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Uranium nitride [U≡N]x is an alternative nuclear fuel that has great potential for the future of nuclear power; however, very little is known about the U≡N functionality. This presentation will show that for the first time a terminal uranium nitride complex can be generated through photolysis of an azide precursor. The transient U≡N fragment is reactive and undergoes insertion into a ligand C-H bond to generate new N-H and N-C bonds. The mechanism of this unprecedented reaction has been evaluated through computational and spectroscopic studies, which reveal that the photochemical azide activation pathway can be shut down through coordination of the terminal azide ligand to the Lewis acid B(C6F5)3. These studies demonstrate that photochemistry can be a powerful tool for inducing redox transformations for organometallic actinide complexes. Additional studies using alternate ligand frameworks led to new photochemical transformations. Recent developments in this area of chemistry will be presented. Host: Cristiano Nisoli, T-4, CNLS, cristiano@lanl.gov |