4.8 Article

Epitaxially Grown Heterostructured SrMn3O6-x-SrMnO3 with High-Valence Mn3+/4+ for Improved Oxygen Reduction Catalysis

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 40, Pages 22043-22050

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202109207

Keywords

heterostructures; perovskites; oxygen reduction reaction; zinc-air batteries

Funding

  1. Natural Science Foundation of China [21875048]
  2. Outstanding Youth Project of Guangdong Natural Science Foundation [2020B1515020028]
  3. Yangcheng Scholars Research Project of Guangzhou [201831820]
  4. Science and Technology Research Project of Guangzhou [202002010007]
  5. Basic Innovation Project of Guangzhou University [2020GDJC-M07]
  6. MacDiarmid Institute for Advanced Materials and Nanotechnology

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The study developed a SrMn3O6-x-SrMnO3 (SMOx-SMO) heterostructure catalyst through epitaxial growth, showing excellent electrocatalyst performance for the oxygen reduction reaction (ORR). The formation of high-valence Mn3+/4+ promoted a positive shift in the d-band center, optimizing the catalytic activity at the heterojunction surface. Applied as an air-electrode catalyst in a rechargeable zinc-air battery, SMOx-SMO demonstrated high output voltage and power density, with cycling stability superior to Pt/C-IrO2 air-electrode catalysts.
Heterostructured catalysts show outstanding performance in electrochemical reactions owing to their beneficial interfacial properties. However, the rational design of heterostructured catalysts with the desired interfacial properties and charge-transfer characteristics is challenging. Herein, we developed a SrMn3O6-x-SrMnO3 (SMOx-SMO) heterostructure through epitaxial growth, which demonstrated excellent electrocatalyst performance for the oxygen reduction reaction (ORR). The formation of high-valence Mn3+/4+ is beneficial for promoting a positive shift in the position of the d-band center, thereby optimizing the adsorption and desorption of ORR intermediates on the heterojunction surface and resulting in improved catalytic activity. When SMOx-SMO was applied as an air-electrode catalyst in a rechargeable zinc-air battery, a high output voltage and power density was achieved, with performance comparable to a battery prepared with Pt/C-IrO2 air-electrode catalysts, albeit with much better cycling stability.

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