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The role of chlorine in global tropospheric chemistry

机译：氯在全球对流层化学的作用

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摘要

We present a comprehensive simulation of tropospheric chlorine within the GEOS-Chem global 3-D model of oxidant-aerosol-halogen atmospheric chemistry. The simulation includes explicit accounting of chloride mobilization from sea salt aerosol by acid displacement of HCl and by other heterogeneous processes. Additional small sources of tropospheric chlorine (combustion, organochlorines, transport from stratosphere) are also included. Reactive gasphase chlorine Cl~*, including Cl, ClO, Cl_2, BrCl, ICl, HOCl, ClNO_3, ClNO_2, and minor species, is produced by the HClC OH reaction and by heterogeneous conversion of sea salt aerosol chloride to BrCl, ClNO_2, Cl_2, and ICl. The model successfully simulates the observed mixing ratios of HCl in marine air (highest at northern midlatitudes) and the associated HNO_3 decrease from acid displacement. It captures the high ClNO_2 mixing ratios observed in continental surface air at night and attributes the chlorine to HCl volatilized from sea salt aerosol and transported inland following uptake by fine aerosol. The model successfully simulates the vertical profiles of HCl measured from aircraft, where enhancements in the continental boundary layer can again be largely explained by transport inland of the marine source. It does not reproduce the boundary layer Cl_2 mixing ratios measured in the WINTER aircraft campaign (1-5 ppt in the daytime, low at night); the model is too high at night, which could be due to uncertainty in the rate of the ClNO_2 CCl~- reaction, but we have no explanation for the high observed Cl_2 in daytime. The global mean tropospheric concentration of Cl atoms in the model is 620 cm~(-3) and contributes 1.0% of the global oxidation of methane, 20% of ethane, 14% of propane, and 4% of methanol. Chlorine chemistry increases global mean tropospheric BrO by 85 %, mainly through the HOBrCCl~- reaction, and decreases global burdens of tropospheric ozone by 7% and OH by 3% through the associated bromine radical chemi
机译：我们在氧化剂 - 气溶胶 - 卤素大气化学地球化学全球3-D模型中综合模拟了对流层氯。该模拟包括通过HCl的酸性位移和其他异质过程从海盐气溶胶的氯化物动员显式核算。还包括额外的小氯化氯（燃烧，有机氯，从平流层运输）的额外小来源。反应性气体Cl〜*，包括Cl，ClO，Cl_2，BrCl，ICL，HOCl，ClNO_3，ClNO_2和次要物种是通过HCLC OH反应产生的，并通过将海盐气溶胶氯化物的异质转化为BRCL，ClNO_2，CL_2和ICL。该模型成功地模拟了海洋空气中HCl的观察到的混合比（在北中间阶段最高），并且相关的HNO_3从酸性位移中减少。它捕获了夜间在欧式表面​​空气中观察到的高ClNO_2混合比，并将氯与海盐气溶胶挥发的HCl归因，并通过细气溶胶进行摄取后运输内陆。该模型成功地模拟了从飞机测量的HCl的垂直轮廓，其中大陆边界层的增强可以再次通过运输海军源的内陆来解释。它不会再现在冬季飞机运动中测量的边界层CL_2混合比（白天在白天，晚上低1-5个PPT）;该模型在夜间过高，这可能是由于CLNO_2 CCL〜 - 反应的速率的不确定性，但我们对白天的高观察到的CL_2没有解释。模型中Cl原子的全局平均浓度为620cm〜（-3），占甲烷全球氧化的1.0％，乙烷的20％，丙烷的14％，4％的甲醇。氯化学通过HOBRCCL〜 - 反应增加了85％的全球平均晶体兄弟，并通过相关的溴激进化学将全球臭氧的全球臭氧量减少7％和哦

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  • 来源
    《Atmospheric chemistry and physics》 |2019年第2期|共23页
  • 作者

    Xuan Wang; Daniel J. Jacob; Sebastian D. Eastham; Melissa P. Sulprizio; Lei Zhu; Qianjie Chen; Becky Alexander; Tomás Sherwen; Mathew J. Evans; Ben H. Lee; Jessica D. Haskins; Felipe D. Lopez-Hilfiker; Joel A. Thornton; Gregory L. Huey; Hong Liao;

  • 作者单位

    School of Engineering and Applied Sciences Harvard University Cambridge Massachusetts USA;

    School of Engineering and Applied Sciences Harvard University Cambridge Massachusetts USA;

    Laboratory for Aviation and the Environment Massachusetts Institute of Technology Cambridge Massachusetts USA;

    School of Engineering and Applied Sciences Harvard University Cambridge Massachusetts USA;

    School of Engineering and Applied Sciences Harvard University Cambridge Massachusetts USA;

    Department of Chemistry University of Michigan Ann Arbor Michigan USA;

    Department of Atmospheric Sciences University of Washington Seattle USA;

    Wolfson Atmospheric Chemistry Laboratories Department of Chemistry University of York York UK;

    Wolfson Atmospheric Chemistry Laboratories Department of Chemistry University of York York UK;

    Department of Atmospheric Sciences University of Washington Seattle USA;

    Department of Atmospheric Sciences University of Washington Seattle USA;

    Laboratory of Atmospheric Chemistry Paul Scherrer Institute Villigen Switzerland;

    Department of Atmospheric Sciences University of Washington Seattle USA;

    School of Earth and Atmospheric Science Georgia Institute of Technology Atlanta GA USA;

    School of Environmental Science and Engineering Nanjing University of Information Science and Technology Nanjing China;

  • 收录信息
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 大气科学（气象学）;
  • 关键词

    The role; chlorine; global tropospheric;

    机译：作用;氯;全球对流层;

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