Rate Coefficients of C1 and C2 Criegee Intermediate Reactions with Formic and Acetic Acid Near the Collision Limit: Direct Kinetics Measurements and Atmospheric Implications

Welz, Oliver; Eskola, Arkke J.; Sheps, Leonid; Rotavera, Brandon; Savee, John D.; Scheer, Adam M.; Osborn, David L.; Lowe, Douglas; Murray Booth, A.; Xiao, Ping; Anwar H. Khan, M.; Percival, Carl J.; Shallcross, Dudley E.; Taatjes, Craig A.

doi:10.1002/anie.201400964

Rate Coefficients of C1 and C2 Criegee Intermediate Reactions with Formic and Acetic Acid Near the Collision Limit: Direct Kinetics Measurements and Atmospheric Implications

Journal Article · Tue Mar 25 00:00:00 EDT 2014 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.201400964· OSTI ID:1623484

Welz, Oliver ^[1]; Eskola, Arkke J. ^[2]; Sheps, Leonid ^[2]; Rotavera, Brandon ^[2]; Savee, John D. ^[2]; Scheer, Adam M. ^[2]; Osborn, David L. ^[2]; Lowe, Douglas ^[3]; Murray Booth, A. ^[3]; Xiao, Ping ^[4]; Anwar H. Khan, M. ^[4]; Percival, Carl J. ^[3]; Shallcross, Dudley E. ^[4]; Taatjes, Craig A. ^[2]

Sandia National Lab. (SNL-CA), Livermore, CA (United States). Combusstion Research Facility; DOE/OSTI
Sandia National Lab. (SNL-CA), Livermore, CA (United States). Combusstion Research Facility
Univ. of Manchester (United Kingdom). The School of Earth and Atmospheric and Environmental Science. The Centre for Atmospheric Science
Bristol Univ. (United Kingdom). School of Chemistry. Biogeochemistry Research Centre

Rate coefficients are directly determined for the reactions of the Criegee intermediates (CI) CH2OO and CH3CHOO with the two simplest carboxylic acids, formic acid (HCOOH) and acetic acid (CH3COOH), employing two complementary techniques: multiplexed photoionization mass spectrometry and cavity-enhanced broadband ultraviolet absorption spectroscopy. The measured rate coefficients are in excess of 1 1010 cm3 s 1 , several orders of magnitude larger than those suggested from many previous alkene ozonolysis experiments and assumed in atmospheric modeling studies. These results suggest that the reaction with carboxylic acids is a substantially more important loss process for CIs than is presently assumed. Implementing these rate coefficients in global atmospheric models shows that reactions between CI and organic acids make a substantial contribution to removal of these acids in terrestrial equatorial areas and in other regions where high CI concentrations occur such as high northern latitudes, and implies that sources of acids in these areas are larger than previously recognized.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC02-05CH11231; AC04-94AL85000

OSTI ID:: 1623484

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 18 Vol. 53; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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