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

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Ding,  Yuxiao
Research Department Schlögl, Max Planck Institute for Chemical Energy Conversion, Max Planck Society;

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Citation

Wu, K.-H., Huang, X., Tahini, H., Kappen, P., Huang, R., Tan, X., et al. (2019). Oxygen Electrocatalysis at Mn-III-O-x-C Hybrid Heterojunction: An Electronic Synergy or Cooperative Catalysis? ACS Applied Materials and Interfaces, 11(1), 706-713. doi:10.1021/acsami.8b16325.


Cite as: https://hdl.handle.net/21.11116/0000-0006-795F-9
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 Mn-III-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 (Delta E-onset = 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 Mn-III-O-x single-layer.