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Chemical Characterization of Secondary Organic Aerosol from Oxidation of Isoprene Hydroxyhydroperoxides

机译：异戊二烯羟基过氧化氢氧化产生的二级有机气溶胶的化学表征

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摘要

Atmospheric oxidation of isoprene under low- NO_x conditions leads to the formation of isoprene hydroxyhydroperoxides (ISOPOOH). Subsequent oxidation of ISOPOOH largely produces isoprene epoxydiols (1EPOX), which are known secondary organic aerosol (SOA) precursors. Although SOA from IEPOX has been previously examined, systematic studies of SOA characterization through a non- . IEPOX route from 1,2-ISOPOOH oxidation are lacking. In the present work, SOA formation from the oxidation of authentic 1,2-ISOPOOH under low-NO_x conditions was systematically examined with varying aerosol compositions and relative humidity. High yields of highly oxidized compounds, including multifunctional organosulfates (OSs) and hydroperoxides, were chemically characterized in both laboratory-generated SOA and fine aerosol samples collected from the southeastern U.S. IEPOX-derived SOA constituents were observed in all experiments, but their concentrations were only enhanced in the presence of acidified sulfate aerosol, consistent with prior work. High-resolution aerosol mass spectrometry (HR-AMS) reveals that 1,2-ISOPOOH-derived SOA formed through non-IEPOX routes exhibits a notable mass spectrum with a characteristic fragment ion at m/z 91. This laboratory-generated mass spectrum is strongly correlated with a factor recently resolved by positive matrix factorization (PMF) of aerosol mass spectrometer data collected in areas dominated by isoprene emissions, suggesting that the non-IEPOX pathway could contribute to ambient SOA measured in the Southeastern United States.
机译：在低NO_x条件下，异戊二烯在大气中的氧化会导致异戊二烯羟基氢过氧化物（ISOPOOH）的形成。随后进行ISOPOOH的氧化，可大量生产异戊二烯环氧二醇（1EPOX），这是已知的次级有机气溶胶（SOA）前体。尽管先前已经检查了来自IEPOX的SOA，但通过非系统方法对SOA表征进行了系统研究。缺乏IEPOX从1,2-ISOPOOH氧化的途径。在目前的工作中，系统地研究了在低NO_x条件下由真实的1,2-ISOPOOH氧化形成的SOA，其中使用了不同的气溶胶成分和相对湿度。在实验室生成的SOA中化学表征了高收率的高氧化化合物，包括多功能有机硫酸盐（OSs）和氢过氧化物，在所有实验中均观察到从美国东南部IEPOX衍生的SOA成分中收集的精细气溶胶样品，但其浓度仅为在酸化的硫酸盐气溶胶存在下增强，与先前的工作一致。高分辨率气溶胶质谱法（HR-AMS）显示，通过非IEPOX途径形成的1,2-ISOPOOH衍生的SOA表现出显着的质谱，特征离子为m / z91。该实验室生成的质谱为与最近由异戊二烯排放占主导的地区收集的气溶胶质谱仪数据的正矩阵分解（PMF）解决的因素密切相关，这表明非IEPOX途径可能对美国东南部的环境SOA有所贡献。

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  • 来源
    《Environmental Science & Technology》 |2016年第18期|9889-9899|共11页
  • 作者

    Matthieu Riva; Sri H. Budisulistiorini; Yuzhi Chen; Zhenfa Zhang; Emma L. DAmbro; Xuan Zhang; Avram Gold; Barbara J. Turpin; Joel A. Thornton; Manjula R. Canagaratna; Jason D. Surratt;

  • 作者单位

    Department of Environmental Sciences and Engineering, Gillings School of Global Public Health, The University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599 United States;

    Department of Environmental Sciences and Engineering, Gillings School of Global Public Health, The University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599 United States;

    Department of Environmental Sciences and Engineering, Gillings School of Global Public Health, The University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599 United States;

    Department of Environmental Sciences and Engineering, Gillings School of Global Public Health, The University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599 United States;

    Department of Atmospheric Sciences, University of Washington, Seattle, Washington 98195 United States;

    Center for Aerosol and Cloud Chemistry, Aerodyne Research, Billerica, Massachusetts 01821 United States;

    Department of Environmental Sciences and Engineering, Gillings School of Global Public Health, The University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599 United States;

    Department of Environmental Sciences and Engineering, Gillings School of Global Public Health, The University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599 United States;

    Department of Atmospheric Sciences, University of Washington, Seattle, Washington 98195 United States;

    Center for Aerosol and Cloud Chemistry, Aerodyne Research, Billerica, Massachusetts 01821 United States;

    Department of Environmental Sciences and Engineering, Gillings School of Global Public Health, The University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599 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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