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Overriding Norrish Type II to Access Cyclopropanols

James W. Pearson, Samantha L. Dudra, Anthony F. Palermo, B Chiu, Julie Dang, Alexis L. Gabbey, Bridget A. B. Henson, Teh Ren Hou, Negin Nabavi, Sophie A. L. Rousseaux

2025Journal of the American Chemical Society9 citationsDOI

Abstract

The propensity for photoexcited aryl ketones to undergo 1,5-hydrogen atom transfer (HAT) reactions is a fundamental process in organic synthesis and polymer degradation. Since its discovery in 1958, Norrish-Yang photocyclization has become a prominent method to access cyclobutanols under mild photoirradiative conditions. Despite its successful extension to larger ring systems, access to medicinally relevant 3-membered rings remains limited due to the strong kinetic preference for 1,5-HAT over 1,4-HAT. In this work, we demonstrate the first photocyclization of β-boryl aryl ketones to cyclopropanols. Our strategy relies on solvent-controlled selective population of the π,π* triplet state over the n,π* triplet state, with the former preferentially undergoing 1,4-boryl group transfer over 1,5-HAT. This protocol proceeds under mild irradiative conditions with excellent functional group tolerance, providing access to a broad range of highly valuable cyclopropanol scaffolds.

Topics & Concepts

ChemistryArylRing (chemistry)PopulationAtom (system on chip)Combinatorial chemistryCarbonyl groupFunctional groupComputational chemistryPhotochemistryStereochemistryGroup (periodic table)Electron transferLeaving groupRange (aeronautics)Reaction mechanismRadical Photochemical ReactionsOrganic Chemistry Cycloaddition ReactionsCyclopropane Reaction Mechanisms
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