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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Reactions of Group V Transition Metal Oxide Cluster Ions with Ethane and Ethylene
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Reactions of Group V Transition Metal Oxide Cluster Ions with Ethane and Ethylene

机译：V族过渡金属氧化物簇离子与乙烷和乙烯的反应

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摘要

Reactions of mass-selected group V transition metal oxide cluster ions (V_Xo_Y~(+-), Nb_xO_y~(+-) and Ta_xO_y~(+-)) with ethane (C_2H_6) and ethylene (C_2H_4) were investigated. The major reaction channels observed during the reactions of C_2 hydrocarbons with M_Xo_Y~+ were association and oxygen transfer. The association channel, M_xO_yC_2H_n~+, where n = 4 or 6, was common to most of the group V transition metal oxide cluster cations examined. However, a reaction channel corresponding to the loss of an oxygen atom from the mass-selected metal oxide cluster, producing M_xO_(y-1)~+, was only observed during the reactions of (V_2O_5)_n~+, where n = 1,2, or 3, with ethane and ethylene and during the reactions of ethylene with Nb_2O_5~+. It is proposed that this reaction pathway is oxygen transfer from the mass-selected metal oxide cluster cation to the neutral hydrocarbon. This oxygen transfer channel is the major pathway observed during the course of reactions of V_2O_5~+, V_4O_(10)~+, and V_6O_(15)~+ with ethane and ethylene, but this reaction pathway is minor or nonexistent in the case of reactions of C_2H_6 and C_2H_4 with stoichiometrically equivalent niobium and tantalum oxide cluster cations. Additionally, the reactions of M_XO_y~- with C_2 hydrocarbons were also examined. In contrast tot he cation results, no reaction products were observed in studies of the interaction of group V transition metal oxide cluster anions with ethane and ethylene. The studies reveal that the identity of the metal, charge state, cluster stoichiometry, and geometric structure strongly influence the ability of the metal oxide cluster to transfer an oxygen atom to the neutral C_2 hydrocarbon.
机译：研究了质量选择的V组过渡金属氧化物簇离子（V_Xo_Y〜（+-），Nb_xO_y〜（+-）和Ta_xO_y〜（+-））与乙烷（C_2H_6）和乙烯（C_2H_4）的反应。 C_2烃与M_Xo_Y〜+反应过程中观察到的主要反应通道是缔合和氧转移。缔合通道M_xO_yC_2H_n〜+，其中n = 4或6，是所研究的大多数V族过渡金属氧化物簇阳离子所共有的通道。但是，仅在（V_2O_5）_n〜+反应期间观察到与从质量选择的金属氧化物簇中失去氧原子相应的反应通道，生成M_xO_（y-1）〜+，其中n = 1 ，2或3，与乙烷和乙烯一起，以及在乙烯与Nb_2O_5〜+反应期间。提出该反应途径是氧从质量选择的金属氧化物簇阳离子转移到中性烃。该氧气传输通道是V_2O_5〜+，V_4O_（10）〜+和V_6O_（15）〜+与乙烷和乙烯反应的过程中观察到的主要途径，但对于以下情况，该反应途径很小或不存在C_2H_6和C_2H_4与化学计量上等价的铌和钽氧化物簇阳离子的反应另外，还研究了M_XO_y〜-与C_2烃的反应。与阳离子结果相反，在研究V族过渡金属氧化物簇阴离子与乙烷和乙烯的相互作用时未观察到反应产物。研究表明，金属的身份，电荷状态，簇化学计量和几何结构强烈影响金属氧化物簇将氧原子转移至中性C_2烃的能力。

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