Structural/surface characterization and catalytic evaluation of rare-earth (Y, Sm and La) doped ceria composite oxides for CH3SH catalytic decomposition

被引:78
作者
He, Dedong [1 ]
Chen, Dingkai [1 ]
Hao, Husheng [1 ]
Yu, Jie [1 ]
Liu, Jiangping [1 ]
Lu, Jichang [1 ]
Liu, Feng [1 ]
Wan, Gengping [1 ,2 ]
He, Sufang [3 ]
Luo, Yongming [1 ]
机构
[1] Kunming Univ Sci & Technol, Fac Environm Sci & Engn, Kunming 650500, Peoples R China
[2] Hainan Univ, Res Ctr Anal & Measurement, Haikou 570228, Peoples R China
[3] Kunming Univ Sci & Technol, Res Ctr Anal & Measurement, Kunming 650093, Peoples R China
基金
中国国家自然科学基金;
关键词
CeO2-based composite oxides; Rare earth; Oxygen vacancies; Surface basicity; CH3SH decomposition; SOLID-SOLUTIONS; METHYL MERCAPTAN; CO OXIDATION; FACILE SYNTHESIS; SOOT OXIDATION; VOC OXIDATION; CEO2; H2S; ADSORPTION; REDUCTION;
D O I
10.1016/j.apsusc.2016.08.129
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
A series of rare earth (Y, Sm and La) doped ceria composite oxides and pure CeO2 were synthesized and evaluated by conducting CH3SH catalytic decomposition test. Several characterization studies, including XRD, BET, Raman, H-2-TPR, XPS, FT-IR, CO2-TPD and CH3SH-TPD, were undertaken to correlate structural and surface properties of the obtained ceria-based catalysts with their catalytic performance for CH3SH decomposition. More oxygen vacancies and increased basic sites exhibited in the rare earth doped ceria catalysts. Y doped ceria sample (Ce(0.75)Yo(0.25)O(2-delta)), with a moderate increase in basic sites, contained more oxygen vacancies. More structural defects and active sites could be provided, and a relatively small amount of sulfur would accumulate, which resulted in better catalytic performance. The developed catalyst presented good catalytic behavior with stability very similar to that of typical zeolite-based catalysts reported previously. However, La doped ceria catalyst (Ce(0.75)Yo(0.25)O(2-delta)) with the highest alkalinity was not the most active one. More sulfur species would be adsorbed and a large amount of cerium sulfide species (Ce2S3) would accumulate, which caused deactivation of the catalysts. The combined effect of increased oxygen vacancies and alkalinity led to the catalytic stability of Ce(0.75)Yo(0.25)O(2-delta) sample was comparable to that of pure CeO2 catalyst. (C) 2016 Elsevier B.V. All rights reserved.
引用
收藏
页码:959 / 967
页数:9
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