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Hexafluoroisopropanol for the Selective Deactivation of Poisonous Nucleophiles Enabling Catalytic Asymmetric Cyclopropanation of Complex Molecules

Jack C. Sharland, David I. Dunstan, Dyuti Majumdar, Jinhai Gao, Kian L. Tan, Hasnain A. Malik, Huw M. L. Davies

2022ACS Catalysis28 citationsDOI

Abstract

In the presence of 1,1,1,3,3,3-hexafluoroisopropanol (HFIP), nucleophilic and reactive reagents are prevented from interacting with a rhodium carbene, allowing asymmetric cyclopropanation to occur with high yield and stereoselectivity on a variety of compounds. A high-throughput screen was conducted on cyclopropanation with a complementary catalytic system in the presence of 90 different poisonous nucleophiles and varying amounts of HFIP (10 equiv, used as reaction solvent). The scope of both the aryl/heteroaryl diazoacetate and the olefin was expanded, and the study culminated in the enantioselective functionalization of complex molecules including API and natural products.

Topics & Concepts

CyclopropanationNucleophileEnantioselective synthesisCarbeneChemistryEthyl diazoacetateArylCatalysisOlefin fiberCombinatorial chemistryReactivity (psychology)RhodiumMoleculeOrganic chemistryPathologyAlternative medicineAlkylMedicineCyclopropane Reaction MechanismsAsymmetric Synthesis and CatalysisAsymmetric Hydrogenation and Catalysis
Hexafluoroisopropanol for the Selective Deactivation of Poisonous Nucleophiles Enabling Catalytic Asymmetric Cyclopropanation of Complex Molecules | Litcius