Chemistry - A European Journal · 2014 · 20 citations · 62 references
Natural SciencesChemistryMedicinal ChemistryCatalysisElectrochemistryOrganic ChemistryCatalytic MechanismsHeterocycle SynthesisHeterocyclic ChemistryHeterocyclic CompoundsOrganic SynthesisAcid CatalysisGeneral Acid CatalysisGeneral Acid-base CatalysisHeterocycle FunctionalizationIntramolecular CatalysisPyrrolidine SynthesisQuaternary Ammonium CompoundsRoom-temperature Synthesis
A cascade reaction that generates pyrrolo- and pyridoindoline motifs from isocyanide precursors under phase-transfer conditions is described. This transformation proceeds at room temperature in the presence of a quaternary ammonium catalyst and base to generate functionalized products containing an all-carbon quaternary stereocentre. Quantum chemical calculations demonstrated that intramolecular general acid catalysis plays a key accelerating role through stabilization of developing charge in the transition state, and that the reaction is best described as a 5-endo dig cyclization, rather than an anionic 6π electrocyclization. Investigations employing chiral phase-transfer catalysts have given promising selectivities to date.
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