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Regio‐ and Diastereoselective Formal [2+2] Cycloaddition of Allenes with Amino‐Functionalized Alkenes by Rare‐Earth‐Catalyzed C(sp<sup>2</sup>)−H Activation

Wenxuan Xu, Xuefeng Cong, Kun An, Shao‐Jie Lou, Zhenghua Li, Masayoshi Nishiura, Tetsuro Murahashi, Zhaomin Hou

2022Angewandte Chemie International Edition31 citationsDOI

Abstract

Abstract The [2+2] cycloaddition of allenes with alkenes is of much interest and importance as a straightforward route for the construction of four‐membered carbocycles but has remained much underexplored to date. Herein we report for the first time the intermolecular regio‐ and diastereoselective formal [2+2] cycloaddition of a wide range of allenes with amino‐functionalized alkenes by half‐sandwich rare‐earth catalysts. The reaction proceeded through an allene C(sp 2 )−H activation mechanism initiated by the site‐selective deprotonation of the allene unit by a rare‐earth metal alkyl species followed by alkene insertion into the resulting metal‐allenyl bond and the subsequent intramolecular cycloaddition to an allene C=C bond. This protocol offers a unique route for the synthesis of a new family of cyclobutane and cyclobutene derivatives which were difficult to access previously.

Topics & Concepts

CycloadditionAlleneAlkeneChemistryIntramolecular forceCyclobuteneDeprotonationStereochemistryAlkylMedicinal chemistryCatalysisOrganic chemistryRing (chemistry)IonCatalytic C–H Functionalization MethodsCatalytic Alkyne ReactionsCyclopropane Reaction Mechanisms