Ethanol dehydration was investigated over commercial H-FER, H-MFI, H-MOR, H-BEA, H-Y and H-USY zeolite samples, and alumina and silica alumina for comparison. The catalysts were characterized using FT-IR spectroscopy of the surface OH groups and of adsorbed CO and pyridine. UV–vis, Raman and TG-DTA were applied to characterize coke, formed more on H-MOR and H-BEA. H-zeolites are definitely more active than silica alumina and alumina on catalyst weight base. The H-MOR sample is the most active but the H-MFI samples with Si/Al2 ratios 280 and 50 show higher reaction rates per Al ion, H-FER and faujasites show highest ethylene yield (99.9% at 573 K). At lower temperature and higher space velocities, diethyl ether is formed with high yield (>70% at 453–473 K on H-BEA and H-MFI (50)). Overconversion of ethylene mainly to aromatics is observed on H-MFI (50). The different behaviour of protonic zeolites can predominantly be explained by confinement effects on the different zeolite cavities
IR spectra of hydroxyl groups, adsorbed CO, pivalonitrile and pyridine on three H-MFI zeolite samples and on two H-Y faujasites are reported and discussed. Samples richer in Al (H-MFI (Si/Al2 = 30) and H-Y (Si/Al2 = 5.1)) show the presence of extraframework species and the presence of Lewis acidity together with Brønsted acidity. H-MFI with lowest Al content (Si/Al2 = 280) does not show any extraframework species (EF) and only presents Brønsted acidity. H-MFI with intermediate Al content (Si/Al2 = 50) possess very small amount of EF species and of Lewis acidity. H-Y with low Al content (Si/Al2 = 30) does not show extraframework species but shows the presence of Lewis acidity together with Brønsted acidity. The role of extraframework material as carrier of Lewis acidity is confirmed. It is proposed that Lewis acidity of low Al-content H-Y can arise from framework tetrahedral Al ions, which can enlarge their coordination to five without any previous dehydroxylation. A support for this hypothesis is given by the reversible shift of the LF OH stretching band, whose extent depends on the strength of the basic molecules: this is certainly not due to a direct interaction of the OH groups responsible for the LF band, which are located in cavities (sodalite cavity and hexagonal prisms) where the molecular probes cannot access
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