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Structural revolution of atomically dispersed Mn sites dictates oxygen reduction performance

Nano Research 2021年第12期14卷 4512-4519页

作者： Zhengkun Yang Xiaolin Wang Mengzhao Zhu Xinyan Leng Wenxing Chen Wenyu Wang Qian Xu Li-Ming Yang Yuen Wu School of Chemistry and Materials Science iChEMHefei National Laboratory for Physical Sciences at the MicroscaleUniversity of Science and Technology of ChinaHefei230026China Hubei Key Laboratory of Bioinorganic Chemistry and Materia Medica Key Laboratory of Material Chemistry for Energy Conversion and StorageMinistry of EducationHubei Key Laboratory of Materials Chemistry and Service FailureHubei Engineering Research Center for Biomaterials and Medical Protective MaterialsSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan430074China Institutes of Physical Science and Information Technology Key Laboratory of Structure and Functional Regulation of Hybrid Materials(Anhui University)Ministry of EducationAnhui Graphene Engineering LaboratoryAnhui UniversityHefei230601China Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing100081China National Synchrotron Radiation Laboratory(NSRL) Hefei230026China

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 MnO_(2) nanowires@ZIF-8 core-shell structure.Under high-temperature,the Mn species break free from core-MnO_(2) 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.

关键词： thermal diffusion coordination repairing single-atom manganese oxygen reduction catalysis fuel cells

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