globalchange  > 气候减缓与适应
DOI: 10.1038/ngeo2046
论文题名:
High levels of molecular chlorine in the Arctic atmosphere
作者: Liao J.; Huey L.G.; Liu Z.; Tanner D.J.; Cantrell C.A.; Orlando J.J.; Flocke F.M.; Shepson P.B.; Weinheimer A.J.; Hall S.R.; Ullmann K.; Beine H.J.; Wang Y.; Ingall E.D.; Stephens C.R.; Hornbrook R.S.; Apel E.C.; Riemer D.; Fried A.; Mauldin R.L.; Smith J.N.; Staebler R.M.; Neuman J.A.; Nowak J.B.
刊名: Nature Geoscience
ISSN: 17520894
出版年: 2014
卷: 7, 期:2
起始页码: 91
结束页码: 94
语种: 英语
Scopus关键词: arctic environment ; atmospheric chemistry ; boundary layer ; chlorine ; concentration (composition) ; marine atmosphere ; oxidant ; peroxy radical ; photolysis ; radical ; Alaska ; Arctic ; Barrow ; United States
英文摘要: Chlorine radicals can function as a strong atmospheric oxidant, particularly in polar regions, where levels of hydroxyl radicals are low. In the atmosphere, chlorine radicals expedite the degradation of methane and tropospheric ozone, and the oxidation of mercury to more toxic forms. Here we present direct measurements of molecular chlorine levels in the Arctic marine boundary layer in Barrow, Alaska, collected in the spring of 2009 over a six-week period using chemical ionization mass spectrometry. We report high levels of molecular chlorine, of up to 400 pptv. Concentrations peaked in the early morning and late afternoon, and fell to near-zero levels at night. Average daytime molecular chlorine levels were correlated with ozone concentrations, suggesting that sunlight and ozone are required for molecular chlorine formation. Using a time-dependent box model, we estimate that the chlorine radicals produced from the photolysis of molecular chlorine oxidized more methane than hydroxyl radicals, on average, and enhanced the abundance of short-lived peroxy radicals. Elevated hydroperoxyl radical levels, in turn, promoted the formation of hypobromous acid, which catalyses mercury oxidation and the breakdown of tropospheric ozone. We therefore suggest that molecular chlorine exerts a significant effect on the atmospheric chemistry of the Arctic. © 2014 Macmillan Publishers Limited. All rights reserved.
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资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/106444
Appears in Collections:气候减缓与适应
科学计划与规划

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作者单位: School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA 30033, United States; Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO 80809, United States; Earth System Research Laboratory, NOAA, Boulder, CO 80305, United States; Combustion Research Facility, Sandia National Laboratories, Livermore, CA 94551, United States; National Center for Atmospheric Research, Boulder, CO 80307, United States; Department of Atmospheric and Oceanic Sciences, University of Colorado Boulder, Boulder, CO 80309, United States; Department of Chemistry, Purdue University, West Lafayette, IN 47907, United States; Department of Land, Air and Water Resources, University of California, Davis, CA 95616, United States; Department of Physics, University of Helsinki, Helsinki FI-00014, Finland; Air Quality Processes Section, Environment Canada, Toronto, M3H 5T4, Canada

Recommended Citation:
Liao J.,Huey L.G.,Liu Z.,et al. High levels of molecular chlorine in the Arctic atmosphere[J]. Nature Geoscience,2014-01-01,7(2)
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