Quantum size effects in ambient CO oxidation catalysed by ligand-protected gold clusters

Olga Lopez-Acevedo*, Katarzyna A. Kacprzak, Jaakko Akola, Hannu Häkkinen

*Corresponding author for this work

Research output: Contribution to journalArticleScientificpeer-review

248 Citations (Scopus)

Abstract

Finely dispersed nanometre-scale gold particles are known to catalyse several oxidation reactions in aerobic, ambient conditions. The catalytic activity has been explained by various complementary mechanisms, including support effects, particle-size-dependent metal-insulator transition, charging effects, frontier orbital interactions and geometric fluxionality. We show, by considering a series of robust and structurally well-characterized ligand-protected gold clusters with diameters between 1.2 and 2.4 nm, that electronic quantum size effects, particularly the magnitude of the so-called HOMO-LUMO energy gap, has a decisive role in binding oxygen to the nano-catalyst in an activated form. This can lead to the oxidation reaction 2CO+O-2 -> 2CO(2) with low activation barriers. Binding of dioxygen is significant only for the smallest particles with a metal core diameter clearly below 2 nm. Our results suggest a potentially viable route to practical applications using ligand-protected gold clusters for green chemistry.

Original languageEnglish
Pages (from-to)329-334
Number of pages6
JournalNATURE CHEMISTRY
Volume2
Issue number4
DOIs
Publication statusPublished - Apr 2010
MoE publication typeA1 Journal article-refereed

Keywords

  • AUGMENTED-WAVE METHOD
  • NANOPARTICLE CATALYSTS
  • CRYSTAL-STRUCTURE
  • METAL-CLUSTERS
  • NANOCLUSTERS
  • CHEMISTRY
  • SUPERATOMS
  • AU-2(-)
  • ATOM

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