Angewandte Chemie International Edition · 2015 · 80 citations · 75 references
Natural SciencesChemistryCatalysisGreen ChemistryOrganometallic ChemistryCatalytic MechanismsHeterocycle SynthesisHeterocyclic ChemistryMolecular BondingReaction MechanismsScaffold DiversificationActivationCatalytic FunctionalizationPyridine ChemistryPyridine SynthesisReactivitySelectivityStructure-reactivity RelationshipsTransition Metal-catalyzed Synthesis
Gold carbene reactivity patterns were accessed by ynamide insertion into a C(sp(3) )H bond. A substantial increase in molecular complexity occurred through the cascade polycyclization of N-allyl ynamides to form fused nitrogen-heterocycle scaffolds. Exquisite selectivity was observed despite several competing pathways in an efficient gold-catalyzed synthesis of densely functionalized C(sp(3) )-rich polycycles and a copper-catalyzed synthesis of fused pyridine derivatives. The respective gold-keteniminium and ketenimine activation pathways have been explored through a structure-reactivity study, and isotopic labeling identified turnover-limiting CH bond-cleavage in both processes.
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Escape from Flatland 2: complexity and promiscuity
Frank Lovering · MedChemComm · 2012 · 1.4K citations