Journal
NANO-MICRO LETTERS
Volume 14, Issue 1, Pages -Publisher
SHANGHAI JIAO TONG UNIV PRESS
DOI: 10.1007/s40820-021-00772-7
Keywords
CO2 reduction; Bismuth; Proton transport; Electron localization; Boron
Funding
- Shanghai Jiao Tong University
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In this study, boron atoms are introduced to modify the local electronic structure of bismuth, enabling high activity and selectivity for the conversion of CO2 into formate. The effects of boron on the reaction mechanism and its concentration-dependent modulation of catalytic properties are revealed through experimental and computational investigations. This study provides in-depth mechanistic insights at the atomic level and offers an effective strategy for the rational design of highly active and selective electrocatalysts for efficient CO2 conversion.
Electrochemical reduction of CO2 to formate is economically attractive but improving the reaction selectivity and activity remains challenging. Herein, we introduce boron (B) atoms to modify the local electronic structure of bismuth with positive valence sites for boosting conversion of CO2 into formate with high activity and selectivity in a wide potential window. By combining experimental and computational investigations, our study indicates that B dopant differentiates the proton participations of rate-determining steps in CO2 reduction and in the competing hydrogen evolution. By comparing the experimental observations with the density functional theory, the dominant mechanistic pathway of B promoted formate generation and the B concentration modulated effects on the catalytic property of Bi are unravelled. This comprehensive study offers deep mechanistic insights into the reaction pathway at an atomic and molecular level and provides an effective strategy for the rational design of highly active and selective electrocatalysts for efficient CO2 conversion.
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