Wang Ching-Huei, Chen Chun-Liang, Weng Hung-Shan
Department of Biochemical Engineering, Kao Yuan Institute of Technology, Kaohsiung 821, Taiwan.
Chemosphere. 2004 Dec;57(9):1131-8. doi: 10.1016/j.chemosphere.2004.08.031.
La(1-x)Sr(x)FeO(3) (x=0.0-1.0) perovskites were prepared and tested for the combustion of methane. X-ray diffraction (XRD) patterns revealed the presence of a single perovskite structure for substitutions 0x0.3, however Fe(2)O(3), SrCO(3) and SrFeO(3) phases were observed for substitutions x>0.3. The results of activity test indicate that with La(1-x)Sr(x)FeO(3) as the catalyst, the combustion of methane can take place at low temperatures around 400 degrees C. Partial substitution of La with Sr increases the activity and an optimal substitution fraction (x=0.5) exists in the La(1-x)Sr(x)FeO(3) catalysts. Catalyst activity can be well correlated to the product of the specific surface area and atomic ratio of Fe to La+Sr on the catalyst surface. Experimental results of O(2)-TPD and CH(4)-TPD in the range of 350-500 degrees C indicate that the amount of oxygen desorbed from the La(1-x)Sr(x)FeO(3) catalysts is far larger than that of methane. Therefore, it can be proposed that the catalytic oxidation of CH(4) over these catalysts proceeds with the surface reaction between CH(4) in the gas phase and the adsorbed O(2). Addition of water vapor or CO(2) to the feed inhibited catalyst activity, but the inhibition was reversible and became negligible at high reaction temperature.
制备了La(1-x)Sr(x)FeO(3)(x = 0.0 - 1.0)钙钛矿并测试其对甲烷燃烧的性能。X射线衍射(XRD)图谱表明,当x在0到0.3之间时,存在单一的钙钛矿结构,然而,当x > 0.3时,观察到了Fe(2)O(3)、SrCO(3)和SrFeO(3)相。活性测试结果表明,以La(1-x)Sr(x)FeO(3)为催化剂,甲烷燃烧可在400℃左右的低温下进行。用Sr部分替代La可提高活性,且在La(1-x)Sr(x)FeO(3)催化剂中存在最佳替代分数(x = 0.5)。催化剂活性与催化剂表面比表面积和Fe与La + Sr原子比的乘积密切相关。在350 - 500℃范围内进行的O(2)-TPD和CH(4)-TPD实验结果表明,从La(1-x)Sr(x)FeO(3)催化剂上脱附的氧量远大于甲烷量。因此,可以提出,在这些催化剂上CH(4)的催化氧化是通过气相中的CH(4)与吸附的O(2)之间的表面反应进行的。向进料中添加水蒸气或CO(2)会抑制催化剂活性,但这种抑制是可逆的,在高反应温度下可忽略不计。