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

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Abstract

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.

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

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Publication details

The article was received on 26 Jan 2019, accepted on 29 Mar 2019 and first published on 30 Mar 2019


Article type: Paper
DOI: 10.1039/C9CP00514E
Citation: Phys. Chem. Chem. Phys., 2019, Advance Article

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

    X. Wang, H. Ma, C. Meng, D. Chen and F. Huang, Phys. Chem. Chem. Phys., 2019, Advance Article , DOI: 10.1039/C9CP00514E

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