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Title: The Reaction of Criegee Intermediate CH2OO with Water Dimer: Primary Products and Atmospheric Impact

Abstract

The rapid reaction of the smallest Criegee intermediate, CH2OO, with water dimers is the dominant removal mechanism for CH2OO in the Earth's atmosphere, but its products are not well understood. This reaction was recently suggested as a significant source of the most abundant tropospheric organic acid, formic acid (HCOOH), which is consistently underpredicted by atmospheric models. Furthermore, using time-resolved measurements of reaction kinetics by UV absorption and product analysis by photoionization mass spectrometry, we show that the primary products of this reaction are formaldehyde and hydroxymethyl hydroperoxide (HMHP), with direct HCOOH yields of less than 10%. Incorporating our results into a global chemistry-transport model further reduces HCOOH levels by 10–90%, relative to previous modeling assumptions, which indicates that the reaction CH2OO + water dimer by itself cannot resolve the discrepancy between the measured and predicted HCOOH levels.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [2];  [2];  [3]
+ Show Author Affiliations
  1. Sandia National Lab. (SNL-CA), Livermore, CA (United States)
  2. Univ. of Bristol, Cantock's Close (United Kingdom)
  3. Univ. of Manchester, Manchester (United Kingdom)
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1374752
Report Number(s):
SAND-2017-8272J
Journal ID: ISSN 1463-9076; 655941
Grant/Contract Number:  
AC04-94AL85000
Resource Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP
Additional Journal Information:
Journal Volume: 19; Journal Issue: 33; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 54 ENVIRONMENTAL SCIENCES

Citation Formats

Sheps, Leonid, Rotavera, Brandon, Eskola, Arkke J., Osborn, David L., Taatjes, Craig A., Au, Kendrew, Shallcross, Dudley E., Khan, M. Anwar H., and Percival, Carl J. The Reaction of Criegee Intermediate CH2OO with Water Dimer: Primary Products and Atmospheric Impact. United States: N. p., 2017. Web. doi:10.1039/c7cp03265j.
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Sheps, Leonid, Rotavera, Brandon, Eskola, Arkke J., Osborn, David L., Taatjes, Craig A., Au, Kendrew, Shallcross, Dudley E., Khan, M. Anwar H., & Percival, Carl J. The Reaction of Criegee Intermediate CH2OO with Water Dimer: Primary Products and Atmospheric Impact. United States. https://doi.org/10.1039/c7cp03265j
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Sheps, Leonid, Rotavera, Brandon, Eskola, Arkke J., Osborn, David L., Taatjes, Craig A., Au, Kendrew, Shallcross, Dudley E., Khan, M. Anwar H., and Percival, Carl J. Fri . "The Reaction of Criegee Intermediate CH2OO with Water Dimer: Primary Products and Atmospheric Impact". United States. https://doi.org/10.1039/c7cp03265j. https://www.osti.gov/servlets/purl/1374752.
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@article{osti_1374752,
title = {The Reaction of Criegee Intermediate CH2OO with Water Dimer: Primary Products and Atmospheric Impact},
author = {Sheps, Leonid and Rotavera, Brandon and Eskola, Arkke J. and Osborn, David L. and Taatjes, Craig A. and Au, Kendrew and Shallcross, Dudley E. and Khan, M. Anwar H. and Percival, Carl J.},
abstractNote = {The rapid reaction of the smallest Criegee intermediate, CH2OO, with water dimers is the dominant removal mechanism for CH2OO in the Earth's atmosphere, but its products are not well understood. This reaction was recently suggested as a significant source of the most abundant tropospheric organic acid, formic acid (HCOOH), which is consistently underpredicted by atmospheric models. Furthermore, using time-resolved measurements of reaction kinetics by UV absorption and product analysis by photoionization mass spectrometry, we show that the primary products of this reaction are formaldehyde and hydroxymethyl hydroperoxide (HMHP), with direct HCOOH yields of less than 10%. Incorporating our results into a global chemistry-transport model further reduces HCOOH levels by 10–90%, relative to previous modeling assumptions, which indicates that the reaction CH2OO + water dimer by itself cannot resolve the discrepancy between the measured and predicted HCOOH levels.},
doi = {10.1039/c7cp03265j},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 33,
volume = 19,
place = {United States},
year = {Fri Aug 04 00:00:00 EDT 2017},
month = {Fri Aug 04 00:00:00 EDT 2017}
}
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https://doi.org/10.1039/c7cp03265j
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