Ammonia Dehydrogenation on Cobalt Cluster Cations Doped with Niobium
Reactivity of bimetallic cobalt-niobium cluster cations, Co n Nb m + (n = 1–4, 6; m = 1–3), toward ammonia was investigated at near thermal energy using a guided ion beam tandem mass spectrometer. The dehydrogenation of NH3 is dominantly observed in the single-collision reactions of all the bimetallic clusters studied here. Most of the clusters containing one niobium atom, Co n Nb+, exhibit large cross sections for the NH3 dehydrogenation compared to the corresponding single-element clusters, Co n+1 + and Nb n+1 +. Density functional theory calculations reveal that both the transition states involved in the first and the second cleavages of N–H bonds of NH3 are significantly stabilized for Co4Nb+, which gives rise to the higher reactivity toward the NH3 dehydrogenation. The multiple-collision reactions of Co n Nb+ (n = 3, 4, and 6) result in the formation of Co n NbN2 +, which can be generated via complete dehydrogenation of two NH3 molecules, in addition to the formation of Co n NbN x H x +.
Publisher URL: https://link.springer.com/article/10.1007/s11244-017-0861-6
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