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Effects of NH_3 and alkaline metals on the formation of particulate sulfate and nitrate in wintertime Beijing

机译:冬季北京地区NH_3和碱金属对硫酸盐和硝酸盐颗粒形成的影响

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摘要

Sulfate and nitrate from secondary reactions remain as the most abundant inorganic species in atmospheric particle matter (PM). Their formation is initiated by oxidation (either in gas phase or particle phase), followed by neutralization reaction primarily by NH_3, or by other alkaline species such as alkaline metal ions if available. The different roles of NH_3 and metal ions in neutralizing H_2SO_4 or HNO_3, however, are seldom investigated. Here we conducted semi-continuous measurements of SO_4~(2-), NO_3~- , NH_4~+, and their gaseous precursors, as well as alkaline metal ions (Na~+, K~+, Ca~(2+)), and Mg~(2+)) in wintertime Beijing. Analysis of aerosol acidity (estimated from a thermodynamic model) indicated that preferable sulfate formation was related to low pH conditions, while high pH conditions promote nitrate formation. Data in different mass fraction ranges of alkaline metal ions showed that in some ranges the role of NH_3 was replaced by alkaline metal ions in the neutralization reaction of H_2SO_4 and HNO3 to form particulate SO_4~(2-) and NO_3~-. The relationships between mass fractions of SO_4~(2-) and HO_3~- in those ranges of different alkaline metal ion content also suggested that alkaline metal ions participate in the competing neutralization reaction of sulfate and nitrate. The implication of the current study is that in some regions the chemistry to incorporate sulfur and nitrogen into particle phase might be largely affected by desert/fugitive dust and sea salt, besides NH_3. This implication is particularly relevant in coastal China and those areas with strong influence of dust storm in the North China Plain (NCP), both of which host a number of megacities with deteriorating air quality.
机译:来自次级反应的硫酸盐和硝酸盐仍然是大气颗粒物(PM)中最丰富的无机物。它们的形成是通过氧化(气相或颗粒相)开始的,然后主要通过NH_3或其他碱性物质(如碱金属离子,如果有)进行中和反应。然而,很少研究NH_3和金属离子在中和H_2SO_4或HNO_3中的不同作用。在这里,我们对SO_4〜(2-),NO_3〜-,NH_4〜+及其气态前体以及碱金属离子(Na〜+,K〜+,Ca〜(2+))进行了半连续测量。和Mg〜(2+))的冬季北京。气溶胶酸度分析(根据热力学模型估算)表明,优选的硫酸盐形成与低pH条件有关,而高pH条件则促进硝酸盐的形成。碱金属离子质量分数范围不同的数据表明,在H_2SO_4和HNO3的中和反应中,NH_3的作用在某些范围内被碱金属离子替代,从而形成颗粒SO_4〜(2-)和NO_3〜-。在不同的碱金属离子含量范围内,SO_4〜(2-)和HO_3〜-的质量分数之间的关系也表明,碱金属离子参与了硫酸盐和硝酸盐的竞争中和反应。当前研究的意义在于,除了NH_3以外,在某些地区,将硫和氮掺入颗粒相的化学反应可能还受到沙漠/逃逸性粉尘和海盐的影响。这对中国沿海地区以及华北平原(NCP)受沙尘暴影响较大的地区尤其重要,这两个地区都拥有许多空气质量不断恶化的特大城市。

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  • 来源
    《The Science of the Total Environment》 |2020年第may15期|137190.1-137190.8|共8页
  • 作者单位

    Key Laboratory of Aerosol Chemistry and Physics State Key Laboratory of Loess and Quaternary Geology CAS Center for Excellence in Quaternary Science and Global Change Institute of Earth and Environment Chinese Academy of Sciences Xi'an 710061 China;

    Department of Civil and Environmental Engineering Faculty of Science and Technology University of Macau Taipa Macau China;

    State Key foint Laboratory of Environmental Simulation and Pollution Control College of Environmental Sciences and Engineering Peking University Beijing China;

    Chongqing Institute of Green and Intelligent Technology Chinese Academy of Sciences Chongqing 400714 China;

    State Key Laboratory of Organic Geochemistry and Guangdong Key Laboratory of Environmental Protection and Resources Utilization Guangzhou Institute of Geochemistry Chinese Academy of Sciences Guangzhou China;

    Key Laboratory of Aerosol Chemistry and Physics State Key Laboratory of Loess and Quaternary Geology CAS Center for Excellence in Quaternary Science and Global Change Institute of Earth and Environment Chinese Academy of Sciences Xi'an 710061 China Centre for Isotope Research (CIO) Energy and Sustainability Research Institute Groningen (ESRIG) University of Groningen the Netherlands;

    Key Laboratory of Aerosol Chemistry and Physics State Key Laboratory of Loess and Quaternary Geology CAS Center for Excellence in Quaternary Science and Global Change Institute of Earth and Environment Chinese Academy of Sciences Xi'an 710061 China School of Physics and Centre for Climate and Air Pollution Studies Ryan Institute National University of Ireland Galway University Road Galway Ireland;

    CAS Key Laboratory for Biological Effects of Nanomaterials and Nanosafety National Centre for Nanoscience and Technology Beijing 100191 China;

    Metrahm China Ltd. Shanghai 200335 China;

    School of Physics and Centre for Climate and Air Pollution Studies Ryan Institute National University of Ireland Galway University Road Galway Ireland;

    Centre for Isotope Research (CIO) Energy and Sustainability Research Institute Groningen (ESRIG) University of Groningen the Netherlands;

    Institute of Inorganic and Analytical Chemistry Johannes Gutenberg University of Mainz Duesbergweg 10-14 Mainz 55128 Germany;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    Sulfate; Nitrate; Ammonia; Alkaline metals;

    机译:硫酸盐硝酸盐氨;碱性金属;

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