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Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
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Preprints
https://doi.org/10.5194/acp-2020-643
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2020-643
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.

  24 Jul 2020

24 Jul 2020

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This preprint is currently under review for the journal ACP.

Global modeling of heterogeneous hydroxymethanesulfonate chemistry

Shaojie Song1, Tao Ma2, Yuzhong Zhang3,4, Lu Shen1, Pengfei Liu5, Ke Li1, Shixian Zhai1, Haotian Zheng1,2, Meng Gao6, Fengkui Duan2, Kebin He2, and Michael B. McElroy1 Shaojie Song et al.
  • 1School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, USA
  • 2State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex, Beijing Key Laboratory of Indoor Air Quality Evaluation and Control, Tsinghua University, Beijing 100084, China
  • 3School of Engineering, Westlake University, Hangzhou 310024, Zhejiang, China
  • 4Institute of Advanced Technology, Westlake Institute for Advanced Study, Hangzhou 310024, Zhejiang, China
  • 5School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA 30332, USA
  • 6Department of Geography, State Key Laboratory of Environmental and Biological Analysis, Hong Kong Baptist University, Hong Kong SAR, China

Abstract. Hydroxymethanesulfonate (HMS) has recently been identified as an abundant organosulfur compound in aerosols during winter haze episodes in northern China. It has also been detected in other regions, although the concentrations are low. Because of the sparse field measurements, the global significance of HMS and its spatial and seasonal patterns remain unclear. Here, we implement HMS chemistry into the GEOS-Chem chemical transport model and conduct multiple global simulations. The developed model accounts for cloud entrainment and gas–aqueous mass transfer within the rate expressions for heterogeneous sulfur chemistry. Our simulations can generally reproduce the available HMS observations, and show that East Asia has the highest HMS concentration, followed by Europe and North America. The simulated HMS shows a seasonal pattern with higher values in the colder period. Photochemical oxidizing capacity affects the competition of formaldehyde with oxidants (such as ozone and hydrogen peroxide) for sulfur dioxide and is a key factor influencing the seasonality of HMS. The highest average HMS concentration (1–3 μg m−3) and HMS/sulfate molar ratio (0.1–0.2) are found in northern China winter. The simulations suggest that aqueous clouds act as the major medium for HMS chemistry while aerosol liquid water may play a role if its rate constant for HMS formation is greatly enhanced compared to cloud water.

Shaojie Song et al.

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Short summary
We simulate the atmospheric chemical processes of an important sulfur-containing organic aerosol species, which is produced by the reaction between sulfur dioxide and formaldehyde. We can predict its distribution on a global scale. We find it is particularly rich in East Asia. This aerosol species is more abundant in the colder season partly because of weaker sunlight.
We simulate the atmospheric chemical processes of an important sulfur-containing organic aerosol...
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