Criegee intermediate-hydrogen sulfide chemistry at the air/water interface

被引：49

作者：

Kumar, Manoj ^{[1
]}

Zhong, Jie ^{[1
]}

Francisco, Joseph S. ^{[1
]}

Zeng, Xiao C. ^{[1
,2
]}

机构：

[1] Univ Nebraska, Dept Chem, Lincoln, NE 68588 USA

[2] Beijing Univ Chem Technol, Beijing Adv Innovat Ctr Soft Matter Sci & Engn, Beijing 100029, Peoples R China

来源：

CHEMICAL SCIENCE | 2017年 / 8卷 / 08期

基金：

美国国家科学基金会;

关键词：

OZONOLYSIS; REACTIVITY; MECHANISM; SURFACE; SULFUR; GAS;

D O I：

10.1039/c7sc01797a

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

We carry out Born-Oppenheimer molecular dynamic simulations to show that the reaction between the smallest Criegee intermediate, CH2OO, and hydrogen sulfide (H2S) at the air/water interface can be observed within few picoseconds. The reaction follows both concerted and stepwise mechanisms with former being the dominant reaction pathway. The concerted reaction proceeds with or without the involvement of one or two nearby water molecules. An important implication of the simulation results is that the Criegee-H2S reaction can provide a novel non-photochemical pathway for the formation of a C-S linkage in clouds and could be a new oxidation pathway for H2S in terrestrial, geothermal and volcanic regions.

引用

页码：5385 / 5391

页数：7

共 46 条

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