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https://doi.org/10.5194/acp-2020-806
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2020-806
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.

  31 Aug 2020

31 Aug 2020

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This preprint is currently under review for the journal ACP.

Aqueous phase oxidation of bisulfite influenced by nitrate photolysis

Lu Chen1, Lingdong Kong1,2, Songying Tong1, Kejing Yang1, Shengyan Jin1, Chao Wang1, and Lin Wang1 Lu Chen et al.
  • 1Department of Environmental Science & Engineering, Jiangwan Campus, Fudan University, No. 2205 Songhu Road, Shanghai, 200438, China
  • 2Institute of Eco-Chongming, East China Normal University, No.3663 Northern Zhongshan Road, Shanghai 200062, China

Abstract. Nitrate aerosol is ubiquitous in the atmosphere, and it can exit in both solid aerosol particles and fog and cloud droplets. Nitrate in the aqueous and particulate phase can undergo photolysis to produce oxidizing active radicals, which will inevitably affect various atmospheric chemical processes. However, the role of nitrate aerosols in these atmospheric photochemical processes remains unclear. In this study, the effects of nitrate photolysis on the aqueous phase oxidation of bisulfite under different conditions were investigated. Results show that nitrate photolysis can significantly promote the oxidation of bisulfite to sulfate. It is found that pH plays a significant role in the reaction, and ammonium sulfate has significant impacts on regulating the pH of solution and the enhancement of sulfate production. We also found an apparent synergism among halogen chemistry, nitrate and its photochemistry and S(IV) aqueous oxidation, especially the oxidation of halide ions by the nitrate photolysis and by the intermediate peroxymonosulfuric acid (HSO5) produced by the free radical chain oxidation of S(IV) in acidic solution leads to the coupling of the redox cycle of halogen with the oxidation of bisulfite, which promotes the continuous aqueous oxidation of bisulfite and the formation of sulfate. In addition, it is also found that O2 is of great significance on nitrate photolysis for the conversion of HSO3, and H2O2 generation during the nitrate photolysis is verified. These results provide a new insight into the heterogeneous aqueous phase oxidation pathways and mechanisms of SO2 in cloud and fog droplets and haze particles.

Lu Chen et al.

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Short summary
The role of nitrate aerosol in atmospheric SO2 oxidation remains unclear. We investigated the effects of nitrate on the aqueous phase oxidation of bisulfite under different conditions. We found the important roles of nitrate photolysis, pH, ammonium and O2 in the oxidation of bisulfite to sulfate, the generation of H2O2, and the synergism with halogen chemistry. These results provide a new insight into the heterogeneous aqueous phase oxidation of SO2 in cloud and fog droplets and haze particles.
The role of nitrate aerosol in atmospheric SO2 oxidation remains unclear. We investigated the...
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