Engineering 3d–2p–4f Gradient Orbital Coupling to Enhance Electrocatalytic Oxygen Reduction

Abstract The development of highly efficient and economical materials for the oxygen reduction reaction (ORR) plays a key role in practical energy conversion technologies. However, the intrinsic scaling relations exert thermodynamic inhibition on realizing highly active ORR electrocatalysts. Herein, a novel and feasible gradient orbital coupling strategy for tuning the ORR performance through the construction of Co 3d‐O 2p‐Eu 4f unit sites on the Eu 2 O 3 –Co model is proposed. Through the gradient orbital coupling, the pristine ionic property between Eu and O atoms is assigned with increased covalency, which optimizes the e g occupancy of Co sites, and weakens the OO bond, thus ultimately breaking the…

• NN
  National Natural Science Foundation of China

  Awards: 22109073, 22072067
• NS
  Natural Science Foundation of Jiangsu Province

  Award: BK20221321
• PA
  Priority Academic Program Development of Jiangsu Higher Education Institutions