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Alkyne Insertion Enabled Vinyl to Acyl 1,5‐Palladium Migration: Rapid Access to Substituted 5‐Membered‐Dihydrobenzofurans and Indolines

Mingruo Ding, Pengcheng Ou, Xuening Li, Yinghua Yu, Mengmeng Niu, Yongjian Yang, Yewei Huang, Zhixiang Wang, Xueliang Huang

2023Angewandte Chemie International Edition23 citationsDOI

Abstract

Abstract “Through space” palladium/hydrogen shift is an efficient strategy to achieve selective functionalization of a specific remote C−H bond. Compared with relatively extensive exploited 1,4‐palladium migration process, the relevant 1,5‐Pd/H shift was far less investigated. We herein report a novel 1,5‐Pd/H shift pattern between a vinyl and an acyl group. Through the pattern, rapid access to 5‐membered‐dihydrobenzofuran and indoline derivatives has been achieved. Further studies have unveiled an unprecedented trifunctionalization (vinylation, alkynylation and amination) of a phenyl ring through 1,5‐palladium migration relayed decarbonylative Catellani type reaction. A series of mechanistic investigations and DFT calculations have provided insights into the reaction pathway. Notably, it was unveiled that the 1,5‐palladium migration in our case prefers a stepwise mechanism involving a Pd IV intermediate.

Topics & Concepts

PalladiumIndolineChemistryAlkyneSurface modificationRing (chemistry)Combinatorial chemistryStereochemistryCatalysisOrganic chemistryPhysical chemistryCatalytic C–H Functionalization MethodsCatalytic Alkyne ReactionsCyclopropane Reaction Mechanisms