Preprint Article Version 1 Preserved in Portico This version is not peer-reviewed

Regulation of Bimetallic Coordination Centers in MOF Catalyst for Electrochemical CO2 Reduction to Formate

Version 1 : Received: 21 August 2023 / Approved: 22 August 2023 / Online: 22 August 2023 (16:10:41 CEST)

A peer-reviewed article of this Preprint also exists.

Yang, R.; Huang, Q.; Sha, X.; Gao, B.; Peng, J. Regulation of Bimetallic Coordination Centers in MOF Catalyst for Electrochemical CO2 Reduction to Formate. Int. J. Mol. Sci. 2023, 24, 13838. Yang, R.; Huang, Q.; Sha, X.; Gao, B.; Peng, J. Regulation of Bimetallic Coordination Centers in MOF Catalyst for Electrochemical CO2 Reduction to Formate. Int. J. Mol. Sci. 2023, 24, 13838.

Abstract

Electrocatalytic reduction of CO2 to valuable chemicals can alleviate the energy crisis, and solve the greenhouse effect. The key is to develop non-noble metal electrocatalysts with high activity, selectivity and stability. Herein, bimetallic MOF materials (BiZn-MOF, BiSn-MOF and BiIn-MOF) were constructed by coordinating the P-zone transition metals Zn, In, Sn and Bi with the organic ligand 3-amino-1H-1,2,4-triazole-5-carboxylic acid (H2atzc) through a rapid microwave synthesis approach. The coordination centers in bimetallic MOF Catalyst were regulated to optimize the catalytic performance to CO2RR. The optimized catalyst BiZn-MOF exhibited high catalytic activity than those of Bi-MOF, BiSn-MOF and BiIn-MOF. The BiZn-MOF exhibited a higher selectivity for formate production with a Faradic efficiency (FE=92%) at a potential of -0.9 V (vs. RHE) with a current density of 13 mA/cm2. The current density maintained for 13 h continuous electrolysis. The electrochemical conversion of CO2 to formic acid mainly follows the *OCHO pathway. The good catalytic performance of BiZn-MOF may be attributed to the Bi-Zn bimetallic coordination centers in the MOF, which can reduce the binding energies of the reaction intermediates by tuning the electronic structure and atomic arrangement. This study provides a feasible strategy for performance optimization of bismuth-based catalysts.

Keywords

electrocatalysis; carbon dioxide; formic acid; coordination centers; bimetallic

Subject

Chemistry and Materials Science, Electrochemistry

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