Preprints
https://doi.org/10.5194/acp-2021-788
https://doi.org/10.5194/acp-2021-788
25 Oct 2021
 | 25 Oct 2021
Status: this preprint has been withdrawn by the authors.

Contribution of the gas-phase reaction between hydroxyl radical and sulfur dioxide to the sulfate aerosol over West Pacific

Yu-Wen Chen, Yi-Chun Chen, Charles C.-K. Chou, Hui-Ming Hung, Shih-Yu Chang, Lisa Eirenschmalz, Michael Lichtenstern, Helmut Ziereis, Hans Schlager, Greta Stratmann, Katharina Kaiser, Johannes Schneider, Stephan Borrmann, Florian Obersteiner, Eric Förster, Andreas Zahn, Wei-Nai Chen, Po-Hsiung Lin, Shuenn-Chin Chang, Maria Dolores Andrés Hernández, Pao-Kuan Wang, and John P. Burrows

Abstract. Sulfate is among the major components of atmospheric aerosols or fine particulate matters. Aerosols loaded with sulfate result in low air quality, damage to ecosystems, and influences on climate change. Sulfate aerosols could originate from that directly emitted to the atmosphere and that produced by atmospheric physicochemical processes. The latter is generated from sulfur dioxide (SO2) via oxidation either in the gas phase reactions or in the aqueous phase. Several mechanisms of SO2 oxidation have been proposed, but the differentiation of the various mechanisms and identification of the sources remain challenging. To meet this need, a new method to estimate the contribution of the gas-phase reaction between hydroxyl radical (OH) and SO2 to the sulfate aerosol is proposed and investigated. Briefly, we consider the OH-reaction rates of the respective trace gases that compete for OH radicals with SO2 in the troposphere, and estimate the fraction of SO2-OH reaction in the total OH reactivity. Then the relationship between sulfate concentration and the SO2-OH reaction is analyzed statistically to investigate the sources of sulfate in aerosols. We test this method using the data from ground-based observations and aircraft measurements made during the Effect of Megacities on the transport and transformation of pollutants on the Regional to Global scales in Asia (EMeRGe-Asia) over the western Taiwan and West Pacific regions. Our results show that the estimated SO2-OH reactivity fraction is well-correlated with sulfate concentration. The sulfate production from SO2-OH reaction accounts for approximately 30 % of the total sulfate in aerosols collected at the surface and near-surface (altitude < 600 m) in our study area, comparable to the estimates from other model simulations. Within its assumptions and limitations, this new method provides a valuable approach to investigate the significance of SO2-OH reaction regionally and globally.

This preprint has been withdrawn.

Yu-Wen Chen, Yi-Chun Chen, Charles C.-K. Chou, Hui-Ming Hung, Shih-Yu Chang, Lisa Eirenschmalz, Michael Lichtenstern, Helmut Ziereis, Hans Schlager, Greta Stratmann, Katharina Kaiser, Johannes Schneider, Stephan Borrmann, Florian Obersteiner, Eric Förster, Andreas Zahn, Wei-Nai Chen, Po-Hsiung Lin, Shuenn-Chin Chang, Maria Dolores Andrés Hernández, Pao-Kuan Wang, and John P. Burrows

Interactive discussion

Status: closed

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on acp-2021-788', Anonymous Referee #1, 06 Jan 2022
  • RC2: 'Comment on acp-2021-788', Anonymous Referee #2, 12 Jan 2022

Interactive discussion

Status: closed

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on acp-2021-788', Anonymous Referee #1, 06 Jan 2022
  • RC2: 'Comment on acp-2021-788', Anonymous Referee #2, 12 Jan 2022
Yu-Wen Chen, Yi-Chun Chen, Charles C.-K. Chou, Hui-Ming Hung, Shih-Yu Chang, Lisa Eirenschmalz, Michael Lichtenstern, Helmut Ziereis, Hans Schlager, Greta Stratmann, Katharina Kaiser, Johannes Schneider, Stephan Borrmann, Florian Obersteiner, Eric Förster, Andreas Zahn, Wei-Nai Chen, Po-Hsiung Lin, Shuenn-Chin Chang, Maria Dolores Andrés Hernández, Pao-Kuan Wang, and John P. Burrows
Yu-Wen Chen, Yi-Chun Chen, Charles C.-K. Chou, Hui-Ming Hung, Shih-Yu Chang, Lisa Eirenschmalz, Michael Lichtenstern, Helmut Ziereis, Hans Schlager, Greta Stratmann, Katharina Kaiser, Johannes Schneider, Stephan Borrmann, Florian Obersteiner, Eric Förster, Andreas Zahn, Wei-Nai Chen, Po-Hsiung Lin, Shuenn-Chin Chang, Maria Dolores Andrés Hernández, Pao-Kuan Wang, and John P. Burrows

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This preprint has been withdrawn.

Short summary
By presenting an approach using EMeRGe-Asia airborne field measurements and surface observations, this study shows that the fraction of OH reactivity due to SO2-OH reaction has a significant correlation with the sulfate concentration. Approximately 30 % of sulfate is produced by SO2-OH reaction. Our results underline the importance of SO2-OH gas-phase oxidation in sulfate formation, and demonstrate that the method can be applied to other regions and under different meteorological conditions.
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