The Effect of the Coordination Environment of Atomically Dispersed Fe and N Co‐doped Carbon Nanosheets on CO2 Electroreduction

Abstract

AbstractSingle‐atom metal and nitrogen co‐doped carbon catalysts have caused an extensive research boom for electrochemical CO2 reduction reaction (CO2RR). The diversity of metal‐N coordination environment at high temperature limits the accurate study of electrocatalytic active sites. In this work, Fe porphyrin is anchored on a nitrogen‐doped graphene substrate through the coordination between Fe and N atoms to form atomically dispersed Fe and N co‐doped graphene nanosheets. The confinement anchoring effect of the nitrogen‐doped graphene substrate prevents Fe atoms from agglomerating into Fe nanoparticles. Apart from that, the different Fe‐N coordination environments and their catalytic effects on CO2RR are investigated by temperature changes. Electrochemical tests and density functional theory (DFT) calculations indicate that the atomically dispersed saturated Fe‐N coordination catalyst have excellent performance for CO2RR and the Faradaic efficiency towards CO can up to 97 % at a potential of −0.5 V (vs. reversible hydrogen electrode, RHE).