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首页> 外文期刊>Environmental Science & Technology >'Sizing' Heterogeneous Chemistry in the Conversion of Gaseous Dimethyl Sulfide to Atmospheric Particles
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'Sizing' Heterogeneous Chemistry in the Conversion of Gaseous Dimethyl Sulfide to Atmospheric Particles

机译：气态二甲基硫硫化物向大气颗粒转化的“定型”异构化学

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The oxidation of biogenic dimethyl sulfide (DMS) emissions is a global source of cloud condensation nuclei. The amounts of the nucleating H_2SO_4(g) species produced in such process, however, remain uncertain. Hydrophobic DMS is mostly oxidized in the gas phase into H_2SO_4(g) + DMSO(g) (dimethyl sulfoxide), whereas water-soluble DMSO is oxidized into H_2SO_4(g) in the gas phase and into SO_4~(2-) + MeSO_3~- (methanesulfo- nate) on water surfaces. R = MeSO_3~-/(non-sea-salt SO_4~(2-)) ratios would therefore gauge both the strength of DMS sources and the extent of DMSO heterogeneous oxidation if R_(het) = MeSO_3~-/SO_4~(2-) for DMSO(aq) + ·OH(g) were known. Here, we report that R_(het) = 2.7, a value obtained from online electrospray mass spectra of DMSO(aq) + ·OH(g) reaction products that quantifies the MeSO_3~- produced in DMSO heterogeneous oxidation on aqueous aerosols for the first time. On this basis, the inverse R dependence on particle radius in size-segregated aerosol collected over Syowa station and Southern oceans is shown to be consistent with the competition between DMSO gas-phase oxidation and its mass accommodation followed by oxidation on aqueous droplets. Geographical R variations are thus associated with variable contributions of the heterogeneous pathway to DMSO atmospheric oxidation, which increase with the specific surface area of local aerosols.
机译：生物二甲基硫醚（DMS）排放物的氧化是云凝结核的全球来源。然而，在这种过程中产生的成核的H_2SO_4（g）种类的数量仍然不确定。疏水性DMS在气相中大部分被氧化为H_2SO_4（g）+ DMSO（g）（二甲亚砜），而水溶性DMSO在气相中被氧化为H_2SO_4（g）并被氧化为SO_4〜（2-）+ MeSO_3 〜-（甲磺酸盐）在水表面。因此，如果R_（het）= MeSO_3〜-/ SO_4〜（2），则R = MeSO_3〜-/（非海盐SO_4〜（2-））的比率将衡量DMS源的强度和DMSO非均相氧化的程度。 -）对于DMSO（aq）+·OH（g）是已知的。在此，我们报告R_（het）= 2.7，该值是从DMSO（aq）+·OH（g）反应产物的在线电喷雾质谱获得的，该值量化了DMSO在水性气雾剂中非均相氧化中产生的MeSO_3〜-。时间。在此基础上，Syowa台站和南大洋上收集到的大小分离的气溶胶中，反R对颗粒半径的依赖性被证明与DMSO气相氧化与其质量调节，然后在水滴上氧化之间的竞争是一致的。因此，地理R变化与非均质途径对DMSO大气氧化的贡献有关，该贡献随着局部气溶胶比表面积的增加而增加。

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  • 来源
    《Environmental Science & Technology》 |2016年第4期|1834-1843|共10页
  • 作者

    Shinichi Enami; Yosuke Sakamoto; Keiichiro Hara; Kazuo Osada; Michael R. Hoffmann; Agustin J. Colussi;

  • 作者单位

    The Hakubi Center for Advanced Research, Kyoto University, Kyoto 606-8302, Japan,Research Institute for Sustainable Humanosphere, Kyoto University, Uji 611-0011, Japan,PRESTO, Japan Science and Technology Agency, Kawaguchi 332-0012, Japan;

    Faculty of Environmental Earth Science, Hokkaido University, Sapporo 060-0610, Japan;

    Department of Earth Science System, Fukuoka University, Fukuoka 814-0180, Japan;

    Graduate School of Environmental Studies, Nagoya University, Nagoya 464-8601, Japan;

    Linde Center for Global Environmental Science, California Institute of Technology, California 91125, United States;

    Linde Center for Global Environmental Science, California Institute of Technology, California 91125, United States;

  • 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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