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Oxidation of [Li(THF)]2[Co(NCtBu2)4] with 1 equiv. of I2 generates Co(NCtBu2)4 in 85% yield. In the solid-state, this complex exhibits a squashed tetrahedral structure about the Co center. DFT calculations reveal this geometry arises, in part, to maximize ketimide-to-cobalt π-donation.
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