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Dynamic restructuring drives catalytic activity on nanoporous gold-silver alloy catalysts.
Zugic, Branko; Wang, Lucun; Heine, Christian; Zakharov, Dmitri N; Lechner, Barbara A J; Stach, Eric A; Biener, Juergen; Salmeron, Miquel; Madix, Robert J; Friend, Cynthia M.
Afiliación
  • Zugic B; Department of Chemistry and Chemical Biology, Harvard University, Cambridge, Massachusetts 02138, USA.
  • Wang L; Department of Chemistry and Chemical Biology, Harvard University, Cambridge, Massachusetts 02138, USA.
  • Heine C; Materials Science Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA.
  • Zakharov DN; Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, USA.
  • Lechner BAJ; Materials Science Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA.
  • Stach EA; Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, USA.
  • Biener J; Nanoscale Synthesis and Characterization Laboratory, Lawrence Livermore National Laboratory, Livermore, California 94550, USA.
  • Salmeron M; Materials Science Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA.
  • Madix RJ; Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts 02138, USA.
  • Friend CM; Department of Chemistry and Chemical Biology, Harvard University, Cambridge, Massachusetts 02138, USA.
Nat Mater ; 16(5): 558-564, 2017 05.
Article en En | MEDLINE | ID: mdl-27992418
ABSTRACT
Bimetallic, nanostructured materials hold promise for improving catalyst activity and selectivity, yet little is known about the dynamic compositional and structural changes that these systems undergo during pretreatment that leads to efficient catalyst function. Here we use ozone-activated silver-gold alloys in the form of nanoporous gold as a case study to demonstrate the dynamic behaviour of bimetallic systems during activation to produce a functioning catalyst. We show that it is these dynamic changes that give rise to the observed catalytic activity. Advanced in situ electron microscopy and X-ray photoelectron spectroscopy are used to demonstrate that major restructuring and compositional changes occur along the path to catalytic function for selective alcohol oxidation. Transient kinetic measurements correlate the restructuring to three types of oxygen on the surface. The direct influence of changes in surface silver concentration and restructuring at the nanoscale on oxidation activity is demonstrated. Our results demonstrate that characterization of these dynamic changes is necessary to unlock the full potential of bimetallic catalytic materials.

Texto completo: 1 Colección: 01-internacional Banco de datos: MEDLINE Idioma: En Revista: Nat Mater Asunto de la revista: CIENCIA / QUIMICA Año: 2017 Tipo del documento: Article País de afiliación: Estados Unidos

Texto completo: 1 Colección: 01-internacional Banco de datos: MEDLINE Idioma: En Revista: Nat Mater Asunto de la revista: CIENCIA / QUIMICA Año: 2017 Tipo del documento: Article País de afiliación: Estados Unidos