f‐p‐d Gradient Orbital Coupling Induced Spin State Enhancement of Atomic Fe Sites for Efficient and Stable Oxygen Reduction Reaction

Abstract Advancing energy conversion technologies requires cost‐efficient electrocatalysts for the oxygen reduction reaction (ORR). Iron phthalocyanine (FePc) emerges as a scalable and economical ORR electrocatalyst. However, the Fe–N 4 configuration in FePc still falls short of the satisfied ORR activity and stability under electrocatalytic conditions. Here, an effective f‐p‐d (Eu–O–Fe) gradient orbital coupling strategy is introduced by integrating FePc with Eu 2 O 3 (FePc/Eu 2 O 3 ) to enhance the spin state and ORR performance of the Fe center through a precisely designed, scalable synthetic approach. The Eu─O bond promotes electron delocalization and shifts the spin state of Fe center from low‐spin to…

• NS
  Natural Science Foundation of Shanghai

  Award: 22ZR1429700
• NN
  National Natural Science Foundation of China

  Awards: 52304332, 52274302