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EPR Studies on the Addition of Ligated Boryl Radicals to Carbonyl Compounds

John C. Walton, Wen Dai, Dennis P. Curran

2020The Journal of Organic Chemistry15 citationsDOIOpen Access PDF

Abstract

-heterocyclic carbene (NHC)-boranes bearing ester substituents were recently found to ring close in 5-endo mode by addition to the oxygen atoms of the ester substituents. The inference from this was that NHC-boryl radicals might add intermolecularly to carbonyl-containing substrates. Several different NHC-boryl radicals were generated by H-atom abstraction from NHC-ligated trihydroborates. Electron paramagnetic resonance (EPR) spectroscopy proved that these did indeed add to the oxygen atoms of diaryl ketones with production of the corresponding bora-ketyl radicals. The same unusual regioselectivity of addition was observed with monoaryl ketones, but no bora-ketyls were observed with dialkyl ketones. Similarly, no bora-ketyl adduct radicals were observed with esters, even esters of benzoic acid. EPR spectroscopic evidence suggested that NHC-boryl radicals were also added to the O-atoms of aromatic aldehydes. Amine-boryl and phosphine-boryl radicals were also observed to add to the O-atom of benzophenone with production of the corresponding ketyl radicals.

Topics & Concepts

KetylRadicalChemistryBenzophenoneElectron paramagnetic resonancePhotochemistryRegioselectivityMedicinal chemistryAdductOrganic chemistryCatalysisNuclear magnetic resonancePhysicsOrganoboron and organosilicon chemistryRadical Photochemical ReactionsCatalytic Cross-Coupling Reactions
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