Litcius/Paper detail

Dicationic Boron Derivatives of Schlenk’s and Thiele’s Hydrocarbon

Philipp Dabringhaus, Andrew Molino, Noah D. McMillion, Robert J. Gilliard

2025Journal of the American Chemical Society15 citationsDOI

Abstract

In recent years, neutral NHC-stabilized boryl radicals have been investigated as reactive species in various organic transformations. However, cationic boron radicals have been significantly less explored. In addition, boron-centered open-shell species with S > 1/2 have emerged as attractive synthetic targets. In this study, we provide a synthetic route to an NHC-stabilized boryl radical cation as a salt of the weakly coordinating [Al(OR F ) 4 ] − ( R F = C(CF 3 ) 3 ) anion. The synthetic procedure was extended to dicationic diboron derivatives of Schlenk’s and Thiele’s hydrocarbons with meta - and para -phenylene coupling units between the spin centers. While most known isolable boron biradicals have a singlet ground-state with a thermally accessible triplet state, the boron version of Schlenk’s hydrocarbon occupies a ground-state triplet spin-state, as shown by combined electron paramagnetic resonance spectroscopy and density functional theory studies. Furthermore, initial reactivity studies of the dications with elemental sulfur and diphenyldiselenide are presented.

Topics & Concepts

ChemistryBoronSinglet stateRadicalCationic polymerizationReactivity (psychology)Ground statePhotochemistryHydrocarbonBoron trichlorideElectron paramagnetic resonanceElectrophileTriplet stateComputational chemistryMedicinal chemistryInorganic chemistryMoleculeOrganic chemistryCatalysisNuclear magnetic resonanceMedicinePhysicsPathologyQuantum mechanicsNuclear physicsExcited stateAlternative medicineOrganoboron and organosilicon chemistryCatalytic Cross-Coupling ReactionsSynthesis and characterization of novel inorganic/organometallic compounds