Title

Directed evolution of a fluorinase for improved fluorination efficiency on a non-native substrate

Conference Dates

September 24-28, 2017

Abstract

Fluorinases offer an environmentally friendly alternative for selective fluorination under mild conditions. However, their diversity is limited in nature and they have yet to be engineered via directed evolution. Herein, we report the directed evolution of the fluorinase FlA1 for improved conversion of a non-native substrate, 5’-chloro-5’-deoxyadenosine (5’-ClDA), to 5’-fluoro-5’-deoxyadenosine (5’-FDA). The evolved variants, fah2081 (A279Y) and fah2114 (F213Y, A279L), were successfully applied in the radiosynthesis of 5’-[18F]FDA, with overall radiochemical conversion (RCC) >3-fold higher than FlA1. Kinetic studies of the 2-step reaction revealed that the variants significantly improved kcat in the conversion of 5’-ClDA to S-adenosyl-L-methionine (SAM) but decreased kcat in the conversion of SAM to 5’-FDA.

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