CO诱导的FeO(111)/Ru(0001)负载Au原子吸附位和电荷的改变

doi:10.1016/S1872-2067(12)60664-0

催化学报 ›› 2013, Vol. 34 ›› Issue (10): 1820-1825.DOI: 10.1016/S1872-2067(12)60664-0

CO诱导的FeO(111)/Ru(0001)负载Au原子吸附位和电荷的改变

欧阳润海, 李微雪

中国科学院大连化学物理研究所催化基础国家重点实验室, 辽宁大连116023

收稿日期:2013-05-29 修回日期:2013-06-17 出版日期:2013-09-29 发布日期:2013-09-29
基金资助:
国家自然科学基金(21173210,21225315);国家重点基础研究发展计划(973计划,2013CB834603).

Adsorbed CO induced change of the adsorption site and charge of Au adatoms on FeO(111)/Ru(0001)

Runhai Ouyang, Wei-Xue Li

State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China

Received:2013-05-29 Revised:2013-06-17 Online:2013-09-29 Published:2013-09-29
Contact: Wei-Xue Li
Supported by:
This work was supported by the National Natural Science Foundation of China (21173210, 21225315) and the National Basic Research Program of China (973 Program, 2013CB834603).

摘要/Abstract

摘要：

采用密度泛函理论研究了CO气氛对FeO(111)/Ru(0001)负载Au原子吸附位、电荷及其稳定性的影响. 首先考察了FeO(111)单层薄膜在Ru(0001)表面上的界面结构. 研究发现,表面莫尔超晶胞内的HCP区域有最小的Fe-O层间距(rumpling),且Fe和O原子均与衬底Ru形成化学键. Au原子在FeO/Ru(0001)上最稳定的吸附在HCP区域的Fe-bridge位. 其中,Au原子诱导两个Fe原子从O原子层的下面翻转到其上面,形成两个Au-Fe键,且Au带负电. 当把体系暴露在CO气氛下后,CO能诱导Au原子从原来最稳定的Fe-bridge位转移到其邻近的O-top位,伴随着Au的电荷从负变到正,形成非常稳定的Au⁺-CO羰基物. 结果表明,反应气氛对负载金属催化剂的化学状态及其稳定性的影响很大; 同时也强调了反应条件下催化剂原位表征的重要性.

关键词: 密度泛函理论, 一氧化碳, 金, 氧化铁薄膜

Abstract:

A first principles study of the influence of CO adsorption on the charge state, adsorption site, and stability of Au adatoms on FeO/Ru(0001) was presented. Calculations were first carried out to explore the detailed interface structure of a bilayer FeO(111) film on Ru(0001). The HCP domain inside the Moire supercell has a rather small rumpling with both the Fe and O atoms directly bonded to the Ru substrate. The most stable adsorption of an Au atom on FeO/Ru(0001) is at the Fe-bridge site in the HCP domain, where Au binds with two flipped Fe atoms and is negatively charged. After exposure to CO, the Au anions at the Fe-bridge site changed their position to the O-top site by overcoming a small barrier of only 0.12 eV, where they formed stable Au⁺-CO species with a significant reduction in the formation energy. The results highlighted the importance of in situ characterization of supported catalysts under reaction conditions, and implications on catalyst stability were also discussed.

Key words: Density functional theory, Carbon monoxide, Gold, Iron oxide film

欧阳润海, 李微雪. CO诱导的FeO(111)/Ru(0001)负载Au原子吸附位和电荷的改变[J]. 催化学报, 2013, 34(10): 1820-1825.

Runhai Ouyang, Wei-Xue Li. Adsorbed CO induced change of the adsorption site and charge of Au adatoms on FeO(111)/Ru(0001)[J]. Chinese Journal of Catalysis, 2013, 34(10): 1820-1825.

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CO诱导的FeO(111)/Ru(0001)负载Au原子吸附位和电荷的改变

Adsorbed CO induced change of the adsorption site and charge of Au adatoms on FeO(111)/Ru(0001)

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