Seasonal Contribution of Isoprene-Derived Organosulfates to Total Water-Soluble Fine Particulate Organic Sulfur in the United States,ACS Earth and Space Chemistry

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Seasonal Contribution of Isoprene-Derived Organosulfates to Total Water-Soluble Fine Particulate Organic Sulfur in the United States
ACS Earth and Space Chemistry ( IF 2.9 ) Pub Date : 2021-08-17 , DOI: 10.1021/acsearthspacechem.1c00102
Yuzhi Chen ₁ , Tracy Dombek ₂ , Jenny Hand ₃ , Zhenfa Zhang ₁ , Avram Gold ₁ , Andrew P. Ault ₄ , Keith E. Levine ₂ , Jason D. Surratt _{1,

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Affiliation

Organosulfates (OSs) are the most abundant class of organosulfur (OrgS) compounds in atmospheric fine particulate matter (PM_2.5). Globally, isoprene-derived OSs (iOSs) are the most abundantly reported OSs; however, total sulfur mass closure in PM_2.5 has not been conducted at the molecular level in order to understand how iOS contributions vary by season and by location in the United States (U.S.). In this work, iOSs were quantitively characterized in PM_2.5 collected from 20 ground sites within the Interagency Monitoring of Protected Visual Environments (IMPROVE) network during the 2016 summer and winter seasons. Total water-soluble sulfur (TWS-S) and sulfur from inorganic sulfate (S_inorg) were also chemically determined, with the imbalance between TWS-S and S_inorg used as an upper-bound estimate of water-soluble OrgS concentrations. Significantly higher fine particulate OrgS concentrations (∼20% of TWS-S) were observed at most sites only in summer, coincident with elevated iOS concentrations in the eastern U.S. On average, iOSs (130 ng m^–3) explained 29 and 4% by mass of OrgS and of organic matter (OM), respectively, in the eastern U.S. In the western U.S., iOSs (11 ng m^–3, on average) accounted for 6 and 0.5% by mass of OrgS and OM, respectively. In winter, iOSs were hardly detected, consistent with reduced isoprene emissions. Our study shows that ∼70 and 80% of OrgS mass in the eastern U.S. and western U.S., respectively, remain unexplained at the molecular level. This study provides critical insights into the abundance, prevalence, and spatial variability of fine particulate iOSs across the U.S.

中文翻译：

异戊二烯衍生的有机硫酸盐对美国水溶性细颗粒有机硫总量的季节性贡献

有机硫酸盐 (OS) 是大气细颗粒物 (PM _2.5 ) 中含量最丰富的一类有机硫 (OrgS) 化合物。在全球范围内，异戊二烯衍生的操作系统 (iOS) 是报道最多的操作系统；然而，PM _{2.5 中的}总硫质量闭合尚未在分子水平上进行，以了解 iOS 贡献如何随季节和美国 (US) 位置而变化。在这项工作中，iOS在 2016 年夏季和冬季期间从受保护视觉环境机构间监测 (IMPROVE) 网络内的 20 个地面站点收集的PM _{2.5 中}进行了定量表征。总水溶性硫 (TWS-S) 和来自无机硫酸盐的硫 (S _inorg) 也被化学确定，TWS-S 和 S _inorg之间的不平衡用作水溶性 OrgS 浓度的上限估计。仅在夏季在大多数地点观察到显着更高的细颗粒 OrgS 浓度（TWS-S 的约 20%），与美国东部的 iOS 浓度升高相吻合平均而言，iOSs (130 ng m ^–3 ) 解释了 29% 和 4%分别在美国东部的 OrgS 和有机质 (OM) 质量在美国西部，iOSs (11 ng m ^–3平均）分别占 OrgS 和 OM 质量的 6% 和 0.5%。在冬季，几乎没有检测到 iOS，这与异戊二烯排放量减少一致。我们的研究表明，在美国东部和美国西部，分别有 70% 和 80% 的 OrgS 质量在分子水平上仍然无法解释。这项研究提供了关于美国细颗粒 iOS 的丰度、流行率和空间变异性的重要见解

更新日期：2021-09-16

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