期刊论文

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

中文

南华大学学报(自然科学版)

1673-0062

2013

27

1

78-82

10.19431/j.cnki.1673-0062.2013.01.018

本校为第一机构

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 tak...