Characterization of the acid strength of SiO[sub 2]-ZrO[sub 2] mixed oxides
- DSM Research B.V., Gelenee (Netherlands)
The preparation of SiO[sub 2]-ZrO[sub 2] mixed oxides and the single oxides SiO[sub 2] and ZrO[sub 2] from H[sub 2]SiF[sub 6] and/or H[sub 2]ZrF[sub 6] is described. The catalysts are characterized using Hammett colour indicators, temperature programmed desorption of ammonia, XRD, XPS, and infrared spectroscopy. New IR bands and absence of XRD crystallinity show mixing of SiO[sub 2] and ZrO[sub 2] on an atomic scale in the amorphous coprecipitate. However, as could be concluded from the difference between surface concentrations of Zr and Si measured with XPS and the mean bulk concentrations, the ZrO[sub 2] precipitates somewhat more quickly than SiO[sub 2]. The acid strength of the SiO[sub 2]-ZrO[sub 2] mixed oxides corresponds to an H[sub 0] value between -11.4 and 13.8 (super-acidity). There is a fair correlation between the surface concentration of strong acid sites, determined from NH[sub 3] TPD, and the performance in the acid catalyzed dehydration of cyclohexanol to cyclohexene. In addition to the concentration of acid sites, their acid strength is an important factor determining the performance of the SiO[sub 2]-ZrO[sub 2] catalysts in the dehydration of cyclohexanol. The acid strength needed for the dehydration of cyclohexanol corresponds to H[sub 0] [<=] +2.8. Chemically mixed SiO[sub 2]-ZrO[sub 2] oxides contain strong acid sites as opposed to the single oxides SiO[sub 2] and ZrO[sub 2], which contain only weak acid sites. XPS shows an oxygen depletion on the surface of the mixed oxides, which indicates that the strong acid sites are of the Lewis type. 27 refs., 11 figs., 4 tabs.
- OSTI ID:
- 6879586
- Journal Information:
- Journal of Catalysis; (United States), Vol. 148:2; ISSN 0021-9517
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
ORGANIC
PHYSICAL AND ANALYTICAL CHEMISTRY
CYCLOHEXANOL
DEHYDRATION
SILICON OXIDES
CATALYTIC EFFECTS
ZIRCONIUM OXIDES
ABSORPTION SPECTROSCOPY
AMMONIA
CHEMICAL PREPARATION
DESORPTION
LEWIS ACIDS
PHOTOELECTRON SPECTROSCOPY
TEMPERATURE DEPENDENCE
X-RAY DIFFRACTION
X-RAY SPECTROSCOPY
ALCOHOLS
CHALCOGENIDES
COHERENT SCATTERING
DIFFRACTION
ELECTRON SPECTROSCOPY
HYDRIDES
HYDROGEN COMPOUNDS
HYDROXY COMPOUNDS
INORGANIC ACIDS
NITROGEN COMPOUNDS
NITROGEN HYDRIDES
ORGANIC COMPOUNDS
OXIDES
OXYGEN COMPOUNDS
SCATTERING
SILICON COMPOUNDS
SORPTION
SPECTROSCOPY
SYNTHESIS
TRANSITION ELEMENT COMPOUNDS
ZIRCONIUM COMPOUNDS
400201* - Chemical & Physicochemical Properties