LAUSR

Abstract Reaction of [UO2Cl2(THF)2]2 with 8 equiv of Li(N=CtBuPh) or 6 equiv of Li(N=CtBu2) affords the uranyl ketimide complexes, [Li(THF)(Et2O)]2[UO2(N=CtBuPh)4] (1) and [Li(THF)(TMEDA)][UO2(N=CtBu2)3] (2), respectively. Complexes 1 and 2 have been fully characterized, including analysis by X-ray crystallography. Most importantly, both complexes feature dative interactions between their lithium counterions and the uranyl oxo ligands. These interactions are likely a consequence of their weaker UO bonds, which are caused by electrostatic repulsion between the anionic N donor atom of the strongly electron donating ketimide ligand and the oxo ligand of the uranyl fragment.