A rational design of manganese electrocatalysts for Lewis acid-assisted carbon dioxide reduction

文献情報

出版日 2019-03-30

DOI 10.1039/C9CP00514E

インパクトファクター 3.676

著者

Xiaoli Wang, Haiyan Ma, Caiyun Meng, Dezhan Chen, Fang Huang

原文を見る

要旨

Herein, the mechanisms of Brønsted acid- and Lewis acid-assisted CO2 electroreduction by Mn(mesbpy)(CO)3Br (1) were investigated by density functional theory calculations. Our results indicate that for the Lewis acid-assisted cycle, an energy sink (13) is present owing to the interaction between Mg(OTf)2 and activated CO2, which is disadvantageous to the apparent activation energy (ΔG≠). Moreover, a series of substituted 13 counterparts were investigated to reduce the energy sink and decrease ΔG≠. Based on our study on the substituent effect, an excellent linear relationship was found between 2e reduction potentials and LUMO energies of substituted 1, and a moderate linear relationship was observed between ΔG of substituted 13 and the 2e reduction potential of substituted 1 counterparts. Moreover, for the CO2 reduction assisted by a Lewis acid, the formyl-substituted complex R8 has been predicted to be a more effective catalyst with lower overpotential and higher catalytic activity than its parent complex 1.

掲載誌

Physical Chemistry Chemical Physics

CiteScore: 5.5

自己引用率: 10.3%

年間論文数: 3036

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