Revealing the Potential-Dependent Rate-Determining Step of Oxygen Reduction Reaction on Single-Atom Catalysts

Single-atom catalysts (SACs) have attracted widespread attention due to their potential to replace platinum-based catalysts in achieving efficient oxygen reduction reaction (ORR), yet the rational optimization of SACs remains challenging due to their elusive reaction mechanisms. Herein, by employing ab initio molecular dynamics simulations and a thermodynamic integration method, we have constructed the potential-dependent free energetics of ORR on a single iron atom catalyst dispersed on nitrogen-doped graphene (Fe–N4/C) and further integrated these parameters into a microkinetic model. We demonstrate that the rate-determining step (RDS) of the ORR on SACs is potential-dependent rather than invariant within…

• GP
  Guangdong Provincial Key Laboratory Of Catalysis

  Award: 2020B121201002
• NK
  National Key Research and Development Program of China

  Award: 2023YFA1509004