A study of global atmospheric budget and distribution of acetone using global atmospheric model STOCHEM-CRI
Open accessAbstract
The impact of including a more detailed VOC oxidation scheme (CRI v2-R5) with a multi-generational approach for simulating tropospheric acetone is investigated using a 3-D global model, STOCHEM-CRI. The CRI v2-R5 mechanism contains photochemical production of acetone from monoterpenes which account for 64% (46.8 Tg/yr) of the global acetone sources in STOCHEM-CRI. Both photolysis and oxidation by OH in the troposphere contributes equally (42%, each) and dry deposition contributes 16% of the atmospheric sinks of acetone. The tropospheric life-time and the global burden of acetone are found to be 18 days and 3.5 Tg, respectively, these values being close to those reported in the study of Jacob et al. (2002). A dataset of aircraft campaign measurements are used to evaluate the inclusion of acetone formation from monoterpenes in the CRI v2-R5 mechanism used in STOCHEM-CRI. The overall comparison between measurements and models show that the parameterised approach in STOCHEM-NAM (no acetone formation from monoterpenes) underpredicts the mixing ratios of acetone in the atmosphere. However, using a detailed monoterpene oxidation mechanism forming acetone has brought the STOCHEM-CRI into closer agreement with measurements with an improvement in the vertical simulation of acetone. The annual mean surface distribution of acetone simulated by the STOCHEM-CRI shows a peak over forested regions where there are large biogenic emissions and high levels of photochemical activity. Year-long observations of acetone and methanol at the Mace Head research station in Ireland are compared with the simulated acetone and methanol produced by the STOCHEM-CRI and found to produce good overall agreement between model and measurements. The seasonal variation of model and measured acetone levels at Mace Head, California, New Hampshire and Minnesota show peaks in summer and dips in winter, suggesting that photochemical production may have the strongest effect on its seasonal trend.
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Photolysis of acetaldehyde is an important loss process, contributing ~10% to the total loss rate for this compound.
“Photolysis of acetaldehyde is also an important loss process, contributing ~10% to the total loss rate for this compound [100-102].”
From Investigation of Biofuel as a Potential Renewable Energy Source (2021) · cites this paper as [100]
Photolysis yields HCO and CH3 radicals, where HCO instantly forms HO2 radicals on reaction with O2.
“Photolysis yields HCO and CH 3 radicals, where HCO instantly forms HO 2 radicals on reaction with O 2 .”
From Investigation of Biofuel as a Potential Renewable Energy Source (2021) · cites this paper as [100]
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- Authors
- Khan, M. A. H., Cooke, M. C., Utembe, S. R., Archibald, A. T., Maxwell, P., Morris, W. C., Xiao, P., Derwent, R. G., Jenkin, M. E., Percival, C. J., Walsh, R. C., Young, T. D. S., Simmonds, P. G., Nickless, G., O'Doherty, S., & Shallcross, D. E.
- Affiliations
- University of Bristol (GB)
- University of Manchester (GB)
- Corresponding author
- Shallcross, D.E.
- ORCID
- Venue
- Atmospheric Environment
- Publisher
- Elsevier BV
- Published
- 2015-07
- Volume
- 112
- Pages
- 269-277
- ISSN
- 1352-2310 (ISSN-L)
- OpenAlex
- W1974677838
- Cited by
- 72
- References
- 54
- Citations by year
- 2026: 3 · 2025: 5 · 2024: 4 · 2023: 7 · 2022: 10 · 2021: 14 · 2020: 6 · 2019: 6 · 2018: 4 · 2017: 10 · 2016: 3
- FWCI
- 3.94
- Type
- journal article
- Language
- en
- Open access
- hybrid
- doi.org
- Locations
- Atmospheric Environment (publishedVersion, cc-by)
- Research Explorer (The University of Manchester) (submittedVersion)
- Explore Bristol Research (submittedVersion)
- Bristol Research (University of Bristol) (submittedVersion)
- Funders
- NERC (NE/J009008/1)
- Bristol ChemLabS
- Topics
- Physical Sciences › Earth and Planetary Sciences › Atmospheric Science › Atmospheric chemistry and aerosols
- Physical Sciences › Environmental Science › Global and Planetary Change › Atmospheric and Environmental Gas Dynamics
- Physical Sciences › Earth and Planetary Sciences › Atmospheric Science › Atmospheric Ozone and Climate
- Keywords
- acetone, tropospheric chemistry, monoterpenes, monoterpene oxidation, photochemical production, atmospheric lifetime, dry deposition, hydroxyl radical oxidation, biogenic emissions, methanol, seasonal variation, Mace Head
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