Combination of flame synthesis and high-throughput experimentation:: The preparation of alumina-supported noble metal particles and their application in the partial oxidation of methane

Mono and multi-noble metal particles on Al2O3 Were prepared in one step by flame spray pyrolysis (FSP) of the corresponding noble metal precursors dissolved in methanol and acetic acid (v/v 1:1) or xylene. The noble metal loading of the catalysts was close to the theoretical composition as determined by WD-XRF and LA-ICP-MS. The preparation method was combined with high-throughput testing using an experimental setup consisting of eight parallel fixed-bed reactors. Samples containing 0.1-5 wt% noble metals (Ru, Rh, Pt, Pd) on Al2O3 were tested in the catalytic partial oxidation of methane. The ignition of the reaction towards carbon monoxide and hydrogen depended on the loading and the noble metal constituents. The selectivity of these noble metal catalysts towards CO and H-2 was similar under the conditions used (methane: oxygen ratio 2: 1, temperature from 300 to 500 degrees C) and exceeded significantly those of gold and silver containing catalysts. Selected catalysts were further analysed using XPS, BET, STEM-EDXS and XANES/EXAFS. The catalysts exhibited generally a specific surface area of more than 100 m(2)/g, and were made up of ca. 10 nm alumina particles on which the smaller noble metal particles (1-2 nm, partially oxidized state) were discernible. XPS investigation revealed an enrichment of noble metals on the alumina surface of all samples. The question of alloy formation was addressed by STEM-EDXS and EXAFS analysis. In some cases, particularly for Pt-Pd and Pt-Rh, alloying close to the bulk alloys was found, in contrast to Pt-Ru being only partially alloyed. In situ X-ray absorption spectroscopy on selected samples was used to gain insight into the oxidation state during ignition and extinction of the catalytic partial oxidation of methane to hydrogen and carbon monoxide. (c) 2006 Elsevier B.V. All rights reserved.