Morphology Effect of CeO2 Support in the Preparation, Metal-Support Interaction, and Catalytic Performance of Pt/CeO2 Catalysts

被引:196
|
作者
Gao, Yuxian [1 ]
Wang, Wendong [1 ]
Chang, Sujie [1 ]
Huang, Weixin [1 ]
机构
[1] Univ Sci & Technol China, Dept Chem Phys, CAS Key Lab Mat Energy Convers, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Peoples R China
基金
中国国家自然科学基金;
关键词
cerium; metal-support interaction; oxidation; platinum; supported catalysts; structure-activity relationships; PREFERENTIAL CO OXIDATION; ADJACENT CRYSTAL PLANES; LOW-INDEX SURFACES; ELECTRONIC-STRUCTURE; SELECTIVE SYNTHESIS; NANOSCALE CERIA; HYDROGEN PROX; SHAPE; NANOCRYSTALS; GAS;
D O I
10.1002/cctc.201300709
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
Pt/CeO2 catalysts with various Pt loadings were prepared by a conventional incipient wetness impregnation method that employed CeO2 cubes (c-CeO2), rods (r-CeO2), and octahedra (o-CeO2) as the support and Pt(NH3)(4)(NO3)(2) as the metal precursor. Their structures and catalytic activities in CO oxidation in excess O-2 and the preferential oxidation of CO in a H-2-rich gas (CO-PROX) were studied, and strong morphology effects were observed. The impregnated Pt precursor interacts more strongly with CeO2 rods and cubes than with CeO2 octahedra, and the reduction/decomposition of the Pt precursor impregnated on CeO2 octahedra is easier than that on CeO2 rods and cubes. With the same Pt loading, the Pt/o-CeO2 catalyst contains the largest fraction of metallic Pt, whereas the Pt/c-CeO2 catalyst contains the largest fraction of Pt2+ species. The reducibility of pure CeO2 and CeO2 in the Pt/CeO2 catalysts follows the order r-CeO2>c-CeO2>o-CeO2, and the reducibility of CeO2 depends on the Pt loading for the Pt/c-CeO2 catalysts but not much for the Pt/r-CeO2 and Pt/o-CeO2 catalysts. The catalytic performance of Pt/CeO2 catalysts in both CO oxidation and the CO-PROX reaction follows the order Pt/r-CeO2>Pt/c-CeO2> Pt/o-CeO2. The Pt-0-CeO2 ensemble is more active than the Pt2+-CeO2 ensemble in the catalysis of CO oxidation in excess O-2. H-2-assisted CO oxidation catalyzed by the Pt/CeO2 catalysts was observed in the CO-PROX reaction, and the Pt2+ species and CeO2 with a large concentration of oxygen vacancies constitute the active structure of the Pt/CeO2 catalyst for the CO-PROX reaction. The effect of the morphology of the CeO2 support in the preparation, metal-support interaction, and catalytic performance of Pt/CeO2 catalysts can be correlated the exposed crystal planes and surface composition/structure of the CeO2 support with different morphologies. These results not only demonstrate that the structure and catalytic performance of oxide-supported catalysts can be tuned by controlling the morphology of the oxide support but also deepens the fundamental understanding of CO oxidation reactions catalyzed by Pt/CeO2 catalysts.
引用
收藏
页码:3610 / 3620
页数:11
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