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Single-Electron Oxidation of Carbene-Coordinated Pnictinidenes–Entry into Heteroleptic Radical Cations and Metalloid Clusters

Julia Krüger, Julia Haak, Christoph Wölper, George E. Cutsail, Gebhard Haberhauer, Stephan Schulz

2022Inorganic Chemistry24 citationsDOI

Abstract

Stable heavy main group element radicals are challenging synthetic targets. Although several strategies have been developed to stabilize such odd-electron species, the number of heavier pnictogen-centered radicals is limited. We report on a series of two-coordinated pnictogen-centered radical cations [(MecAAC)EGa(Cl)L][B(C6F5)4] (MecAAC = [H2C(CMe2)2NDipp]C; Dipp = 2,6-i-Pr2C6H3; E = As 1, Sb 2, Bi 3; L = HC[C(Me)NDipp]2) synthesized by one-electron oxidation of L(Cl)Ga-substituted pnictinidenes (MecAAC)EGa(Cl)L (E = As I, Sb II, Bi III). 1–3 were characterized by electron paramagnetic resonance (EPR) spectroscopy and single crystal X-ray diffraction (sc-XRD) (1, 2), while quantum chemical calculations support their description as carbene-coordinated pnictogen-centered radical cations. The low thermal stability of 3 enables access to metalloid bismuth clusters as shown by formation of [{LGa(Cl)}3Bi6][B(C6F5)4] (4).

Topics & Concepts

PnictogenChemistryElectron paramagnetic resonanceCarbeneRadicalMain group elementCrystallographyBismuthMetalloidTransition metalMetalOrganic chemistryNuclear magnetic resonanceCatalysisPhysicsQuantum mechanicsSuperconductivitySynthesis and characterization of novel inorganic/organometallic compoundsOrganoboron and organosilicon chemistryOrganometallic Complex Synthesis and Catalysis