期刊
ACS CATALYSIS
卷 10, 期 1, 页码 743-750出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.9b04043
关键词
CO2 reduction; Electrocatalyst; Bismuth oxide; Formate; Rate-determining
资金
- Fundamental Research Funds for the Central Universities [2018KFYXKJC044, 2018KFYYXJJ121, 2017KFXKJC002, 2017KFYXJJ164]
- National 1000 Young Talents Program of China
- WNLO of HUST
Electrochemical conversion of carbon dioxide (CO2) into high-value chemical products has become a dramatic research area because of the efficient exploitation of carbon resources and simultaneous reduction of atmospheric CO2 concentration. Herein, we report the bismuth-based catalyst in the efficient electroconversion of CO2 for the formation of formate with a maximum Faradaic efficiency of 91% and partial current density of similar to 8 mA cm(-2) at -0.9 V vs RHE. Experimental and theoretical results show that the bismuth-oxygen structure of bismuth oxides is beneficial for a higher adsorption of CO2 and the rate-determining route switching from the initial fast pre-equilibrium of electron transfer process to the subsequent hydrogenation step, accompanied by a lower free energy of intermediate. This work may offer valuable insights into crystal structure engineering to achieve efficient electrocatalysts for selective CO2 reduction toward generation of valuable products.
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