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| DOI | 10.5194/acp-21-13973-2021 |
| Global tropospheric halogen (Cl, Br, I) chemistry and its impact on oxidants | |
| Wang X.; Jacob D.J.; Downs W.; Zhai S.; Zhu L.; Shah V.; Holmes C.D.; Sherwen T.; Alexander B.; Evans M.J.; Eastham S.D.; Neuman J.A.; Veres P.R.; Koenig T.K.; Volkamer R.; Huey L.G.; Bannan T.J.; Percival C.J.; Lee B.H.; Thornton J.A. | |
| 发表日期 | 2021 |
| ISSN | 1680-7316 |
| 起始页码 | 13973 |
| 结束页码 | 13996 |
| 卷号 | 21期号:18 |
| 英文摘要 | We present an updated mechanism for tropospheric halogen (Clĝ€¯+ĝ€¯Brĝ€¯+ĝ€¯I) chemistry in the GEOS-Chem global atmospheric chemical transport model and apply it to investigate halogen radical cycling and implications for tropospheric oxidants. Improved representation of HOBr heterogeneous chemistry and its pH dependence in our simulation leads to less efficient recycling and mobilization of bromine radicals and enables the model to include mechanistic sea salt aerosol debromination without generating excessive BrO. The resulting global mean tropospheric BrO mixing ratio is 0.19ĝ€¯ppt (parts per trillion), lower than previous versions of GEOS-Chem. Model BrO shows variable consistency and biases in comparison to surface and aircraft observations in marine air, which are often near or below the detection limit. The model underestimates the daytime measurements of Cl2 and BrCl from the ATom aircraft campaign over the Pacific and Atlantic, which if correct would imply a very large missing primary source of chlorine radicals. Model IO is highest in the marine boundary layer and uniform in the free troposphere, with a global mean tropospheric mixing ratio of 0.08ĝ€¯ppt, and shows consistency with surface and aircraft observations. The modeled global mean tropospheric concentration of Cl atoms is 630ĝ€¯cm-3, contributing 0.8ĝ€¯% of the global oxidation of methane, 14ĝ€¯% of ethane, 8ĝ€¯% of propane, and 7ĝ€¯% of higher alkanes. Halogen chemistry decreases the global tropospheric burden of ozone by 11ĝ€¯%, NOx by 6ĝ€¯%, and OH by 4ĝ€¯%. Most of the ozone decrease is driven by iodine-catalyzed loss. The resulting GEOS-Chem ozone simulation is unbiased in the Southern Hemisphere but too low in the Northern Hemisphere. © Copyright: |
| 语种 | 英语 |
| scopus关键词 | atmospheric chemistry; atmospheric transport; bromine; chlorine; iodine; oxidant; pH; troposphere |
| 来源期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS
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| 文献类型 | 期刊论文 |
| 条目标识符 | http://gcip.llas.ac.cn/handle/2XKMVOVA/246572 |
| 作者单位 | School of Energy and Environment, City University of Hong Kong, Hong Kong; City University of Hong Kong, Shenzhen Research Institute, Shenzhen, China; School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, United States; Department of Atmospheric Sciences, University of Washington, Seattle, WA, United States; School of Environmental Science and Engineering, Southern University of Science and Technology, Shenzhen, China; Department of Earth, Ocean, and Atmospheric Science, Florida State University, Tallahassee, FL, United States; Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, United Kingdom; National Centre for Atmospheric Science, University of York, York, United Kingdom; Laboratory for Aviation and the Environment, Massachusetts Institute of Technology, Cambridge, MA, United States; NOAA Chemical Sciences Laboratory (CSL), Boulder, CO, United States; Cooperative Institute for Research in Environmental Sciences, University of Colorado... |
| 推荐引用方式 GB/T 7714 | Wang X.,Jacob D.J.,Downs W.,et al. Global tropospheric halogen (Cl, Br, I) chemistry and its impact on oxidants[J],2021,21(18). |
| APA | Wang X..,Jacob D.J..,Downs W..,Zhai S..,Zhu L..,...&Thornton J.A..(2021).Global tropospheric halogen (Cl, Br, I) chemistry and its impact on oxidants.ATMOSPHERIC CHEMISTRY AND PHYSICS,21(18). |
| MLA | Wang X.,et al."Global tropospheric halogen (Cl, Br, I) chemistry and its impact on oxidants".ATMOSPHERIC CHEMISTRY AND PHYSICS 21.18(2021). |
| 条目包含的文件 | 条目无相关文件。 | |||||
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