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Size and Shape-controlled Pd Nanocrystals on ZnO and SiO2: When the Nature of the Support Determines the Active Phase

Authors

  • Dr. Micaela Crespo-Quesada,

    1. Group of Catalytic Reaction Engineering, Ecole Polytechnique Fédérale de Lausanne, 1015 Lausanne (Switzerland)
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  • Dr. Songhak Yoon,

    1. Laboratory for Solid State Chemistry and Catalysis, Swiss Federal Laboratories for Materials Science and Technology, 8600 Dübendorf (Switzerland)
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  • Prof. Mingshang Jin,

    1. Metal Nanomaterials and Catalysis Research Group, Frontier Institute of Science and Technology, 710054 Xi'an (P.R. China)
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  • Prof. Younan Xia,

    1. The Wallace H. Coulter Department of Biomedical Engineering, School of Chemistry and Biochemistry and School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, 30332 Atlanta (USA)
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  • Prof. Anke Weidenkaff,

    1. Laboratory for Solid State Chemistry and Catalysis, Swiss Federal Laboratories for Materials Science and Technology, 8600 Dübendorf (Switzerland)
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  • Prof. Lioubov Kiwi-Minsker

    Corresponding author
    1. Group of Catalytic Reaction Engineering, Ecole Polytechnique Fédérale de Lausanne, 1015 Lausanne (Switzerland)
    • Group of Catalytic Reaction Engineering, Ecole Polytechnique Fédérale de Lausanne, 1015 Lausanne (Switzerland)

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Abstract

The structure sensitivity of acetylene hydrogenation was studied over size-controlled cubic and octahedral Pd nanocrystals (NCs) supported on ZnO and SiO2. Acetylene hydrogenation was found to be structure sensitive [with Pd(1 1 1) in octahedra being more active than Pd(1 0 0) in cubes]. However, the response was found to vary depending on the redox properties of the support. The catalytically active and selective palladium carbide (PdCx) phase was readily formed on the SiO2-supported Pd NCs (much faster on cubes than on octahedra), whereas a markedly less active PdZn phase was preferentially formed on the ZnO-supported Pd nanocrystals. Here we show that the structure sensitivity of a chemical reaction is a complex phenomenon that originates from the reconstruction of the active phase in response to the reactive environment, which is ultimately determined by the support used.

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