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Visible-Light-Induced Dearomatization via [2+2] Cycloaddition or 1,5-Hydrogen Atom Transfer: Divergent Reaction Pathways of Transient Diradicals

Min Zhu, Xiǎo Zhang, Chao Zheng, Shu‐Li You

2020ACS Catalysis116 citationsDOI

Abstract

Visible-light-induced dearomatization reaction via energy-transfer mechanism is an emerging strategy for the synthesis of highly strained polycyclic molecules. Transient, high-energy diradical species are typically involved in this type of reaction as key intermediates. Herein, we report the visible-light-induced divergent dearomatization of indole-tethered O-methyl oximes, in which the reactions of the open-shelled singlet diradical intermediates toward competitive [2 + 2] cycloaddition or 1,5-hydrogen atom transfer can be achieved with exclusive selectivity. The mechanism has been well supported by a series of experimental and computational investigations. The dearomatization reactions allow the facile synthesis of structurally appealing indoline-fused azetidines and related polycyclic molecules with high efficiency.

Topics & Concepts

DiradicalCycloadditionChemistryPhotochemistryHydrogen atomIndolineReactive intermediateMoleculeSinglet stateIndole testCombinatorial chemistryCatalysisComputational chemistryStereochemistryOrganic chemistryExcited statePhysicsNuclear physicsAlkylRadical Photochemical ReactionsCatalytic C–H Functionalization MethodsSynthesis and Catalytic Reactions
Visible-Light-Induced Dearomatization via [2+2] Cycloaddition or 1,5-Hydrogen Atom Transfer: Divergent Reaction Pathways of Transient Diradicals | Litcius