Unrestricted study of the Eley-Rideal formation of H(2) on graphene using a new multidimensional graphene-H-H potential: role of the substrate.
Unrestricted study of the Eley-Rideal formation of H(2) on graphene using a new multidimensional graphene-H-H potential: role of the substrate.
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使用新的多维石墨烯-H-H 势对石墨烯上 H(2) 的 Eley-Rideal 形成进行无限制研究：基材的作用。
DOI：
10.1039/b818614f
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发表时间：
2009
期刊：
影响因子：
--
通讯作者：
V. Sidis
中科院分区：
文献类型：
--
作者：
D. Bachellerie;M. Sizun;F. Aguillon;D. Teillet;N. Rougeau;V. Sidis
布伦纳势适用于处理石墨烯表面氢原子的化学相互作用和反应。调整后的势再现了 DFT 计算数据的几个重要特征，并揭示了表面吸附 H 原子时的扩展褶皱。该势用于以比以前更现实的方式进行研究，Eley-Rideal 抽象反应在 H + H-石墨烯碰撞中以能量 E(col)< 或 = 0.2 eV 产生 H(2)。石墨烯表面由 200 个碳原子组成的板代表，研究是使用经典分子动力学在以化学吸附轴为中心的圆柱体中垂直入射进行的。本研究的一个亮点是，当气相 H 原子到达时，吸附剂 C 原子被吸引并拉出其周围的表面原子。由此形成的小丘保持褶皱状，直到新形成的分子被释放。导致反应的冲击参数范围取决于碰撞能量，并由入口通道电势的形状控制；在此范围内的反应概率为100%。平均而言，在研究的 E(col) 范围内，可用能量 (3.92 eV + E(col)) 共享为：69-52% 为内能，11-23% 为平移能，20-25% 为传递到表面的能量。此外，新生 H(2) 分子的平均振动和旋转能级分别为 v = 5-4 和 j = 2-4。
The Brenner potential is adapted to handle chemical interactions and reactions of H atoms at a graphene surface. The adapted potential reproduces several important features of DFT computed data and reveals an extended puckering of the surface upon its adsorption of an H atom. This potential is used to investigate in a much more realistic way than has been done before, the Eley-Rideal abstraction reaction producing H(2) in H + H-graphene collisions at energies E(col)< or = 0.2 eV. The graphene surface is represented by a slab of 200 carbon atoms and the study is carried out using classical molecular dynamics for vertical incidences in a cylinder centered about the chemisorption axis. A highlight of the present study is that upon the arrival of the gas phase H atom, the adsorbent C atom is attracted and pulls out its surrounding surface atoms. The hillock thus formed remains puckered until the newly formed molecule is released. The range of impact parameters leading to reaction depends on the collision energy and is governed by the shape of the entrance channel potential; the reaction probability in this range is 100%. On average, in the studied E(col) range, the available energy (3.92 eV + E(col)) is shared as: 69-52% for the internal energy, 11-23% for the translation energy and 20-25% for the energy imparted to the surface. Also, the average vibration and rotation energy levels of the nascent H(2) molecule are, respectively, v = 5-4 and j = 2-4.