Welch, AE; (2008) Multifunctional microporous metallosilicate catalysts. Doctoral thesis , UCL (University College London).

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Abstract

The work reported in this thesis is concerned with the synthesis and characterisation of a range of metallosilicate materials. A range of heteroatom containing materials with 3D framework structures were synthesised from amorphous cogel precursors, via a facile hydrothermal process. Titanosilicate, aluminosilicate and ferrisilicate materials were synthesised and characterisation of these materials demonstrated that the heteroatoms encompassed within them were in the ideal coordination geometry for active catalysis. These materials were compared to those synthesised from conventional means using a variety of techniques including, XRD, NMR, FTIR, TPD-MS and catalysis. Both the framework materials and their amorphous precursors were employed as catalysts for a range of oxidative and acidic reactions. The catalysis results demonstrated that although the amorphous cogel precursors were catalytically active and to some degree selective, the framework materials were more effective catalysts (regardless of the nature of the incorporated heteroatom). A range of bimetallosilicate materials were also synthesised from cogel precursors, these framework materials contained two of the heteroatoms previously employed (titanium, iron or aluminium). These materials were similarly characterised and their catalytic properties also evaluated. The differing chemical nature of the inserted heteroatoms allowed one catalyst to behave as both an active oxidative and an acidic catalyst.

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