Mo2CS2–MXene Supported Single-Atom Catalysts for Efficient and Selective CO2 Electrochemical Reduction

DFT studies were performed for electrochemical reduction of CO 2 to C 1 products using single transition metal supported on Mo 2 CS 2 -MXene. Among the SACs studied, Fe, Co, Ni, and Ru SACs are potential catalysts for CO 2 RR. • Single atom supported on sulfur terminated MXene (Mo 2 CS 2 ) has been investigated for electrochemical conversion of CO 2 . • Binding energy and AIMD results suggest that the single metal atoms tend to occupy the Mo-top site on the Mo 2 CS 2 surface. • Fe, Co, and Ru supported by Mo 2 CS 2 catalysts selectively produce CH 4 and Ni primarily produces HCOOH. Single-atom catalysts (SACs) recently attracted considerable attention in heterogeneous catalysis, owing to high atom-utilization and unique properties. In this paper, we investigated geometry, electronic structure, stabilities, catalytic activity, and selectivity of the various TM@Mo 2 CS 2 (TM = Fe, Co, Ni, Cu, Ru. Rh, Pd, Ag, Os, Ir, Pt, and Au) anchored SACs for CO 2 electrochemical reduction using periodic density functional theory and ab-initio molecular dynamics calculations. The single metal atoms tend to occupy the Mo-top site on the Mo 2 CS 2 surface. Possible different reaction pathways to produce various C 1 products such as CO, HCOOH, HCHO, CH 3 OH, and CH 4 have been investigated for Fe, Co, Ni, and Ru supported SACs. Among the SACs investigated, Fe, Co, and Ru supported by Mo 2 CS 2 catalysts selectively produce CH 4 , whereas Ru@Mo 2 CS 2 has the lowest overpotential of 0.24 V. Ni primarily produces HCOOH with an overpotential is 0.37 V. Therefore, this research demonstrated the significant potential of Mo 2 CS 2 surface for a single-atom catalyst for selective CO 2 reduction and other electrochemical applications.