Chemical evolution of atmospheric organic carbon over multiple generations of oxidation.
Chemical evolution of atmospheric organic carbon over multiple generations of oxidation.
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DOI：
10.1038/s41557-018-0002-2
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发表时间：
2018-04
期刊：
影响因子：
21.8
通讯作者：
Kroll JH
中科院分区：
文献类型：
--
作者：
Isaacman-VanWertz G;Massoli P;O'Brien R;Lim C;Franklin JP;Moss JA;Hunter JF;Nowak JB;Canagaratna MR;Misztal PK;Arata C;Roscioli JR;Herndon ST;Onasch TB;Lambe AT;Jayne JT;Su L;Knopf DA;Goldstein AH;Worsnop DR;Kroll JH
大气有机碳（OC）的演变，因为它经历氧化的关键大气物种，包括颗粒物，臭氧和氧化剂的浓度具有控制性的影响。然而，在数小时至数天的大气处理过程中，OC的完全表征一直受到其极端化学复杂性的阻碍。在这里，我们在实验室中研究α-蒎烯的多代氧化，用几种最先进的分析技术表征产物。虽然一些早期产品的量化仍然难以捉摸，但在实验结束时实现了完全的碳封闭（在测量不确定性范围内）。这些结果提供了新的见解氧化对OC属性（挥发性，氧化态和反应性）和OC的大气生命周期的影响。在以官能化反应和颗粒生长为特征的初始阶段之后，碎片化反应占主导地位，形成较小的物种。经过大约一天的大气老化后，大多数碳被封存在两个长期储存库中，即挥发性氧化气体和低挥发性颗粒物。内容摘要：我们量化和描述了一个高度复杂的不断演变的大气系统中几乎所有的有机碳：a-蒎烯的多代氧化。我们观察到，官能团的初始添加很快让位于裂解反应，有机碳最终被隔离在耐化学性的储层中：有机气溶胶和长寿命的气相物种。
The evolution of atmospheric organic carbon (OC) as it undergoes oxidation has a controlling influence on concentrations of key atmospheric species, including particulate matter, ozone, and oxidants. However, full characterization of OC over hours to days of atmospheric processing has been stymied by its extreme chemical complexity. Here we study the multigenerational oxidation of α-pinene in the laboratory, characterizing products with several state-of-the-art analytical techniques. While quantification of some early-generation products remains elusive, full carbon closure is achieved (within measurement uncertainty) by the end of the experiments. These results provide new insights into the effects of oxidation on OC properties (volatility, oxidation state, and reactivity) and the atmospheric lifecycle of OC. Following an initial period characterized by functionalization reactions and particle growth, fragmentation reactions dominate, forming smaller species. After approximately one day of atmospheric aging, most carbon is sequestered in two long-lived reservoirs, volatile oxidized gases and low-volatility particulate matter. Table of Contents Summary:We quantify and characterize nearly all organic carbon in a highly complex evolving atmospheric system: the multi-generational oxidation of a-pinene. We observe that initial addition of functional groups quickly gives way to fragmentation reactions, with organic carbon ultimately becoming sequestered in chemically-resistant reservoirs: organic aerosol and long-lived gas-phase species.
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影响因子：
2.9
作者：
Kroll, Jesse H.;Lim, Christopher Y.;Wilson, Kevin R.
通讯作者：
Wilson, Kevin R.
影响因子：
3.4
作者：
Daumit, Kelly E.;Kessler, Sean H.;Kroll, Jesse H.
通讯作者：
Kroll, Jesse H.
DOI：
10.1073/pnas.1115186109
发表时间：
2012-08-21
影响因子：
11.1
作者：
Donahue, Neil M.;Henry, Kaytlin M.;Baltensperger, Urs
通讯作者：
Baltensperger, Urs
影响因子：
6.3
作者：
Canagaratna, M. R.;Jimenez, J. L.;Worsnop, D. R.
通讯作者：
Worsnop, D. R.
影响因子：
6.3
作者：
Chan, A. W. H.;Kreisberg, N. M.;Goldstein, A. H.
通讯作者：
Goldstein, A. H.