Electrochemical Reduction of CO₂ via Single-Atom Catalysts Supported on -In₂Se₃

In this work, the electrochemical CO2 reductionreaction (CO2RR) over transition metal and & alpha;-In2Se3 monolayer catalysts was investigated by densityfunctional theory (DFT) and an effective screening medium method-referenceinteraction site model (ESM-RISM). On the basis of the scaling relationshipbetween the adsorption free energies of intermediates, we constructedthe relationships between oxygen-bound intermediates with *O and carbon-boundintermediates with *CHO. The calculation results indicate that *OCHOintermediates are more favorable for the first hydrogenation of CO2 on M@In2Se3 catalysts; thus, the adsorptionenergy of oxygen-bound species determines the catalytic performanceof M@In2Se3. The Co@In2Se3 & DARR;-C was predicted to be the most promising catalyst with alow limiting potential of -0.385 V as determined by the computationalhydrogen electrode method. Constant potential calculations also demonstratethat the M@In2Se3 catalysts hold great potentialfor highly efficient CO2RR. This work provides a fundamentalunderstanding for the rational design of ferroelectric single-atomcatalysts for the purpose of highly efficient electrocatalytic CO2 reduction.