CO Oxidation Mechanism on CeO-Supported Au Nanoparticles.

Density functional theory was used to study the CO oxidation catalytic activity of CeO-supported Au nanoparticles (NPs). Experimental observations on CeO show that the surface of CeO is enriched with oxygen vacancies. We compare CO oxidation by a Au NP supported on stoichiometric CeO (Au@CeO-STO) an...

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Publicado en:Journal of the American Chemical Society Vol. 134; no. 3; pp. 1560 - 1571
Autores principales: Hyun You Kim, Hyuck Mo Lee, Henkelman, Graeme
Formato: Artículo
Publicado: American Chemical Society 1/25/2012
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Acceso en línea:Ver este registro en EBSCOhost
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      dt: 1/25/2012
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      pub: American Chemical Society
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        10.1021/ja207510v
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        atl: CO Oxidation Mechanism on CeO-Supported Au Nanoparticles.
      aug:
        au:
          Hyun You Kim
          Hyuck Mo Lee
          Henkelman, Graeme
        affil:
          Department of Chemistry and Biochemistry, University of Texas at Austin, Austin, Texas 78712-0165, United States
          Department of Materials Science and Engineering, KAIST, 291 Daehak-ro, Yuseong-gu, Daejeon, Korea
      su:
        Density functionals
        Oxidation of carbon monoxide
        Cerium oxides
        Gold
        Nanoparticles
      sug:
        subj:
          Density functionals
          Oxidation of carbon monoxide
          Cerium oxides
          Gold
          Nanoparticles
      ab: Density functional theory was used to study the CO oxidation catalytic activity of CeO-supported Au nanoparticles (NPs). Experimental observations on CeO show that the surface of CeO is enriched with oxygen vacancies. We compare CO oxidation by a Au NP supported on stoichiometric CeO (Au@CeO-STO) and partially reduced CeO with three vacancies (Au@CeO-3VAC). The structure of the Au NP was chosen to minimize structural rearrangement during CO oxidation. We suggest three CO oxidation mechanisms by Au@CeO: CO oxidation by coadsorbed O, CO oxidation by a lattice oxygen in CeO, and CO oxidation by O bound to a Au-Ce anchoring site. Oxygen vacancies are shown to open a new CO oxidation pathway by O bound to a Au-Ce anchoring site. Our results provide a design strategy for CO oxidation on supported Au catalysts. We suggest lowering the vacancy formation energy of the supporting oxide, and using an easily reducible oxide to increase the concentration of reduced metal ions, which act as anchoring sites for O molecules.
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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