Study on syngas methanation mechanism over Ni4/MCM-41 catalyst based on density functional theory

IF 2.1 4区 化学 Q3 CHEMISTRY, PHYSICAL
Jiaying Zhang
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引用次数: 1

Abstract

The density functional theory method is employed to systematically explore the mechanism of syngas methanation on the Ni4/MCM-41 catalyst surface. The calculation results show that the optimal pathway of CH4 formation is CO + H → CHO + H → CH2O + H → CH3O → CH3 + H → CH4 with the rate-determining step of CH3O direct dissociation. Because the activation energy for the direct dissociation of CH3O species is much lower than that for the CH3OH formation (198.6 vs 264.8 kJ mol−1), there is almost no by-product CH3OH that appeared in the products of the syngas methanation over the Ni4/MCM-41 catalyst. Compared with other conventional nickel-based methanation catalysts, Ni4/MCM-41 catalyst is an excellent methanation catalyst with high selectivity of CH4.
基于密度泛函理论的Ni4/MCM-41催化剂合成气甲烷化机理研究
采用密度泛函理论方法对Ni4/MCM-41催化剂表面合成气甲烷化机理进行了系统探讨。计算结果表明,CH4的最佳生成途径为CO + H→CHO + H→CH2O + H→ch30→CH3 + H→CH4,其中ch30直接解离为决定速率的步骤。由于在Ni4/MCM-41催化剂上合成气甲烷化反应的产物中,ch30直接解离的活化能远低于CH3OH生成的活化能(198.6 vs 264.8 kJ mol−1),因此几乎没有副产物CH3OH出现。与其他传统镍基甲烷化催化剂相比,Ni4/MCM-41催化剂具有较高的CH4选择性,是一种优异的甲烷化催化剂。
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来源期刊
CiteScore
2.10
自引率
0.00%
发文量
5
审稿时长
2.3 months
期刊介绍: The journal covers the fields of kinetics and mechanisms of chemical processes in the gas phase and solution of both simple and complex systems.
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