Quantifying Asymmetric Coordination to Correlate with Oxygen Reduction Activity in Fe‐Based Single‐Atom Catalysts

Abstract Precisely manipulating asymmetric coordination configurations and examining electronic effects enable to tunethe intrinsic oxygen reduction reaction (ORR) activity of single‐atom catalysts (SACs). However, the lackof a definite relationship between coordination asymmetry and catalytic activity makes the rational design of SACs ambiguous. Here, we propose a concept of “asymmetry degree” to quantify asymmetric coordination configurations and assess the effectiveness of active moieties in Fe‐based SACs. A theoretical framework is established, elucidating the volcanic relationship between asymmetry degree and ORR activity by constructing a series of Fe‐based SAC models doped with non‐metal atoms (B, P, S,…

• NN
  National Natural Science Foundation of China

  Awards: 52422314, 52231008, U23A20687
• AS
  Austrian Science Fund

  Awards: 10.55776/COE5, I4434N, 10.55776/I4434-N, 55776/COE5