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  • Coordination of Atomic Co-Pt Coupling Species at Carbon Defects as Active Sites for Oxygen Reduction Reaction

    Author(s)
    Zhang, Longzhou
    Fischer, Julia Melisande Theresa Agatha
    Jia, Yi
    Yan, Xuechen
    Xu, Wei
    Wang, Xiyang
    Chen, Jun
    Yang, Dongjiang
    Liu, Hongwei
    Zhuang, Linzhou
    Hanke, Marlies
    Searles, Debra J
    Huang, Keke
    Feng, Shouhua
    Brown, Christopher L
    Yao, Xiangdong
    Griffith University Author(s)
    Yan, Xuecheng
    Jia, Yi
    Year published
    2018
    Metadata
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    Abstract
    Platinum (Pt) is the state-of-the-art catalyst for oxygen reduction reaction (ORR), but its high cost and scarcity limit its large-scale use. However, if the usage of Pt reduces to a sufficiently low level, this critical barrier may be overcome. Atomically dispersed metal catalysts with high activity and high atom efficiency have the possibility to achieve this goal. Herein, we report a locally distributed atomic Pt-Co nitrogen–carbon-based catalyst (denoted as A-CoPt-NC) with high activity and robust durability for ORR (267 times higher than commercial Pt/C in mass activity). The A-CoPt-NC shows a high selectivity for the ...
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    Platinum (Pt) is the state-of-the-art catalyst for oxygen reduction reaction (ORR), but its high cost and scarcity limit its large-scale use. However, if the usage of Pt reduces to a sufficiently low level, this critical barrier may be overcome. Atomically dispersed metal catalysts with high activity and high atom efficiency have the possibility to achieve this goal. Herein, we report a locally distributed atomic Pt-Co nitrogen–carbon-based catalyst (denoted as A-CoPt-NC) with high activity and robust durability for ORR (267 times higher than commercial Pt/C in mass activity). The A-CoPt-NC shows a high selectivity for the 4e– pathway in ORR, differing from the reported 2e– pathway characteristic of atomic Pt catalysts. Density functional theory calculations suggest that this high activity originates from the synergistic effect of atomic Pt-Co located on a defected C/N graphene surface. The mechanism is thought to arise from asymmetry in the electron distribution around the Pt/Co metal centers, as well as the metal atoms’ coordination with local environments on the carbon surface. This coordination results from N8V4 vacancies (where N8 represents the number of nitrogen atoms and V4 indicates the number of vacant carbon atoms) within the carbon shell, which enhances the oxygen reduction reaction via the so-called synergistic effect.
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    Journal Title
    Journal of the American Chemical Society
    Volume
    140
    Issue
    34
    DOI
    https://doi.org/10.1021/jacs.8b04647
    Subject
    Chemical sciences
    Other chemical sciences not elsewhere classified
    Publication URI
    http://hdl.handle.net/10072/384271
    Collection
    • Journal articles

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