A Nanocomposite of Bismuth Clusters and Bi2O2CO3 Sheets for Highly Efficient Electrocatalytic Reduction of CO2 to Formate

• Published in: Angewandte Chemie International Edition Vol. 62; no. 3
• Main Authors: Lin, Li, He, Xiaoyang, Zhang, Xia‐Guang, Ma, Wenchao, Zhang, Biao, Wei, Diye, Xie, Shunji, Zhang, Qinghong, Yi, Xiaodong, Wang, Ye
• Format: Journal Article
• Language: English
• Published: Weinheim Wiley Subscription Services, Inc 16.01.2023
• Edition: International ed. in English
• Subjects: Bismuth; Carbon dioxide; Carbon Dioxide Reduction; Catalysts; Chemical reduction; Clusters; Current density; Electrochemistry; Energy conversion; Energy conversion efficiency; Formic Acid; Heterogeneous Catalysis; Nanocomposites; Selectivity
• DOI: 10.1002/anie.202214959
• ISSN: 1433-7851

The renewable‐electricity‐driven CO2 reduction to formic acid would contribute to establishing a carbon‐neutral society. The current catalyst suffers from limited activity and stability under high selectivity and the ambiguous nature of active sites. Herein, we report a powerful Bi2S3‐derived catalyst that demonstrates a current density of 2.0 A cm−2 with a formate Faradaic efficiency of 93 % at −0.95 V versus the reversible hydrogen electrode. The energy conversion efficiency and single‐pass yield of formate reach 80 % and 67 %, respectively, and the durability reaches 100 h at an industrial‐relevant current density. Pure formic acid with a concentration of 3.5 mol L−1 has been produced continuously. Our operando spectroscopic and theoretical studies reveal the dynamic evolution of the catalyst into a nanocomposite composed of Bi0 clusters and Bi2O2CO3 nanosheets and the pivotal role of Bi0−Bi2O2CO3 interface in CO2 activation and conversion. An electrocatalyst derived from Bi2S3 is very powerful for the reduction of CO2 to formic acid, achieving a current density of 2.0 A cm−2 with a formate Faradaic efficiency of 93 % and a single‐pass formate yield of 67 %. The active catalyst is composed of Bi nanoclusters on Bi2O2CO3 nanosheets and the interfacial Bi site plays a pivotal role.