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Au and Pt Remain Unoxidized on a CeO2-Based Catalyst during the Water-Gas Shift Reaction.
Reina, Tomas R; Gonzalez-Castaño, Miriam; Lopez-Flores, Victor; Martínez T, L Marcela; Zitolo, Andrea; Ivanova, Svetlana; Xu, Wenquian; Centeno, Miguel Angel; Rodriguez, Jose A; Odriozola, Jose Antonio.
Afiliación
  • Reina TR; Inorganic Chemistry Department and Materials Science Institute, University of Seville─CSIC, 41092 Sevilla, Spain.
  • Gonzalez-Castaño M; Department of Chemical and Process Engineering, University of Surrey, Guildford GU2 7XH, United Kingdom.
  • Lopez-Flores V; Inorganic Chemistry Department and Materials Science Institute, University of Seville─CSIC, 41092 Sevilla, Spain.
  • Martínez T LM; Inorganic Chemistry Department and Materials Science Institute, University of Seville─CSIC, 41092 Sevilla, Spain.
  • Zitolo A; Synchrotron SOLEIL, L'Orme des Merisiers, B.P. 48, 91192 Gif-sur-Yvette, France.
  • Ivanova S; Inorganic Chemistry Department and Materials Science Institute, University of Seville─CSIC, 41092 Sevilla, Spain.
  • Xu W; Synchrotron SOLEIL, L'Orme des Merisiers, B.P. 48, 91192 Gif-sur-Yvette, France.
  • Centeno MA; Inorganic Chemistry Department and Materials Science Institute, University of Seville─CSIC, 41092 Sevilla, Spain.
  • Rodriguez JA; Chemistry Department, Brookhaven National Laboratory, 98 Rochester Street, Upton, New York 11973, United States.
  • Odriozola JA; Inorganic Chemistry Department and Materials Science Institute, University of Seville─CSIC, 41092 Sevilla, Spain.
J Am Chem Soc ; 144(1): 446-453, 2022 Jan 12.
Article en En | MEDLINE | ID: mdl-34928589
The active forms of Au and Pt in CeO2-based catalysts for the water-gas shift (WGS) reaction are an issue that remains unclear, although it has been widely studied. On one hand, ionic species might be responsible for weakening the Ce-O bonds, thus increasing the oxygen mobility and WGS activity. On the other hand, the close contact of Au or Pt atoms with CeO2 oxygen vacancies at the metal-CeO2 interface might provide the active sites for an efficient reaction. In this work, using in situ X-ray absorption spectroscopy, we demonstrate that both Au and Pt remain unoxidized during the reaction. Remarkable differences involving the dynamics established by both species under WGS atmospheres were recognized. For the prereduced Pt catalyst, the increase of the conversion coincided with a restructuration of the Pt atoms into cuboctahedrical metallic particles without significant variations on the overall particle size. Contrary to the relatively static behavior of Pt0, Au0 nanoparticles exhibited a sequence of particle splitting and agglomeration while maintaining a zero oxidation state despite not being located in a metallic environment during the process. High WGS activity was obtained when Au atoms were surrounded by oxygen. The fact that Au preserves its unoxidized state indicates that the chemical interaction between Au and oxygen must be necessarily electrostatic and that such an electrostatic interaction is fundamental for a top performance in the WGS process.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2022 Tipo del documento: Article País de afiliación: España Pais de publicación: Estados Unidos
Texto completo
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2022 Tipo del documento: Article País de afiliación: España Pais de publicación: Estados Unidos