Nitrene Transfer Catalyzed by a Non-Heme Iron Enzyme and Enhanced by Non-Native Small-Molecule Ligands
J. Am. Chem. Soc. 2019, 141, 19585-19588, 10.1021/jacs.9b11608
Transition-metal catalysis is a powerful tool for the construction of chemical bonds. Here we show that Pseudomonas savastanoi ethylene-forming enzyme, a non-heme iron enzyme, can catalyze olefin aziridination and nitrene C−H insertion, and that these activities can be improved by directed evolution. The nonheme iron center allows for facile modification of the primary coordination sphere by addition of metalcoordinating molecules, enabling control over enzyme activity and selectivity using small molecules.
Metal: FeLigand type: Amino acidHost protein: Pseudomonas savastanoi ethylene-forming enzyme (PsEFE)Anchoring strategy: NativeOptimization: GeneticReaction: C-H aminationMax TON: 730ee: 61PDB: 6CBANotes: Additional reaction: aziridination