Non-native Photobiocatalysis: Using Non-Natural Single Electron Transfer Reactions to Enable the Enantioselective Synthesis of Amines

Lead Research Organisation: University of Cambridge
Department Name: Chemistry

Abstract

Year 1: Generic training activities for all first-year student members of the CDT.

Year 2-4: Enzymes are attractive catalysts for asymmetric synthesis as they enable selectivities and efficiencies that surpass those of conventional chemical methods while also possessing a unique mode of optimisation, allowing their chemical structures to be tailored towards a specific substrate and selectivity outcomes, via protein engineering. However, the applications of enzymatic catalysis have been generally restricted to reactions found in nature. Recently, exploiting non-natural reaction mechanisms within native enzymes has emerged as an attractive strategy for expanding the synthetic repertoire of biocatalysis and has the potential to address many long-standing selectivity and reactivity challenges in chemical synthesis. This project will carry out an initial exploration into the viability of conducting non-natural single electron transfer reactions within imine reductases (IREDs) to enable the photo-biocatalytic asymmetric synthesis of alkyl amines. Accurate determination of enantioselectivity from crude reaction mixtures on a micromolar scale remains an ongoing challenge. We hope the eventual development of a robust high-throughput methodology to generate standardised datasets will facilitate future enzymatic optimisation through linking sequence to activity.

Publications

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Studentship Projects

Project Reference Relationship Related To Start End Student Name
EP/S024220/1 31/05/2019 30/11/2027
2468416 Studentship EP/S024220/1 30/09/2020 29/09/2024 James Robinson