Angewandte Chemie International Edition · 2014 · 341 citations · 43 references
Natural SciencesChemical EngineeringChemistryCatalysisInorganic ChemistryOrganic ChemistryDiversity-oriented SynthesisHeterocycle SynthesisOrganic SynthesisRedox CatalysisRedox-active MaterialsCatalytic Cycle AnalysisCatalytic Cycle MechanismsIsoquinoline ChemistryIsoquinoline SynthesisManganese CatalysisManganese ChemistryManganese Oxide CatalystsManganese Redox Chemistry
Described herein is a manganese-catalyzed dehydrogenative [4+2] annulation of NH imines and alkynes, a reaction providing highly atom-economical access to diverse isoquinolines. This transformation represents the first example of manganese-catalyzed CH activation of imines; the stoichiometric variant of the cyclomanganation was reported in 1971. The redox neutral reaction produces H2 as the major byproduct and eliminates the need for any oxidants, external ligands, or additives, thus standing out from known isoquinoline synthesis by transition-metal-catalyzed CH activation. Mechanistic studies revealed the five-membered manganacycle and manganese hydride species as key reaction intermediates in the catalytic cycle.
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Adding Aliphatic C–H Bond Oxidations to Synthesis
M. Christina White · Science · 2012 · 709 citations