After more than 50 years, the synthesis and electronic structure of the first and only reported "U complex" [U(bipy) ] (1) has been reinvestigated. Additionally, its one-electron reduced product [Na(THF) ][U(bipy) ] (2) has been newly discovered. High resolution crystallographic analyses combined with magnetic and computational data show that 1 and its derivative 2 are best described as highly reduced species containing mid-to-high-valent uranium ligated by redox non-innocent ligands.
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