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首页> 外文期刊>Environmental Science & Technology >Organic Peroxides and Sulfur Dioxide in Aerosol: Source of Particulate Sulfate
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Organic Peroxides and Sulfur Dioxide in Aerosol: Source of Particulate Sulfate

机译：气溶胶中的有机过氧化物和二氧化硫：颗粒状硫酸盐的来源

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Sulfur oxides (SOx) are important atmospheric trace species in both gas and particulate phases, and sulfate is a major component of atmospheric aerosol. One potentially important source of particulate sulfate formation is the oxidation of dissolved SO2 by organic peroxides, which comprises a major fraction of secondary organic aerosol (SOA). In this study, we investigated the reaction kinetics and mechanisms between SO2 and condensed-phase peroxides. pH-dependent aqueous phase reaction rate constants between S(IV) and organic peroxide standards were measured. Highly oxygenated organic peroxides with O/C > 0.6 in alpha-pinene SOA react rapidly with S(IV) species in the aqueous phase. The reactions between organic peroxides and S(IV) yield both inorganic sulfate and organosulfates (OS), as observed by electrospray ionization ion mobility mass spectrometry. For the first time, S-34-labeling experiments in this study revealed that dissolved SO2 forms OS via direct reactions without forming inorganic sulfate as a reactive intermediate. Kinetics of OS formation was estimated semiquantitatively, and such reaction was found to account for 30-60% of sulfur reacted. The photochemical box model GAMMA was applied to assess the implications of the measured SO2 consumption and OS formation rates. Our findings indicate that this novel pathway of SO2-peroxide reaction is important for sulfate formation in submicron aerosol.
机译：硫氧化物（SOx）在气相和颗粒相中都是重要的大气痕量物质，而硫酸盐是大气气溶胶的主要成分。潜在的重要的颗粒状硫酸盐形成来源是有机过氧化物对溶解的SO2的氧化，该过氧化物包含大部分的次级有机气溶胶（SOA）。在这项研究中，我们研究了SO2与冷凝相过氧化物之间的反应动力学和机理。测量了S（IV）和有机过氧化物标准溶液之间pH依赖的水相反应速率常数。在α-pine烯SOA中O / C> 0.6的高度氧化的有机过氧化物与水相中的S（IV）物种迅速反应。如通过电喷雾电离离子迁移质谱法所观察到的，有机过氧化物与S（IV）之间的反应会同时产生无机硫酸盐和有机硫酸盐（OS）。这项研究中的S-34标记实验首次显示，溶解的SO2通过直接反应形成OS，而没有形成无机硫酸盐作为反应性中间体。半定量估计OS形成的动力学，发现该反应占反应的硫的30-60％。应用光化学箱模型GAMMA评估测得的SO2消耗和OS形成速率的影响。我们的发现表明，这种SO2-过氧化物反应的新途径对于亚微米气溶胶中硫酸盐的形成很重要。

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