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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Intracluster Ion-Molecule Reactions of Ti~+ with Methanol Clusters
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Intracluster Ion-Molecule Reactions of Ti~+ with Methanol Clusters

机译：Ti〜+与甲醇团簇的团簇内离子分子反应

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摘要

The intracluster ion-molecule reactions occurring within the titanium/methanol heterocluster ions are studied using a simple cluster source based on the mixing of the laser-ablated plasma with the supersonic expansion of a methanol vapor seeded in Ar carrier gas. The product ions are detected using a reflectron time-of-flight mass spectrometer. The mass spectra exhibit a major sequence of cluster ions with the formula Ti~+(CH_3O)_2(CH_3-OH)_n, which are attributed to the hydrogen elimination reactions (-2H or -H_2) of Ti~+ ion within the heteroclusters. In addition, heterocluster ions of the types Ti~+(CH_3O)(CH_3OH)_n and Ti~+(CH_3O)_3(CH_3OH)_n also emerge throughout the observed mass spectra, indicating that consecutive H-eliminations by the Ti~+ ion occur for up to three methanol molecules. The results from isotope-labeling experiments suggest that H-elimination is the reaction path for O-H bond breaking in Ti~+-methanol heteroclusters. The observed TiOH~+ and TiO~+ ions are interpreted as arising from the insertion of Ti~+ ions into the C-O bond in CH_3OH, followed by CH_3- and CH_4-elimination, respectively, from the [HO-Ti~+-CH_3] intermediate. The experiments also show that the chemical reactivity of heterocluster ions is greatly influenced by cluster size and argon stagnation pressure. The reaction energetics and formation mechanisms of the observed heterocluster ions are also discussed.
机译：使用简单的簇源，基于激光烧蚀的等离子体与注入Ar载气中的甲醇蒸气的超音速膨胀的混合，研究了钛/甲醇杂簇离子中发生的簇内离子分子反应。使用反射电子飞行时间质谱仪检测产物离子。质谱显示簇离子的主要序列，分子式为Ti〜+（CH_3O）_2（CH_3-OH）_n，这归因于杂原子团中Ti〜+离子的氢消除反应（-2H或-H_2） 。此外，在整个观察到的质谱图中还会出现类型为Ti〜+（CH_3O）（CH_3OH）_n和Ti〜+（CH_3O）_3（CH_3OH）_n的杂簇离子，表明Ti〜+离子连续消除了H最多可出现三个甲醇分子。同位素标记实验结果表明，H-消除是Ti〜+-甲醇杂簇中O-H键断裂的反应路径。观察到的TiOH〜+和TiO〜+离子被解释为是由于将Ti〜+离子插入CH_3OH中的CO键中，然后分别从[HO-Ti〜+ -CH_3]中消除了CH_3-和CH_4-。 ]中级。实验还表明，杂簇离子的化学反应性受团簇大小和氩气停滞压力的很大影响。还讨论了所观察到的杂簇离子的反应能和形成机理。

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