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Discussion papers
https://doi.org/10.5194/acp-2018-1111
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2018-1111
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 05 Nov 2018

Research article | 05 Nov 2018

Review status
This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

A potential source of atmospheric sulfate from O2-induced SO2 oxidation by ozone

Narcisse Tchinda Tsona and Lin Du Narcisse Tchinda Tsona and Lin Du
  • Environment Research Institute, Shandong University, Binhai Road 72, 266237 Shandong, China

Abstract. It was formerly demonstrated that O2SOO forms at collisions rate in the gas-phase as a result of SO2 reaction with O2. Hereby, we present a theoretical investigation of the chemical fate of O2SOO by reaction with O3 in the gas-phase, based on ab initio calculations. Two main mechanisms were found for the title reaction, with fundamentally different products: (i) formation of a van der Waals complex followed by electron transfer and further decomposition to O2+SO2+O3 and (ii) formation of a molecular complex from O2 switching by O3, followed by SO2 oxidation to SO3 within the complex. Both reactions are exergonic, but separated by relatively low energy barriers. The products in the former mechanism would likely initiate other SO2 oxidations as shown in previous studies, whereas the latter mechanism closes a path wherein SO2 is oxidized to SO3. The latter reaction is atmospherically relevant since it forms the SO3 ion, hereby closing the SO2 oxidation path initiated by O2. The main atmospheric fate of SO3 is nothing but sulfate formation. Exploration of the reactions kinetics indicates that the path of reaction (ii) is highly facilitated by humidity. For this path, we found an overall rate constant of 4.0×10−11cm3molecule−1s−1 at 298K and 50% relative humidity. The title reaction provides a new mechanism for sulfate formation from ion-induced SO2 oxidation in the gas-phase and highlights the importance of including such mechanism in modelling sulfate-based aerosol formation rates.

Narcisse Tchinda Tsona and Lin Du
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Status: open (until 31 Dec 2018)
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Narcisse Tchinda Tsona and Lin Du
Narcisse Tchinda Tsona and Lin Du
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Short summary
We used ab initio calculations to explore a new path for ion-induced SO2 oxidation by ozone in the gas-phase. We find that, initiated by the superoxide ion, SO2 can readily oxidize to SO3. The reaction is facilitated by the presence of water, being ~ 4 orders of magnitude faster than the reaction in the absence of water. Depending on the altitude and temperature, it is estimated that this reaction may contribute to 0.1–3.1 % of the total atmospheric sulfuric acid.
We used ab initio calculations to explore a new path for ion-induced SO2 oxidation by ozone in...
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