Ru Nanocrystals with Shape-Dependent Surface-Enhanced Raman Spectra and Catalytic Properties: Controlled Synthesis and DFT Calculations.

Despite its multidisciplinary interests and technological importance the shape control of Ru nanocrystals still remains a great challenge. In this article we demonstrated a facile hydrothermal approach toward the controlled synthesis of Ru nanocrystals with the assistance of first-principles calcula...

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Publicado en:Journal of the American Chemical Society Vol. 134; no. 50; pp. 20479 - 20490
Autores principales: An-Xiang Yin, Wen-Chi Liu, Jun Ke, Wei Zhu, Jun Gu, Ya-Wen Zhang, Chun-Hua Yan
Formato: Artículo
Publicado: American Chemical Society 12/19/2012
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Acceso en línea:Ver este registro en EBSCOhost
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      dt: 12/19/2012
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        atl: Ru Nanocrystals with Shape-Dependent Surface-Enhanced Raman Spectra and Catalytic Properties: Controlled Synthesis and DFT Calculations.
      aug:
        au:
          An-Xiang Yin
          Wen-Chi Liu
          Jun Ke
          Wei Zhu
          Jun Gu
          Ya-Wen Zhang
          Chun-Hua Yan
        affil: Beijing National Laboratory for Molecular Sciences State Key Laboratory of Rare Earth Materials Chemistry and Applications PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry College of Chemistry and Molecular Engineering Peking University Beijing 100871 China
      su:
        Nanocrystals spectra
        Ruthenium catalyst synthesis
        Surface enhanced Raman effect
        Density functionals
        Molecular shapes
        Carbon monoxide
        Catalyst selectivity
      sug:
        subj:
          Nanocrystals spectra
          Ruthenium catalyst synthesis
          Surface enhanced Raman effect
          Density functionals
          Molecular shapes
          Carbon monoxide
          Catalyst selectivity
      ab: Despite its multidisciplinary interests and technological importance the shape control of Ru nanocrystals still remains a great challenge. In this article we demonstrated a facile hydrothermal approach toward the controlled synthesis of Ru nanocrystals with the assistance of first-principles calculations. For the first time Ru triangular and irregular nanoplates as well as capped columns with tunable sizes were prepared with high shape selectivity. In consistency with the experimental observations and density functional theory (DFT) calculations confirmed that both the intrinsic characteristics of Ru crystals and the adsorption of certain reaction species were responsible for the shape control of Ru nanocrystals. Ultrathin Ru nanoplates exposed a large portion of (0001) facets due to the lower surface energy of Ru(0001). The selective adsorption of oxalate species on Ru(10-10) would retard the growth of the side planes of the Ru nanocrystals while the gradual thermolysis of the oxalate species would eliminate their adsorption effects leading to the shape evolution of Ru nanocrystals from prisms to capped columns. The surface-enhanced Raman spectra (SERS) signals of these Ru nanocrystals with 4-mercaptopyridine as molecular probes showed an enhancement sequence of capped columns > triangle nanoplates > nanospheres probably due to the sharp corners and edges in the capped columns and nanoplates as well as the shrunk interparticle distance in their assemblies. CO-selective methanation tests on these Ru nanocrystals indicated that the nanoplates and nanospheres had comparable activities but the former has much better CO selectivity than the latter.
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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