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首页> 外文期刊>Environmental Science & Technology >Secondary Organic Aerosol Production from Aqueous Reactions of Atmospheric Phenols with an Organic Triplet Excited State
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Secondary Organic Aerosol Production from Aqueous Reactions of Atmospheric Phenols with an Organic Triplet Excited State

机译：大气苯酚与有机三重态激发态的水溶液反应产生次级有机气溶胶

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摘要

Condensed-phase chemistry plays a significant role in the formation and evolution of atmospheric organic aerosols. Past studies of the aqueous photoformation of secondary organic aerosol (SOA) have largely focused on hydroxyl radical oxidation, but here we show that triplet excited states of organic compounds (~3C~*) can also be important aqueous oxidants. We studied the aqueous photoreactions of three phenols (phenol, guaiacol, and syringol) with the aromatic carbonyl 3,4-dimethoxybenzaldehyde (DMB); all of these species are emitted by biomass burning. Under simulated sunlight, DMB forms a triplet excited state that rapidly oxidizes phenols to form low-volatility SOA. Rate constants for these reactions are fast and increase with decreasing pH and increasing methoxy substitution of the phenols. Mass yields of aqueous SOA are near 100% for all three phenols. For typical ambient conditions in areas with biomass combustion, the aqueous oxidation of phenols by ~3C~* is faster than by hydroxyl radical, although rates depend strongly on pH, oxidant concentrations, and the identity of the phenol. Our results suggest that ~3C~* can be the dominant aqueous oxidant of phenols in areas impacted by biomass combustion and that this is a significant pathway for forming SOA.
机译：冷凝相化学在大气有机气溶胶的形成和演化中起着重要作用。过去对次级有机气溶胶（SOA）的水性光形成的研究主要集中在羟基自由基的氧化上，但在这里我们表明有机化合物（〜3C〜*）的三重激发态也可能是重要的水性氧化剂。我们研究了三种酚（苯酚，愈创木酚和丁香酚）与芳香族羰基3,4-二甲氧基苯甲醛（DMB）的水反应。所有这些物种都是通过生物质燃烧排放的。在模拟的阳光下，DMB形成三重激发态，该态会迅速氧化苯酚以形成低挥发性SOA。这些反应的速率常数很快，并且随着pH降低和酚的甲氧基取代增加而增加。对于所有三种酚，SOA水溶液的质量产率均接近100％。在生物质燃烧区域的典型环境条件下，酚的水溶液〜3C〜*的水溶液氧化速度比羟基自由基快，尽管其速率主要取决于pH值，氧化剂浓度和酚的种类。我们的结果表明，〜3C〜*可能是受生物质燃烧影响的区域中酚类的主要氧化剂，这是形成SOA的重要途径。

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  • 来源
    《Environmental Science & Technology》 |2014年第2期|1049-1057|共9页
  • 作者

    Jeremy D. Smith; Vicky Sio; Lu Yu; Qi Zhang; Cort Anastasio;

  • 作者单位

    Department of Land, Air and Water Resources, University of California-Davis, 1 Shields Avenue, Davis, California 95616, United States,Agricultural and Environmental Chemistry Graduate Group, University of California-Davis, 1 Shields Avenue, Davis, California 95616, United States;

    Department of Land, Air and Water Resources, University of California-Davis, 1 Shields Avenue, Davis, California 95616, United States;

    Agricultural and Environmental Chemistry Graduate Group, University of California-Davis, 1 Shields Avenue, Davis, California 95616, United States,Department of Environmental Toxicology, University of California-Davis, 1 Shields Avenue, Davis, California 95616, United States;

    Agricultural and Environmental Chemistry Graduate Group, University of California-Davis, 1 Shields Avenue, Davis, California 95616, United States,Department of Environmental Toxicology, University of California-Davis, 1 Shields Avenue, Davis, California 95616, United States;

    Department of Land, Air and Water Resources, University of California-Davis, 1 Shields Avenue, Davis, California 95616, United States,Agricultural and Environmental Chemistry Graduate Group, University of California-Davis, 1 Shields Avenue, Davis, California 95616, 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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