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The design of model systems for biocatalysis

This dissertation discusses a number of very different approaches towards generating models for biocatalysis. After a brief introduction to biocatalysis, the next two chapters detail two different approaches to generating enzyme-like systems possessing binding sites with catalytic functions. Two further chapters discuss systems designed to model the catalytic function of two very different proton transfer enzymes. A collaborative project in the catalytic antibody field is described in Chapter 2. The background to efforts towards fashioning catalytic sites for lactamisation, decarboxylation and proton transfer is presented. The syntheses of substrates required for these studies were undertaken and the results from the studies (insofar as they are available) are discussed. A second collaborative project attempting to use polymer imprinting technology to generate catalytic binding sites is described in Chapter 3. After a brief overview of the conception and aims of the project, details are given of monomer syntheses, polymerisation procedures and subsequent kinetic studies. Two systems intended for use as models for the general acid catalysis observed in lysozyme have been synthesised. The reasoning behind the designed features of the compounds is presented in the context of a brief review of lysozyme and previous models. Proton transfer from carbon acids is usually a difficult process. A number of enzymes have evolved to catalyse this difficult reaction. The design and synthesis of a model for such an enzyme is described. Detailed kinetic studies upon the new substrate revealed that the intended reaction course is not followed. It is possible that a new type of mechanism is being observed. A discussion of possible mechanistic pathways which the molecule may be following is presented with their relative merits and precedents.

Identiferoai:union.ndltd.org:bl.uk/oai:ethos.bl.uk:604130
Date January 1999
CreatorsHodgson, D. R. W.
PublisherUniversity of Cambridge
Source SetsEthos UK
Detected LanguageEnglish
TypeElectronic Thesis or Dissertation

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