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Title: The development of catalysts for the partial oxidation of ethane
Author: Sonntag, Olivier
ISNI:       0000 0001 3471 3277
Awarding Body: Nottingham Trent University
Current Institution: Nottingham Trent University
Date of Award: 2006
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In this study iron containing bulk and porous materials were developed and characterised for their application as potential heterogeneous catalysts for the partial oxidation of ethane to ethanol. The catalysts comprised bulk and supported iron phosphates as well as supported iron and bimetallic iron-gold. The chosen supports were zeolites of MFI structure and the porous silicate MCM-41, which were modified either during their synthesis or post-synthetically. The physical properties of the catalysts were analysed by means of X-ray diffraction, atomic absorption, nitrogen adsorption at 77 K, temperature programmed reduction, ammonia adsorption and desorption, nitric oxide adsorption. The catalytic properties of the materials were evaluated by testing them for the partial oxidation of ethane in the gas phase, using either nitrous oxide or oxygen as oxidising agent. Difficulties were encountered in the synthesis of crystalline iron phosphates, but the bulk properties of the silica and silica-alumina supports were merely affected by their postsynthetic treatments; surface areas and long-range order were retained in most cases. The effect of the reducibility of transition metals present or the acidity of the materials on their catalytic properties were investigated. It is believed that some degree of Bronsted acidity is necessary for the production of the hydroxylated oxygenate. Gold only slightly enhanced the oxidative capabilities of the catalysts, and best results were obtained with Fe-ZSM-5 and Fe-MFI materials, when using nitrous oxide as oxidising agent. Following studies of the adsorption of nitrous oxide on the materials, it was decided that the active site for partial oxidative activity was an iron dimer or oligomer of Fe404 structure, similarly as to the oxidation of benzene to phenol.
Supervisor: Not available Sponsor: Not available
Qualification Name: Thesis (Ph.D.) Qualification Level: Doctoral
EThOS ID:  DOI: Not available