镍基催化上甲烷部分氧化反应机理的量化计算  

Theoretical Investigation of the Partial Oxidation Reactions Mechanism of Methane over Nickel

作　　者：龙威[1] 周昕[1] 罗虹[1] 邓昌爱[1] 

机构地区：[1]南华大学化学化工学院,湖南衡阳421001

出　　处：《南华大学学报（自然科学版）》2013年第1期78-82,共5页Journal of University of South China：Science and Technology

摘　　要：采用密度泛函(DFT)及二级微扰(MP2)方法,结合混合基组对镍基催化上甲烷部分氧化反应机理进行了研究.计算结果表明,甲烷部分氧化的反应包含六步,其中有两步是副反应,各步的热焓分别为:212.46、-413.46、-69.65、135.28、-94.69、-42.25 kJ/mol.第一步甲烷的逐步脱氢是强吸热的,第五步为生成CO的关键反应且较容易发生,其活化能仅为44.59 kJ/mol.The mechanism of the partical oxidation reaction＇s mechanism of methane based on nickel was investigated by DFT and MP2 methods with mixed basis set. The research showed that on Ni-based catalysts, there were six steps involved in the reaction system and two steps were side reaction. The heats of reaction of the six steps were： 212. 46, -413.46, -69.65,135.28, -94.69, -42.25 kJ/mol. The first step of methane＇s releasing hydrogen atom were endothermic. The fifth critical of coloradb-generation step was easy to take place, and its activation energy was only 44.59 kJ/mol.

关 键 词：甲烷部分氧化 反应机理 量子化学 密度泛函 

分 类 号：O623.11[理学—有机化学]