Fundamental Investigation for the Structure and Dynamics of the Ultrafine Metal Particles over the Solid Surface

实用催化剂，如三元催化剂和燃烧催化剂已经得到了大量的开发和研究。然而，它们最初是经验的，而不是理论的。因此，有必要建立与此类催化剂发展相关的新课程和评价方法。本研究采用分子动力学（MD）模拟、基于密度泛函（DF）方法的量子化学（QC）计算和计算机图形学（CG）方法研究了超细金属颗粒在固体表面等表面上的精细结构和动力学。本文重点研究了：(1)超细金颗粒在不同氧化物表面的烧结机理和表面结构，以及载体与金属之间界面的作用；(2)基于EAM-MD方法更精确地描述原子间相互作用，再现了金属表面重构并分析了其机理；(3)元负载催化剂的电子态及其氧化态；(4)基于扩展DF方法（考虑周期边界条件）对支撑-金属模型的研究，该模型与实际催化剂相比更为明显。结果表明：(1)可以获得超细金属颗粒动力学行为的详细信息；(2)与传统的MD方法相比，可以更详细地考虑固体表面动力学的可能性；(3)可以提示负载Pd催化剂和负载Rh催化剂之间电子态差异的重要性；(4)可以更准确地估计吸附剂和吸附物之间的相互作用。因此，我们认为我们的研究取得了进展，取得了成功，取得了重要而富有成效的成果。此外，我们将尝试在更多样化的模型系统中提取更多有用的信息。少

Practical catalysts such as the three-way catalyst and combustion catalyst have been considerably developed and investigated. However, they were originally empirical rather than theoretical. Thus it is necessary to establish new courses and evaluation methods concerned with such developments of catalyst. In this investigation we studied the fine structure and the dynamics of the ultrafine metal particles over the solid surfaces and so on by using molecular dynamics (MD) simulation, quantum chemical (QC) calculations based on density functional (DF) method and computer graphics (CG). Particularly we investigated in detail : (1) sintering mechanism and the surface structure of ultrafine gold particles over various oxides surfaces and the roles of the interface between the supports and metals, (2) reproducing the metal surface reconstruction and analysis of its mechanism by using more accurate description of interatomic interaction based on EAM-MD method, (3) the electronic states of meta … More l supported catalysts and their oxidized states ; the methane adsorption and activation process over the metal cluster and over the metal oxide cluster by QC calculations based on DF methods, and (4) the studies based on the extended DF method (taking into account the periodic boundary condition) for the support - metal models which are more apparent system compared with the real catalyst. As results, it was clarified that : (1) detailed information of the dynamic behaviors of the ultrafine metal particles can be obtained, (2) the possibilities of the more detail consideration for the dynamics in the solid surface compared with the conventional MD method, (3) the importance of the difference of the electronics states between supported Pd catalyst and supported Rh catalyst can suggest, and (4) the interaction between the adsorbent and the adsorbate can be estimated more accurate. So it is considered that our investigation progressed and was successful to obtain important and fruitful results. Futhermore we will try to extract more useful infomation assuming more diversified model system. Less