Herein we report the first example of a mononuclear uranium complex, [U(NP(pip))] (1-U), that selectively reduces dioxygen to produce a terminal oxo complex, [UO(NP(pip))] (2-U; [NP(pip)] is tris(piperidinyl)imidophosphorane). Reactions between 1-U and the heavier elemental chalcogens, S or Se, result in six-coordinate U(VI) complexes, [U(κ-E)(NP(pip))] (E = S (3-U) or Se (4-U)).
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