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The Role of Nitrogen Dioxide in the Production of Sulfate during Chinese Haze-Aerosol Episodes

Li, Lijie and Hoffmann, Michael R. and Colussi, Agustin J. (2018) The Role of Nitrogen Dioxide in the Production of Sulfate during Chinese Haze-Aerosol Episodes. Environmental Science and Technology, 52 (5). pp. 2686-2693. ISSN 0013-936X. https://resolver.caltech.edu/CaltechAUTHORS:20180131-114107312

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Abstract

Haze events in China megacities involve the rapid oxidation of SO_2 to sulfate aerosol. Given the weak photochemistry that takes place in these optically thick hazes, it has been hypothesized that SO_2 is mostly oxidized by NO_2 emissions in the bulk of pH > 5.5 aerosols. Because NO_2(g) dissolution in water is very slow and aerosols are more acidic, we decided to test such a hypothesis. Herein, we report that > 95% of NO_2(g) disproportionates [2NO_2(g) + H_2O(l) = H+ + NO_3–(aq) + HONO (R1)] upon hitting the surface of NaHSO_3 aqueous microjets for < 50 μs, thereby giving rise to strong NO_3– (m/z 62) signals detected by online electrospray mass spectrometry, rather than oxidizing HSO_3– (m/z 81) to HSO_4– (m/z 97) in the relevant pH 3–6 range. Because NO_2(g) will be consumed via R1 on the surface of typical aerosols, the oxidation of S(IV) may in fact be driven by the HONO/NO_2– generated therein. S(IV) heterogeneous oxidation rates are expected to primarily depend on the surface density and liquid water content of the aerosol, which are enhanced by fine aerosol and high humidity. Whether aerosol acidity affects the oxidation of S(IV) by HONO/NO_2– remains to be elucidated.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1021/acs.est.7b05222DOIArticle
http://pubs.acs.org/doi/abs/10.1021/acs.est.7b05222PublisherArticle
https://pubs.acs.org/doi/suppl/10.1021/acs.est.7b05222PublisherSupporting Information
ORCID:
AuthorORCID
Li, Lijie0000-0002-7988-6208
Hoffmann, Michael R.0000-0001-6495-1946
Colussi, Agustin J.0000-0002-3400-4101
Additional Information:© 2018 American Chemical Society. Received: October 11, 2017; Revised: January 12, 2018; Accepted: January 29, 2018; Published: January 29, 2018. The authors acknowledge financial support from the National Science Foundation (Grants AC-1238977 and AGS-1744353). The authors declare no competing financial interest.
Funders:
Funding AgencyGrant Number
NSFAGS-1238977
NSFAGS-1744353
Issue or Number:5
Record Number:CaltechAUTHORS:20180131-114107312
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20180131-114107312
Official Citation:Role of Nitrogen Dioxide in the Production of Sulfate during Chinese Haze-Aerosol Episodes. Lijie Li, Michael R. Hoffmann, and Agustín J. Colussi. Environmental Science & Technology 2018 52 (5), 2686-2693 DOI: 10.1021/acs.est.7b05222
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:84603
Collection:CaltechAUTHORS
Deposited By: Ruth Sustaita
Deposited On:31 Jan 2018 22:18
Last Modified:13 Apr 2020 23:07

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