Abstract: Electrochemical reductions of CO2 (ECRR) and N2 (ENRR) can not only reduce CO2 emissions in the air but also make use of N2 and H2O, the most extensive resources on earth, to produce high value-added chemicals, which has become one of the hot research directions. In this study, the formation energy (Ef) and dissolution potential (Udiss) of 96 two-dimensional catalysts derived from different defect sites of monoclinic crystal boron nitride (BN) were calculated, and the catalysts with thermodynamic and electrochemical stability were selected. The suitable catalysts for producing HCOOH (Ga/In@N-BN), CO (Sn@BN), and CH3OH (Co@N-BN) by ECRR and NH3 (Fe@BN) by ENRR were predicated based on a selective calculation method. The results obtained can provide guidance for the design and development of new catalysts for ECRR and ENRR.

Binhao Qin, Yu-Hang Li, Qiao Zhang, Guangxing Yang, Haiyan Wang, Yupeng Zhang, and Feng Peng*. Mechanistic Insights into the Electrochemical Reduction of CO2 and N2 on the Regulation of a Boron Nitride Defect-Derived Two-Dimensional Catalyst using Density Functional Theory Calculations, J. Phys. Chem. Lett. , 2021, 12, 30, 7151–7158.