Total oxidation of propene at low temperature over Co3O4-CeO2 mixed oxides:: Role of surface oxygen vacancies and bulk oxygen mobility in the catalytic activity

被引:245
作者
Liotta, L. F. [1 ]
Ousmane, M. [2 ,4 ,5 ,6 ]
Di Carlo, G. [2 ]
Pantaleo, G. [1 ]
Deganello, G. [1 ,2 ]
Marci, G. [3 ]
Retailleau, L. [4 ,5 ,6 ]
Giroir-Fendler, A. [4 ,5 ,6 ]
机构
[1] ISMN CNR, I-90146 Palermo, Italy
[2] Univ Palermo, Dipartimento Chim Inorgan & Analit Stanislao Cann, I-90128 Palermo, Italy
[3] Univ Palermo, Dipartimento Ingn Chim Proc & Mat, I-90128 Palermo, Italy
[4] Univ Lyon, F-69003 Lyon, France
[5] Univ Lyon 1, F-69622 Villeurbanne, France
[6] IRCELYON, CNRS, UMR 5256, F-69622 Villeurbanne, France
关键词
propene total oxidation; C3H6-TPR; TPD experiments; surface oxygen vacancies; SEM characterization;
D O I
10.1016/j.apcata.2008.05.038
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
Co3O4, CeO2 and Co3O4-CeO2 mixed oxides with Co/Ce nominal atomic ratio 0.1:5, prepared by co-precipitation method with sodium carbonate, were tested in the oxidation of propene under lean condition and the catalyst stability was checked by performing three consecutive heating-cooling cycles. Characterization of the textural properties were performed by surface area measurement BET, X-ray diffraction (XRD) and scanning electron microscopy (SEM) measurements. Among the Co3O4-CeO2 mixed oxides, Co3O4 (30 Wt%)-CeO2 (70 wt%) gives the best activity attaining full propene conversion at 250 degrees C. This sample is characterized by the presence of Co3O4 particles well dispersed and in good contact with ceria according to BET and XRD data and as evidenced by SEM micrographs. Oxygen temperature-programmed desorption (O-2-TPD) and C3H6-temperature-programmed reduction (C3H6-TPR) experiments were carried out in order to study the surface and bulk oxygen mobility and to correlate it to the activity. At temperature around 200 degrees C, O-2-TPD experiments showed the desorption of mobile surface oxygen species for the most active samples, Co3O4 and Co3O4 (30 wt%)-CeO2 (70 wt%). C3H6-TPR experiments for both of the oxides also evidenced a high reactivity at low temperature, especially, for Co3O4 (30 wt%)-CeO2 (70 wt%) giving at 345 degrees C an intense peak of CO2 formation. Conversely, the ceria sample showed by C3H6-TPR much less pronounced oxygen bulk mobility, starting to react with propene above 500 degrees C and forming only CO. In this case, the catalytic activity of ceria was explained in terms of formation of surface oxygen vacancies which are relevant to the propene oxidation in presence of gaseous oxygen. (c) 2008 Elsevier B.V. All rights reserved.
引用
收藏
页码:81 / 88
页数:8
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