First-principles investigation of transition metal atom M (M = Cu, Ag, Au) adsorption on CeO2(110)

被引:55
作者
Cui, Lixia [1 ,2 ]
Tang, Yuanhao [1 ]
Zhang, Hua [1 ]
Hector, Louis G., Jr. [3 ]
Ouyang, Chuying [4 ]
Shi, Siqi [1 ,2 ]
Li, Hong [2 ]
Chen, Liquan [2 ]
机构
[1] Zhejiang Sci Tech Univ, Dept Phys, Ctr Optoelect Mat & Devices, Hangzhou 310018, Peoples R China
[2] Chinese Acad Sci, Renewable Energy Lab, Inst Phys, Beijing 100190, Peoples R China
[3] Gen Motors R&D Ctr, Warren, MI 48090 USA
[4] Jiangxi Normal Univ, Dept Phys, Nanchang 330022, Peoples R China
基金
中国国家自然科学基金;
关键词
GAS SHIFT REACTION; CO OXIDATION; PREFERENTIAL OXIDATION; CATALYTIC-ACTIVITY; SURFACE-STRUCTURE; OXIDE; CEO2; DENSITY; NANOPARTICLES; DEACTIVATION;
D O I
10.1039/c2cp22720g
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
Transition metal atom M (M = Cu, Ag, Au) adsorption on CeO2(110), a technologically important catalytic support surface, is investigated with density-functional theory within the DFT + U formalism. A set of model configurations was generated by placing M at three surface sites, viz., on top of an O, an O bridge site, and a Ce bridge site. Prior to DFT optimization, small distortions in selected Ce-O distances were imposed to explore the energetics associated with reduction of Ce4+ to Ce3+ due to charge transfer to Ce during M adsorption. Charge redistribution is confirmed with spin density isosurfaces and site projected density of states. We demonstrate that Cu and Au atoms can be oxidized to Cu2+ and Au2+, although the adsorption energy, E-ads, of Au2+ is less favorable and, unlike Cu2+, it has not been experimentally observed. Oxidation of Ag always results in Ag+. For M adsorption at an O bridge site, E-ads(2NN) > E-ads(3NN) > E-ads(1NN) where NN denotes the nearest neighbor Ce3+ site relative to M. Alternatively, for M adsorption at a Ce bridge site, E-ads(3NN) > E-ads(2NN) > E-ads(1NN). The adsorption behavior of M on CeO2 (110) is compared with M adsorption on CeO2(111).
引用
收藏
页码:1923 / 1933
页数:11
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