题 目：Revealing the chemical logic of diverse non-heme iron enzyme catalysis in natural products assembly
报告人：Wei-Chan Chang 博士 North Carolina State University
摘 要：Revealing the chemical logic of diverse non-heme iron enzyme catalysis in natural products assembly Non-heme iron, 2-oxo-glutarate and molecular oxygen dependent enzymes catalyze a broad array of synthetically challenging transformations, ranging from hydroxylation, demethylation, halogenation, epimerization, endoperoxidation, ring expansion and etc. In the last decade, mechanistic investigations on this enzyme family have revealed an emerging paradigm where diverse reaction outcome can be attributed from: (1) the electronic structures of the Fe(IV)-oxo species; (2) participation of polar or redox-active residues in the secondary coordination sphere; and (3) the intrinsic properties of the substrates. To explore the chemical logic governing diverse, but controlled, reaction outcomes, we take a complementary approach including mechanistic probe design, transient kinetics dissection and spectroscopic characterization to provide experimental support for revealing chemical logic of diverse reaction outcomes.