Substantial Impact of Spin State Evolution in OER/ORR Catalyzed by Fe–N–C

The Fe-embedded N-doped graphene (Fe–N–C) is the most representative single atom catalyst (SAC) that has shown great potentiality in electrocatalysis, such as oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). However, the active moiety of Fe–N–C is still elusive due to contradictory experimental results. Moreover, early simulations mainly focus on the thermodynamic potential of adsorbates, while the effect of spin multiplicity receives little attention. To explore the role of spin multiplicity in electrocatalysis, we employ the constant-potential density functional theory (DFT) to systematically study the structural evolution of the high-spin (HS) and intermediate-spin (IS) FeN4 site (marked…

• NN
  National Natural Science Foundation of China

  Award: 22303039
• NS
  Natural Science Foundation of Jiangsu Province

  Award: BK20220929
• NU
  Nanjing University of Science and Technology

  Award: TSXK2022D002