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  • Few-layer graphdiyne doped with sp-hybridized nitrogen atoms at acetylenic sites for oxygen reduction electrocatalysis

    Author(s)
    Zhao, Yasong
    Wan, Jiawei
    Yao, Huiying
    Zhang, Lijuan
    Lin, Kaifeng
    Wang, Lei
    Yang, Nailiang
    Liu, Daobin
    Song, Li
    Zhu, Jia
    Gu, Lin
    Liu, Lei
    Zhao, Huijun
    Li, Yuliang
    Wang, Dan
    Griffith University Author(s)
    Zhao, Huijun
    Wang, Dan
    Year published
    2018
    Metadata
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    Abstract
    The oxygen reduction reaction (ORR) is a fundamental reaction for energy storage and conversion. It has mainly relied on platinum-based electrocatalysts, but the chemical doping of carbon-based materials has proven to be a promising strategy for preparing metal-free alternatives. Nitrogen doping in particular provides a diverse range of nitrogen forms. Here, we introduce a new form of nitrogen doping moieties —sp-hybridized nitrogen (sp-N) atoms into chemically defined sites of ultrathin graphdiyne, through pericyclic replacement of the acetylene groups. The as-prepared sp-N-doped graphdiyne catalyst exhibits overall good ...
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    The oxygen reduction reaction (ORR) is a fundamental reaction for energy storage and conversion. It has mainly relied on platinum-based electrocatalysts, but the chemical doping of carbon-based materials has proven to be a promising strategy for preparing metal-free alternatives. Nitrogen doping in particular provides a diverse range of nitrogen forms. Here, we introduce a new form of nitrogen doping moieties —sp-hybridized nitrogen (sp-N) atoms into chemically defined sites of ultrathin graphdiyne, through pericyclic replacement of the acetylene groups. The as-prepared sp-N-doped graphdiyne catalyst exhibits overall good ORR performance, in particular with regards to peak potential, half-wave potential and current density. Under alkaline conditions it was comparable to commercial Pt/C, and showed more rapid kinetics. And although its performances are a bit lower than those of Pt/C in acidic media they surpass those of other metal-free materials. Taken together, experimental data and density functional theory calculations suggest that the high catalytic activity originates from the sp-N dopant, which facilitates O2 adsorption and electron transfer on the surface of the catalyst. This incorporation of chemically defined sp-N atoms provides a new synthetic route to high-performance carbon-based and other metal-free catalysts.
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    Journal Title
    Nature Chemistry
    Volume
    10
    DOI
    https://doi.org/10.1038/s41557-018-0100-1
    Subject
    Chemical Sciences not elsewhere classified
    Chemical Sciences
    Publication URI
    http://hdl.handle.net/10072/382064
    Collection
    • Journal articles

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