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The synthesis and structure of the uranium(IV) compound UI2(OCH2CH2CH2CH2I)2(Ph3PO)2 (1) is described. Compound 1 is formed from the ring opening of THF from UI4(CH3CN)4.

The uranium(III) iodide complex UI 3 (THF) 4 reacts cleanly at ambient temperature with 1 equiv of sodium and potassium pentamethylcyclopentadienide salts in tetrahydrofuran to form the mono-ring uranium(III) complex (η-C 5 Me 5 )UI 2 (THF) 3 (1). Additionally, reaction of UI 3 (THF) 4 with 2 equiv or more of K(C 5 Me 5 ) in THF solution leads to the formation of the bis-ring adduct (η-C 5 Me 5 ) 2 UI(THF) (2) in high yield. In the solid state 1 exhibits a pseudooctahedral mer,trans ligand geometry with the C 5 Me 5 ligand occupying one axial position. U-I bond lengths range from 3.161(1) to 3.179(1) Å, while U-O distances to the THF ligands lie in the range 2.496(8)-2.594(10) Å. 1 also provides a convenient entry into a variety of other mono-ring complexes of uranium(III). In the presence of excess pyridine, the coordinated THF ligands of 1 are readily displaced to form the tris(pyridine) adduct (η-C 5 Me 5 )UI 2 (py) 3 (3), which exhibits a mer,trans ligand geometry in the solid state similar to that of 1. Metathesis of the iodide ligands in 1 with 2 equiv of KN(SiMe 3 ) 2 affords the bis(amido) complex (η-C 5 Me 5 )U[N(SiMe 3 ) 2 ] 2 (4). An X-ray diffraction study of this molecule reveals that methyl groups from both amido ligands are involved in agostic interactions with the uranium-(III) center.