Tailoring the d‐Orbital Splitting Manner of Single Atomic Sites for Enhanced Oxygen Reduction

Abstract Regulating the electronic states of single atomic sites around the Fermi level remains a major concern for boosting the electrocatalytic oxygen reduction reaction (ORR). Herein, a Fe d‐orbital splitting manner modulation strategy by constructing axial coordination on FeN 4 sites is presented. Experimental investigations and theoretical calculations reveal that the axial tractions induce the distortion of square‐planar field (FeN 4 SP ), up to the quasi‐octahedral coordination (FeN 4 O 1 OC quasi ), thus leading to the electron rearrangement with a diluted spin polarization. The declined population of unpaired electrons in d z 2 , d x z and d yz states engenders a moderate adsorption of ORR…

• NN
  National Natural Science Foundation of China

  Awards: 21905070, 51802059, 22075062, 21673064
• KT
  Key Technology Research and Development Program of Shandong

  Award: 2022CXGC010305
• FR
  Fundamental Research Funds for the Central Universities

  Award: FRFCU5710051922