Effect of the Aerosol-Phase State on Secondary Organic Aerosol Formation from the Reactive Uptake of Isoprene-Derived Epoxydiols (IEPOX)

Effect of the Aerosol-Phase State on Secondary Organic Aerosol Formation from the Reactive Uptake of Isoprene-Derived Epoxydiols (IEPOX)
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气溶胶相状态对异戊二烯衍生环氧二醇 (IEPOX) 反应吸收形成的二次有机气溶胶的影响

DOI:
10.1021/acs.estlett.8b00044
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发表时间:
2018
影响因子:
10.9
通讯作者:
Jayne, John T.
Jayne, John T.
中科院分区:
环境科学与生态学2区
文献类型:
--
作者:
Zhang, Yue;Chen, Yuzhi;Lambe, Andrew T.;Olson, Nicole E.;Lei, Ziying;Craig, Rebecca L.;Zhang, Zhenfa;Gold, Avram;Onasch, Timothy B.;Jayne, John T.

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酸催化的气相和颗粒相组分之间的反应是大气二次有机气溶胶(SOA)形成的关键。气溶胶相态被认为通过改变颗粒内的扩散速率来影响气溶胶颗粒对气相前体的反应性吸收。然而,很少有实验研究探讨了反应性吸收过程中的气溶胶相态的确切作用。本文系统地研究了反式-β-异戊二烯环氧二醇(trans-β-IEPOX)在酸性硫酸盐颗粒表面的反应吸收系数(γ)。γ IEPOX是SOA涂层厚度和相对湿度的函数。当SOA涂层在吸收之前存在时,γ IEPOX降低,在某些情况下降低到原始值的一半,特别是当涂层厚度>15 nm时。IEPOX损失的酸催化反应吸收产生SOA与其他已知的大气汇(气相氧化或沉积)相比的昼夜趋势是通过模拟实验涂层效应与来自美国东南部的现场数据。由于下午(12:00至7:00 p.m.,当地时间),对应于生产水平最高的时期。
Acid-catalyzed reactions between gas- and particle-phase constituents are critical to atmospheric secondary organic aerosol (SOA) formation. The aerosol-phase state is thought to influence the reactive uptake of gas-phase precursors to aerosol particles by altering diffusion rates within particles. However, few experimental studies have explored the precise role of the aerosol-phase state on reactive uptake processes. This laboratory study systematically examines the reactive uptake coefficient (γ) oftrans-β-isoprene epoxydiol (trans-β-IEPOX), the predominant IEPOX isomer, on acidic sulfate particles coated with SOA derived from α-pinene ozonolysis. γIEPOXis obtained for core-shell particles, the morphology of which was confirmed by microscopy, as a function of SOA coating thickness and relative humidity. γIEPOXis reduced, in some cases by half of the original value, when SOA coatings are present prior to uptake, especially when coating thicknesses are >15 nm. The diurnal trend of IEPOX lost to acid-catalyzed reactive uptake yielding SOA compared with other known atmospheric sinks (gas-phase oxidation or deposition) is derived by modeling the experimental coating effect with field data from the southeastern United States. IEPOX-derived SOA is estimated to be reduced by 16–27% due to preexisting organic coatings during the afternoon (12:00 to 7:00 p.m., local time), corresponding to the period with the highest level of production.
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DOI: 10.4209/aaqr.2015.05.0346
发表时间: 2016
影响因子: 4
作者:
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根据 SOA 颗粒的聚结时间估算其粘度范围
DOI: --
发表时间: 2014
期刊:
影响因子: --
作者:
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通讯作者: A. Virtanen
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发表时间: 2012-01-01
影响因子: 5.1
作者:
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