Perspective on Theoretical Models for CO2 Electrochemical Reduction

The electrochemical reduction of CO2 (CO2RR) is a promising alternative to achieve carbon neutrality and the sustainable development of human civilization. Rational design of electrocatalysts for CO2RR requires thorough understanding of catalytically active sites and corresponding reaction mechanisms from the atomic level, where theoretical computations and simulations are indispensable. In this perspective, we summarize the recent progress in simulating CO2RR from both thermodynamic and kinetic aspects, including different methods for describing solvent–ion effects and applied potentials. In addition, a brief overview of applications of machine learning (ML) to the design of CO2RR catalysts is presented, and the simulation of electrocatalytic processes is also discussed, considering the solvent model under a constant potential by ML. Finally, an outlook is provided for the future development of computational models and their applications to CO2RR.