Abstract

AbstractThe 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.

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