Journal
INTERNATIONAL JOURNAL OF MASS SPECTROMETRY
Volume 195, Issue -, Pages 149-170Publisher
ELSEVIER SCIENCE BV
DOI: 10.1016/S1387-3806(99)00170-0
Keywords
bond activation; thermochemistry; niobium; transition metal ions; bond energies
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The kinetic energy dependence of the reactions of Nb+ (D-5) With methane, ethane, and propane have been studied using guided ion beam mass spectrometry. It is found that dehydrogenation is efficient and the dominant process at low energies in all three reaction systems. At high energies, products resulting from both C-H and C-C cleavage processes are appreciable. The observation of dihydride and hydride-methyl niobium cation products provides insight into the reaction mechanisms operating in these processes. The results for Nb+ are compared with those for the first-row transition metal congener V+ and the differences in behavior and mechanism discussed. Modeling of the endothermic reaction cross sections yields the 0 K bond dissociation energies (in electron volts) of D-0(Nb-H) > 2.3 +/- 0.1, D-0(Nb+-2H) = 4.64 +/- 0.06, D-0(Nb+-C) = 5.28 +/- 0.15, D-0(Nb+-CH) = 6.02 +/- 0.20, D-0(Nb+-CH2) = 4.44 +/- 0.09, D-0(Nb+-CH3) = 2.06 +/- 0.11, D-0[Nb+-(H)(CH3)] = 4.78 +/- 0.11, D-0(Nb+-C2H) = 4.34 +/- 0.19, D-0(Nb+-C2H2) = 2.90 +/- 0.06, D-0(Nb+-C2H3) = 3.43 +/- 0.21, D-0(Nb+-C2H4) = 2.8 +/- 0.3, D-0(Nb+-C2H5) = 2.45 +/- 0.12, D-0(Nb+-C3H2) = 5.25 +/- 0.19, and lower limits for D-0(Nb+- C3H3) greater than or equal to 3.76 +/- 0.23 and D-0(Nb+-C3H5) greater than or equal to 1.4 +/- 0.1. The observation of exothermic processes sets lower limits for the bond energies of Nb+ to propyne and propene of 2.84 and 1.22 eV, respectively. (C) 2000 Elsevier Science B.V.
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