Journal of Catalysis, Vol.306, 109-115, 2013
High-temperature calcination improves the catalytic properties of alumina-supported Pd@ceria prepared by self assembly
The effect of varying the calcination temperature from 773 to 1073 K was examined on catalysts prepared from Pd@CeO2, core shell nanoparticles adsorbed on silane-functionalized gamma-Al2O3 (Pd@CeO2/Si-Al2O3). Calcining to higher temperatures increased rates per gram catalyst for the methane-oxidation reaction significantly. The Pd@CeO2/Si-Al2O3 catalyst calcined to 773 X was unstable for methane-steam reforming (MSR) due to deep reduction of the catalyst while the catalyst calcined at 1073 K showed reasonable stable rates. CO adsorption, monitored using volumetric uptakes and FTIR, indicated adsorption on the Pd was suppressed following reduction at 673 K in H-2 when the catalyst had been calcined at only 773 K, but not after 1073 K. Pulse-reactor measurements demonstrated that catalysts calcined at either 773 X or 1073 X were heavily reduced under MSR reaction conditions at 673 K but that the catalyst heated to 1073 K could be re-oxidized by H2O at this temperature, while the 773-K sample could not be. It is suggested that increasing calcination temperature modifies the structure of the ceria shell, which in turn changes the ceria redox properties. (C) 2013 Elsevier Inc. All rights reserved.
Keywords:Methane oxidation;Methane-steam reforming;Core-shell catalysts;Calcination temperature;Ceria;Pd