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

Acetic acid (CH 3COOH) is one of the most abundant carboxylic acids in the troposphere. In the study, the tropospheric chemistry of CH 3COOH is investigated using the 3-D global chemistry transport model, STOCHEM-CRI. The highest mixing ratios of surface CH 3COOH are found in the tropics by as much as 1.6 ppb in South America. The model predicts the seasonality of CH 3COOH 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 3COOH are 1.6–1.8 days and 0.45–0.61 Tg, respectively. The reactions of the peroxyacetyl radical (CH 3CO 3) with the hydroperoxyl radical (HO 2) and other organic peroxy radicals (RO 2) are found to be the principal sources of tropospheric CH 3COOH in the model, but the model-measurement discrepancies suggest the possible unknown or underestimated sources which can contribute large fractions of the CH 3COOH burden. The major sinks of CH 3COOH in the troposphere are wet deposition, dry deposition, and OH loss. However, the reaction of CH 3COOH with Criegee intermediates is proposed to bemore » a potentially significant chemical loss process of tropospheric CH 3COOH that has not been previously accounted for in global modeling studies. Inclusion of this loss process reduces the tropospheric CH 3COOH 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 3COOH are underpredicted even more so in current global models.« less
Authors:
ORCiD logo [1] ;  [1] ; ORCiD logo [1] ;  [1] ;  [2] ; ORCiD logo [2] ;  [1] ;  [3] ; ORCiD logo [1]
  1. Univ. of Bristol, Bristol (United Kingdom)
  2. Sandia National Lab. (SNL-CA), Livermore, CA (United States)
  3. California Inst. of Technology (CalTech), La Canada Flintridge, CA (United States). Jet Propulsion Lab.
Publication Date:
Report Number(s):
SAND2018-6899J
Journal ID: ISSN 2169-897X; 664978
Grant/Contract Number:
AC04-94AL85000; AC02-05CH11231; 702794
Type:
Published Article
Journal Name:
Journal of Geophysical Research: Atmospheres
Additional Journal Information:
Journal Volume: 123; Journal Issue: 11; Journal ID: ISSN 2169-897X
Publisher:
American Geophysical Union
Research Org:
Sandia National Lab. (SNL-CA), Livermore, 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:
1454283
Alternate Identifier(s):
OSTI ID: 1454284; OSTI ID: 1459928

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., and Shallcross, Dudley E.. Investigating the Tropospheric Chemistry of Acetic Acid Using the Global 3-D Chemistry Transport Model, STOCHEM-CRI. United States: N. p., Web. doi:10.1029/2018JD028529.
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.. Investigating the Tropospheric Chemistry of Acetic Acid Using the Global 3-D Chemistry Transport Model, STOCHEM-CRI. United States. doi:10.1029/2018JD028529.
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., and Shallcross, Dudley E.. 2018. "Investigating the Tropospheric Chemistry of Acetic Acid Using the Global 3-D Chemistry Transport Model, STOCHEM-CRI". United States. doi:10.1029/2018JD028529.
@article{osti_1454283,
title = {Investigating the Tropospheric Chemistry of Acetic Acid Using the Global 3-D Chemistry Transport Model, STOCHEM-CRI},
author = {Khan, M. Anwar H. and Lyons, Kyle and Chhantyal-Pun, Rabi and McGillen, Max R. and Caravan, Rebecca L. and Taatjes, Craig A. and Orr-Ewing, Andrew J. and Percival, Carl J. and Shallcross, Dudley E.},
abstractNote = {Acetic acid (CH3COOH) is one of the most abundant carboxylic acids in the troposphere. In the study, the tropospheric chemistry of CH3COOH is investigated using the 3-D global chemistry transport model, STOCHEM-CRI. The highest mixing ratios of surface CH3COOH are found in the tropics by as much as 1.6 ppb in South America. The model predicts the seasonality of CH3COOH 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 CH3COOH are 1.6–1.8 days and 0.45–0.61 Tg, respectively. The reactions of the peroxyacetyl radical (CH3CO3) with the hydroperoxyl radical (HO2) and other organic peroxy radicals (RO2) are found to be the principal sources of tropospheric CH3COOH in the model, but the model-measurement discrepancies suggest the possible unknown or underestimated sources which can contribute large fractions of the CH3COOH burden. The major sinks of CH3COOH in the troposphere are wet deposition, dry deposition, and OH loss. However, the reaction of CH3COOH with Criegee intermediates is proposed to be a potentially significant chemical loss process of tropospheric CH3COOH that has not been previously accounted for in global modeling studies. Inclusion of this loss process reduces the tropospheric CH3COOH level significantly which can give even larger discrepancies between model and measurement data, suggesting that the emissions inventory and the chemical production sources of CH3COOH are underpredicted even more so in current global models.},
doi = {10.1029/2018JD028529},
journal = {Journal of Geophysical Research: Atmospheres},
number = 11,
volume = 123,
place = {United States},
year = {2018},
month = {5}
}