Achieving Free‐Electron Transfer Reversal and dz 2 ‐Orbital Occupancy Modulation on Core‐shell NiS@Au Cocatalysts for Highly Selective H 2 O 2 Photosynthesis

Abstract Spontaneous free‐electron migration usually occurs on the interface between host photocatalysts and cocatalysts, but the influences of the charge transfer direction on the two‐electron oxygen reduction reaction (2e − ‐ORR) of cocatalysts have not been taken seriously. Herein, an innovative electron‐transfer reversal is proposed to direct the free‐electron transfer in a way that enables highly selective 2e − ‐ORR on Au cocatalysts. To this end, metallic Au nanoparticles are originally loaded on NiS particles to fabricate novel core–shell NiS@Au cocatalysts on g‐C 3 N 4 surface by a directional photodeposition procedure. XAS spectra and DFT calculations disclose that the intergrated NiS induces a…

• NN
  National Natural Science Foundation of China

  Awards: 22402126, U22A20147, 22272110, 22178224
• BA
  Basic and Applied Basic Research Foundation of Guangdong Province

  Award: 2023A1515110535