Why Do Weak-Binding M–N–C Single-Atom Catalysts Possess Anomalously High Oxygen Reduction Activity?

Single-atom catalysts (SACs) with metal–nitrogen–carbon (M–N–C) structures are widely recognized as promising candidates in oxygen reduction reactions (ORR). According to the classical Sabatier principle, optimal 3d metal catalysts, such as Fe/Co–N–C, achieve superior catalytic performance due to the moderate binding strength. However, the substantial ORR activity demonstrated by weakly binding M–N–C catalysts such as Ni/Cu–N–C challenges current understandings, emphasizing the need to explore new underlying mechanisms. In this work, we integrated a pH-field coupled microkinetic model with detailed experimental electron state analyses to verify a novel key step in the ORR reaction pathway of weak-binding…

• NC
  National Computational Infrastructure
• HF
  Hirose Foundation
• UO
  University of Sydney
• NN
  National Natural Science Foundation of China

  Award: 22309109
• SJ
  Shanghai Jiao Tong University
• AC
  Australian Centre for Microscopy and Microanalysis, University of Sydney
• AR
  Australian Research Council

  Award: FT210100218
• JS
  Japan Society for the Promotion of Science

  Awards: JP24K23068, JP23K13703
• IF
  Institute for Materials Research, Tohoku University
• NC
  National Cancer Institute
• DO
  Division of Materials Research