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DOI10.1016/j.atmosenv.2021.118248
Intercomparison of the representations of the atmospheric chemistry of pre-industrial methane and ozone in earth system and other global chemistry-transport models
Derwent R.G.; Parrish D.D.; Archibald A.T.; Deushi M.; Bauer S.E.; Tsigaridis K.; Shindell D.; Horowitz L.W.; Khan M.A.H.; Shallcross D.E.
发表日期2021
ISSN1352-2310
卷号248
英文摘要An intercomparison has been set up to study the representation of the atmospheric chemistry of the pre-industrial troposphere in earth system and other global tropospheric chemistry-transport models. The intercomparison employed a constrained box model and utilised tropospheric trace gas composition data for the pre-industrial times at ninety mid-latitude surface locations. Incremental additions of four organic compounds: methane, ethane, acetone and propane, were used to perturb the constrained box model and generate responses in hydroxyl radicals and tropospheric ozone at each location and with each chemical mechanism. Although the responses agreed well across the chemical mechanisms from the selected earth system and other global tropospheric chemistry-transport models, there were differences in the detailed responses between the chemical mechanisms that could be tracked down by sensitivity analysis to differences in the representation of C1–C3 chemistry. Inter-mechanism ranges in NOx compensation points were about 0.17 ± 0.12 when expressed relative to the inter-mechanism average. Monte Carlo uncertainty analysis carried out with a single chemical mechanism put the intra-mechanism range a factor of three higher at 0.50 ± 0.12. Similar differences between inter-mechanism and intra-mechanism ranges were found for hydroxyl radical depletion but were up to a factor of six wider for ozone formation from incremental additions of organic compounds. The cause of the discrepancies between the inter- and intra-mechanism ranges was found to be the large uncertainties that are present in the laboratory determinations of the rate coefficients and product channel branching ratios of some key chemical reactions involving organic peroxy radicals and hydroperoxides. Whilst these large uncertainties are present in the laboratory determinations, there will be irreducible uncertainties in the predictions from the earth system and other chemistry-transport models of methane and tropospheric ozone trends since pre-industrial times and hence their contributions to the radiative forcing of climate change. Further definitive laboratory studies of the reaction rates and product yields of the reactions of the simple organic peroxy radicals and hydroperoxides are required to resolve and reduce current uncertainties in earth system and chemistry-transport model predictions. © 2021 Elsevier Ltd
语种英语
scopus关键词Acetone; Atmospheric movements; Atmospheric radiation; Chemical analysis; Climate change; Climate models; Methane; Ozone; Reaction rates; Sensitivity analysis; Troposphere; Uncertainty analysis; Chemical mechanism; Chemistry transport model; Compensation points; Global chemistry transport model; Laboratory determinations; Laboratory studies; Organic peroxy radicals; Tropospheric chemistry; Atmospheric chemistry; acetone; ethane; hydroperoxide; hydroxyl radical; methane; ozone; peroxy radical; propane; atmospheric chemistry; hydroxyl radical; industrial emission; methane; ozone; radiative forcing; sensitivity analysis; trace gas; troposphere; uncertainty analysis; Article; atmospheric deposition; atmospheric transport; biogeochemistry; boundary layer; chemical reaction; decomposition; industrial area; photolysis; priority journal; temperature dependence; troposphere; water vapor
来源期刊ATMOSPHERIC ENVIRONMENT
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/248558
作者单位rdscientific, Newbury, Berkshire RG14 6LH, United Kingdom; David D. Parrish, LLC, Boulder, CO, United States; Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge, CB2 1EW, United Kingdom; National Centre for Atmospheric Science, United Kingdom; Meteorological Research Institute, Japan Meteorological Agency, Tsukuba, Japan; NASA Goddard Institute for Space Studies, New York, United States; Center for Climate Systems Research, Columbia University, New York, United States; Nicholas School of the Environment, Duke University, Durham, NC 27708, United States; NOAA Geophysical Fluid Dynamics Laboratory, PrincetonNJ, United States; Biogeochemistry Research Centre, School of Chemistry, University of Bristol, Cantock's Close, Bristol BS8 1TS, United Kingdom; Department of Chemistry, University of Western Cape, Robert Sobukwe Road, Bellville7375, South Africa
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GB/T 7714
Derwent R.G.,Parrish D.D.,Archibald A.T.,et al. Intercomparison of the representations of the atmospheric chemistry of pre-industrial methane and ozone in earth system and other global chemistry-transport models[J],2021,248.
APA Derwent R.G..,Parrish D.D..,Archibald A.T..,Deushi M..,Bauer S.E..,...&Shallcross D.E..(2021).Intercomparison of the representations of the atmospheric chemistry of pre-industrial methane and ozone in earth system and other global chemistry-transport models.ATMOSPHERIC ENVIRONMENT,248.
MLA Derwent R.G.,et al."Intercomparison of the representations of the atmospheric chemistry of pre-industrial methane and ozone in earth system and other global chemistry-transport models".ATMOSPHERIC ENVIRONMENT 248(2021).
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