Oxygen Electrocatalysis at MnIII–Ox–C Hybrid Heterojunction: An Electronic Synergy or Cooperative Catalysis?

Autor: Rui Huang, Xin Tan, Ling-Yun Jang, Ian R. Gentle, Xing Huang, Dang Sheng Su, Peter Kappen, Hassan A. Tahini, Dawei Wang, Sean C. Smith, Kuang-Hsu Wu, Wei Qi, Rose Amal, Yuxiao Ding
Rok vydání: 2018
Předmět:
Zdroj: ACS Applied Materials & Interfaces. 11:706-713
ISSN: 1944-8252
1944-8244
DOI: 10.1021/acsami.8b16325
Popis: 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.
Databáze: OpenAIRE