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Title: Multiphase Mechanism for the Production of Sulfuric Acid from SO 2 by Criegee Intermediates Formed During the Heterogeneous Reaction of Ozone with Squalene

Here we report a new multiphase reaction mechanism by which Criegee intermediates (CIs), formed by ozone reactions at an alkene surface, convert SO 2 to SO 3 to produce sulfuric acid, a precursor for new particle formation (NPF). During the heterogeneous ozone reaction, in the presence of 220 ppb SO 2, an unsaturated aerosol (squalene) undergoes rapid chemical erosion, which is accompanied by NPF. A kinetic model predicts that the mechanism for chemical erosion and NPF originate from a common elementary step (CI + SO 2) that produces both gas phase SO 3 and small ketones. At low relative humidity (RH = 5%), 20% of the aerosol mass is lost, with 17% of the ozone-surface reactions producing SO 3. At RH = 60%, the aerosol shrinks by 30%, and the yield of SO 3 is <5%. In conclusion, this multiphase formation mechanism of H 2SO 4 by CIs is discussed in the context of indoor air quality and atmospheric chemistry.
Authors:
 [1] ;  [2] ;  [2] ; ORCiD logo [1] ; ORCiD logo [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Univ. of California, Berkeley, CA (United States)
Publication Date:
Grant/Contract Number:
AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 9; Journal Issue: 12; Related Information: Copyright © 2018 American Chemical Society.; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1461172

Heine, Nadja, Arata, Caleb, Goldstein, Allen H., Houle, Frances A., and Wilson, Kevin R.. Multiphase Mechanism for the Production of Sulfuric Acid from SO2 by Criegee Intermediates Formed During the Heterogeneous Reaction of Ozone with Squalene. United States: N. p., Web. doi:10.1021/acs.jpclett.8b01171.
Heine, Nadja, Arata, Caleb, Goldstein, Allen H., Houle, Frances A., & Wilson, Kevin R.. Multiphase Mechanism for the Production of Sulfuric Acid from SO2 by Criegee Intermediates Formed During the Heterogeneous Reaction of Ozone with Squalene. United States. doi:10.1021/acs.jpclett.8b01171.
Heine, Nadja, Arata, Caleb, Goldstein, Allen H., Houle, Frances A., and Wilson, Kevin R.. 2018. "Multiphase Mechanism for the Production of Sulfuric Acid from SO2 by Criegee Intermediates Formed During the Heterogeneous Reaction of Ozone with Squalene". United States. doi:10.1021/acs.jpclett.8b01171.
@article{osti_1461172,
title = {Multiphase Mechanism for the Production of Sulfuric Acid from SO2 by Criegee Intermediates Formed During the Heterogeneous Reaction of Ozone with Squalene},
author = {Heine, Nadja and Arata, Caleb and Goldstein, Allen H. and Houle, Frances A. and Wilson, Kevin R.},
abstractNote = {Here we report a new multiphase reaction mechanism by which Criegee intermediates (CIs), formed by ozone reactions at an alkene surface, convert SO2 to SO3 to produce sulfuric acid, a precursor for new particle formation (NPF). During the heterogeneous ozone reaction, in the presence of 220 ppb SO2, an unsaturated aerosol (squalene) undergoes rapid chemical erosion, which is accompanied by NPF. A kinetic model predicts that the mechanism for chemical erosion and NPF originate from a common elementary step (CI + SO2) that produces both gas phase SO3 and small ketones. At low relative humidity (RH = 5%), 20% of the aerosol mass is lost, with 17% of the ozone-surface reactions producing SO3. At RH = 60%, the aerosol shrinks by 30%, and the yield of SO3 is <5%. In conclusion, this multiphase formation mechanism of H2SO4 by CIs is discussed in the context of indoor air quality and atmospheric chemistry.},
doi = {10.1021/acs.jpclett.8b01171},
journal = {Journal of Physical Chemistry Letters},
number = 12,
volume = 9,
place = {United States},
year = {2018},
month = {6}
}