Journal of the American Chemical Society · 2001 · 45 citations · 10 references
Natural SciencesChemistryMedicinal ChemistryNatural Product BiosynthesisOrganic ChemistrySynthetic Medicinal ChemistryHeterocycle SynthesisHeterocyclic ChemistryOrganic SynthesisRetrosynthetic AnalysisTerpenoid BiosynthesisAbsolute Configuration AssignmentAbsolute Configuration DeterminationClaisen CondensationClaisen RearrangementEnantioselective SynthesisKinetic ControlKinetic Control Of AssemblyOxonium Ions
A short efficient enantioselective synthesis of both (+)- and (-)-saudin, a naturally occurring hypoglycemic diterpene, is described. This synthesis establishes the absolute configuration of natural (-)-saudin for the first time. The key steps include the enantioselective construction of a dimethyl Hagemann's ester by an asymmetric Michael reaction and establishment of the key 1,3 disposed quaternary centers by means of a novel Ti(IV) promoted Claisen rearrangement. The assembly of the polycyclic ketal skeleton was likely under kinetic control proceeding via formation of the C1oxygen-C7 bond through an oxonium ion intermediate in the final stage.
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