Mo2CS2-MXene supported single-atom catalysts for efficient and selective CO2 electrochemical reduction

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@Mo2CS2 (TM = Fe, Co, Ni, Cu, Ru. Rh, Pd, Ag, Os, Ir, Pt, and Au) anchored SACs for CO2 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 Mo2CS2 surface. Possible different reaction pathways to produce various C1 products such as CO, HCOOH, HCHO, CH3OH, and CH4 have been investigated for Fe, Co, Ni, and Ru supported SACs. Among the SACs investigated, Fe, Co, and Ru supported by Mo2CS2 catalysts selectively produce CH4, whereas Ru@Mo2CS2 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 Mo2CS2 surface for a single-atom catalyst for selective CO2 reduction and other electrochemical applications.