Rational design of graphdiyne-based single-atom catalysts for electrochemical CO 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 (TM) (TM = Fe, Ru, Os, Co, Rh, Ir) single-atom catalysts (SACs) with isolated loading on GDY were designed for electrochemical CO reduction reaction (CORR) 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 CORR over Os/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 CORR.