Synergistic effect between transition metal single atom and SnS2 toward deep CO2 reduction.

The electrochemical reduction of CO2 is an efficient channel to facilitate energy conversion, but the rapid design and rational screening of high-performance catalysts remain a great challenge. In this work, we investigated the relationships between the configuration, energy, and electronic properties of SnS2 loaded with transition metal single atom (TM@SnS2) and analyzed the mechanism of CO2 activation and reduction by using density functional theory. The "charge transfer bridge" promoted the adsorption of CO2 on TM@SnS2, thus enhancing the binding of HCOOH∗ to the catalyst for further hydrogenation and reduction to high-value CH4. The research revealed that the binding free energy of COOH∗ on TM@SnS2 formed a "volcano curve" with the limiting potential of CO2 reduction to CH4, and the TM@SnS2 (TM = Cr, Ru, Os, and Pt) at the "volcano top" exhibited a high CH4 activity.