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首页> 外文期刊>Environmental Science & Technology >Efficient Conversion of NO to NO_2 on SO_2-Aged MgO under Atmospheric Conditions
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Efficient Conversion of NO to NO_2 on SO_2-Aged MgO under Atmospheric Conditions

机译：在大气条件下高效地转换为SO_2-AGED MgO的NO_2

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摘要

The NO-NO_2 cycle determines the formation of O_3 and hence plays a critical role in the oxidizing capacity of troposphere. Traditional view concluded that the heterogeneous oxidation of NO to NO_2 was negligible due to the weak reactivity of NO on aerosols, compared to the homogeneous oxidation process. However, the results here reported for the first time that SO_2 can greatly promote the heterogeneous transformation of NO into NO_2 and HONO on MgO particles under ambient conditions. The uptake coefficients of NO were increased by 2-3 orders of magnitudes on SO_2-aged MgO, compared to the fresh sample. Based on spectroscopic characterization and density functional theory (DFT) calculations, the active sites for the adsorption and oxidation of NO were determined to be sulfates, where an intermediate [SO_4-NO] complex was formed during the adsorption. The decomposition of this species led to the formation of NO_2 and the change of sulfate configuration. The formed NO_2 could further react with surface sulfite to form HONO and sulfate. The conversion of NO to NO_2 and HONO on the SO_2-aged MgO surface under ambient conditions contributes a new formation pathway of NO_2 and HONO and could be quite helpful for understanding the source of atmospheric oxidizing capacity as well as the formation of air pollution complexes in polluted regions such as the northern China.
机译：No-No_2循环决定了O_3的形成，因此在对流层的氧化能力中起着关键作用。传统观点得出结论，与均匀氧化过程相比，由于气溶胶上的缺乏反应性，NO〜2的非均相氧化是可忽略不计的。然而，这里的结果首次报道了SO_2可以在环境条件下大大促进NO_2和MgO颗粒中的NO_2和Hono的异质转化。与新鲜样品相比，在SO_2老年的MgO上增加了NO的摄取系数增加了2-3次倍数。基于光谱性表征和密度官能理论（DFT）计算，测定吸附和氧化的活性位点是硫酸盐，其中在吸附过程中形成中间体[SO_4-NO]复合物。该物种的分解导致形成NO_2和硫酸盐构型的变化。形成的NO_2可以进一步与表面亚硫酸盐反应形成隆起和硫酸盐。在环境条件下，在SO_2老年的MGO表面上对NO_2和HONO的转化有助于NO_2和HONO的新形成途径，并且可以非常有助于理解大气氧化能力的来源以及空气污染复合物的形成污染地区，如北方。

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  • 来源
    《Environmental Science & Technology》 |2020年第19期|11848-11856|共9页
  • 作者

    Chang Liu; Honghong Wang; Qingxin Ma; Jinzhu Ma; Zhe Wang; Linlin Liang; Wanyun Xu; Gen Zhang; Xiaoye Zhang; Tao Wang; Hong He;

  • 作者单位

    State Key Laboratory of Severe Weather & Key Laboratory of Atmospheric Chemistry of China Meteorological Administration Chinese Academy of Meteorological Sciences Beijing 100081 China Department of Civil and Environmental Engineering The Hong Kong Polytechnic University Kowloon Hong Kong 999077 China;

    State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Beijing 100085 China Center for Excellence in Urban Atmospheric Environment Institute of Urban Environment Chinese Academy of Sciences Xiamen 361021 China;

    Department of Civil and Environmental Engineering The Hong Kong Polytechnic University Kowloon Hong Kong 999077 China State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Beijing 100085 China Center for Excellence in Urban Atmospheric Environment Institute of Urban Environment Chinese Academy of Sciences Xiamen 361021 China College of Resources and Environment University of Chinese Academy of Sciences Beijing 100049 China;

    State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Beijing 100085 China Center for Excellence in Urban Atmospheric Environment Institute of Urban Environment Chinese Academy of Sciences Xiamen 361021 China College of Resources and Environment University of Chinese Academy of Sciences Beijing 100049 China;

    Division of Environment and Sustainability The Hong Kong University of Science and Technology Kowloon 999077 Hong Kong China;

    State Key Laboratory of Severe Weather & Key Laboratory of Atmospheric Chemistry of China Meteorological Administration Chinese Academy of Meteorological Sciences Beijing 100081 China;

    State Key Laboratory of Severe Weather & Key Laboratory of Atmospheric Chemistry of China Meteorological Administration Chinese Academy of Meteorological Sciences Beijing 100081 China;

    State Key Laboratory of Severe Weather & Key Laboratory of Atmospheric Chemistry of China Meteorological Administration Chinese Academy of Meteorological Sciences Beijing 100081 China;

    State Key Laboratory of Severe Weather & Key Laboratory of Atmospheric Chemistry of China Meteorological Administration Chinese Academy of Meteorological Sciences Beijing 100081 China Center for Excellence in Urban Atmospheric Environment Institute of Urban Environment Chinese Academy of Sciences Xiamen 361021 China;

    Department of Civil and Environmental Engineering The Hong Kong Polytechnic University Kowloon Hong Kong 999077 China;

    State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Beijing 100085 China Center for Excellence in Urban Atmospheric Environment Institute of Urban Environment Chinese Academy of Sciences Xiamen 361021 China College of Resources and Environment University of Chinese Academy of Sciences Beijing 100049 China;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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