Quantum Chemical Modelling Case Studies Relevant to Metal Oxide Dissolution and Catalysis

被引:16
作者
Gerson, A. R. [1 ]
Jones, R. [1 ]
Simpson, D. [1 ]
Pacchioni, G. [2 ]
Bredow, T. [3 ]
机构
[1] Univ S Australia, Ian Wark Res Inst, Commonwealth ARC Special Res Ctr Particle & Mat I, Mawson Lakes, SA 5095, Australia
[2] Univ Milano Bicocca, Ist Nazl Fis Mat, Dipartimento Sci Mat, I-20125 Milan, Italy
[3] Leibniz Univ Hannover, D-30167 Hannover, Germany
关键词
D O I
10.1007/BF02373562
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Over the past 20 years quantum-chemical methods have been developed sufficiently so that they can now be applied to the elucidation of the complex mechanistic processes that occur during metal oxide dissolution and catalysis reactions. Many of the reactions occurring during these processes are not directly accessible to experimental techniques and therefore quantum-chemical modelling can be applied to probe the individual reaction steps involved in the overall mechanism. Quantum chemistry provides the means of calculating the electronic properties of solids (e. g. band structures) structural properties of solids and surfaces (for instance surface relaxation and rumpling) heats of formation and reaction, activation energies, spectroscopic excitation energies and vibrational frequencies. Three case studies are described, which have been chosen to cover a range of quantum chemical applications and methodologies. These case studies are a) the dissolution mechanism of MgO, b) the parameterisation of titanium dioxide for the determination of electronic properties and c) the mechanism and energetics of adsorption of Pd onto rutile. These case studies utilise Hartree-Fock semiempirical and ab initio quantum-chemical methods as well as density functional methodologies. A range of model types are used, namely cluster models embedded in pseudo-atoms, 3-dimensional periodic models and 2-dimensional periodic surface models.
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收藏
页码:290 / 309
页数:20
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