Abstract： To study the reaction mechanism between CaS and SO₂ in desulfurization reaction, stable molecular configurations of reactants, intermediates, transition state, and products were optimized at the 6-311G++ (d, p) level, using the B3LYP method in density functional theory, and the corresponding energy values of them were obtained. The results show that the reaction of SO₂ and CaS forms chain intermediate IM1 firstly, then transient state TS is generated by S and O atoms forming chemical bond. Intermediates IM_2,IM₃ and IM₄ are generated through molecular rearrangement and energy configuration of TS, product CaSO₄and sulfur are finally generated. The energy barrier of intermediate IM₄ to product P₁ is the greatest, which shows that it is the rate-determining step.

Keywords: desulfurization reaction; reaction mechanism; density functional theory; quantum chemistry

中图分类号：TB99      文献标志码：A

文章编号：1008-5548（2015）04-0053-04

DOI:10.13732/j.issn.1008-5548.2015.04.012

收稿日期：2014-12-11， 修回日期：2014-12-24，在线出版时间：2015-08-26。

基金项目：国家自然科学基金项目，编号：51106077；(北京化工大学)化工资源有效利用国家重点实验室开放基金项目， 编号：CRE-2013-C-302； 山东省优秀中青年科学家科研奖励基 金 项 目 ， 编 号 ：BS2011NJ007。

第一作者简介：张聪（1989—），男，硕士研究生，研究方向为烟气脱硫脱硝。 E-mail: zhangcong0424@126.com。