La2CoAlO6催化剂的制备及其甲烷催化燃烧性能

doi:10.3866/PKU.WHXB20110502

物理化学学报 >> 2011, Vol. 27 >> Issue (05): 1169-1175.doi: 10.3866/PKU.WHXB20110502

La₂CoAlO₆催化剂的制备及其甲烷催化燃烧性能

张慧敏¹,胡瑞生¹, 胡佳楠¹, 张玉龙²

1. 内蒙古大学化学化工学院, 稀土材料化学与物理重点实验室, 呼和浩特 010021;
2. Western Research Institute, 365 N 9St, Laramie, Wyoming, USA

收稿日期:2011-01-13 修回日期:2011-03-03 发布日期:2011-04-28
通讯作者: 胡瑞生 E-mail:cehrs@imu.edu.cn
基金资助:
国家自然科学基金(20763003), 教育部春晖计划(Z2007-1-01029)及内蒙古自然科学基金(2008 0404 MS 0123)资助项目

Preparation and Catalytic Activities of La₂CoAlO₆ for Methane Combustion

ZHANG Hui-Min¹, HU Rui-Sheng¹, HU Jia-Nan¹, ZHANG Yu-Long²

1. Key Laboratory of Rare Earth Materials Chemistry and Physics, School of Chemistry and Chemical Engineering, Inner Mongolia University, Hohhot 010021, P. R. China;
2. Western Research Institute, 365 N 9St, Laramie, Wyoming, USA

Received:2011-01-13 Revised:2011-03-03 Published:2011-04-28
Contact: HU Rui-Sheng E-mail:cehrs@imu.edu.cn
Supported by:
The project was supported by the National Natural Science Foundation of China (20763003) and Chun Hui Plans of the Ministry of Education of China (Z2007-1-01029) and Natural Science Foundation of Inner Mongolia, China (2008 0404 MS 0123).

摘要/Abstract

摘要：

采用溶胶-凝胶法, 以柠檬酸为络合剂制备了新型稀土双钙钛矿催化材料La₂CoAlO₆, 利用X射线粉末衍射(XRD)、H₂-程序升温还原(H₂-TPR)、比表面(BET)、扫描电镜(SEM)、傅里叶变换红外(FT-IR)光谱和磁性测试等手段对其进行了表征, 以甲烷催化燃烧反应为探针考察了其催化活性. 结果表明, 在空气气氛中, 经过1100 °C焙烧3 h后, 可以形成稳定的单相稀土双钙钛矿型化合物La₂CoAlO₆, 且该化合物表现出较好的甲烷催化燃烧活性, 起燃温度(T₁₀)和完全转化温度(T₉₀)分别为434.1和657.4 °C. 与稀土单钙钛矿型催化剂LaCoO₃和LaAlO₃相比, 其T₁₀分别降低了56.5和138.2 °C, T₉₀分别降低了84.6和108.9 °C. H₂-程序升温还原结果表明, 稀土双钙钛矿型化合物La₂CoAlO₆有较低的还原温度, 并且经过H₂-程序升温还原反应后, La₂CoAlO₆样品XRD图中的所有衍射峰均向小角度方向发生了移动. 扫描电子显微镜的结果表明, 稀土双钙钛矿型催化剂La₂CoAlO₆表现出无规则的片状形貌及较强的抗烧结性. 此外还发现稀土双钙钛矿型催化剂La₂CoAlO₆的磁滞回线较为特殊.

关键词: 稀土, 双钙钛矿, 单钙钛矿, 甲烷催化燃烧, 溶胶-凝胶法

Abstract:

A novel rare earth double perovskite-type catalyst (La₂CoAlO₆) was prepared by the sol-gel method using citric acid as complex agent. The catalyst was characterized by X-ray powder diffraction (XRD), H₂-temperature-programmed reduction (H₂-TPR), specific surface area (BET), scanning electron microscopy (SEM), Fourier transform infrared (FT-IR) spectroscopy, and magnetic property measurement. This catalyst was evaluated for methane combustion. The results showed that a single-phase rare earth double perovskite oxide La₂CoAlO₆ could be formed by calcination at 1100 °C for 3 h. La₂CoAlO₆ gives good catalytic activity for methane combustion. It has a light-off temperature (T₁₀) of 434.1 °C and a total conversion temperature (T₉₀) of 657.4 °C. Compared with the single rare earth perovskite-type oxides LaCoO₃ and LaAlO₃, the T₁₀ decreased by 56.5 and 138.2 °C, and T₉₀ decreased by 84.6 and 108.9 °C, respectively. The FT-IR results indicate that all the synthesized oxides possess perovskite-type structures. Furthermore, the La₂CoAlO₆ samples showed excellent catalytic activity for methane combustion, which could be related to the decrease in reduction temperature that was observed in the H₂-TPR experiments. This was probably because of the increased oxygen mobility that was promoted by the presence of aluminum. In addition, the rare earth double perovskite-type oxide La₂CoAlO₆ has a platelet morphology and is resistant to sintering. We also found that the double perovskite oxide La₂CoAlO₆ had special magnetic properties.

Key words: Rare earth, Double perovskite, Single perovskite, Methane catalytic combustion, Sol-gel method

张慧敏, 胡瑞生, 胡佳楠, 张玉龙. La₂CoAlO₆催化剂的制备及其甲烷催化燃烧性能[J]. 物理化学学报, 2011, 27(05), 1169-1175. doi: 10.3866/PKU.WHXB20110502

ZHANG Hui-Min, HU Rui-Sheng, HU Jia-Nan, ZHANG Yu-Long. Preparation and Catalytic Activities of La₂CoAlO₆ for Methane Combustion[J]. Acta Phys. -Chim. Sin. 2011, 27(05), 1169-1175. doi: 10.3866/PKU.WHXB20110502

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB20110502

https://www.whxb.pku.edu.cn/CN/Y2011/V27/I05/1169

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La₂CoAlO₆催化剂的制备及其甲烷催化燃烧性能

Preparation and Catalytic Activities of La₂CoAlO₆ for Methane Combustion

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