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Mullane, Kimberly C.,Ryu, Ho,Cheisson, Thibault,Grant, Lauren N.,Park, Ji Young,Manor, Brian C.,Carroll, Patrick J.,Baik, Mu-Hyun,Mindiola, Daniel J.,Schelter, Eric J. American Chemical Society 2018 JOURNAL OF THE AMERICAN CHEMICAL SOCIETY - Vol.140 No.36
<P>Uranium complexes in the +3 and +4 oxidation states were prepared using the anionic PN<SUP>-</SUP> (PN<SUP>-</SUP> = (<I>N</I>-(2-(diisopropylphosphino)-4-methylphenyl)-2,4,6-trimethylanilide) ligand framework. New complexes include the halide starting materials, (PN)<SUB>2</SUB>U<SUP>III</SUP>I (<B>1</B>) and (PN)<SUB>2</SUB>U<SUP>IV</SUP>Cl<SUB>2</SUB> (<B>2</B>), which both yield (PN)<SUB>2</SUB>U<SUP>IV</SUP>(N<SUB>3</SUB>)<SUB>2</SUB> (<B>3</B>) by reaction with NaN<SUB>3</SUB>. Compound <B>3</B> was reduced with potassium graphite to produce a putative, transient uranium-nitrido moiety that underwent an intramolecular C-H activation to form a rare example of a parent imido complex, [K(THF)<SUB>3</SUB>][(PN)U<SUP>IV</SUP>(═NH)[<SUP><I>i</I></SUP>Pr<SUB>2</SUB>P(C<SUB>6</SUB>H<SUB>3</SUB>Me)N(C<SUB>6</SUB>H<SUB>2</SUB>Me<SUB>2</SUB>CH<SUB>2</SUB>)]] (<B>4</B>). Calculated reaction energy profiles strongly suggest that a C-H insertion becomes unfavorable when a reductant is present, offering a distinctively different reaction pathway than previously observed for other uranium nitride complexes.</P> [FIG OMISSION]</BR>