Angewandte Chemie International Edition · 2015 · 121 citations · 23 references
Natural SciencesBiochemistryChemistryBiocatalysisEnzymologyOrganic ChemistryAmino Acid ChemistryAmino Acid-derived Natural ProductsChemoenzymatic SynthesisHigh-throughput SynthesisOrganic SynthesisPeptide ChemistryCascade Chemoenzymatic SynthesisChemoenzymatic Cascade ReactionsChemoenzymatic DerivatizationHigh-throughput Cascade ScreeningPhenylalanine Ammonia-lyase PathwayPhenylalanine BiosynthesisPhenylalanine-derived Natural ProductsStereoselective Oxidation
The synthesis of substituted D-phenylalanines in high yield and excellent optical purity, starting from inexpensive cinnamic acids, has been achieved with a novel one-pot approach by coupling phenylalanine ammonia lyase (PAL) amination with a chemoenzymatic deracemization (based on stereoselective oxidation and nonselective reduction). A simple high-throughput solid-phase screening method has also been developed to identify PALs with higher rates of formation of non-natural D-phenylalanines. The best variants were exploited in the chemoenzymatic cascade, thus increasing the yield and ee value of the D-configured product. Furthermore, the system was extended to the preparation of those L-phenylalanines which are obtained with a low ee value using PAL amination.
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