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Research Article

Structural revolution of atomically dispersed Mn sites dictates oxygen reduction performance

Zhengkun Yang1,3,§( ), Xiaolin Wang2,§, Mengzhao Zhu1,§, Xinyan Leng3, Wenxing Chen4, Wenyu Wang1, Qian Xu5, Li-Ming Yang2( ), Yuen Wu1( )
School of Chemistry and Materials Science, iChEM, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei 230026, China
Hubei Key Laboratory of Bioinorganic Chemistry and Materia Medica; Key Laboratory of Material Chemistry for Energy Conversion and Storage, Ministry of Education; Hubei Key Laboratory of Materials Chemistry and Service Failure; Hubei Engineering Research Center for Biomaterials and Medical Protective Materials; School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan 430074, China
Institutes of Physical Science and Information Technology, Key Laboratory of Structure and Functional Regulation of Hybrid Materials (Anhui University), Ministry of Education, Anhui Graphene Engineering Laboratory, Anhui University, Hefei 230601, China
Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China
National Synchrotron Radiation Laboratory (NSRL), Hefei 230026, China

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Abstract

An efficient preparation and local coordination environment regulation of isolated single-atom sites catalysts (ISASC) for improved activity is still challenging. Herein, we develop a solid phase thermal diffusion strategy to synthesize Mn ISASC on highly uniform nitrogen-doped carbon nanotubes by employing MnO2 nanowires@ZIF-8 core-shell structure. Under high-temperature, the Mn species break free from core-MnO2 lattice, which will be trapped by carbon defects derived from shell-ZIF-8 carbonization, and immobilized within carbon substrate. Furthermore, the poly-dispersed Mn sites with two nitrogen-coordinated centers can be controllably renovated into four-nitrogen-coordinated Mn sites using NH3 treatment technology. Both experimental and computational investigations indicate that the symmetric coordinated Mn sites manifest outstanding oxygen reduction activity and superior stability in alkaline and acidic solutions. This work not only provides efficient way to regulate the coordination structure of ISASC to improve catalytic performance but also paves the way to reveal its significant promise for commercial application.

Keywords

thermal diffusioncoordination repairingsingle-atom manganeseoxygen reduction catalysisfuel cells

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Nano Research
Volume 14 Issue 12,
December 2021
Pages 4512-4519
DOI: 10.1007/s12274-021-3823-z
Cite this article:
Yang Z, Wang X, Zhu M, et al. Structural revolution of atomically dispersed Mn sites dictates oxygen reduction performance. Nano Research, 2021, 14(12): 4512-4519. https://doi.org/10.1007/s12274-021-3823-z
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Received: 14 July 2021
Revised: 13 August 2021
Accepted: 16 August 2021
Published: 16 September 2021
© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021
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