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supported palladium catalysts; precious metal-catalysts; H bond activation; hydrocarbon oxidation; particle-size; toluene combustion; low emissions; temperature; platinum; oxygen
Abstract:
The progressive activation of a Pd(2 wt %)/gamma-alumina catalyst under the reaction conditions of catalytic combustion of methane (CCM) was studied. The reasons of this activation were investigated by XPS, CO-chemisorption, and HR-TEM. The removal of carbon from the surface cannot explain the observed activation process. Sintering of the palladium particles was detected but this parameter alone does not fully explain the activation process of the catalyst. HR-TEM imaging evidences (i) that PdO is present both in the fresh and the active catalyst and (ii) that the PdO nanoparticles sinter and restructure (surface roughening) during the reaction. Development of preferential faces was not observed. It is suggested that this restructuring may be responsible for the activation process by facilitating the formation of an active oxygen layer on the PdO surface. CCM on Pd/gamma-Al2O3 depends on the thermal history of the catalyst and is a structure-sensitive reaction.
