Heterogeneous interactions between SO<sub>2</sub> and organic peroxides in submicron aerosol

Wang, Shunyao; Liu, Tengyu; Jang, Jinmyung; Abbatt, Jonathan P. D.; Chan, Arthur W. H.

doi:https://doi.org/10.5194/acp-21-6647-2021

Articles | Volume 21, issue 9

https://doi.org/10.5194/acp-21-6647-2021

© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.

https://doi.org/10.5194/acp-21-6647-2021

© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.

Articles | Volume 21, issue 9

Research article

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04 May 2021

Research article | Highlight paper |

| 04 May 2021

Heterogeneous interactions between SO₂ and organic peroxides in submicron aerosol

Shunyao Wang, Tengyu Liu, Jinmyung Jang, Jonathan P. D. Abbatt, and Arthur W. H. Chan

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AC: Author comment | RC: Referee comment | SC: Short comment | EC: Editor comment

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RC1: 'Review for Wang, Liu, Jang, Abbott, and Chan.', Anonymous Referee #1, 28 Oct 2020
- AC1: 'Reply on RC1', Shunyao Wang, 09 Feb 2021
RC2: 'Review for Wang et al.', Anonymous Referee #2, 20 Jan 2021
- AC2: 'Reply on RC2', Shunyao Wang, 09 Feb 2021

Peer-review completion

AR: Author's response | RR: Referee report | ED: Editor decision

AR by Shunyao Wang on behalf of the Authors (12 Feb 2021) Author's response Author's tracked changes Manuscript

ED: Referee Nomination & Report Request started (20 Feb 2021) by Hang Su

RR by Anonymous Referee #2 (24 Feb 2021)

ED: Publish subject to minor revisions (review by editor) (09 Mar 2021) by Hang Su

Dear authors,

I am close to accept your paper for publication in ACP, and please find a few comments as detailed below.
Page 3 “Reactive nitrogen species (such as NO2) have also been put forward to account for the missing sulfate at relatively high aerosol pH (close to 7) (Wang et al., 2016; Cheng et al., 2016).”
Cheng et al. (2016) suggested NO2 as a major contributor for the missing sulfate a pH range of ~5 to ~6. I would suggest being more specific about the pH range in Cheng et al. (2016) because “close to 7” might be misleading.

Page 3 “However, such high aerosol pH is not substantiated by thermodynamic models, which conclude that pH ranges between 4 and 5 even in polluted regions (Song et al., 2018;Guo et al., 2017)”.
For the aerosol pH range, later studies (e.g., Shi et al. 2017; Ding et al. 2019) show that the modelled aerosol pH in Beijing can go beyond the range of 4-5, even >6. I would suggest updating this and related statement. Note that Cheng et al. (2016) highlighted the importance of both NH3 and dust in regulating aerosol pH. Guo et al. (2017), however, didn’t consider the contribution of dusts. Moreover, higher RH and higher aerosol concentrations may lead to further increase of aerosol pH (Zheng et al. 2020).

Sincerely,

Hang Su

Reference:
Ding, J., Zhao, P., Su, J., Dong, Q., Du, X., and Zhang, Y.: Aerosol pH and its driving factors in Beijing, Atmos. Chem. Phys., 19, 7939-7954, 10.5194/acp-19-7939-2019, 2019.
Shi, G., Xu, J., Peng, X., Xiao, Z., Chen, K., Tian, Y., Guan, X., Feng, Y., Yu, H., Nenes, A., and Russell, A. G.: pH of Aerosols in a Polluted Atmosphere: Source Contributions to Highly Acidic Aerosol, Environ. Sci. Technol., 51, 4289-4296, 10.1021/acs.est.6b05736, 2017.
Zheng, G., Su, H., Wang, S., Andreae, M. O., Pöschl, U., and Cheng, Y.: Multiphase buffer theory explains contrasts in atmospheric aerosol acidity, Science, 369, 1374-1377, 10.1126/science.aba3719, 2020.

Sincerely,

Hang Su

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AR by Shunyao Wang on behalf of the Authors (11 Mar 2021) Author's response Author's tracked changes Manuscript

ED: Publish as is (11 Mar 2021) by Hang Su

AR by Shunyao Wang on behalf of the Authors (12 Mar 2021) Author's response Manuscript

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Short summary

Discrepancies between atmospheric modeling and field observations, especially in highly polluted cities, have highlighted the lack of understanding of sulfate formation mechanisms and kinetics. Here, we directly quantify the reactive uptake coefficient of SO₂ onto organic peroxides and study the important governing factors. The SO₂ uptake rate was observed to depend on RH, peroxide amount and reactivity, pH, and ionic strength, which provides a framework to better predict sulfate formation.

Heterogeneous interactions between SO2 and organic peroxides in submicron aerosol

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Heterogeneous interactions between SO₂ and organic peroxides in submicron aerosol