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Kinetically Controlled Synthesis of Rhodium Nanocrystals with Different Shapes and a Comparison Study of Their Thermal and Catalytic Properties

  • Ming Zhao
    Ming Zhao
    School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
    More by Ming Zhao
  • Zitao Chen
    Zitao Chen
    The Wallace H. Coulter Department of Biomedical Engineering, Georgia Institute of Technology and Emory University, Atlanta, Georgia 30332, United States
    More by Zitao Chen
  • Yifeng Shi
    Yifeng Shi
    School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
    More by Yifeng Shi
  • Zachary D. Hood
    Zachary D. Hood
    School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
    Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • Zhiheng Lyu
    Zhiheng Lyu
    School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
    More by Zhiheng Lyu
  • Minghao Xie
    Minghao Xie
    School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
    More by Minghao Xie
  • Miaofang Chi
    Miaofang Chi
    Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
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  • , and 
  • Younan Xia*
    Younan Xia
    School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
    School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
    The Wallace H. Coulter Department of Biomedical Engineering, Georgia Institute of Technology and Emory University, Atlanta, Georgia 30332, United States
    *Email: [email protected]
    More by Younan Xia
Cite this: J. Am. Chem. Soc. 2021, 143, 16, 6293–6302
Publication Date (Web):April 14, 2021
https://doi.org/10.1021/jacs.1c02734
Copyright © 2021 American Chemical Society

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    Abstract

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    We report the synthesis of Rh nanocrystals with different shapes by controlling the kinetics involved in the growth of preformed Rh cubic seeds. Specifically, Rh nanocrystals with cubic, cuboctahedral, and octahedral shapes can all be obtained from the same cubic seeds under suitable reduction kinetics for the precursor. The success of such a synthesis also relies on the use of a halide-free precursor to avoid oxidative etching, as well as the involvement of a sufficiently high temperature to remove Br ions from the seeds while ensuring adequate surface diffusion. The availability of Rh nanocrystals with cubic and octahedral shapes allows for an evaluation of the facet dependences of their thermal and catalytic properties. The data from in situ electron microscopy studies indicate that the cubic and octahedral Rh nanocrystals can keep their original shapes up to 700 and 500 °C, respectively. When tested as catalysts for hydrazine decomposition, the octahedral nanocrystals exhibit almost 4-fold enhancement in terms of H2 selectivity relative to the cubic counterpart. As for ethanol oxidation, the order is reversed, with the cubic nanocrystals being about three times more active than the octahedral sample.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.1c02734.

    • TEM images and XPS data of Rh cubic seeds and Rh nanocrystals prepared under different experimental conditions are provided. XRD pattern of the Rh octahedra prepared using the standard protocol is also included (PDF)

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