A density functional theory study on the mechanism of Dimethyl ether carbonylation over heteropolyacids catalyst

大纲

摘要
关键词

化学科学与工程前沿（英文）

2021年第15卷第2期页码 319-329

A density functional theory study on the mechanism of Dimethyl ether carbonylation over heteropolyacids catalyst

展示更多

10.1007/s11705-020-1957-2

引用这篇文章

摘要

Dimethyl ether (DME) carbonylation is considered as a key step for a promising route to produce ethanol from syngas. Heteropolyacids (HPAs) are proved to be efficient catalysts for DME carbonylation. In this work, the reaction mechanism of DME carbonylation was studied theoretically by using density functional theory calculations on two typical HPA models (HPW, HSiW). The whole process consists of three stages: DME dissociative adsorption, insertion of CO into methoxyl group and formation of product methyl acetate. The activation barriers of all possible elementary steps, especially two possible paths for CO insertion were calculated to obtain the most favorable reaction mechanism and rate-limiting step. Furthermore, the effect of the acid strength of Brønsted acid sites on reactivity was studied by comparing the activation barriers over HPW and HSiW with different acid strength, which was determined by calculating the deprotonation energy, Mulliken population analyses and adsorption energies of pyridine.

关键词

dimethyl ether ; carbonylation ; mechanism ; heteropolyacids ; density functional theory

上一篇本期文章

本期文章下一篇

阅读量

下载量

大纲

Figures(5)

标签(1)

其他(2)

化学科学与工程前沿（英文）

A density functional theory study on the mechanism of Dimethyl ether carbonylation over heteropolyacids catalyst

摘要

关键词

评论

大纲

Figures(5)

标签(1)

其他(2)

化学科学与工程前沿（英文）

A density functional theory study on the mechanism of Dimethyl ether carbonylation over heteropolyacids catalyst

摘要

关键词

评论

相关研究