物理化学学报 >> 2004, Vol. 20 >> Issue (08S): 1045-1054.doi: 10.3866/PKU.WHXB200408zk23

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金属氧化物表面化学吸附和反应的量子化学簇模型方法研究

徐昕;吕鑫;王南钦;张乾二   

  1. 厦门大学化学系，固体表面物理化学国家重点实验室，理论化学研究中心，物理化学研究所，厦门　361005
  • 收稿日期:2004-01-02 修回日期:2004-05-15 发布日期:2004-08-15
  • 通讯作者: 徐昕 E-mail:xinxu@xmu.edu.cn

Cluster Modeling of Chemisorption and Reactions on Metal Oxide Surfaces

Xu Xin;Lü Xin;Wang Nan-Qin;Zhang Qian-Er   

  1. State Key Laboratory for Physical Chemistry of Solid Surfaces ＆ Center for Theoretical Chemistry, Department of Chemistry ＆ Institute of Physical Chemistry, Xiamen University, Xiamen　361005
  • Received:2004-01-02 Revised:2004-05-15 Published:2004-08-15
  • Contact: Xu Xin E-mail:xinxu@xmu.edu.cn

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摘要： 综述了本研究小组利用量子化学簇模型方法研究金属氧化物表面化学吸附和反应的工作.提出了选簇的三个原则，即电中性原则、化学配比原则和配位原则.发现在符合前两个原则的基础上，一个具有最饱和配位、或最少悬空键的簇往往是一个用于化学吸附研究的好的簇模型.与此同时，探讨了如何恰当地考虑大块固体本底的长程影响，提出了用球电荷模拟簇模型的环境、环境与簇体进行电荷自洽的SPC簇模型方法.利用该模型研究了一系列具有催化背景的重要体系，包括H2/ZnO、O/MgO、NO/MgO、N2O/ MgO、N2O/Li/MgO、CO/MgO、CO/NiO等.

关键词: 簇模型方法, 氧化物, 化学吸附, 表面反应, 量子化学

Abstract: The research on the cluster modeling of chemisorption and reactions on metal oxide surfaces in our group has been reviewed. Three principles, namely, neutrality principle, stoichiometrical principle and coordination principle were proposed for building up cluster models of metal oxides. Good correlation between the topologic parameters Nc(βc), Na(βa) and Nd(βd) with the stability of clusters has been shown. The problem of how the ways of embedding affect the calculated electronic properties of the substrate clusters and the adsorption properties has been investigated. Based on these, we proposed an SPC model, which is a stoichiometric cutout cluster embedded in a spherically expanded point charge surrounding with charges being self-consistently determined. We have successfully applied the SPC model to a variety of important systems, including H2/ZnO, O/MgO, NO/MgO, N2O/MgO, N2O/Li/MgO, CO/MgO and CO/NiO.

Key words: Cluster modeling, Oxide, Chemisorption, Surface reaction, Quantum chemistry