The development of catalysts for the partial oxidation of ethane

Sonntag, O, 2006. The development of catalysts for the partial oxidation of ethane. PhD, Nottingham Trent University.

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Abstract

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 post-synthetic 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 Brønsted 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.

Item Type:	Thesis
Creators:	Sonntag, O.
Date:	2006
ISBN:	9781369313581
Identifiers:	Number Type PQ10183071 Other
Divisions:	Schools > School of Science and Technology
Record created by:	Linda Sullivan
Date Added:	17 Sep 2020 13:41
Last Modified:	28 Jun 2023 09:57
URI:	https://irep.ntu.ac.uk/id/eprint/40759

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