(Experimental and kinetic modeling of acid/base redox reactions over metal oxide catalysts)
During the past three years, our studies of metal oxide catalysts have been directed in several important areas. One of our major directions has been the development of microcalorimetry as a tool for the measurement and formulation of a thermodynamic scale of surface acidity. Studies in this area have involved a series of silica-supported metal oxides as well as several zeolite catalysts used in catalytic cracking. A second direction of research has been the preparation and study of thin-film oxide materials as models of vanadia/titania catalysts for the selective reduction of nitric oxide. These materials are well-suited for ultra-high vacuum investigations (e.g., XPS, AES, TPD) and they thereby provide valuable information about the kinetics and surface bonding energetics of the elementary steps comprising the reaction mechanism. Our studies funded by the Department of Energy have also involved microkinetic simulations of the oxidations of methane, methanol, formaldehyde and carbon monoxide over silica-supported molybdena and vanadia. The objective of this work was to determine whether a physically realistic reaction network of surface reaction steps could be constructed that would describe quantitatively the oxidation kinetics and selectivities of the above four reactants over a wide range of reaction conditions. The final direction that we have followed utilized solid state NMR techniques to characterize the coordination state of aluminum cations on silica-alumina catalysts and silica/alumina/molybdena materials. These studies give insight into the factors controlling the dispersion of alumina on silica and the mobility of molybdena on silica/alumina under oxidizing conditions at elevated temperatures. The following sections will describe in greater detail our results in each of the above four research efforts.
- Research Organization:
- Wisconsin Univ., Madison, WI (USA). Dept. of Chemical Engineering
- Sponsoring Organization:
- DOE/ER
- DOE Contract Number:
- FG02-84ER13183
- OSTI ID:
- 6740083
- Report Number(s):
- DOE/ER/13183-4; ON: DE90013835
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
37 INORGANIC
ORGANIC
PHYSICAL AND ANALYTICAL CHEMISTRY
ALUMINIUM OXIDES
CATALYTIC EFFECTS
MOLYBDENUM OXIDES
VANADIUM OXIDES
ACTIVATION ENERGY
CATALYSTS
CHEMICAL REACTION KINETICS
METHANE
NITROGEN OXIDES
NMR SPECTRA
PROGRESS REPORT
REDUCTION
SILICA
ALKANES
ALUMINIUM COMPOUNDS
CHALCOGENIDES
CHEMICAL REACTIONS
DOCUMENT TYPES
ENERGY
HYDROCARBONS
KINETICS
MINERALS
MOLYBDENUM COMPOUNDS
NITROGEN COMPOUNDS
ORGANIC COMPOUNDS
OXIDE MINERALS
OXIDES
OXYGEN COMPOUNDS
REACTION KINETICS
REFRACTORY METAL COMPOUNDS
SILICON COMPOUNDS
SILICON OXIDES
SPECTRA
TRANSITION ELEMENT COMPOUNDS
VANADIUM COMPOUNDS
360204* - Ceramics
Cermets
& Refractories- Physical Properties
400201 - Chemical & Physicochemical Properties