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    Universal Approach to Fabricating Graphene-Supported Single-Atom Catalysts from Doped ZnO Solid Solutions

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    Author
    Meng, J; Li, J; Liu, J; Zhang, X; Jiang, G; Ma, L; Hu, ZY; Xi, S; Zhao, Y; Yan, M; ...
    Date
    2020-08-26
    Source Title
    ACS Central Science
    Publisher
    American Chemical Society
    University of Melbourne Author/s
    Liu, Zhe; Wang, Peiyao
    Affiliation
    Mechanical Engineering
    Metadata
    Show full item record
    Document Type
    Journal Article
    Citations
    Meng, J., Li, J., Liu, J., Zhang, X., Jiang, G., Ma, L., Hu, Z. Y., Xi, S., Zhao, Y., Yan, M., Wang, P., Liu, X., Li, Q., Liu, J. Z., Wu, T. & Mai, L. (2020). Universal Approach to Fabricating Graphene-Supported Single-Atom Catalysts from Doped ZnO Solid Solutions. ACS Central Science, 6 (8), pp.1431-1440. https://doi.org/10.1021/acscentsci.0c00458.
    Access Status
    Access this item via the Open Access location
    URI
    http://hdl.handle.net/11343/254234
    DOI
    10.1021/acscentsci.0c00458
    Open Access URL
    http://doi.org/10.1021/acscentsci.0c00458
    Abstract
    Single-atom catalysts (SACs) have attracted widespread interest for many catalytic applications because of their distinguishing properties. However, general and scalable synthesis of efficient SACs remains significantly challenging, which limits their applications. Here we report an efficient and universal approach to fabricating a series of high-content metal atoms anchored into hollow nitrogen-doped graphene frameworks (M-N-Grs; M represents Fe, Co, Ni, Cu, etc.) at gram-scale. The highly compatible doped ZnO templates, acting as the dispersants of targeted metal heteroatoms, can react with the incoming gaseous organic ligands to form doped metal-organic framework thin shells, whose composition determines the heteroatom species and contents in M-N-Grs. We achieved over 1.2 atom % (5.85 wt %) metal loading content, superior oxygen reduction activity over commercial Pt/C catalyst, and a very high diffusion-limiting current (6.82 mA cm-2). Both experimental analyses and theoretical calculations reveal the oxygen reduction activity sequence of M-N-Grs. Additionally, the superior performance in Fe-N-Gr is mainly attributed to its unique electron structure, rich exposed active sites, and robust hollow framework. This synthesis strategy will stimulate the rapid development of SACs for diverse energy-related fields.

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