Litcius/Paper detail

Isolation of an Annulated 1,4‐Distibabenzene Diradicaloid

Henric Steffenfauseweh, Dennis Rottschäfer, Yury V. Vishnevskiy, Beate Neumann, Hans‐Georg Stammler, Dariusz W. Szczepanik, Rajendra S. Ghadwal

2023Angewandte Chemie International Edition42 citationsDOIOpen Access PDF

Abstract

Abstract The first 1,4‐distibabenzene‐1,4‐diide compound [(ADC)Sb] 2 ( 5 ) based on an anionic dicarbene (ADC) (ADC=PhC{N(Dipp)C} 2 , Dipp=2,6‐ i Pr 2 C 6 H 3 ) is reported as a bordeaux‐red solid. Compound 5 , featuring a central six‐membered C 4 Sb 2 ring with formally Sb I atoms may be regarded as a base‐stabilized cyclic bis‐stibinidene in which each of the Sb atoms bears two lone‐pairs of electrons. 5 undergoes 2 e‐oxidation with Ph 3 C[B(C 6 F 5 ) 4 ] to afford [(ADC)Sb] 2 [B(C 6 F 5 ) 4 ] 2 ( 6 ) as a brick‐red solid. Each of the Sb atoms of 6 has an unpaired electron and a lone‐pair. The broken‐symmetry open‐shell singlet diradical solution for ( 6 ) 2+ is calculated to be 2.13 kcal mol −1 more stable than the closed‐shell singlet. The diradical character of ( 6 ) 2+ according to SS‐CASSCF (state‐specific complete active space self‐consistent field) and UHF (unrestricted Hartree‐Fock) methods amounts to 36 % and 39 %, respectively. Treatments of 6 with (PhE) 2 yield [(ADC)Sb(EPh)] 2 [B(C 6 F 5 ) 4 ] 2 ( 7 ‐E) (E=S or Se). Reaction of 5 with (cod)Mo(CO) 4 affords [(ADC)Sb] 2 Mo(CO) 4 ( 8 ).

Topics & Concepts

DiradicalLone pairUnpaired electronChemistrySinglet stateCrystallographyOpen shellStereochemistryExcited stateAtomic physicsMoleculePhysicsOrganic chemistrySynthesis and characterization of novel inorganic/organometallic compoundsOrganoboron and organosilicon chemistryOrganometallic Complex Synthesis and Catalysis