Doping and pretreatment optimized the adsorption of *OCHO on bismuth for the electrocatalytic reduction of CO2 to formate

Meng Tian; Shanshan Wu; Yang Hu; Zhaori Mu; Zhi Li; Yichao Hou; Pinxian Xi; Chun-Hua Yan

doi:10.1039/d2nr06638f

Doping and pretreatment optimized the adsorption of *OCHO on bismuth for the electrocatalytic reduction of CO₂ to formate

Nanoscale. 2023 Mar 2;15(9):4477-4487. doi: 10.1039/d2nr06638f.

Authors

Meng Tian¹, Shanshan Wu¹, Yang Hu¹, Zhaori Mu¹, Zhi Li¹, Yichao Hou¹, Pinxian Xi¹, Chun-Hua Yan^{1

2}

Affiliations

¹ State Key Laboratory of Applied Organic Chemistry, Frontiers Science Center for Rare Isotopes, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, China. xipx@lzu.edu.cn.
² Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials Chemistry and Applications, PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, College of Chemistry and Molecular Engineering Peking University, Beijing 100871, China.

PMID: 36752707
DOI: 10.1039/d2nr06638f

Abstract

Electrocatalytic reduction of CO₂ to formate is considered as a promising method to achieve carbon neutrality, and the introduction of heteroatoms is an effective strategy to improve the catalytic activity and selectivity of catalysts. However, the structural reconstruction behavior of catalysts driven by voltage is usually ignored. Therefore, we used Cu/Bi₂S₃ as a model to reveal the dynamic reduction process in different atmospheric environments. The catalyst showed an outstanding faradaic efficiency of 94% for formate and a long-term stability of 100 h, and exhibited a high current density of 280 mA cm^-2 in a flow cell. The experimental results and theoretical calculations show that the introduction of copper enhances the adsorption of CO₂, accelerates the charge transfer and reduces the formation barrier of *OCHO, thus promoting the formation of formate. This work draws attention to the effects of saturated gases in the electrolyte during structural evolution and provides a possibility for designing catalysts with high catalytic activity.