Characterization of methoxy adsorption on some transition metals: a first principles density functional theory study.
Characterization of methoxy adsorption on some transition metals: a first principles density functional theory study.
复制标题
DOI：
10.1063/1.1839552
复制
发表时间：
2005-01
期刊：
影响因子：
--
通讯作者：
Guichang Wang;Yu-Hua Zhou;J. Nakamura
中科院分区：
文献类型：
--
作者：
Guichang Wang;Yu-Hua Zhou;J. Nakamura
基于梯度密度泛函理论，给出了甲氧基在Au(111)、Ag(111)、Cu(111)、Pt(111)、Pd(111)、Ni(111)、Rh(111)和Fe(100)表面的吸附计算结果，并对决定金属反应性的一些关键物理性质给出了一致的图像。这8种金属分为两类：一类是d电子已填满(IB组)，另一类是d电子未填满但超过一半(组)。计算得到的吸附能与实验数据以及以前的理论计算结果非常吻合。重要的是，利用B.Hammer和J.K.Norskov的分析，自然(伦敦)376,232(1995)以及R.M.Lambert和G.Pacchioni(Kluwer Academy，Dordrecht，1997)编辑的《在支撑的团簇和薄膜上的化学吸附和反应》，结合能已经选择性地与这两类金属的d带中心和与吸附物质(耦合矩阵元素)重叠的金属d带轨道的大小线性相关。并通过对吸附键合性质的分析，提出了造成这种差异的可能原因。
Based on the gradient-density functional theory, calculation results of methoxy adsorption on Au(111), Ag(111), Cu(111), Pt(111), Pd(111), Ni(111), Rh(111), and Fe(100) surfaces are presented, and a consistent picture for some key physical properties determining the reactivity of metals appears. These eight metals belong to two groups: either with filled d electrons (group IB) or with unfilled but more than half filled d electrons (group VIII). The calculated adsorption energies are quite in agreement with the experimental data as well as the previous theoretical calculation results. Importantly, using the analysis of B. Hammer and J. K. Norskov, Nature (London) 376, 232 (1995) and in Chemisorption and Reactivity on Supported Clusters and Thin Films, edited by R. M. Lambert and G. Pacchioni (Kluwer Academic, Dordrecht, 1997), pp. 285-351, the binding energies have selectively been linearly correlated to the d-band center and to the size of the metal d-band orbital overlapping with the adsorbate (coupling matrix element) for these two groups of metals. And by analyzing the nature of the adsorption bonding, the possible reason of this difference is suggested.