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Synthesis of Rhodium Complexes with Chiral Diene Ligands via Diastereoselective Coordination and Their Application in the Asymmetric Insertion of Diazo Compounds into E−H Bonds

Nikita M. Ankudinov, Denis Chusov, Yulia V. Nelyubina, Dmitry S. Perekalin

2021Angewandte Chemie International Edition41 citationsDOI

Abstract

Abstract A new method for the synthesis of chiral diene rhodium catalysts is introduced. The readily available racemic tetrafluorobenzobarrelene complexes [(R 2 ‐TFB)RhCl] 2 were separated into two enantiomers via selective coordination of one of them with the auxiliary S ‐salicyl‐oxazoline ligand. One of the resulting chiral complexes with an exceptionally bulky diene ligand [( R , R ‐ i Pr 2 ‐TFB)RhCl] 2 was an efficient catalyst for the asymmetric insertion of diazoesters into B−H and Si−H bonds giving the functionalized organoboranes and silanes with high yields (79–97 %) and enantiomeric purity (87–98 % ee ). The stereoselectivity of separation via auxiliary ligand and that of the catalytic reaction was predicted by DFT calculations.

Topics & Concepts

ChemistryRhodiumLigand (biochemistry)OxazolineEnantiomerDieneStereoselectivityDiazoCatalysisChiral ligandStereochemistryEnantioselective synthesisEnantiomeric excessMedicinal chemistryCombinatorial chemistryOrganic chemistryNatural rubberBiochemistryReceptorCyclopropane Reaction MechanismsCatalytic C–H Functionalization MethodsAsymmetric Hydrogenation and Catalysis
Synthesis of Rhodium Complexes with Chiral Diene Ligands via Diastereoselective Coordination and Their Application in the Asymmetric Insertion of Diazo Compounds into E−H Bonds | Litcius