Dynamics of interfacial reactions between O(3P) atoms and long-chain liquid hydrocarbons
Dynamics of interfacial reactions between O(3P) atoms and long-chain liquid hydrocarbons
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DOI：
10.1088/0031-8949/76/3/n06
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发表时间：
2007-09-01
期刊：
影响因子：
2.9
通讯作者：
McKendrick, Kenneth G.
中科院分区：
文献类型：
--
作者：
Allan, Mhairi;Bagot, Paul A. J.;McKendrick, Kenneth G.
简要总结了近年来在理解气液界面碰撞动力学方面所取得的进展。在这种情况下，我们描述了一种有前途的新方法来实验研究气液界面反应，我们已经介绍了。这是基于液体表面以上的反应性气相原子的激光光解产生和由此产生的新生产物的激光光谱探测。该技术用于长链液态烃角鲨烷（2,6,10,15,19,23-六甲基四烷）表面O（P-3）原子的反应。激光诱导荧光检测新生氢氧根揭示了其内部和平移能量分布之间的机械诊断相关性。振动激发的OH分子能够逃离表面。至少有两个贡献的产品旋转分布被确定，确认和扩展了之前的假设参与直接和捕获-解吸机制。我们简要地推测了未来的实验和理论发展，这可能是解决许多目前尚未解决的机制问题所必需的，以及其他类型的气液界面反应。
Recent progress that has been made towards understanding the dynamics of collisions at the gas-liquid interface is summarized briefly. We describe in this context a promising new approach to the experimental study of gas-liquid interfacial reactions that we have introduced. This is based on laser-photolytic production of reactive gas-phase atoms above the liquid surface and laser-spectroscopic probing of the resulting nascent products. This technique is illustrated for reaction of O(P-3) atoms at the surface of the long-chain liquid hydrocarbon squalane ( 2,6,10,15,19,23-hexamethyltetracosane). Laser-induced fluorescence detection of the nascent OH has revealed mechanistically diagnostic correlations between its internal and translational energy distributions. Vibrationally excited OH molecules are able to escape the surface. At least two contributions to the product rotational distributions are identified, confirming and extending previous hypotheses of the participation of both direct and trapping-desorption mechanisms. We speculate briefly on future experimental and theoretical developments that might be necessary to address the many currently unanswered mechanistic questions for this, and other, classes of gas-liquid interfacial reaction.