Electrochemical reduction of CO2 to value-added chemicals and fuels shows great promise in contributing to reducing the energy crisis and environment problems. This progress has been slowed by a lack of stable, efficient and selective catalysts. In this paper, density functional theory (DFT) was used to study the catalytic performance of the first transition metal series anchored TM-Bβ12 monolayers as catalysts for electrochemical reduction of CO2. The results show that the TM-Bβ12 monolayer structure has excellent catalytic stability and electrocatalytic selectivity. The primary reduction product of Sc-Bβ12 is CO and the overpotential is 0.45 V. The primary reduction product of the remaining metals (Ti-Zn) is CH4, where Fe-Bβ12 has the minimum overpotential of 0.45 V. Therefore, these new catalytic materials are exciting. Furthermore, the underlying reaction mechanisms of CO2 reduction via the TM-Bβ12 monolayers have been revealed. This work will shed insights on both experimental and theoretical studies of electroreduction of CO2.
Bibliographical noteFunding Information:
J.–H. L. and L.-M. Y. gratefully acknowledge support from the National Natural Science Foundation of China (21673087 and 21873032), Startup Fund (2006013118 and 3004013105) from Huazhong University of Science and Technology, and the Fundamental Research Funds for the Central Universities (2019kfyRCPY116). The authors thank the Minnesota Supercomputing Institute (MSI) at the University of Minnesota for supercomputing resources.
© The Royal Society of Chemistry 2019.