Science · 2014 · 222 citations · 34 references
Natural SciencesChemistryCatalysisChemical KineticsOrganic ChemistryCatalyst DesignCatalytic MaterialsCatalytic MechanismsCatalytic Reaction KineticsChiral SeparationAsymmetric CatalysisC - H Bond FunctionalizationCatalytic Reaction MechanismsChiral KineticsEnantioselective CatalysisEnantioselective SynthesisKinetic Resolution
Asymmetric carbon-hydrogen (C-H) activation reactions often rely on desymmetrization of prochiral C-H bonds on the same achiral molecule, using a chiral catalyst. Here, we report a kinetic resolution via palladium-catalyzed enantioselective C-H iodination in which one of the enantiomers of a racemic benzylic amine substrates undergoes faster aryl C-H insertion with the chiral catalysts than the other. The resulting enantioenriched C-H functionalization products would not be accessible through desymmetrization of prochiral C-H bonds. The exceedingly high relative rate ratio (k(fast)/k(slow) up to 244), coupled with the subsequent iodination of the remaining enantiomerically enriched starting material using a chiral ligand with the opposite configuration, enables conversion of both substrate enantiomers into enantiomerically pure iodinated products.
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Biotinylated Rh(III) Complexes in Engineered Streptavidin for Accelerated Asymmetric C–H Activation
Todd K. Hyster, Livia Knörr, Thomas R. Ward et al. · Science · 2012 · 806 citations · Full text
Bing‐Feng Shi, Nathan Maugel, Yanghui Zhang et al. · Angewandte Chemie International Edition · 2008 · 686 citations