Wyles, Joanna K; (1999) Heteroatom-substituted aluminophosphates. Doctoral thesis (Ph.D), UCL (University College London).

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Abstract

The work described in this thesis focuses on the synthesis and structural properties of heteroatom-substituted aluminophosphates with the chabazite structure, an important class of materials in the field of catalysis. Efforts have been made to design new template molecules for the synthesis of these materials, to understand the overall framework structure and derive the coordination geometry around the heteroatom both in the as-synthesised state and after producing the active catalyst. Two new organic molecules have been identified and used in the synthesis of heteroatom substituted aluminophosphates; these templates were chosen using two techniques: the de novo computer code ZEBEDDE predicted the template 4- piperidinopiperidine would produce a material with a chabazite structure; using rational design the template 1,3,3-trimethyl-6-azabicyclo[3.2.1]octane (TMABO) was identified for the synthesis of a small pore aluminophosphate. Chabazite type materials were produced in both cases. From a detailed characterisation using both laboratory and synchrotron radiation based techniques, we have been able to study the active sites in these materials and therefore predict their catalytic performance. A detailed study has also been carried out on the differences in the structure, stability and redox properties of CoAPO-34 synthesised using four different templates. From this study we are able to propose the best preparative route to produce a good catalyst for, in particular, the shape selective oxidation of linear alkanes.

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