Litcius/Paper detail

Iron-Catalyzed Enantioselective Multicomponent Cross-Couplings of α-Boryl Radicals

Cassandra R. Youshaw, Ming‐Hsiu Yang, Achyut Ranjan Gogoi, Ángel Rentería‐Gómez, Lei Liu, Lukas M. Morehead, Osvaldo Gutiérrez

2023Organic Letters21 citationsDOIOpen Access PDF

Abstract

Despite recent interest in the development of iron-catalyzed transformations, methods that use iron-based catalysts capable of controlling the enantioselectivity in carbon–carbon cross-couplings are underdeveloped. Herein, we report a practical and simple protocol that uses commercially available and expensive iron salts in combination with chiral bisphosphine ligands to enable the regio- and enantioselective (up to 91:9) multicomponent cross-coupling of vinyl boronates, (fluoro)alkyl halides, and Grignard reagents. Preliminary mechanistic studies are consistent with rapid formation of an α-boryl radical followed by reversible radical addition to monoaryl bisphosphine-Fe(II) and subsequent enantioselective inner-sphere reductive elimination. From a broader perspective, this work provides a blueprint to develop asymmetric Fe-catalyzed multicomponent cross-couplings via the use of alkenes as linchpins to translocate alkyl radicals, modify their steric and electronic properties, and induce stereocontrol.

Topics & Concepts

Enantioselective synthesisChemistryRadicalSteric effectsCatalysisCombinatorial chemistryAlkylReagentHalideOrganic chemistryCatalytic C–H Functionalization MethodsRadical Photochemical ReactionsOrganoboron and organosilicon chemistry