Low temperature CO oxidation over the ceria oxide catalysts doped with Fe, Ni and Cu
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摘要: 采用水热合成法制备了一系列不同金属掺杂的Ce-M（M=Fe、Ni和Cu）复合氧化物，运用低温N2吸附-脱附、XRD、H2-TPR、拉曼光谱和XPS等表征技术对Ce-M复合氧化物的结构与其CO低温氧化反应性能之间的关系进行了关联。结果表明，将Fe、Ni和Cu掺入CeO2明显提高了其氧空位的含量，提升了晶格氧的流动性，从而使Ce-M催化剂的还原能力和催化活性高于纯CeO2。其中，CeCu催化剂氧空位最多、还原能力最好，催化活性最高，130 ℃下即可将CO完全氧化；其次是CeNi催化剂，180 ℃时实现CO完全氧化；与之相比，CeFe催化剂的活性最差，200 ℃时的CO转化率仅为92%。Abstract: A series of ceria oxide catalysts doped with Fe, Ni and Cu were prepared by hydrothermal method and they characterized by N2 sorption, XRD, H2-TPR, Raman spectra and XPS; the relationship between the structure of Ce-M mixed oxides and their catalytic performance in low temperature CO oxidation were then investigated. The results reveal that the incorporation of Fe, Ni and Cu metal ions into CeO2 can remarkably increase the amount of oxygen vacancies in the doped samples, which is beneficial to the migration of the lattice oxygen; as a result, the doped Ce-M mixed oxides exhibit much higher reducibility and catalytic activity than the pure CeO2. Among them, the CeCu catalyst with most oxygen vacancies exhibits the highest activity in CO oxidation, with a complete CO conversion at 130℃; over CeNi catalyst, in the next, a complete CO conversion is obtained at 180℃. On the contrary, CeFe catalyst is least active and the conversion of CO is only 92% at 200℃.
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Key words:
- doped ceria /
- iron oxide /
- nickel oxide /
- copper oxide /
- oxygen vacancies /
- CO oxidation
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图 1 CeO2及Ce-M复合氧化物催化剂的XRD谱图
Figure 1 XRD patterns of CeO2 and Ce-M mixed oxides with different dopants
图 2 CeO2及Ce-M复合氧化物催化剂的H2-TPR谱图
Figure 2 H2-TPR profiles of CeO2 and Ce-M mixed oxides with different dopants
图 3 CeO2及Ce-M复合氧化物催化剂的拉曼光谱谱图
Figure 3 Raman spectra of CeO2 and Ce-M mixed oxides with different dopants
图 4 CeO2及Ce-M复合氧化物催化剂的Ce 3d XPS谱图
Figure 4 Ce 3d XPS spectra of CeO2 and Ce-M mixed oxides with different dopants
图 5 CeO2及Ce-M复合氧化物催化剂的O 1s XPS谱图
Figure 5 O 1s XPS spectra of CeO2 and Ce-M mixed oxides with different dopants
图 6 CeO2及Ce-M复合氧化物催化剂的CO转化率随反应温度的变化
Figure 6 Catalytic activity of CeO2 and Ce-M mixed oxides with different dopants in CO oxidation
表 1 Ce-M复合氧化物催化剂的ICP检测
Table 1 ICP analysis results of various Ce-M mixed oxides
表 2 CeO2及Ce-M复合氧化物催化剂的比表面积和XRD分析
Table 2 Surface area and XRD results of CeO2 and Ce-M mixed oxides with different dopants
表 3 CeO2及Ce-M复合氧化物催化剂的拉曼光谱和XPS分析
Table 3 Raman and XPS analysis results of CeO2 and Ce-M mixed oxides with different dopants
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