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克里吉中间体化学与对流层臭氧分解反应的研究前沿

Research frontiers in the chemistry of Criegee intermediates and tropospheric ozonolysis.

作者信息

Taatjes Craig A, Shallcross Dudley E, Percival Carl J

机构信息

Combustion Research Facility, Sandia National Laboratories, Mailstop 9055, Livermore, California, 94551 USA.

出版信息

Phys Chem Chem Phys. 2014 Feb 7;16(5):1704-18. doi: 10.1039/c3cp52842a.

Abstract

The chemistry of carbonyl oxides, known as Criegee intermediates, is central to many aspects of tropospheric chemistry. For decades it has been known that these reactive species, whose electronic structure contains zwitterionic and biradical character, are formed in the ozonolysis of alkenes. However it is only recently that direct measurements of their reaction kinetics have become possible. In this perspective we describe the most recent progress in understanding the reactivity of these historically elusive molecules, explore the atmospheric chemistry implications of new experimental discoveries, and propose important new areas for investigation.

摘要

羰基氧化物(即所谓的克里奇中间体)的化学性质在对流层化学的诸多方面都起着核心作用。几十年来,人们一直知道这些反应性物种在烯烃的臭氧分解过程中形成,其电子结构具有两性离子和双自由基特征。然而,直到最近才有可能直接测量它们的反应动力学。在这篇综述中,我们描述了在理解这些长期以来难以捉摸的分子的反应活性方面的最新进展,探讨了新实验发现对大气化学的影响,并提出了重要的新研究领域。

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