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After more than 50 years, the synthesis and electronic structure of the first and only reported “U0 complex” [U(bipy)4] (1) has been reinvestigated. Additionally, its one‐electron reduced product [Na(THF)6][U(bipy)4] (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...
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