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Controlled Synthesis of Nanosized Palladium icosahedra and Their Catalytic Activity towards Formic-Acid Oxidation

Authors

  • Tian Lv,

    1. The Wallace H. Coulter Department of Biomedical Engineering, Georgia Institute of Technology and Emory University, School of Chemistry & Biochemistry and School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia, 30332 (USA)
    2. Engineering Research Center for Nanophotonics and Advanced Instruments, Ministry of Education, Department of Physics, East China Normal University, Shanghai 200062 (PR China)
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    • These two authors contributed equally to this work.

  • Yi Wang,

    1. The Wallace H. Coulter Department of Biomedical Engineering, Georgia Institute of Technology and Emory University, School of Chemistry & Biochemistry and School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia, 30332 (USA)
    2. Education Ministry Key Laboratory on Luminescence and Real-Time Analysis, School of Chemistry and Chemical Engineering, Southwest University, Chongqing 400715 (PR China)
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    • These two authors contributed equally to this work.

  • Dr. Sang-Il Choi,

    1. The Wallace H. Coulter Department of Biomedical Engineering, Georgia Institute of Technology and Emory University, School of Chemistry & Biochemistry and School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia, 30332 (USA)
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  • Dr. Miaofang Chi,

    1. Materials Science and Technology Division, Oak Ridge National Laboratory (ORNL), Oak Ridge, Tennessee 37830 (USA)
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  • Dr. Jing Tao,

    1. Condensed Matter Physics and Materials Science Department, Brookhaven National Laboratory (BNL), Upton, New York 11973 (USA)
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  • Prof. Likun Pan,

    1. Engineering Research Center for Nanophotonics and Advanced Instruments, Ministry of Education, Department of Physics, East China Normal University, Shanghai 200062 (PR China)
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  • Prof. Cheng Zhi Huang,

    1. Education Ministry Key Laboratory on Luminescence and Real-Time Analysis, School of Chemistry and Chemical Engineering, Southwest University, Chongqing 400715 (PR China)
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  • Dr. Yimei Zhu,

    1. Condensed Matter Physics and Materials Science Department, Brookhaven National Laboratory (BNL), Upton, New York 11973 (USA)
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  • Prof. Younan Xia

    Corresponding author
    1. The Wallace H. Coulter Department of Biomedical Engineering, Georgia Institute of Technology and Emory University, School of Chemistry & Biochemistry and School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia, 30332 (USA)
    • The Wallace H. Coulter Department of Biomedical Engineering, Georgia Institute of Technology and Emory University, School of Chemistry & Biochemistry and School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia, 30332 (USA)

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Abstract

Pd icosahedra with sizes controlled in the range of 5–35 nm were synthesized in high purity through a combination of polyol reduction and seed-mediated growth. The Pd icosahedra were obtained with purity >94 % and uniform sizes controlled in the range of 5–17 nm by using ethylene glycol as both the reductant and solvent. The studies indicate that the formation of Pd nanocrystals with an icosahedral shape was very sensitive to the reaction kinetics. The success of this synthesis relies on the use of HCl to manipulate the reaction kinetics and thus control the twin structure and shape of the resultant nanocrystals. The size of the Pd icosahedra could be further increased up to 35 nm by seed-mediated growth, with 17 nm Pd icosahedra serving as seeds. The multiply twinned Pd icosahedra could grow into larger sizes, and their shape and multiply twinned structure were preserved. Thanks to the presence of twin defects, the Pd icosahedra showed a catalytic current density towards formic-acid oxidation that was 1.9 and 11.6 times higher than that of single-crystal Pd octahedra, which were also fully covered by {111} facets, and commercial Pd/C, respectively.

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