Investigating the Tropospheric Chemistry of Acetic Acid Using the Global 3‐D Chemistry Transport Model, STOCHEM‐CRI

Khan, M. Anwar H.; Lyons, Kyle; Chhantyal‐Pun, Rabi; McGillen, Max R.; Caravan, Rebecca L.; Taatjes, Craig A.; Orr‐Ewing, Andrew J.; Percival, Carl J.; Shallcross, Dudley E.

doi:10.1029/2018JD028529

Title: Investigating the Tropospheric Chemistry of Acetic Acid Using the Global 3‐D Chemistry Transport Model, STOCHEM‐CRI

Journal Article · Wed Jun 13 00:00:00 EDT 2018 · Journal of Geophysical Research: Atmospheres

DOI:https://doi.org/10.1029/2018JD028529· OSTI ID:1454283

^[1]; Lyons, Kyle ^[1];

^[1]; McGillen, Max R. ^[1]; Caravan, Rebecca L. ^[2];

^[2]; Orr‐Ewing, Andrew J. ^[1]; Percival, Carl J. ^[3];

^[1]

School of Chemistry University of Bristol Bristol UK
Combustion Research Facility Sandia National Laboratories Livermore CA USA
Jet Propulsion Laboratory California Institute of Technology Pasadena CA USA

Abstract Acetic acid (CH ₃ COOH) is one of the most abundant carboxylic acids in the troposphere. In the study, the tropospheric chemistry of CH ₃ COOH is investigated using the 3‐D global chemistry transport model, STOCHEM‐CRI. The highest mixing ratios of surface CH ₃ COOH are found in the tropics by as much as 1.6 ppb in South America. The model predicts the seasonality of CH ₃ COOH reasonably well and correlates with some surface and flight measurement sites, but the model drastically underpredicts levels in urban and midlatitudinal regions. The possible reasons for the underprediction are discussed. The simulations show that the lifetime and global burden of CH ₃ COOH are 1.6–1.8 days and 0.45–0.61 Tg, respectively. The reactions of the peroxyacetyl radical (CH ₃ CO ₃ ) with the hydroperoxyl radical (HO ₂ ) and other organic peroxy radicals (RO ₂ ) are found to be the principal sources of tropospheric CH ₃ COOH in the model, but the model‐measurement discrepancies suggest the possible unknown or underestimated sources which can contribute large fractions of the CH ₃ COOH burden. The major sinks of CH ₃ COOH in the troposphere are wet deposition, dry deposition, and OH loss. However, the reaction of CH ₃ COOH with Criegee intermediates is proposed to be a potentially significant chemical loss process of tropospheric CH ₃ COOH that has not been previously accounted for in global modeling studies. Inclusion of this loss process reduces the tropospheric CH ₃ COOH level significantly which can give even larger discrepancies between model and measurement data, suggesting that the emissions inventory and the chemical production sources of CH ₃ COOH are underpredicted even more so in current global models.

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Research Organization:: Sandia National Lab. (SNL-CA), Livermore, CA (United States)

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

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

OSTI ID:: 1454283

Alternate ID(s):: OSTI ID: 1454284; OSTI ID: 1459928

Report Number(s):: SAND2018-6899J

Journal Information:: Journal of Geophysical Research: Atmospheres, Journal Name: Journal of Geophysical Research: Atmospheres Vol. 123 Journal Issue: 11; ISSN 2169-897X

Publisher:: American Geophysical Union (AGU)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 15 works

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