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Copper-Catalyzed Aerobic Aminooxygenation of Cinnamyl <i>N</i> -Alkoxycarbamates via Substrate-Promoted Catalyst Activation

Caitlyn P. McNichol, Ethan M. DeCicco, Amanda M. Canfield, Daniel P. Carstairs, Shauna M. Paradine

2023ACS Catalysis16 citationsDOIOpen Access PDF

Abstract

High Resolution Image Download MS PowerPoint Slide We report a method for a ligand-enabled, copper-catalyzed aerobic aminooxygenation of internal alkenes. The synergistic combination of a phenanthroline-based ligand and substrate coordination promotes reduction of Cu(II) to Cu(I), resulting in a cyclization that proceeds via an amidyl radical pathway rather than a previously established aminocupration pathway. The complementary reactivity enabled by this switch in reaction mechanism provides access to different substrate classes and a considerably broadened scope for this transformation. Experimental evidence supports a free radical mechanism involving substrate-promoted reduction to Cu(I) as well as the role of O 2 as both oxidant and functionalizing agent.

Topics & Concepts

CatalysisChemistrySubstrate (aquarium)Reactivity (psychology)Ligand (biochemistry)CopperCombinatorial chemistryRadicalReaction mechanismPhotochemistryOrganic chemistryReceptorBiochemistryPathologyOceanographyAlternative medicineMedicineGeologySynthesis and Catalytic ReactionsCatalytic C–H Functionalization MethodsSulfur-Based Synthesis Techniques