NDLI: Infrared spectroscopic studies of the reactions of alcohols over group IVB metal oxide catalysts. Part 1.—Propan-2-ol over TiO2, ZrO2 and HfO2

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Journal of the Chemical Society, Faraday Transactions 1 Vol - 85 Issue - 6

Journal of the Chemical Society, Faraday Transactions 1 Vol - 85 Issue - 5

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Infrared spectroscopic studies of the reactions of alcohols over group IVB metal oxide catalysts. Part 1.—Propan-2-ol over TiO₂, ZrO₂ and HfO₂

Content Provider	Royal Society of Chemistry (RSC)
Author	Hussein, Gamal A. M. Sheppard, Norman Fahim, Radamis B. Zaki, Mohamed I.
Copyright Year	1989
Abstract	Infrared spectroscopy has been used to analyse the gas-phase reaction products and the related adsorbed species obtained between room temperature and 400 °C from the dehydrogenation/dehydration reactions of propan-2-ol over a series of differently calcined catalysts of TiO2, ZrO2 and HfO2. The ZrO2 and HfO2 results were independent of the calcination pretreatment, and the surfaces of these oxides, like that from a TiO2 sample calcined at 800 °C, were dehydroxylated. Different results were obtained from a TiO2 sample calcined at 300 °C which had a hydroxylated surface. The acidic sites and reactivities of the surfaces of TiO2(300 °C) and TiO2(800 °C) were explored by pyridine adsorption and infrared spectroscopy. Only Lewis-acid sites were detected by pyridine.On raising the reaction temperature, in all cases the dehydrogenation reaction to give acetone occurred either before or simultaneously to the onset of the dehydration reaction to give propene. Acetone production was most pronounced over ZrO2 and HfO2 but also occurred more with TiO2(800 °C) than with TiO2(300 °C). The dehydrogenation reaction was largely quenched by pre-adsorbed pyridine on both TiO2 samples. The TiO2(300 °C) catalyst showed the presence of adsorbed propan-2-ol and 2-propoxide groups at room temperature. The dehydroxylated ZrO2, HfO2 and TiO2(800 °C) samples only showed appreciable amounts of 2-propoxide groups. In each case the 2-propoxide ions occurred in two different forms, presumably formed by adsorption on different types of sites.Both the acetone and propene products appeared as absorptions from 2-propoxide surface species decreased in intensity, so the latter are clearly reactive species. Gas-phase acetone production was followed by the chemisorption of acetone at a higher temperature. This subsequently decomposed to give surface acetate species, and finally at 400 °C to give CO2 and methane in the gas phase. Propene did not give rise to adsorbed species, or to further products in the gas phase.At the higher temperatures, above 300 °C, the reaction was always selective in favour of the dehydration reaction. However, each of the dehydroxylated catalysts showed some selectivity in favour of the dehydrogenation reaction over the earliest temperature range for alcohol decomposition, between 200 and 250 °C.A discussion is given of possible mechanistic pathways for the production of surface 2-propoxide species and the two types of products, based on the infrared-supported assumption that the different adsorbed forms of 2-propoxide [and possibly adsorbed propan-2-ol on TiO2(300 °C)] are reactive intermediates.
Starting Page	1723
Ending Page	1741
Page Count	19
File Format	PDF
ISSN	03009599
Volume Number	85
Issue Number	7
Journal	Journal of the Chemical Society, Faraday Transactions 1
DOI	10.1039/F19898501723
Language	English
Publisher	Royal Society of Chemistry
Access Restriction	Open
Subject Keyword	Methane Infrared spectroscopy Chemisorption Calcination Surface 2 Isopropyl alcohol Hafnium(IV) oxide Propene Pyridine Adsorption Dehydrogenation Zirconium dioxide Dehydration reaction Acetone
Content Type	Text
Resource Type	Article
Subject	Chemistry

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