Atomically Dispersed Metal–Nitrogen–Carbon Catalysts with d -Orbital Electronic Configuration-Dependent Selectivity for Electrochemical CO 2 -to-CO Reduction

A variety of atomically dispersed transition-metal-anchored nitrogen-doped carbon (M–N–C) electrocatalysts have shown encouraging electrochemical CO2 reduction reaction (CO2RR) performance, with the underlying fundamentals of central transition-metal atom determined CO2RR activity and selectivity yet remaining unclear. Herein, a universal impregnation-acid leaching method was exploited to synthesize various M–N–C (M: Fe, Co, Ni, and Cu) single-atom catalysts (SACs), which revealed d-orbital electronic configuration-dependent activity and selectivity toward CO2RR for CO production. Notably, Ni–N–C exhibits a very high CO Faradaic efficiency (FE) of 97% at −0.65 V versus RHE and above 90% CO selectivity in the…

• NN
  National Natural Science Foundation of China

  Awards: 52225606, 51888103, 52142604
• NS
  Natural Science Foundation of Shaanxi Province

  Award: 2019JCW-10
• QX
  Qian Xuesen Laboratory for Space Technology, China Aerospace Science and Technology Corporation

  Award: TKTSPY-2020-02-01
• FR
  Fundamental Research Funds for the Central Universities