Rational design of graphdiyne-based single-atom catalysts for electrochemical CO2 reduction reaction

Graphdiyne (GDY) has achieved great success in the application of two-dimensional carbon materials in recent years due to its excellent electrochemical catalytic capacity. Considering the unique electronic structure of GDY, transition metal (TM₁) (TM = Fe, Ru, Os, Co, Rh, Ir) single-atom catalysts (SACs) with isolated loading on GDY were designed for electrochemical CO₂ reduction reaction (CO₂RR) with density functional theoretical (DFT) calculations. The charge density difference and projected densities of states have been systematically calculated. The mechanism of electrochemical catalysis and the reaction pathway of CO₂RR over Os₁/GDY catalysts have also been investigated and high catalytic activity was found for the generation of methane. The calculated results provide a theoretical basis for the design of efficient GDY-based SACs for electrochemical CO₂RR.