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Nat Chem. 2010 Apr;2(4):329-34. doi: 10.1038/nchem.589. Epub 2010 Mar 24.

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

Author information

1
Department of Physics, Nanoscience Center, University of Jyväskylä, FI-40014 Jyväskylä, Finland.

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.

PMID:
21124516
DOI:
10.1038/nchem.589

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