改进溶胶-凝胶法合成CeO2-ZrO2固溶体及催化性能研究

doi:10.3724/SP.J.1077.2010.00820

无机材料学报 ›› 2010, Vol. 25 ›› Issue (8): 820-824.DOI: 10.3724/SP.J.1077.2010.00820 CSTR: 32189.14.SP.J.1077.2010.00820

改进溶胶-凝胶法合成CeO₂-ZrO₂固溶体及催化性能研究

袁文辉¹, 周辰辰¹, 李莉²

(华南理工大学 1. 化学与化工学院; 2. 环境科学与工程学院, 广州510640)

收稿日期:2009-12-15 修回日期:2010-02-06 出版日期:2010-08-20 网络出版日期:2010-07-19
基金资助:
国家自然科学基金(20976057); NSFC-广东联合基金(U0834004)

Study on Catalytic Properties of Nano-CeO₂-ZrO₂ Mixed Oxides Prepared by Modified Sol-Gel Method

YUAN Wen- Hui¹, ZHOU Chen-Chen¹, LI Li²

(1. School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, China; 2. College of Environmental Science and Engineering, South China University of Technology, Guangzhou 510640, China)

Received:2009-12-15 Revised:2010-02-06 Published:2010-08-20 Online:2010-07-19

摘要/Abstract

摘要：

以Ce(NO₃)₃·6H₂O和ZrO(NO₃)₂·2H₂O为原料采用改进溶胶-凝胶法合成了纳米级铈锆固溶体, 考察了不同铈锆摩尔比和温度条件对制备固溶体的粒度、晶型和还原性能的影响, 获得了优化工艺条件. 采用XRD、比表面积测定(BET)、扫描电子显微镜(SEM)、程序升温还原(TPR)进行表征. 结果表明: 此方法制备的固溶体均为立方萤石结构的铈锆固溶体复合氧化物, 其比表面积可达92m²/g; 450℃焙烧制备的样品具有良好的还原活性. 在常压固定床流动体系中进行乙醇水蒸气重整反应结果表明: 当n(Ce):n(Zr)=3:1时, CeO₂-ZrO₂固溶体比CeO₂和其它比例的固溶体具有更高的催化活性和对氢气的选择性. ZrO₂的引入不但改进了CeO₂的热稳定性, 而且提高了CeO₂的还原能力.

关键词: 氢气, 乙醇水蒸气重整反应, 纳米CeO₂-ZrO₂, 改进溶胶-凝胶法

Abstract:

The nanosized CeO₂-ZrO₂solid solutions were prepared by modified Sol-Gel method with Ce(NO₃)₃·6H₂O and ZrO(NO₃)₂·2H₂O as starting materials. The effects of different Ce/Zr molar ratio and calcination temperature on the particle size, crystal type and reducibility were studied to obtain optimal preparation condition. CeO₂-ZrO₂ solid solution was characterized by XRD, SEM and TPR measurements. Results show that the highest specific surface area of CeO₂-ZrO₂ solid solution is 92m²/g while Ce/Zr molar ratio is 3: 1. CeO₂-ZrO₂solid solution prepared by modified Sol-Gel method is fluorite structured. TPR results show that CeO₂-ZrO₂solid solution calcined at 450℃ has good catalytic reducibility. Catalytic properties are estimated through a fix-bed reactor under atmospheric pressure. CeO₂-ZrO₂solid solution with Ce/Zr molar ratio of 3: 1 show higher catalytic activity and selectivity to ethanol steam reforming reaction than those of CeO₂ and other molar ratio CeO₂-ZrO₂ solid solution. Both reducibility and heat stability of CeO₂can be improved with the addition of ZrO₂.

Key words: hydrogen production, steam reforming of ethanol, nanosized CeO₂-ZrO₂, modified Sol-Gel method

中图分类号:

TQ174

袁文辉, 周辰辰, 李莉. 改进溶胶-凝胶法合成CeO₂-ZrO₂固溶体及催化性能研究[J]. 无机材料学报, 2010, 25(8): 820-824.

YUAN Wen- Hui, ZHOU Chen-Chen, LI Li. Study on Catalytic Properties of Nano-CeO₂-ZrO₂ Mixed Oxides Prepared by Modified Sol-Gel Method[J]. Journal of Inorganic Materials, 2010, 25(8): 820-824.

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改进溶胶-凝胶法合成CeO₂-ZrO₂固溶体及催化性能研究

Study on Catalytic Properties of Nano-CeO₂-ZrO₂ Mixed Oxides Prepared by Modified Sol-Gel Method

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