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间位取代酚的光化学排列

Photochemical permutation of meta-substituted phenols.

作者信息

Alonso Maialen, Lonardi Giovanni, Arpa Enrique M, Roure Baptiste, Ruffoni Alessandro, Leonori Daniele

机构信息

Institute of Organic Chemistry, RWTH Aachen University, Aachen, Germany.

Department of Chemistry, University of Manchester, Manchester, UK.

出版信息

Nat Commun. 2025 Aug 13;16(1):7502. doi: 10.1038/s41467-025-62549-5.

Abstract

Phenols and their derivatives are highly relevant motifs in pharmaceuticals, natural products, and other functional materials. Conventional strategies for phenol synthesis rely on classical aromatic functionalization, which is often dictated by electronic and steric factors. Herein, we report an alternative approach for phenol synthesis where irradiation in the presence of Lewis or Brønsted acids enables the selective migration of alkyl and aryl groups from meta to either the ortho or para positions. This method exploits the intrinsic photochemical properties of phenolic arenium ions and their rearrangement via 4π electrocyclization and following "1,2-methylene shift". By leveraging selective photoexcitation of these species, we can achieve precise control over the directionality of the permutation process. Specifically, short-wavelength irradiation (λ = 310 nm) promotes meta→para migration, while longer-wavelength irradiation (λ = 390 nm) meta→ortho. This approach offers a late-stage method to use readily available phenols as templates for the preparation of other isomers without de novo synthesis. The applicability of the method has been demonstrated on the isomerization of poly-substituted derivatives including some bioactive species.

摘要

酚类及其衍生物是药物、天然产物和其他功能材料中高度相关的结构单元。传统的酚合成策略依赖于经典的芳香族官能团化反应,这通常受电子和空间因素的支配。在此,我们报道了一种酚合成的替代方法,即在路易斯酸或布朗斯特酸存在下进行光照,能够使烷基和芳基从间位选择性迁移至邻位或对位。该方法利用了酚鎓离子的固有光化学性质及其通过4π电环化和随后的“1,2-亚甲基迁移”进行的重排。通过利用这些物种的选择性光激发,我们可以实现对排列过程方向性的精确控制。具体而言,短波长光照(λ = 310 nm)促进间位→对位迁移,而长波长光照(λ = 390 nm)促进间位→邻位迁移。这种方法提供了一种后期方法,可将现成的酚用作模板来制备其他异构体,而无需从头合成。该方法的适用性已在包括一些生物活性物种在内的多取代衍生物的异构化反应中得到证明。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7f0c/12350626/8222235b7471/41467_2025_62549_Fig1_HTML.jpg

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