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Design of Hemilabile N,N,N-Ligands in Copper-Catalyzed Enantioconvergent Radical Cross-Coupling of Benzyl/Propargyl Halides with Alkenylboronate Esters

Pengfei Wang, Jiao Yu, Kai-Xin Guo, Shengpeng Jiang, Ji‐Jun Chen, Qiang‐Shuai Gu, Ji‐Ren Liu, Xin Hong, Zhong‐Liang Li, Xin‐Yuan Liu

2022Journal of the American Chemical Society57 citationsDOI

Abstract

) cross-coupling of alkyl halides with alkenylboronate esters is an appealing tool in the assembly of synthetically valuable enantioenriched alkenes owing to the ready availability, low toxicity, and air/moisture stability of alkenylboronate esters. Here, we report a copper/chiral N,N,N-ligand catalytic system for the enantioconvergent cross-coupling of benzyl/propargyl halides with alkenylboronate esters (>80 examples) with good functional group tolerance. The key to the success is the rational design of hemilabile N,N,N-ligands by mounting steric hindrance at the ortho position of one coordinating quinoline ring. Thus, the newly designed ligand could not only promote the radical cross-coupling process in the tridentate form but also deliver enantiocontrol over highly reactive alkyl radicals in the bidentate form. Facile follow-up transformations highlight its potential utility in the synthesis of various enantioenriched building blocks as well as in the late-stage functionalization for drug discovery.

Topics & Concepts

ChemistryPropargylLigand (biochemistry)Steric effectsAlkylHalideQuinolineDenticityCatalysisRadicalCombinatorial chemistryStereochemistryMedicinal chemistryOrganic chemistryMetalReceptorBiochemistryRadical Photochemical ReactionsCatalytic C–H Functionalization MethodsSulfur-Based Synthesis Techniques
Design of Hemilabile N,N,N-Ligands in Copper-Catalyzed Enantioconvergent Radical Cross-Coupling of Benzyl/Propargyl Halides with Alkenylboronate Esters | Litcius