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Reactivity of atomically dispersed Pt(2+) species towards H2: model Pt-CeO2 fuel cell catalyst.
Lykhach, Yaroslava; Figueroba, Alberto; Camellone, Matteo Farnesi; Neitzel, Armin; Skála, Tomás; Negreiros, Fabio R; Vorokhta, Mykhailo; Tsud, Nataliya; Prince, Kevin C; Fabris, Stefano; Neyman, Konstantin M; Matolín, Vladimír; Libuda, Jörg.
Afiliação
  • Lykhach Y; Lehrstuhl für Physikalische Chemie II, Friedrich-Alexander-Universität Erlangen-Nürnberg, Egerlandstrasse 3, 91058 Erlangen, Germany. yaroslava.lykhach@fau.de.
  • Figueroba A; Departament de Química Física and Institut de Quimica Teòrica i Computacional (IQTCUB), Universitat de Barcelona, c/Martí Franquès 1, 08028 Barcelona, Spain.
  • Camellone MF; CNR-IOM DEMOCRITOS, Istituto Officina dei Materiali, Consiglio Nazionale delle Ricerche and SISSA, Via Bonomea 265, I-34136, Trieste, Italy.
  • Neitzel A; Lehrstuhl für Physikalische Chemie II, Friedrich-Alexander-Universität Erlangen-Nürnberg, Egerlandstrasse 3, 91058 Erlangen, Germany. yaroslava.lykhach@fau.de.
  • Skála T; Charles University, Faculty of Mathematics and Physics, Department of Surface and Plasma Science, V Holesovickách 2, 18000 Prague, Czech Republic.
  • Negreiros FR; CNR-IOM DEMOCRITOS, Istituto Officina dei Materiali, Consiglio Nazionale delle Ricerche and SISSA, Via Bonomea 265, I-34136, Trieste, Italy.
  • Vorokhta M; Charles University, Faculty of Mathematics and Physics, Department of Surface and Plasma Science, V Holesovickách 2, 18000 Prague, Czech Republic.
  • Tsud N; Charles University, Faculty of Mathematics and Physics, Department of Surface and Plasma Science, V Holesovickách 2, 18000 Prague, Czech Republic.
  • Prince KC; Elettra-Sincrotrone Trieste SCpA, Strada Statale 14, km 163.5, 34149 Basovizza-Trieste, Italy and IOM, Strada Statale 14, km 163.5, 34149 Basovizza-Trieste, Italy.
  • Fabris S; CNR-IOM DEMOCRITOS, Istituto Officina dei Materiali, Consiglio Nazionale delle Ricerche and SISSA, Via Bonomea 265, I-34136, Trieste, Italy.
  • Neyman KM; Departament de Química Física and Institut de Quimica Teòrica i Computacional (IQTCUB), Universitat de Barcelona, c/Martí Franquès 1, 08028 Barcelona, Spain and Institució Catalana de Recerca i Estudis Avançats (ICREA), 08010 Barcelona, Spain.
  • Matolín V; Charles University, Faculty of Mathematics and Physics, Department of Surface and Plasma Science, V Holesovickách 2, 18000 Prague, Czech Republic.
  • Libuda J; Lehrstuhl für Physikalische Chemie II, Friedrich-Alexander-Universität Erlangen-Nürnberg, Egerlandstrasse 3, 91058 Erlangen, Germany. yaroslava.lykhach@fau.de and Erlangen Catalysis Resource Center, Friedrich-Alexander-Universität Erlangen-Nürnberg, Egerlandstrasse 3, 91058 Erlangen, Germany.
Phys Chem Chem Phys ; 18(11): 7672-9, 2016 Mar 21.
Article em En | MEDLINE | ID: mdl-26908194
The reactivity of atomically dispersed Pt(2+) species on the surface of nanostructured CeO2 films and the mechanism of H2 activation on these sites have been investigated by means of synchrotron radiation photoelectron spectroscopy and resonant photoemission spectroscopy in combination with density functional calculations. Isolated Pt(2+) sites are found to be inactive towards H2 dissociation due to high activation energy required for H-H bond scission. Trace amounts of metallic Pt are necessary to initiate H2 dissociation on Pt-CeO2 films. H2 dissociation triggers the reduction of Ce(4+) cations which, in turn, is coupled with the reduction of Pt(2+) species. The mechanism of Pt(2+) reduction involves reverse oxygen spillover and formation of oxygen vacancies on Pt-CeO2 films. Our calculations suggest the existence of a threshold concentration of oxygen vacancies associated with the onset of Pt(2+) reduction.

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Revista: Phys Chem Chem Phys Assunto da revista: BIOFISICA / QUIMICA Ano de publicação: 2016 Tipo de documento: Article País de afiliação: Alemanha País de publicação: Reino Unido

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Revista: Phys Chem Chem Phys Assunto da revista: BIOFISICA / QUIMICA Ano de publicação: 2016 Tipo de documento: Article País de afiliação: Alemanha País de publicação: Reino Unido