期刊
NATURE CHEMISTRY
卷 5, 期 9, 页码 775-781出版社
NATURE PORTFOLIO
DOI: 10.1038/NCHEM.1721
关键词
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资金
- Spanish Science and Innovation Ministry [CSD2009-00050, SEV 2012 0267, MAT2011-28009, MAT2010-20442]
- Xunta de Galicia [Grupos Ref.Comp.2010/41]
- National Centre for Research Resources [5 G12RR013646-12]
- National Institute on Minority Health and Health Disparities from the National Institutes of Health [G12MD007591]
- National Science Foundation [DMR-1103730]
- PREM: NSF PREM [DMR 0934218]
- Consejo Nacional De Ciencia y Tecnologia
- Consejo Superior de Investigaciones Cientificas
- Division Of Materials Research
- Direct For Mathematical & Physical Scien [1103730] Funding Source: National Science Foundation
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.
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