Increasing Isoprene Epoxydiol-to-Inorganic Sulfate Aerosol Ratio Results in Extensive Conversion of Inorganic Sulfate to Organosulfur Forms: Implications for Aerosol Physicochemical Properties.
Increasing Isoprene Epoxydiol-to-Inorganic Sulfate Aerosol Ratio Results in Extensive Conversion of Inorganic Sulfate to Organosulfur Forms: Implications for Aerosol Physicochemical Properties.
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DOI：
10.1021/acs.est.9b01019
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发表时间：
2019-06
影响因子：
11.4
通讯作者：
M. Riva;Yuzhi Chen;Yue Zhang;Ziying Lei;Nicole E. Olson;Hallie C. Boyer;S. Narayan;L. Yee;H. Green;T. Cui;Zhenfa Zhang;K. Baumann;M. Fort;E. Edgerton;S. Budisulistiorini;C. Rose;I. Ribeiro;Rafael L E Oliveira;Erickson O Dos Santos;C. Machado;S. Szopa;Yue Zhao;E. Alves;Suzane S. de Sá;Weiwei Hu;E. Knipping;S. Shaw;S. Duvoisin Júnior;R. D. de Souza;B. Palm;J. Jimenez;M. Glasius;A. Goldstein;H. Pye;A. Gold;B. Turpin;W. Vizuete;S. Martin;J. Thornton;C. Dutcher;A. Ault;J. Surratt
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文献类型：
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作者：
M. Riva;Yuzhi Chen;Yue Zhang;Ziying Lei;Nicole E. Olson;Hallie C. Boyer;S. Narayan;L. Yee;H. Green;T. Cui;Zhenfa Zhang;K. Baumann;M. Fort;E. Edgerton;S. Budisulistiorini;C. Rose;I. Ribeiro;Rafael L E Oliveira;Erickson O Dos Santos;C. Machado;S. Szopa;Yue Zhao;E. Alves;Suzane S. de Sá;Weiwei Hu;E. Knipping;S. Shaw;S. Duvoisin Júnior;R. D. de Souza;B. Palm;J. Jimenez;M. Glasius;A. Goldstein;H. Pye;A. Gold;B. Turpin;W. Vizuete;S. Martin;J. Thornton;C. Dutcher;A. Ault;J. Surratt
异戊二烯环氧二醇（IEPOX），关键的异戊二烯氧化产物，与无机硫酸盐气溶胶的酸驱动的多相化学产生大量的二次有机气溶胶（SOA）通过形成有机硫化合物。然而，无机硫酸盐转化为有机硫酸盐的程度和影响尚不清楚。在这篇文章中，我们证明了大量的无机硫酸盐的消耗发生，这与IEPOX-无机硫酸盐的浓度比（IEPOX/Sulfinorg），通过实验室测量确定的增加。2007年至2016年在田纳西州Look Rock观测到的总硫气溶胶的特征表明，随着人为Sulfinorg的持续下降，有机硫质量分数可能会继续增加，这与我们的实验室发现一致。我们进一步表明，有机硫化合物大大修改关键气溶胶的性质，如酸度，形态，粘度和相态。这些新的机制的见解表明，SO2排放量的变化，特别是在异戊二烯为主的环境中，将显着改变生物SOA的物理化学性质。因此，IEPOX/Sulfinorg将在了解历史气候和确定未来生物SOA对全球气候和空气质量的影响方面发挥重要作用。
Acid-driven multiphase chemistry of isoprene epoxydiols (IEPOX), key isoprene oxidation products, with inorganic sulfate aerosol yields substantial amounts of secondary organic aerosol (SOA) through the formation of organosulfur compounds. The extent and implications of inorganic-to-organic sulfate conversion, however, are unknown. In this article, we demonstrate that extensive consumption of inorganic sulfate occurs, which increases with the IEPOX-to-inorganic sulfate concentration ratio (IEPOX/Sulfinorg), as determined by laboratory measurements. Characterization of the total sulfur aerosol observed at Look Rock, Tennessee, from 2007 to 2016 shows that organosulfur mass fractions will likely continue to increase with ongoing declines in anthropogenic Sulfinorg, consistent with our laboratory findings. We further demonstrate that organosulfur compounds greatly modify critical aerosol properties, such as acidity, morphology, viscosity, and phase state. These new mechanistic insights demonstrate that changes in SO2 emissions, especially in isoprene-dominated environments, will significantly alter biogenic SOA physicochemical properties. Consequently, IEPOX/Sulfinorg will play an important role in understanding the historical climate and determining future impacts of biogenic SOA on the global climate and air quality.