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

Single-atom catalysts (SACs) have displayed unprecedented activity and selectivity for electrochemical CO reduction reaction (CORR). Herein, a series of metal single atoms embedded on nitrogen-doped graphene (M-NG, where M = In, Tl, Ge, Sn, Pb, Sb, and Bi) is systematically evaluated as CORR electrocatalysts by density functional theory (DFT) calculations. The computational results show that most M-NG exhibit better CORR selectivity over the hydrogen evolution reaction (HER). Ge/Pb-NG exhibits excellent electrocatalytic performance in the generation of HCOOH from the CORR with low limiting potentials of -0.292 and -0.306 V, 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 CORR catalysts. The results of this work highlight M-NG as an ideal electrochemical for the electrocatalytic CORR.