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    One-Pot Pyrolysis Method to Fabricate Carbon Nanotube Supported Ni Single-Atom Catalysts with Ultrahigh Loading

    90782.pdf (1.525Mb)
    Access Status
    Open access
    Authors
    Zhao, S.
    Cheng, Yi
    Veder, Jean-Pierre
    Johannessen, B.
    Saunders, M.
    Zhang, L.
    Liu, C.
    Chisholm, M.F.
    De Marco, Roland
    Liu, Jian
    Yang, S.Z.
    Jiang, San Ping
    Date
    2018
    Type
    Journal Article
    
    Metadata
    Show full item record
    Citation
    Zhao, S. and Cheng, Y. and Veder, J.P. and Johannessen, B. and Saunders, M. and Zhang, L. and Liu, C. et al. 2018. One-Pot Pyrolysis Method to Fabricate Carbon Nanotube Supported Ni Single-Atom Catalysts with Ultrahigh Loading. ACS Applied Energy Materials. 1 (10): pp. 5286-5297.
    Source Title
    ACS Applied Energy Materials
    DOI
    10.1021/acsaem.8b00903
    ISSN
    2574-0962
    Faculty
    Faculty of Science and Engineering
    School
    WASM: Minerals, Energy and Chemical Engineering
    John de Laeter Centre (JdLC)
    Funding and Sponsorship
    http://purl.org/au-research/grants/arc/DP180100568
    http://purl.org/au-research/grants/arc/DP180100731
    Remarks

    This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Energy Materials, copyright © American Chemical Society, after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acsaem.8b00903.

    URI
    http://hdl.handle.net/20.500.11937/90958
    Collection
    • Curtin Research Publications
    Abstract

    The practical application of single atom catalysts (SACs) is constrained by the low achievable loading of single metal atoms. Here, nickel SACs stabilized on a nitrogen-doped carbon nanotube structure (NiSA-N-CNT) with ultrahigh Ni atomic loading up to 20.3 wt % have been successfully synthesized using a new one-pot pyrolysis method employing Ni acetylacetonate (Ni(acac)2) and dicyandiamide (DCD) as precursors. The yield and formation of NiSA-N-CNT depends strongly on the Ni(acac)2/DCD ratio and annealing temperature. Pyrolysis at 350 and 650 °C led to the formation of Ni single atom dispersed melem and graphitic carbon nitride (Ni-melem and Ni-g-C3N4). Transition from a stacked and layered Ni-g-C3N4 structure to a bamboo-shaped tubular NiSA-N-CNT structure most likely occurs via a solid-to-solid curling or rolling-up mechanism, thermally activated at temperatures of 700-900 °C. Extended X-ray absorption fine structure (EXAFS) experiments and simulations show that Ni single atoms are stabilized in the N-CNT structure through nitrogen coordination, forming a structure with four nearest N coordination shell surrounded by two carbon shells, Ni-N4. The NiSA-N-CNT catalysts show an excellent activity and selectivity for the electrochemical reduction of CO2, achieving a turnover frequency (TOF) of 11.7 s-1 at -0.55 V (vs RHE), but a low activity for the O2 reduction and O2 evolution reactions, as compared to Ni nanoparticles supported on N-CNTs.

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