- ELSEVIER SCIENCE BV
Reactions of vanadium and niobium nitride cluster cations, V(n)Nm(+) and NbnNm+ (n = 3-6; m = n, n-1), with NH3 were studied using a guided ion beam tandem mass spectrometer. Two main reactions are observed at a near-thermal energy under single collision conditions: simple adsorption of NH3 and adsorption of decomposed NH (i.e., dehydrogenation of NH3). The total reaction cross section and the branching fraction between these two reactions change significantly with the number of atoms and the composition of the cluster. The specific equiatomic vanadium nitride clusters, V4N4+ and V6N6+, are relatively inert and exhibit only simple NH3 adsorption with low probabilities, which can be understood by considering the stable structures (cube and cuboid) resembling subunits of bulk VN. In contrast, most of the other clusters including Nb4N4+ are found to be highly reactive and give rise to the NH3 dehydrogenation. The multiple collision reactions of NbnNm+ with (n,m)= (3,2), (4,3), and (4,4) result in the complete dehydrogenation of ammonia to give the product ions of NbnNmN2+. (C) 2016 Published by Elsevier B.V.
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