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

Binhao Qin; Yu-Hang Li; Qiao Zhang; Guangxing Yang; Haiyan Wang; Yupeng Zhang; Feng Peng

doi:10.1021/acs.jpclett.1c01920

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 Aug 5;12(30):7151-7158. doi: 10.1021/acs.jpclett.1c01920. Epub 2021 Jul 23.

Authors

Binhao Qin^{1

2

3}, Yu-Hang Li⁴, Qiao Zhang¹, Guangxing Yang³, Haiyan Wang², Yupeng Zhang², Feng Peng¹

Affiliations

¹ School of Chemistry and Chemical Engineering, Guangzhou University, Guangzhou 510006, China.
² China-Ukraine Institute of Welding, Guangdong Academy of Sciences, Guangzhou 510651, China.
³ School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, China.
⁴ School of Chemistry, Sun Yat-sen University, Guangzhou 510275, China.

PMID: 34297571
DOI: 10.1021/acs.jpclett.1c01920

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 (E_f) and dissolution potential (U_diss) 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.