Anchoring Single Copper Atoms to Microporous Carbon Spheres as High-Performance Electrocatalyst for Oxygen Reduction Reaction |
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| Authors: | Lingbo Zong Kaicai Fan Weicui Wu Lixiu Cui Lili Zhang Bernt Johannessen Dongchen Qi Huajie Yin Yun Wang Porun Liu Lei Wang Huijun Zhao |
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| Affiliation: | 1. Key Laboratory of Eco-chemical Engineering, Key Laboratory of Optic-Electric Sensing and Analytical Chemistry of Life Science, Taishan Scholar Advantage and Characteristic Discipline Team of Eco-Chemical Process and Technology, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao, 266042 China;2. Centre for Catalysis and Clean Energy, School of Environment and Science, Griffith University, Queensland, 4222 Australia;3. Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, 110016 China;4. Australian Synchrotron, Australia's Nuclear Science and Technology Organisation, Victoria, 3168 Australia;5. Centre for Materials Science, School of Chemistry and Physics, Queensland University of Technology, Queensland, 4001 Australia |
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| Abstract: | Although the carbon-supported single-atom (SA) electrocatalysts (SAECs) have emerged as a new form of highly efficient oxygen reduction reaction (ORR) electrocatalysts, the preferable sites of carbon support for anchoring SAs are somewhat elusive. Here, a KOH activation approach is reported to create abundant defects/vacancies on the porous graphitic carbon nanosphere (CNS) with selective adsorption capability toward transition-metal (TM) ions and innovatively utilize the created defects/vacancies to controllably anchor TM–SAs on the activated CNS via TM Nx coordination bonds. The synthesized TM-based SAECs (TM-SAs@N-CNS, TM: Cu, Fe, Co, and Ni) possess superior ORR electrocatalytic activities. The Cu-SAs@N-CNS demonstrates excellent ORR and oxygen evolution reaction (OER) bifunctional electrocatalytic activities and is successfully applied as a highly efficient air cathode material for the Zn–air battery. Importantly, it is proposed and validated that the N-terminated vacancies on graphitic carbons are the preferable sites to anchor Cu-SAs via a Cu (N C2)3(N C) coordination configuration with an excellent promotional effect toward ORR. This synthetic approach exemplifies the expediency of suitable defects/vacancies creation for the fabrication of high-performance TM-based SAECs, which can be implemented for the synthesis of other carbon-supported SAECs. |
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| Keywords: | carbon vacancy oxygen reduction reaction porous carbon rechargeable Zn–air batteries single-atom catalysts |
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