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Structural Characterization of Lactone-Containing MW 212 Organosulfates Originating from Isoprene Oxidation in Ambient Fine Aerosol.
Environmental Science & Technology ( IF 11.4 ) Pub Date : 2020-01-22 , DOI: 10.1021/acs.est.9b06190
Paulina Wach 1, 2 , Grzegorz Spólnik 2 , Jason D Surratt 3 , Kacper Blaziak 4 , Krzysztof J Rudzinski 1 , Ying-Hsuan Lin 5 , Willy Maenhaut 6 , Witold Danikiewicz 2 , Magda Claeys 7 , Rafal Szmigielski 1
Affiliation  

Isoprene (C5H8) is the main non-methane hydrocarbon emitted into the global atmosphere. Despite intense research, atmospheric transformations of isoprene leading to secondary organic aerosol (SOA) are still not fully understood, including its multiphase chemical reactions. Herein, we report on the detailed structural characterization of atmospherically relevant isoprene-derived organosulfates (OSs) with a molecular weight (MW) of 212 (C5H8SO7), which are abundantly present in both ambient fine aerosol (PM2.5) and laboratory-generated isoprene SOA. The results obtained from smog chamber-generated isoprene SOA and aqueous-phase laboratory experiments coupled to the S(IV)-autooxidation chemistry of isoprene, 3-methyl-2(5H)-furanone, and 4-methyl-2(5H)-furanone, allowed us for the first time to fully elucidate the isomeric structures of the MW 212 OSs. By applying liquid chromatography interfaced to electrospray ionization high-resolution mass spectrometry, we firmly confirmed six positional isomers of the MW 212 OSs in PM2.5 collected from different sites in Europe and the United States. Our results also show that despite the low solubility of isoprene in water, aqueous-phase or multiphase chemistry can play an important role in the formation of OSs from isoprene. Possible formation mechanisms for the MW 212 OSs are also tentatively proposed.

中文翻译:

源自内环境精细气溶胶中异戊二烯氧化反应的含内酯的MW 212有机硫酸盐的结构表征。

异戊二烯(C5H8)是排放到全球大气中的主要非甲烷碳氢化合物。尽管进行了深入的研究,但对异戊二烯在大气中导致二次有机气溶胶(SOA)的转化仍不完全清楚,包括其多相化学反应。本文中,我们报告了有关大气中异戊二烯衍生的有机硫酸盐(OSs)的分子量(MW)为212(C5H8SO7)的详细结构特征,这些物质大量存在于环境精细气溶胶(PM2.5)和实验室生成的异戊二烯SOA。从烟雾室生成的异戊二烯SOA和水相实验室实验获得的结果与异戊二烯,3-甲基-2(5H)-呋喃酮和4-甲基-2(5H)-的S(IV)-自氧化化学偶联呋喃酮,使我们首次能够完全阐明MW 212 OS的异构体结构。通过将液相色谱与电喷雾电离高分辨率质谱联用,我们坚定地确认了从欧洲和美国不同地点收集的PM2.5中MW 212 OS的六个位置异构体。我们的结果还表明,尽管异戊二烯在水中的溶解度低,但水相或多相化学反应在异戊二烯形成OS的过程中仍可发挥重要作用。还初步提出了MW 212 OS的可能形成机制。水相或多相化学在异戊二烯形成OS的过程中可以发挥重要作用。还初步提出了MW 212 OS的可能形成机制。水相或多相化学在异戊二烯形成OS的过程中可以发挥重要作用。还初步提出了MW 212 OS的可能形成机制。
更新日期:2020-01-23
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