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首页> 美国卫生研究院文献>Proceedings of the National Academy of Sciences of the United States of America >Chemical Dynamics Special Feature: Chemical dynamics of vibrationally excited molecules: Controlling reactions in gases and on surfaces
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Chemical Dynamics Special Feature: Chemical dynamics of vibrationally excited molecules: Controlling reactions in gases and on surfaces

机译：化学动力学特性：振动激发分子的化学动力学：控制气体和表面上的反应

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摘要

Experimental studies of the chemical reaction dynamics of vibrationally excited molecules reveal the ability of different vibrations to control the course of a reaction. This Perspective describes those studies for the prototypical reaction of vibrationally excited methane and its isotopologues in gases and on surfaces and looks to the prospects of similar studies in liquids. The influences of vibrational excitation on the CH bond cleavage in a single collision reaction with Cl and in dissociative adsorption on a Ni surface bear some striking similarities. Both reactions are bond-selective processes in which the initial preparation of a molecular eigenstate containing a large component of CH stretching results in preferential cleavage of that bond. It is possible to cleave either the CH bond or CD bond in the reaction of Cl with CH3D, CH2D2, or CHD3 and, similarly, to use initial excitation of the CH stretch to promote dissociation of CHD3 to CD3 and H on a Ni surface. Different vibrational modes, such as the symmetric and antisymmetric stretches in CH3D or CH4, lead to very different reactivities, and molecules with the symmetric stretching vibration excited can be as much as 10 times more reactive than ones with the antisymmetric stretch excited. The origin of this behavior lies in the change in the vibrational motion induced by the interaction with the atomic reaction partner or the surface.
机译：振动激发分子的化学反应动力学的实验研究揭示了不同振动控制反应过程的能力。本《观点》描述了有关在气体和表面上振动激发的甲烷及其同位素异构体的原型反应的研究，并展望了在液体中进行类似研究的前景。在与Cl的单次碰撞反应中以​​及在Ni表面的解离吸附中，振动激发对CH键断裂的影响具有某些惊人的相似之处。这两个反应都是键选择过程，其中最初制备包含CH拉伸大部分成分的分子本征态会导致该键的优先裂解。在Cl与CH3D，CH2D2或CHD3的反应中，有可能断裂CH键或CD键，并且类似地，使用CH链的初始激发来促进CHD3分解为Ni表面上的CD3和H。不同的振动模式（例如CH3D或CH4中的对称和反对称拉伸）会导致非常不同的反应性，受对称拉伸振动激发的分子的反应性可能比受反对称拉伸激发的分子高10倍。这种行为的根源在于与原子反应伙伴或表面相互作用引起的振动运动的变化。

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