Low-temperature oxidation of carbon monoxide with gold(III) ions supported on titanium oxide

Angew Chem Int Ed Engl. 2014 Mar 17;53(12):3245-9. doi: 10.1002/anie.201308206. Epub 2014 Feb 19.

Abstract

Au/TiO2 catalysts prepared by a deposition-precipitation process and used for CO oxidation without previous calcination exhibited high, largely temperature-independent conversions at low temperatures, with apparent activation energies of about zero. Thermal treatments, such as He at 623 K, changed the conversion-temperature characteristics to the well-known S-shape, with activation energies slightly below 30 kJ mol(-1). Sample characterization by XAFS and electron microscopy and a low-temperature IR study of CO adsorption and oxidation showed that CO can be oxidized by gas-phase O2 at 90 K already over the freeze-dried catalyst in the initial state that contained Au exclusively in the +3 oxidation state. CO conversion after activation in the feed at 303 K is due to Au(III)-containing sites at low temperatures, while Au(0) dominates conversion at higher temperatures. After thermal treatments, CO conversion in the whole investigated temperature range results from sites containing exclusively Au(0).

Keywords: CO oxidation; active sites; gold; spectroscopy; titanium dioxide.