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Discussion papers
https://doi.org/10.5194/acp-2018-1352
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2018-1352
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 14 Jan 2019

Research article | 14 Jan 2019

Review status
This discussion paper is a preprint. A revision of the manuscript was accepted for the journal Atmospheric Chemistry and Physics (ACP).

Heterogeneous sulfate aerosol formation mechanisms during wintertime Chinese haze events: Air quality model assessment using observations of sulfate oxygen isotopes in Beijing

Jingyuan Shao1,2, Qianjie Chen2,3, Yuxuan Wang4, Xiao Lu1, Pengzhen He5, Yele Sun6, Viral Shah2,7, Randall V. Martin8, Sajeev Philip9, Shaojie Song7, Yue Zhao10, Zhouqing Xie5, Lin Zhang1, and Becky Alexander2 Jingyuan Shao et al.
  • 1Laboratory for Climate and Ocean-Atmosphere Studies, Department of Atmospheric and Oceanic Sciences, School of Physics, Peking University, Beijing 100871, China
  • 2Department of Atmospheric Sciences, University of Washington, Seattle, WA 98195, USA
  • 3Department of Chemistry, University of Michigan, MI 48109, USA
  • 4Department of Earth and Atmospheric Sciences, University of Houston, Houston, TX 77204, USA
  • 5Anhui Province Key Laboratory of Polar Environment and Global Change, School of Earth and Space Sciences, University of Science and Technology of China, Hefei, Anhui 230026, China
  • 6State Key Laboratory of Atmospheric Boundary Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China
  • 7School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, USA
  • 8Department of Physics and Atmospheric Science, Dalhousie University, Halifax, Nova Scotia, Canada
  • 9NASA postdoctoral program, NASA Ames Research Center, Moffett Field, CA, USA
  • 10School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China

Abstract. Air quality models have not been able to reproduce the magnitude of the observed concentrations of fine particulate matter (PM2.5) during wintertime Chinese haze events. The discrepancy has been at least partly attributed to low biases in modeled sulfate production rates due to the lack of heterogeneous sulfate production on aerosols in the models. In this study, we explicitly implement four heterogeneous sulfate formation mechanisms into a regional chemical transport model, in addition to gas-phase and in-cloud sulfate production. We compare the model results with observations of sulfate concentrations and oxygen isotopes (Δ17O(SO42−)) in the winter of 2014–2015, the latter of which is highly sensitive to the relative importance of different sulfate production mechanisms. Model results suggest that heterogeneous sulfate production on aerosols accounts for about 20 % of sulfate production in clean and polluted conditions, partially reducing the modeled low bias in sulfate concentrations. Model sensitivity studies in comparison with the Δ17O(SO42−) observations suggest that heterogeneous sulfate formation is dominated by transition metal ion catalyzed oxidation of SO2.

Jingyuan Shao et al.
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Status: final response (author comments only)
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Jingyuan Shao et al.
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Short summary
Sulfate is a key species contributing to particle formation and growth during wintertime Chinese haze events. This study combines observations and modeling of oxygen isotope signature in sulfate aerosol to investigate its formation mechanisms, with a focus on heterogeneous production on aerosol surface via H2O2, O3, NO2 and trace metals catalyzed oxidation. Contributions from different formation pathways are presented.
Sulfate is a key species contributing to particle formation and growth during wintertime Chinese...
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