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

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.

doi:10.1039/c7cp03265j

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

Journal Article · Fri Aug 04 00:00:00 EDT 2017 · Physical Chemistry Chemical Physics. PCCP

DOI:https://doi.org/10.1039/c7cp03265j· OSTI ID:1374752

Sheps, Leonid ^[1]; Rotavera, Brandon ^[1]; Eskola, Arkke J. ^[1]; Osborn, David L. ^[1]; Taatjes, Craig A. ^[1]; Au, Kendrew ^[1]; Shallcross, Dudley E. ^[2]; Khan, M. Anwar H. ^[2]; Percival, Carl J. ^[3]

Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Univ. of Bristol, Cantock's Close (United Kingdom)
Univ. of Manchester, Manchester (United Kingdom)

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.

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Research Organization:: Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC04-94AL85000

OSTI ID:: 1374752

Report Number(s):: SAND-2017-8272J; 655941

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Vol. 19, Issue 33; ISSN 1463-9076

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 65 works

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