No abstract

International audienceToluene hydrogenation was studied over catalysts based on Pt supported on large pore zeolites (HUSY and HBEA) with different metal/acid ratios. Acidity of zeolites was assessed by pyridine adsorption followed by FTIR showing only small changes before and after Pt introduction. Metal dispersion was determined by H 2-O 2 titration and verified by a linear correlation with the intensity of Pt 0-CO band obtained by in situ FTIR. It was also observed that the electronic properties of Pt 0 clusters were similar for the different catalysts. Catalytic tests showed rapid catalyst deactivation with an activity loss of 80-95% after 60 min. of reaction. The turnover frequency of fresh catalysts depended both on metal dispersion and the support. For the same support, it changed by a 1.7-fold (HBEA) and 4.0-fold (HUSY) showing that toluene hydrogenation is structure-sensitive, i.e. hydrogenating activity is not a unique function of accessible metal. This was proposed to be due to the contribution to the overall activity of the hydrogenation of adsorbed toluene on acid sites via hydrogen spillover. Taking into account the role of zeolite acidity, the catalysts series were compared by the activity per total adsorbing sites which was observed to increase steadily with n Pt /(n Pt +n A). An increase of the accessible Pt atoms leads to an increase on the amount of spilled over 1 hydrogen available in acid sites therefore increasing the overall activity. Pt/HBEA catalysts were found to be more active per total adsorbing site than Pt/HUSY which is proposed to be due to an augmentation in the efficiency of spilled over hydrogen diffusion related to the proximity between Pt clusters and acid sites. The intervention of Lewis acid sites in a greater extent than that measured by pyridine adsorption may also contribute to this higher activity of Pt/HBEA catalysts. These results reinforce the importance of model reactions as a closer perspective to the relevant catalyst properties in reaction conditions

MFI-type materials with a lamellar morphology were successfully synthesized by using mononitrogen surfactants specifically designed by molecular modelling. The mononitrogen surfactants directed the recrystallization of a crystalline layered polysilicate formed in situ, the magadiite, into a zeolite ZSM-5.Moreover, the surfactants allow the preservation of the lamellar shape of the magadiite and inhibit a further growth into one dimension, leading to the formation of zeolite ZSM-5 nanosheets with a thickness comprised between 2 and 3 nm and a Si/Al ratio of 24. This simple approach paves a new way for obtaining zeolite materials of controlled size and shape for specific catalytic applications.

No abstract