Angewandte Chemie International Edition · 2019 · 89 citations · 38 references
Natural SciencesChemical EngineeringChemistryCatalysisComputational ChemistryOrganic ChemistryCatalysis ModelingCatalyst DesignCatalytic MechanismsCoordination ChemistryHeterocycle SynthesisMetal CatalysisCatalytic Cycle AnalysisCatalytic Cycle MechanismsCatalytic Reaction MechanismsCopper CatalysisCopper-catalyzed OxidationCopper-mediated OxidationNitrogen HeterocyclesOxidation Catalysis
The dual function of the N-F bond as an effective oxidant and subsequent nitrogen source in intramolecular aliphatic C-H functionalization reactions is explored. Copper catalysis is demonstrated to exercise full regio- and chemoselectivity control, which opens new synthetic avenues to nitrogenated heterocycles with predictable ring sizes. For the first time, a uniform catalysis manifold has been identified for the construction of both pyrrolidine and piperidine cores. The individual steps of this new copper oxidation catalysis were elucidated by control experiments and computational studies, clarifying the singularity of the N-F function and characterizing the catalytic cycle to be based on a copper(I/II) manifold.
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Jeremy N. Harvey, Massimiliano Aschi, Helmut Schwarz et al. · Theoretical Chemistry Accounts · 1998 · 913 citations
Natural Sciences, Chemistry, Physics +17