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Zusammenfassung:
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−Ox
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 (ΔEonset= 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−2mg(M)−1 over the MnIII−Ox single-layer.
