| Abstract Scope |
It is of great importance to advance the sustainable technology that converts CO2 into fuels and value-added chemicals via cost-effective electrocatalysis. Transition metal (TM=Fe, Co, or Ni) and nitrogen (N) doped nano-carbon (denoted as TM-N-C) catalysts have been demonstrated to be capable of catalyzing CO2 reduction (CO2RR) to CO with a reasonable activity and amazingly high selectivity. For a rational design of these TM-N-C catalysts, we have performed density functional theory (DFT) calculations to investigate CO2RR on various TM-N4 active sites (TM = Fe, Co, Ni). Specifically, three different TM-N4 moieties were studied, such as the TM-N4 moiety embedded in the graphene basal plane, the porphyrin-like moiety and/or the TM-N4 moiety bridging the edges of two adjacent graphene layers. Our DFT calculations predicted that the CO2RR could happen at the proposed active sites under an electrode potential more positive than that for competing hydrogen evolution reaction. |