Litcius/Paper detail

N‐Heterocyclic Carbene‐Assisted Reversible Migratory Coupling of Aminoborane at Magnesium

D. Akachukwu, Nathan C. Frey, Diane A. Dickie, Charles Edwin Webster, Robert J. Gilliard

2022Angewandte Chemie International Edition11 citationsDOI

Abstract

Abstract A combined synthetic and theoretical investigation of N‐heterocyclic carbene (NHC) adducts of magnesium amidoboranes is presented, which involves a rare example of reversible migratory insertion within a normal valent s ‐block element. The reaction of (NHC)Mg(N(SiMe 3 ) 2 ) 2 ( 1 ) and dimethylamine borane yields the tris(amide) adduct (NHC−BN)Mg(NMe 2 BH 3 )(N(SiMe 3 ) 2 ) ( 2 ; NHC−BN = NHC−BH 2 NMe 2 ). In addition to Me 2 N=BH 2 capture at the NHC C−Mg bond, mechanistic investigations suggest the likelihood of aminoborane migratory insertion from an RMg(NMe 2 BH 2 NMe 2 BH 3 ) intermediate. To elucidate these processes, the carbene complexes (NHC)Mg(NMe 2 BH 3 ) 2 ( 8 ) and (NHC)Mg(NMe 2 BH 2 NMe 2 BH 3 ) 2 ( 9 ) were synthesized, and a dynamic migration of Me 2 N=BH 2 between Mg−N and NHC C−Mg bonds was observed in 9 . This unusual reversible migratory insertion is presumably induced by dissimilar charge localization in the − {NMe 2 BH 2 NMe 2 BH 3 } anion, as well as the capacity of NHCs to reversibly capture Me 2 N=BH 2 in the presence of Lewis acidic magnesium species.

Topics & Concepts

ChemistryCarbeneDimethylamineAdductBoraneMedicinal chemistryMigratory insertionMagnesiumInsertion reactionStereochemistryAmideOrganic chemistryCatalysisHydrogen Storage and MaterialsOrganoboron and organosilicon chemistrySynthesis and characterization of novel inorganic/organometallic compounds