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Controllable synthesis of benzoxazinones and 2-hydroxy-3-indolinones by visible-light-promoted 5-endo-dig N-radical cyclization cascade

Tong‐De Tan, Tong‐Yi Zhai, Yang Liu, Long Li, Peng‐Cheng Qian, Qing Sun, Jin‐Mei Zhou, Long‐Wu Ye

2021Cell Reports Physical Science16 citationsDOIOpen Access PDF

Abstract

In recent years, significant advances have been made on photoredox-catalyzed N-radical addition to C-C unsaturated bond via N-H bond cleavage. However, these N-centered radical additions have so far been mostly limited to the alkenes, and to our knowledge, N-radical 5-endo-dig cyclizations of alkynes have been less exploited. Herein, we disclose an 5-endo-dig N-radical cascade cyclization of o-ethynylacetamides by photoredox catalysis involving rare radical cleavage of C-C triple bond, allowing the practical and controllable synthesis of a diverse array of valuable benzoxazinones and 2-hydroxy-3-indolinones in moderate to good yields under mild conditions. Furthermore, a mechanistic rationale for this radical cyclization cascade is supported by various control experiments and theoretical calculations.

Topics & Concepts

CascadeChemistryRadical cyclizationBond cleavagePhotoredox catalysisCleavage (geology)PhotochemistryCatalysisRadicalCombinatorial chemistryMedicinal chemistryOrganic chemistryPhotocatalysisMaterials scienceChromatographyComposite materialFracture (geology)Radical Photochemical ReactionsCatalytic C–H Functionalization MethodsSulfur-Based Synthesis Techniques