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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Reactions of Tantalum Oxide Cluster Cations with 1-Butene, 1,3-Butadiene, and Benzene
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Reactions of Tantalum Oxide Cluster Cations with 1-Butene, 1,3-Butadiene, and Benzene

机译：氧化钽簇阳离子与1-丁烯，1,3-丁二烯和苯的反应

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摘要

Branching ratios for the reactions of 1-butene, 1,3-butadiene, and benzene with stoichiometric tantalum oxide clusters (TaO_(2-3)~+, Ta_2O_(4-5)~+, and Ta_3O_(7-8)~+) are reported. The major reaction product for most of the clusters is cracking of the C2-C3 bond of 1-butene and 1,3-butadiene to produce Ta_xO_yC_2H_4~+. Additionally, Ta_2O_4~+ was the most reactive cluster toward cracking the C2-C3 bond of both 1-butene and 1,3-butadiene. For a majority of these clusters there were additional cracking channels to produce Ta_xO_yCH_3~+ and Ta_xO_yC_3H_z~+, where z = 5 - 6, which occur under multiple collision conditions for 1-butene and 1,3-butadiene. Under multiple collision conditions, TaO_2~+, Ta_2O_4~+, and Ta_3O_7~+ exhibited the reaction channels of Ta_xO_yC_5H_9~+ and Ta_xO_yC_6H_(10)~+ when reacted with 1-butene. In reactions with 1,3-butadiene, secondary reaction channels of Ta_xO_yC_5H_7~+ and Ta_xO_yC_6H_8~+ were also observed for TaO_2~+, Ta_2O_(4-5)~+, Ta_3O_7~+. Additionally, under multiple collision conditions, TaO_2~+ and Ta_2O_4~+ also displayed reaction channels of Ta_xO_yC_7H_9~+ and Ta_xO_yC_8H_(10)~+. Reactions of most of the stoichiometric tantalum oxide clusters with benzene showed a cracking channel forming Ta_xO_yC_4H_4~+ and a dehydration channel to form Ta_xO_(y-1)C_6H_4~+. The most reactive cluster toward cracking benzene was Ta_3O_8~+, and the most reactive cluster toward the dehydration reaction was TaO_2~+. Reactions of the aforementioned unsaturated hydrocarbons with oxygen-rich clusters (TaO_(4-5)~+, Ta_2O_(6-7)~+, and Ta_3O_(9-10)~+) are also reported. The major reaction channel of most of these clusters involves loss of molecular oxygen to form the smaller, more stable stoichiometric clusters, which then proceed to react with or associate the hydrocarbon gas.
机译：1-丁烯，1,3-丁二烯和苯与化学计量的氧化钽簇（TaO_（2-3）〜+，Ta_2O_（4-5）〜+和Ta_3O_（7-8）〜的反应的支化比+）被报告。大多数簇的主要反应产物是1-丁烯和1,3-丁二烯的C2-C3键裂解生成Ta_xO_yC_2H_4〜+。另外，Ta_2O_4〜+是最易断裂1-丁烯和1,3-丁二烯C2-C3键的簇。对于大多数这些团簇，存在额外的裂化通道以产生Ta_xO_yCH_3〜+和Ta_xO_yC_3H_z〜+，其中z = 5-6，它们在1-丁烯和1,3-丁二烯的多种碰撞条件下发生。在多种碰撞条件下，TaO_2〜+，Ta_2O_4〜+和Ta_3O_7〜+与1-丁烯反应时均显示出Ta_xO_yC_5H_9〜+和Ta_xO_yC_6H_（10）〜+的反应通道。在与1,3-丁二烯的反应中，还观察到Ta_xO_yC_5H_7〜+和Ta_xO_yC_6H_8〜+的次要反应通道TaO_2〜+，Ta_2O_（4-5）〜+，Ta_3O_7〜+。另外，在多个碰撞条件下，TaO_2〜+和Ta_2O_4〜+还显示了Ta_xO_yC_7H_9〜+和Ta_xO_yC_8H_（10）〜+的反应通道。大多数化学计量的氧化钽簇与苯的反应显示出形成Ta_xO_yC_4H_4〜+的裂化通道和形成Ta_xO_（y-1）C_6H_4〜+的脱水通道。裂解苯中反应性最高的簇是Ta_3O_8〜+，脱水反应中反应性最高的簇是TaO_2〜+。还报道了上述不饱和烃与富氧簇（TaO_（4-5）〜+，Ta_2O_（6-7）〜+和Ta_3O_（9-10）〜+）的反应。这些簇中大多数的主要反应通道涉及分子氧的损失，以形成更小，更稳定的化学计量簇，然后使之与烃类气体发生反应或缔合。

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