Article Dans Une Revue Journal of the American Chemical Society Année : 2022

Reactivity of Multimetallic Thorium Nitrides Generated by Reduction of Thorium Azides

Résumé

Thorium nitrides are likely intermediates in the reported cleavage and functionalization of dinitrogen by molecular thorium complexes and are attractive compounds for the study of multiple bond formation in f-element chemistry, but only one example of thorium nitride isolable from solution was reported. Here, we show that stable multimetallic azide/nitride thorium complexes can be generated by reduction of thorium azide precursors.a route that has failed so far to produce Th nitrides. Once isolated, the thorium azide/nitride clusters, M3Th = N = Th (M = K or Cs), are stable in solutions probably due to the presence of alkali ions capping the nitride, but their synthesis requires a careful control of the reaction conditions (solvent, temperature, nature of precursor, and alkali ion). The nature of the cation plays an important role in generating a nitride product and results in large structural differences with a bent Th = N = Th moiety found in the K-bound nitride as a result of a strong K-nitride interaction and a linear arrangement in the Cs-bound nitride. Reactivity studies demonstrated the ability of Th nitrides to cleave CO in ambient conditions yielding CN-.

Dates et versions

hal-03714653 , version 1 (05-07-2022)

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Citer

Fang-Che Hsueh, Luciano Barluzzi, Megan Keener, Thayalan Rajeshkumar, Laurent Maron, et al.. Reactivity of Multimetallic Thorium Nitrides Generated by Reduction of Thorium Azides. Journal of the American Chemical Society, 2022, 144 (7), pp.3222-3232. ⟨10.1021/jacs.1c13150⟩. ⟨hal-03714653⟩
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