Mode-Specific Chemisorption of CH4 on Pt{110}-(1 x 2) Explored by First-Principles Molecular Dynamics
Mode-Specific Chemisorption of CH4 on Pt{110}-(1 x 2) Explored by First-Principles Molecular Dynamics
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DOI：
10.1021/jp207746q
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发表时间：
2011-11-10
影响因子：
3.7
通讯作者：
Jenkins, S. J.
中科院分区：
文献类型：
--
作者：
Sacchi, M.;Wales, D. J.;Jenkins, S. J.
通过对势能面定义的反应途径的振动分析，以及在时间反转中，通过对CH4缔合解吸的第一性原理分子动力学模拟，研究了CH4在Pt{110}-（1 × 2）上的化学吸附，并用密度泛函理论明确地处理了电子结构。我们发现对称伸缩振动v(1)与反应坐标强耦合；因此，我们的结果为最近报道的状态分辨反应性测量提供了坚实的理论基础，这些测量表明激发v(1)正模是增强反应的最有效方法。概率。
The chemisorption of CH4 on Pt{110}-(1 x 2) has been studied by vibrational analysis of the reaction pathway defined by the potential energy surface and, in time reversal, by first-principles molecular dynamics simulations of CH4 associative desorption, with the electronic structure treated explicitly using density functional theory. We find that the symmetric stretch vibration v(1) is strongly coupled to the reaction coordinate; our results therefore provide a firm theoretical basis for recently reported state-resolved reactivity measurements, which show that excitation of the v(1) normal mode is the most efficient, way to enhance the reaction. probability.