Exceptional oxidation activity with size-controlled supported gold clusters of low atomicity

Avelino Corma, Patricia Concepción, Mercedes Boronat, Maria J. Sabater, Javier Navas, Miguel José Yacaman, Eduardo Larios, Alvaro Posadas, M. Arturo López-Quintela, David Buceta, Ernest Mendoza, Gemma Guilera, Alvaro Mayoral

Research output: Contribution to journalArticlepeer-review

300 Scopus citations

Abstract

The catalytic activity of gold depends on particle size, with the reactivity increasing as the particle diameter decreases. However, investigations into behaviour in the subnanometre regime (where gold exists as small clusters of a few atoms) began only recently with advances in synthesis and characterization techniques. Here we report an easy method to prepare isolated gold atoms supported on functionalized carbon nanotubes and their performance in the oxidation of thiophenol with O 2. We show that single gold atoms are not active, but they aggregate under reaction conditions into gold clusters of low atomicity that exhibit a catalytic activity comparable to that of sulfhydryl oxidase enzymes. When clusters grow into larger nanoparticles, catalyst activity drops to zero. Theoretical calculations show that gold clusters are able to activate thiophenol and O 2 simultaneously, and larger nanoparticles are passivated by strongly adsorbed thiolates. The combination of both reactants activation and facile product desorption makes gold clusters excellent catalysts.

Original languageEnglish (US)
Pages (from-to)775-781
Number of pages7
JournalNature Chemistry
Volume5
Issue number9
DOIs
StatePublished - Sep 2013
Externally publishedYes

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)

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