Investigating the Tropospheric Chemistry of Acetic Acid Using the Global 3‐D Chemistry Transport Model, STOCHEM‐CRI
Abstract
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 reactionmore »
- Authors:
-
- 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
- Publication Date:
- Research Org.:
- Sandia National Lab. (SNL-CA), Livermore, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1454283
- Alternate Identifier(s):
- OSTI ID: 1454284; OSTI ID: 1459928
- Report Number(s):
- SAND2018-6899J
Journal ID: ISSN 2169-897X
- Grant/Contract Number:
- DE‐AC02‐05CH11231; AC04-94AL85000
- Resource Type:
- Published Article
- Journal Name:
- Journal of Geophysical Research: Atmospheres
- Additional Journal Information:
- Journal Name: Journal of Geophysical Research: Atmospheres Journal Volume: 123 Journal Issue: 11; Journal ID: ISSN 2169-897X
- Publisher:
- American Geophysical Union (AGU)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
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., 2018.
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. https://doi.org/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. Wed .
"Investigating the Tropospheric Chemistry of Acetic Acid Using the Global 3‐D Chemistry Transport Model, STOCHEM‐CRI". United States. https://doi.org/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 = {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.},
doi = {10.1029/2018JD028529},
journal = {Journal of Geophysical Research: Atmospheres},
number = 11,
volume = 123,
place = {United States},
year = {Wed Jun 13 00:00:00 EDT 2018},
month = {Wed Jun 13 00:00:00 EDT 2018}
}
https://doi.org/10.1029/2018JD028529
Web of Science
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