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F(H2O)+CH3I Ligand Exchange Reaction Dynamics
Bj?rn Bastian, Tim Michaelsen, Milan On?ák, Jennifer Meyer, Roland Wester*
Institut für Ionenphysik und Angewandte Physik, Universit?t Innsbruck, Technikerstraβe 25, 6020 Innsbruck, Austria
Abstract:
Single hydration of the gas phase F?(H2O)+CH3I→[FCH3I]?+H2O reaction allows to probe solvent effects on a fundamental nucleophilic substitution reaction. At the same time, the addition of a solvent molecule opens alternative product channels. Here, we present crossed beam imaging results on the dynamics of the F?(H2O)+CH3I→[FCH3I]?+H2O ligand exchange pathway at collision energies between 0.3 and 2.6 eV. Product kinetic energies are constrained by the stability requirement of the weakly bound product complexes. This implies substantial internal excitation of the water molecule and disfavors effcient energy redistribution in an intermediate complex, which is reflected by the suppression of low kinetic energies as collision energy increases. At 0.3 eV, internal nucleophilic displacement is important and is discussed in light of the competing nucleophilic substitution pathways that form I? and I?(H2O).
Key words:  Reaction dynamics, Ligand exchange, Microsolvation, Crossed beams, Velocity map imaging
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Supplymentary:   CJCP2002018SP.pdf
F(H2O)+CH3I配体交换反应动力学
Bj?rn Bastian, Tim Michaelsen, Milan On?ák, Jennifer Meyer, Roland Wester*
奥地利因斯布鲁克大学离子物理与应用物理研究所,因斯布鲁克 6020
摘要:
本文介绍F?(H2O)+CH3I→[FCH3I]?+H2O在交叉分子束碰撞能量0.3∽2.6 eV的配体交换动力学成像结果. 产物的动能受到弱键结合配合物的稳定性的影响,大量水分子的内部激发不利于中间物有效的能量重新分配,随着碰撞增加,低动能受到抑制. 在0.3 eV时,内部亲核取代非常重要,为形成I?和I?(H2O)的竞争性亲核取代途径提供了依据.
关键词:  反应动力学,配体交换,微溶剂,分子束,速度成像
DOI:10.1063/1674-0068/cjcp2002018
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