Oxygen Electrocatalysis at Mn III -O x -C Hybrid Heterojunction: An Electronic Synergy or Cooperative Catalysis? Academic Article uri icon

abstract

  • The interface at the metal oxide-carbon hybrid heterojunction is the source to the well-known "synergistic effect" in catalysis. Understanding the structure-function properties is key for designing more advanced catalyst-support systems. Using a model MnIII-O x single-layer catalyst on carbon, we herein report a full elucidation to the catalytic synergism at the hybrid heterojunction in the oxygen reduction reaction (ORR). The successful fabrication of the single-layer catalyst from bottom-up is fully characterized by the X-ray absorption fine structure and high-resolution transmission electron microscopy. For oxygen electrocatalysis over this model hybrid heterostructure, our results, from both theory and experiment, show that the synergistic ORR truly undergoes a cooperated two-step electrocatalysis with catalytic promotion (Δ Eonset = 60 mV) near the heterojunction and over the single-layer catalyst through an interfacial electronic interplay, rather than an abstruse transition towards a one-step dissociative pathway. Finally, we report a superior peroxide-reducing activity of 432.5 mA cm-2 mg(M)-1 over the MnIII-O x single-layer.

authors

  • Wu, KH
  • Huang, X
  • Tahini, H
  • Kappen, Peter
  • Huang, R
  • Tan, X
  • Jang, LY
  • Ding, Y
  • Smith, SC
  • Qi, W
  • Gentle, IR
  • Su, DS
  • Amal, R
  • Wang, DW

publication date

  • 2019