The Role of Reducible Oxide–Metal Cluster Charge Transfer in Catalytic Processes: New Insights on the Catalytic Mechanism of CO Oxidation on Au/TiO from ab Initio Molecular Dynamics.
To probe metal particle/reducible oxide interactions density functional theory based ab initio molecular dynamics studies were performed on a prototypical metal cluster (Au) supported on reducible oxides (rutile TiO(110)) to implicitly account for finite temperature effects and the role of excess su...
| Publicado en: | Journal of the American Chemical Society Vol. 135; no. 29; pp. 10673 - 10684 |
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| Autores principales: | , , , , |
| Formato: | Artículo |
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American Chemical Society
7/24/2013
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| Materias: | |
| Acceso en línea: | Ver este registro en EBSCOhost |
| fields | @attributes: recordID: 1 pdfLink: plink: https://search.ebscohost.com/login.aspx?direct=true&db=hlh&AN=89597003&site=ehost-live header: @attributes: shortDbName: hlh uiTerm: 89597003 longDbName: Humanities International Complete uiTag: AN controlInfo: bkinfo: jinfo: jid: 00027863 ACS jtl: Journal of the American Chemical Society issn: 00027863 maglogo: N pubinfo: dt: 7/24/2013 vid: 135 iid: 29 pid: 997 pub: American Chemical Society artinfo: ui: 89597003 10.1021/ja402063v ppf: 10673 ppct: 11 formats: tig: atl: The Role of Reducible Oxide–Metal Cluster Charge Transfer in Catalytic Processes: New Insights on the Catalytic Mechanism of CO Oxidation on Au/TiO from ab Initio Molecular Dynamics. aug: au: Yang-Gang Wang Yeohoon Yoon Glezakou, Vassiliki-Alexandra Jun Li Rousseau, Roger affil: Department of Chemistry, Tsinghua University, Beijing, 100084, China Institute for Interfacial Catalysis, Pacific Northwest National Laboratory, Richland, Washington 99352, United States su: Metal clusters Oxidation of carbon monoxide Molecular dynamics Density functional theory Charge transfer Catalytic activity Gold clusters Titanium dioxide films sug: subj: Metal clusters Oxidation of carbon monoxide Molecular dynamics Density functional theory Charge transfer Catalytic activity Gold clusters Titanium dioxide films ab: To probe metal particle/reducible oxide interactions density functional theory based ab initio molecular dynamics studies were performed on a prototypical metal cluster (Au) supported on reducible oxides (rutile TiO(110)) to implicitly account for finite temperature effects and the role of excess surface charge in the metal oxide. It is found that the charge state of the Au particle is negative in a reducing chemical environment whereas in the presence of oxidizing species coadsorbed to the oxide surface the cluster obtained a net positive charge. In the context of the well-known CO oxidation reaction, charge transfer facilitates the plasticization of Au, which allows for a strong adsorbate induced surface reconstruction upon addition of CO leading to the formation of mobile Au–CO species on the surface. The charging/discharging of the cluster during the catalytic cycle of CO oxidation enhances and controls the amount of O adsorbed at oxide/cluster interface and strongly influences the energetics of all redox steps in catalytic conversions. A detailed comparison of the current findings with previous studies is presented, and generalities about the role of surface-adsorbate charge transfer for metal cluster/reducible oxide interactions are discussed. pubtype: Academic Journal doctype: Article src: R language: English refInfo: copyright: @attributes: flag: Y dt: @attributes: year: 2013 holdings: @attributes: islocal: N |
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