Letter

Nature 437, 1132-1135 (20 October 2005) | doi:10.1038/nature04190; Received 6 May 2005; Accepted 2 September 2005

Tunable gold catalysts for selective hydrocarbon oxidation under mild conditions

Mathew D. Hughes1, Yi-Jun Xu1, Patrick Jenkins1, Paul McMorn1, Philip Landon1, Dan I. Enache1, Albert F. Carley1, Gary A. Attard1, Graham J. Hutchings1, Frank King2, E. Hugh Stitt2, Peter Johnston3, Ken Griffin3 & Christopher J. Kiely4

  1. School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT, UK
  2. Johnson Matthey Catalysts, PO Box 1, Teeside TS23 1LB, UK
  3. Johnson Matthey Catalysts, Orchard Road, Royston, Herts SG8 5HE, UK
  4. Center for Advanced Materials and Nanotechnology, Lehigh University, 5 East Packer Avenue, Bethlehem, Pennsylvania 18015, USA

Correspondence to: Graham J. Hutchings1 Correspondence and requests for materials should be addressed to G.J.H. (Email: hutch@cardiff.ac.uk).

Oxidation is an important method for the synthesis of chemical intermediates in the manufacture of high-tonnage commodities, high-value fine chemicals, agrochemicals and pharmaceuticals: but oxidations are often inefficient1. The introduction of catalytic systems using oxygen from air is preferred for 'green' processing2. Gold catalysis is now showing potential in selective redox processes3, 4, 5, 6, particularly for alcohol oxidation7, 8, 9, 10 and the direct synthesis of hydrogen peroxide11, 12. However, a major challenge that persists is the synthesis of an epoxide by the direct electrophilic addition of oxygen to an alkene13. Although ethene is epoxidized efficiently using molecular oxygen with silver catalysts in a large-scale industrial process14, this is unique because higher alkenes can only be effectively epoxidized using hydrogen peroxide15, 16, 17, hydroperoxides16 or stoichiometric oxygen donors. Here we show that nanocrystalline gold catalysts can provide tunable active catalysts for the oxidation of alkenes using air, with exceptionally high selectivity to partial oxidation products (approx98%) and significant conversions. Our finding significantly extends the discovery by Haruta18, 19 that nanocrystalline gold can epoxidize alkenes when hydrogen is used to activate the molecular oxygen; in our case, no sacrificial reductant is needed. We anticipate that our finding will initiate attempts to understand more fully the mechanism of oxygen activation at gold surfaces, which might lead to commercial exploitation of the high redox activity of gold nanocrystals.

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