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JOURNAL ARTICLE
RESEARCH SUPPORT, NON-U.S. GOV'T
RESEARCH SUPPORT, U.S. GOV'T, NON-P.H.S.
Ammonia Activation, H 2 Evolution and Nitride Formation from a Molybdenum Complex with a Chemically and Redox Noninnocent Ligand.
Journal of the American Chemical Society 2017 May 4
Treatment of the bis(imino)pyridine molybdenum η6 -benzene complex (iPr PDI)Mo(η6 -C6 H6 ) (iPr PDI, 2,6-(2,6-iPr2 C6 H3 N═CMe)2 C5 H3 N) with NH3 resulted in coordination induced haptotropic rearrangement of the arene to form (iPr PDI)Mo(NH3 )2 (η2 -C6 H6 ). Analogous η2 -ethylene and η2 -cyclohexene complexes were also synthesized, and the latter was crystallographically characterized. All three compounds undergo loss of the η2 -coordinated ligand followed by N-H bond activation, bis(imino)pyridine modification, and H2 loss. A dual ammonia activation approach has been discovered whereby reversible M-L cooperativity and coordination induced bond weakening likely contribute to dihydrogen formation. Significantly, the weakened N-H bonds in (iPr PDI)Mo(NH3 )2 (η2 -C2 H4 ) enabled hydrogen atom abstraction and synthesis of a terminal nitride from coordinated ammonia, a key step in NH3 oxidation.
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