贵金属团簇/CeO2的界面结构和化学活性对CeO2晶面的依赖性的理论研究

项目名称： 贵金属团簇/CeO2的界面结构和化学活性对CeO2晶面的依赖性的理论研究

项目编号： No.U1504108

项目类型： 联合基金项目

立项/批准年度： 2016

项目学科： 数理科学和化学

项目作者： 马东伟

作者单位： 安阳师范学院

项目金额： 27万元

中文摘要： 固体催化剂在生产可持续能源和保护环境清洁等领域起着重要作用。暴露在固体催化剂表面的晶面是影响其催化性能的一个关键因素。CeO2负载贵金属团簇（贵金属团簇/CeO2）催化剂的催化性能对CeO2晶面的强烈依赖性得到了大量实验验证及初步理论关注，但是其微观机制仍亟需进一步深入探索。本项目拟利用基于密度泛函理论的第一性原理方法，从原子层次和电子结构方面对比研究贵金属团簇在CeO2三个最稳定晶面的吸附，阐明贵金属团簇/CeO2界面几何结构和电子结构对CeO2晶面的依赖性；进一步对比研究反应相关气体分子在界面的吸附，阐明贵金属团簇/CeO2界面化学活性对CeO2晶面的依赖性。本项目的研究将为揭示贵金属团簇/CeO2催化剂催化性能对CeO2晶面的依赖性的微观机制提供理论参考，对设计和开发实用高效贵金属团簇/CeO2催化剂具有重要理论价值。

中文关键词： 贵金属团簇/CeO2；界面结构；化学活性；晶面依赖性；第一性原理计算

英文摘要： Solid catalysts play important roles in the fields, such as producing sustainable energies and keeping environments clean. The crystal plane exposed on the surface of solid catalysts is a key factor controlling their catalytic performances. Lots of experiments have shown that the catalytic performance of the catalysts of noble-metal clusters supported on CeO2 (noble-metal clusters/CeO2) is strongly dependent on the crystal plane of CeO2, which also preliminarily gains theoretical attention. However, there is an urgent need for further exploring the relevant microscopic mechanisms. By using first-principles calculations based on density functional theory, the current project from the atomic level and the electronic structure will comparatively investigate the adsorption of noble-metal clusters on the three most stable CeO2 surface and clarify the dependence of geometrical and electronic structures of the noble-metal clusters/CeO2 interfaces on the crystal plane of CeO2. Furthermore, we will comparatively investigate the adsorption of the gas molecules involved in the reaction at the noble-metal clusters/CeO2 interfaces and clarify the dependence of chemical activities of the interfaces on the crystal plane of CeO2. The project will provide a theoretical reference for unrevealing the microscopic mechanism behind the dependence of the catalytic performances of the noble-metal clusters/CeO2 catalysts on the crystal plane of CeO2, and has important theoretical value in designing and developing the practical and efficient noble-metal clusters/CeO2 catalysts.

英文关键词： noble-metal clusters/CeO2;interfacial structure;chemical activity;crystal-plane dependence;first-principles calculation