Litcius/Paper detail

Umpolung of an Aliphatic Ketone to a Magnesium Ketone‐1,2‐diide Complex with Vicinal Dianionic Charge

Stuart Burnett, Connor Bourne, Alexandra M. Z. Slawin, Tanja van Mourik, Andreas Stasch

2022Angewandte Chemie International Edition13 citationsDOIOpen Access PDF

Abstract

Abstract The new β‐diketimine i PrDip nacnacH, HC( i PrCNDip) 2 H, Dip=2,6‐ i Pr 2 ‐C 6 H 3 , was converted to the magnesium(I) complex [{( i PrDip nacnac)Mg} 2 ] and reaction with 2‐adamantanone (OAd) afforded the ketone‐1,2‐diide complex [{( i PrDip nacnac)Mg} 2 (μ‐OAd)]. The complex contains the first stable dianion of an aliphatic ketone with an electropositive metal and shows an OAd 2− unit with long C−O bond and pyramidal carbon centre. DFT studies reveal an anionic charge on both neighbouring C and O atoms. Reductions of aliphatic ketones with magnesium(I) complexes show that these likely proceed via highly reactive dianions and afforded a 1 : 1 mixture of an alkoxide and an enolate when an enolisable ketone was used, and rapid CH activations reactions, e.g., of stabilising ligand moieties, when non‐enolisable ketones were employed.

Topics & Concepts

KetoneChemistryUmpolungAlkoxideMagnesiumMedicinal chemistryLigand (biochemistry)AlkylNucleophileOrganic chemistryCatalysisBiochemistryReceptorCoordination Chemistry and OrganometallicsN-Heterocyclic Carbenes in Organic and Inorganic ChemistryOrganometallic Complex Synthesis and Catalysis