Isoprene epoxydiols as precursors to secondary organic aerosol formation: acid-catalyzed reactive uptake studies with authentic compounds.
Isoprene epoxydiols as precursors to secondary organic aerosol formation: acid-catalyzed reactive uptake studies with authentic compounds.
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DOI：
10.1021/es202554c
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发表时间：
2012-01-03
影响因子：
11.4
通讯作者：
Surratt, Jason D.
中科院分区：
文献类型：
--
作者：
Lin, Ying-Hsuan;Zhang, Zhenfa;Docherty, Kenneth S.;Zhang, Haofei;Budisulistiorini, Sri Hapsari;Rubitschun, Caitlin L.;Shaw, Stephanie L.;Knipping, Eladio M.;Edgerton, Eric S.;Kleindienst, Tadeusz E.;Gold, Avram;Surratt, Jason D.
异戊二烯环氧二醇（IEPOX）是由异戊二烯在低nox条件下光氧化形成的，最近根据质谱证据被提出作为二次有机气溶胶（SOA）的前体。在本研究中，我们以高纯度（约99%）合成了ipox异构体，并通过一系列受控暗室研究和反应产物分析，研究了它们通过反应摄取形成SOA的潜力。IEPOX衍生的SOA基本上只在酸性气溶胶存在下观察到，β-IEPOX的保守下限产率为4.7-6.4%，δ-IEPOX为3.4-5.5%，这为IEPOX异构体是异戊二烯SOA的前体提供了直接证据。这些室内研究表明，IEPOX的摄取解释了在环境气溶胶中发现的已知异戊二烯SOA示踪剂的形成，包括2-甲基四醇、c5 -烯三醇、二聚体和IEPOX衍生的有机硫酸盐。此外，我们发现酸化硫酸盐气溶胶上的反应性吸收支持了先前未报道的酸催化ipox在颗粒相中对顺式和反式3-甲基四氢呋喃-3,4-二醇（3- methf -3,4-二醇）的分子内重排。通过气溶胶质谱（AMS）对这些新型示踪化合物的分析表明，它们有助于AMS有机气溶胶光谱的正矩阵分解（PMF），这些光谱来自受酸性气溶胶存在影响的低氮氧化物、异戊二烯主导的区域。
Isoprene epoxydiols (IEPOX), formed from the photooxidation of isoprene under low-NOx conditions, have recently been proposed as precursors of secondary organic aerosol (SOA) on the basis of mass spectrometric evidence. In the present study, IEPOX isomers were synthesized in high purity (> 99%) to investigate their potential to form SOA via reactive uptake in a series of controlled dark chamber studies followed by reaction product analyses. IEPOX-derived SOA was substantially observed only in the presence of acidic aerosols, with conservative lower-bound yields of 4.7–6.4% for β-IEPOX and 3.4–5.5% for δ-IEPOX, providing direct evidence for IEPOX isomers as precursors to isoprene SOA. These chamber studies demonstrate that IEPOX uptake explains the formation of known isoprene SOA tracers found in ambient aerosols, including 2-methyltetrols, C5-alkene triols, dimers, and IEPOX-derived organosulfates. Additionally, we show reactive uptake on the acidified sulfate aerosols supports a previously unreported acid-catalyzed intramolecular rearrangement of IEPOX to cis- and trans-3-methyltetrahydrofuran-3,4-diols (3-MeTHF-3,4-diols) in the particle phase. Analysis of these novel tracer compounds by aerosol mass spectrometry (AMS) suggests that they contribute to a unique factor resolved from positive matrix factorization (PMF) of AMS organic aerosol spectra collected from low-NOx, isoprene-dominated regions influenced by the presence of acidic aerosols.
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影响因子：
11.4
作者：
Kroll, JH;Ng, NL;Seinfeld, JH
通讯作者：
Seinfeld, JH
影响因子：
11.4
作者：
Chan, Man Nin;Surratt, Jason D.;Seinfeld, John H.
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Seinfeld, John H.
影响因子：
11.4
作者：
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Elrod, Matthew J.
影响因子：
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影响因子：
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作者：
Slowik, J. G.;Brook, J.;Abbatt, J. P. D.
通讯作者：
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