Cu在Zr掺杂CeO_2(111)表面吸附特性的第一性原理研究  

First-principles studies on the adsorption of Cu on the Zr-doped CeO_2(111) surface

作　　者：殷岩[1] 陈留定[1] 朱川川[1] 靳义华[1] 秦天明[1] 张岩星[1] 路战胜[1] 杨宗献[1] 

机构地区：[1]河南师范大学物理与信息工程学院河南省光伏材料重点实验室,新乡453007

出　　处：《原子与分子物理学报》2013年第5期819-823,共5页Journal of Atomic and Molecular Physics

基　　金：国家自然科学基金(11174070;11147006)

摘　　要：采用第一原理计算方法,计算并分析了Cu在Zr掺杂的CeO2(111)表面吸附的吸附能及所形成的Cu/Ce0.75Zr0.25O2(111)界面体系的吸附结构和电子结构.结果表明:1)Cu在Ce0.75Zr0.25O2(111)表面上邻近Zr原子的次层O的顶位吸附最强;2)Zr的掺杂增强了Cu与CeO2衬底的作用;3)Cu的吸附在Ce0.75Zr0.25O2(111)表面的O2p-Ce4f态之间引入了新的间隙态,这些间隙态主要来自于Cu3d与衬底O2p的杂化作用,这是Cu与Ce0.75Zr0.25O2有较强作用的主要原因;4)吸附的Cu被Ce0.75Zr0.25O2氧化为Cuδ+,并伴随着表面Ce4+→Ce3+的转化,该反应可以总结为:Cu/Ce4+→Cuδ+/Ce3+.First-principles calculations are performed to study the adsorption properties of Cu on the Zr- doped CeO2 （111） surface. The strong interaction is found between the Cu adatom and the Zr-doped CeO2（111） surface and the Cu adatom prefers to stay neighboring to a surface Zr dopant and at the top site of a subsurface oxygen. The strong interaction between the Cu3d and O2p is mainly responsible for the strong adsorption of the Cu adatom on the Zr-doped CeO2 （111） surface. The Zr dopant would en- hance the interaction between Cu and CeO2. The Cu adatom is oxidized to Cuδ＋ mainly by its next nea- rest-neighbor Ce accompanied by the conversion of Ce4＋→Ce3＋.

关 键 词：Zr掺杂CeO2 CU 吸附特性 密度泛函理论 

分 类 号：O485[理学—固体物理]