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. 2017 Mar 1;139(8):2916-2919.
doi: 10.1021/jacs.7b00002. Epub 2017 Feb 15.

Ammonia Oxidation by Abstraction of Three Hydrogen Atoms from a Mo-NH3 Complex

Papri Bhattacharya  1 , Zachariah M Heiden  2 , Eric S Wiedner  1 , Simone Raugei  1 , Nicholas A Piro  3 , W Scott Kassel  3 , R Morris Bullock  1 , Michael T Mock  1
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Ammonia Oxidation by Abstraction of Three Hydrogen Atoms from a Mo-NH3 Complex

Papri Bhattacharya et al. J Am Chem Soc. .

Abstract

We report ammonia oxidation by homolytic cleavage of all three H atoms from a [Mo-NH3]+ complex using the 2,4,6-tri-tert-butylphenoxyl radical to yield a Mo-alkylimido ([Mo═NR]+) complex (R = 2,4,6-tri-tert-butylcyclohexa-2,5-dien-1-one). Chemical reduction of [Mo═NR]+ generates a terminal Mo≡N nitride complex upon N-C bond cleavage, and a [Mo═NH]+ complex is formed by protonation of the nitride. Computational analysis describes the energetic profile for the stepwise removal of three H atoms from [Mo-NH3]+ and formation of [Mo═NR]+.

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