CexPr1-xO2-δ复合氧化物的制备、表征及CO和CH4氧化性能研究

无机材料学报

Ce_xPr_1-xO_2-δ复合氧化物的制备、表征及CO和CH₄氧化性能研究

闫宗兰; 林霞; 罗建海; 谢冠群; 罗孟飞

浙江师范大学物理化学研究所, 金华 321004

收稿日期:2004-05-29 修回日期:2004-07-08 出版日期:2005-05-20 网络出版日期:2005-05-20

Characterization and Preparation of Ce_xPr_1-xO_2-δ Mixed Oxides and the Catalytic Activity for CO and CH₄

YAN Zong-Lan; LIN Xia; LUO Jian-Hai; XIE Guan-Qun; LUO Meng-Fei

Institute of Physical Chemistry; Zhejiang Normal University; Jinhua 321004; China

Received:2004-05-29 Revised:2004-07-08 Published:2005-05-20 Online:2005-05-20

摘要/Abstract

摘要： 采用溶胶-凝胶法制备了Ce_xPr_1-xO_2-δ复合氧化物,用XRD和Raman光谱对复合氧化物的体相和表面结构进行了表征.结果表明,当x≥0.5时Pr离子完全进入CeO₂晶格中形成单一立方相固溶体. Ce_xPr_1-xO_2-δ(x>0.3)复合氧化物在465和1150cm^-1附近出现具有CaF₂
结构的Raman特征峰,和由氧空穴引起的不对称振动产生的570和195cm^-1 Raman 谱峰.固溶体的形成使还原温度降低,提高了复合氧化物的还原性能.CO氧化活性表明氧空穴的存在对CO氧化活性有一定的对应关系;而CH₄氧化活性则与还原温度和强度有关.

关键词: Ce_xPr_1-xO_2-δ复合氧化物, Raman, XRD, CO氧化, CH₄氧化

Abstract: A series of Ce_xPr_1-xO_2-δ mixed oxides were synthesized by the sol-gel method and characterized by Raman and XRD techniques. The results show that when x value is changed from 1.0 to 0.5, only a cubic
phase CeO₂ appears. The samples are very well crystallized on decreasing x from 0.50 to 0.99. It can be explained to form an ordered array of O vacancies caused by the insertion of Pr atom completely
into the CeO₂ crystal lattice. For Ce_xPr_1-xO_2-δ samples 465cm^-1 and 1150cm^-1 Raman peaks are attributed to the Raman active F_2g mode of CeO₂. The broad peak at
about 570cm^-1 in the region 0.3≤x≤ 0.99 can be linked to lattice defects resulting in oxygen vacancies. The new band at about ^195cm-1 may be attributed to the asymmetric vibration that is caused
by the formation of oxygen vacancies. TPR profiles of Pr₆O₁₁ and CeO₂ have two reduction peaks respectively. The reduction process of Pr₆O₁₁is: PrO_1.83→PrO_1.61→PrO_1.5;
For CeO₂, the peak of low temperature attributed to the reduction of the surface cmoxygen of CeO₂, the peak of high temperature
attributed to the reduction of bulk CeO₂. The reduction peak temperature of Ce_xPr_1-xO_2-δ mixed oxides is lower than that of Pr₆O₁₁ and CeO₂, which indicates that the formation
of Ce_xPr_1-xO_2-δ solid solutions improves the reduction-oxidation behavior. The activity of Ce_xPr_1-xO_2-δ for CO oxidation indicates that the existing of the oxygen vacancies
favors CO oxidation; while the activity of CH₄ oxidation is related to the temperature and the area of the reduction-oxidation peak.

Key words: Ce_xPr_1-xO_2-δ mixed oxides, XRD, Raman, CO, CH₄, oxidation

中图分类号:

O643

闫宗兰,林霞,罗建海,谢冠群,罗孟飞. Ce_xPr_1-xO_2-δ复合氧化物的制备、表征及CO和CH₄氧化性能研究[J]. 无机材料学报.

YAN Zong-Lan,LIN Xia,LUO Jian-Hai,XIE Guan-Qun,LUO Meng-Fei. Characterization and Preparation of Ce_xPr_1-xO_2-δ Mixed Oxides and the Catalytic Activity for CO and CH₄[J]. Journal of Inorganic Materials.

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Ce_xPr_1-xO_2-δ复合氧化物的制备、表征及CO和CH₄氧化性能研究

Characterization and Preparation of Ce_xPr_1-xO_2-δ Mixed Oxides and the Catalytic Activity for CO and CH₄

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