Single-Atom-Embedded Nitrogen-Doped Graphene as Efficient Electrocatalysts for the CO2 Reduction Reaction

Single-atom catalysts (SACs) have displayed unprecedented activity and selectivity for electrochemical CO2 reduction reaction (CO2RR). Herein, a series of metal single atoms embedded on nitrogen-doped graphene (M–N4G, where M = In, Tl, Ge, Sn, Pb, Sb, and Bi) is systematically evaluated as CO2RR electrocatalysts by density functional theory (DFT) calculations. The computational results show that most M–N4G exhibit better CO2RR selectivity over the hydrogen evolution reaction (HER). Ge/Pb–N4G exhibits excellent electrocatalytic performance in the generation of HCOOH from the CO2RR with low limiting potentials of −0.292 and −0.306 eV, which surpass the performance of the vast majority of electrocatalysts. Adsorption energy of the key intermediate *HCOO can be used as an effective reactivity reaction descriptor to screen promising CO2RR catalysts. The results of this work highlight M–N4G as an ideal electrochemical for the electrocatalytic CO2RR.