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Abstract

This dissertation describes both new applications and methodology for the engineering and identification of biocatalysts. Significant portions of this thesis also discuss specifically the characterization, identification, and improvement of flavin-dependent halogenases. This family of enzymes is capable of site-selective halogenation of aryl C-H bonds using benign halide sources and molecular oxygen as the terminal oxidant. Prior to the work in this dissertation, these enzymes had been demonstrated as competent catalysts for regio- and enantio- selective transformations and, importantly, very amenable for improvement by directed evolution. These efforts from our lab had focused largely on the single halogenase RebH as a template for evolution in large part as a result of the dearth of explored enzymes.

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