 %, 41 %, and 22 % in Europe, the United States 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.
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