Theoretical studies of atmospheric reaction mechanisms in the troposphere.
Theoretical studies of atmospheric reaction mechanisms in the troposphere.
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DOI：
10.1039/c2cs35070j
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发表时间：
2012-09
影响因子：
46.2
通讯作者：
L. Vereecken;J. S. Francisco
中科院分区：
文献类型：
--
作者：
L. Vereecken;J. S. Francisco
大气的化学性质包含了大量的反应，这些反应作用于过多的中间产物。这些反应，顺序和平行发生，产生相互交织和不可简化的机制，描述了大气中有机和无机化合物的复杂化学变化。这个系统的复杂性在于，它需要结合实验，理论和建模方法来阐明各个反应的特征，以及它们之间的相互作用。在这篇综述中，我们描述了最近的结果，从量子化学和理论动力学研究相关的大气化学。本文首先总结了最常用的理论方法。然后，它检查的VOC氧化引发通道的OH，O（3），NO（3）和Cl，随后的反应的烷基，烷氧基，烷基过氧和Criegee中间体在随后的氧化步骤中的活性。具体的系统，如芳烃的氧化和VOC氧化中OH再生的知识现状也进行了讨论，以及一些无机反应。
The chemistry of the atmosphere encompasses a vast number of reactions acting on a plethora of intermediates. These reactions, occurring sequentially and in parallel, give rise to intertwined and irreducible mechanisms describing the complex chemical transformations of organic and inorganic compounds in the atmosphere. The complexity of this system is that it requires combined experimental, theoretical, and modeling approaches to elucidate the characteristics of the individual reactions, and their mutual interaction. In this review, we describe recent results from quantum chemical and theoretical kinetic studies of relevance to atmospheric chemistry. The review first summarizes the most commonly used theoretical methodologies. It then examines the VOC oxidation initiation channels by OH, O(3), NO(3) and Cl, followed by the reactions of the alkyl, alkoxy, alkylperoxy and Criegee intermediates active in the subsequent oxidation steps. Specific systems such as the oxidation of aromatics and the current state of knowledge on OH-regeneration in VOC oxidation are also discussed, as well as some inorganic reactions.