Halogen bonding-induced 1,3-carbohydroxylation of allyl carboxylates <i>via</i> 1,2-cationic acyloxy migration (1,2-CAM)

Halogen bonding has emerged as a powerful yet underexplored tool for modulating radical reactivity. Here we demonstrate that halogen-bonding interactions between alkyl iodides and water can lower the C-I bond dissociation energy, enabling visible-light-induced photolysis to generate alkyl radicals under mild conditions. Harnessing this activation mode, we achieved a previously unknown 1,3-carbohydroxylation of allyl carboxylates, wherein radical addition is coupled with 1,2-cationic acyloxy migration (CAM) to furnish β-acyloxy alcohols. The transformation exhibits broad structural tolerance, accommodating diverse esters, thioesters, amides, and perfluoroalkyl iodides, and is effective in the late-stage diversification of natural products and drug-derived scaffolds. Mechanistic studies, including isotopic labeling, radical trapping, UV-vis spectroscopy, and DFT calculations, reveal a pathway in which halogen bonding initiates radical alkene addition, followed by rearrangement and carbocation capture. These findings showcase halogen-bonding-assisted photochemistry as a viable platform for radical-cationic cascades, opening new opportunities for reaction development.

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Publication Details

Journal
Chemical Science
Published
2025-12-24
DOI
https://doi.org/10.1039/d5sc08514d
Primary Topic
Radical Photochemical Reactions
Type
article
Field-Weighted Citation Impact
0.00

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article

Halogen bonding-induced 1,3-carbohydroxylation of allyl carboxylates via 1,2-cationic acyloxy migration (1,2-CAM)

Djamaladdin G. Musaev, Ming‐Yu Ngai, Arman Khosravi, Sahil Sharma et al.
Chemical Science
Radical Photochemical Reactions
article

Halogen bonding-induced 1,3-carbohydroxylation of allyl carboxylates via 1,2-cationic acyloxy migration (1,2-CAM)

Djamaladdin G. Musaev, Ming‐Yu Ngai, Arman Khosravi, Sahil Sharma, Loay Bedda, Gaoyuan Zhao
article en

Abstract

Halogen bonding has emerged as a powerful yet underexplored tool for modulating radical reactivity. Here we demonstrate that halogen-bonding interactions between alkyl iodides and water can lower the C-I bond dissociation energy, enabling visible-light-induced photolysis to generate alkyl radicals under mild conditions. Harnessing this activation mode, we achieved a previously unknown 1,3-carbohydroxylation of allyl carboxylates, wherein radical addition is coupled with 1,2-cationic acyloxy migration (CAM) to furnish β-acyloxy alcohols. The transformation exhibits broad structural tolerance, accommodating diverse esters, thioesters, amides, and perfluoroalkyl iodides, and is effective in the late-stage diversification of natural products and drug-derived scaffolds. Mechanistic studies, including isotopic labeling, radical trapping, UV-vis spectroscopy, and DFT calculations, reveal a pathway in which halogen bonding initiates radical alkene addition, followed by rearrangement and carbocation capture. These findings showcase halogen-bonding-assisted photochemistry as a viable platform for radical-cationic cascades, opening new opportunities for reaction development.

Chemical ScienceVol. 17(7)
Emory University (US), Purdue University West Lafayette (US)
National Science Foundation, Purdue University, Emory University, University of Pittsburgh, National Institutes of Health, Center for Research Computing, University of Pittsburgh, Office of Advanced Cyberinfrastructure, Division of Chemistry
Openalex Percentile: Top 33%
Radical Photochemical Reactions
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Halogen bonding-induced 1,3-carbohydroxylation of allyl carboxylates <i>via</i> 1,2-cationic acyloxy migration (1,2-CAM) — Djamaladdin G. Musaev, Ming‐Yu Ngai, et al. · Chemical Science (2025) | TGRS Research Map | TGRS