Role of the nanoscale in catalytic CO oxidation by supported Au and Pt nanostructures

Sergey Rashkeev, Andrew R. Lupini, Steven H. Overbury, Stephen J. Pennycook, Sokrates T. Pantelides

Research output: Contribution to journalArticle

105 Citations (Scopus)

Abstract

Experiments have found that the catalytic activity of Au increases sharply for supported nanoparticles smaller than 5 nm, while Pt exhibits the opposite behavior. Several authors, seeking to explain the nanoscale Au activity, reached conflicting conclusions, attributing it to different nanoscale features or to a particular bilayer structure that is independent of size. Here, we report an extensive theoretical study of a large ensemble of Ti O2 -supported Au and Pt nanoparticles and show that several nanoscale features collectively result in the observed contrasting behavior. Low coordination is accompanied by bond weakening in Au and strengthening in Pt, while perimeter sites are active only for Au. Though there are orbital-occupancy differences for catalytically active and inactive configurations, there is insignificant variation in physical-charge transfer. Finally, we report atomically resolved Z -contrast images that confirm bond weakening in catalytically active Ti O2 -supported Au nanoparticles.

Original languageEnglish
Article number035438
JournalPhysical Review B - Condensed Matter and Materials Physics
Volume76
Issue number3
DOIs
Publication statusPublished - 30 Jul 2007
Externally publishedYes

Fingerprint

Catalytic oxidation
Carbon Monoxide
Nanostructures
Nanoparticles
nanoparticles
oxidation
image contrast
catalytic activity
Charge transfer
Catalyst activity
charge transfer
orbitals
configurations
Experiments

ASJC Scopus subject areas

  • Condensed Matter Physics

Cite this

Role of the nanoscale in catalytic CO oxidation by supported Au and Pt nanostructures. / Rashkeev, Sergey; Lupini, Andrew R.; Overbury, Steven H.; Pennycook, Stephen J.; Pantelides, Sokrates T.

In: Physical Review B - Condensed Matter and Materials Physics, Vol. 76, No. 3, 035438, 30.07.2007.

Research output: Contribution to journalArticle

Rashkeev, Sergey ; Lupini, Andrew R. ; Overbury, Steven H. ; Pennycook, Stephen J. ; Pantelides, Sokrates T. / Role of the nanoscale in catalytic CO oxidation by supported Au and Pt nanostructures. In: Physical Review B - Condensed Matter and Materials Physics. 2007 ; Vol. 76, No. 3.
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