催化学报

催化学报 ›› 2014, Vol. 35 ›› Issue (10): 1768-1778.DOI: 10.1016/S1872-2067(14)60182-0

• 论文 • 上一篇    

LaXCoO3 (X = Mg, Ca, Sr, Ce) 催化剂的制备及其催化乙醇水蒸气重整制氢

马飞a,b, 丁振武a,c, 储伟a,c, 郝世雄a,d, 齐涛b   

  1. a 四川大学化工学院, 四川 成都 610065;
    b 中国科学院过程工程研究所湿法冶金清洁技术国家工程实验室, 北京 100190;
    c 四川省环境保护环境催化材料工程技术研究中心, 四川 成都 610064;
    d 四川理工学院化工系, 四川 自贡 643000
  • 收稿日期:2014-04-25 修回日期:2014-06-28 出版日期:2014-09-28 发布日期:2014-09-30
  • 通讯作者: 储伟
  • 基金资助:

    国家重点基础研究发展计划（973计划，2011CB201202）.

Preparation of LaXCoO3 (X = Mg, Ca, Sr, Ce) catalysts and their performance for steam reforming of ethanol to hydrogen

Fei Maa,b, Zhenwu Dinga,c, Wei Chua,c, Shixiong Haoa,d, Tao Qib   

  1. a Department of Chemical Engineering, Sichuan University, Chengdu 610065, Sichuan, China;
    b National Engineering Laboratory for Hydrometallurgical Cleaner Production Technology, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China;
    c Sichuan Provincial Engineering Technology Center for Environmental Protection Catalytic Materials, Chengdu 610064, Sichuan, China;
    d Department of Chemical Engineering, Sichuan University of Science and Engineering, Zigong 643000, Sichuan, China
  • Received:2014-04-25 Revised:2014-06-28 Online:2014-09-28 Published:2014-09-30
  • Supported by:

    This work was supported by the National Basic Research Program of China (973 Program, 2011CB201202).

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摘要：

以PEG 400为分散剂，采用一步柠檬酸络合法制备了LaXCoO3 （X = Mg，Ca，Sr，Ce；La：X = 3：2）复合催化剂. 采用X射线衍射、红外光谱、扫描电镜、X射线光电子能谱、N2吸附-脱附和H2程序升温还原等技术对复合催化剂进行了表征，考察了不同元素A位取代对LaCoO3钙钛矿结构的影响，进而研究了其对乙醇水蒸气重整制氢的催化性能和稳定性. 结果表明，在高含量取代时，只有Ce取代的样品能够保持单一的钙钛矿晶型；Ca或Sr取代的样品产生的CO3O4分离相有利于复合催化剂活性中心钴的还原；Sr或Ce取代的样品在反应中表现出较好的活性和稳定性，Sr取代的样品活性更高.

关键词: 柠檬酸络合法, 钙钛矿, 钴, 复合催化剂, 乙醇水蒸气重整, 氢气

Abstract:

Perovskite nanocomposite catalysts LaXCoO3 (X = Mg, Ca, Sr, or Ce; n(La):n(X) = 3:2) have been prepared by a citric acid-complexing method and used for steam reforming of ethanol (SRE), leading to hydrogen generation. The samples were characterized by X-ray diffraction, infrared spectroscopy, scanning electron microscopy, X-ray photoelectron spectroscopy, N2 adsorption-desorption, and H2 temperature-programmed reduction. The effects of elemental substitution in the LaCoO3 perovskite were studied, and the catalytic performance and primary stability of the hydrogen production from SRE were investigated. In the highly substituted samples, only the Ce-doped sample was isolated as the pure perovskite phase. The presence of a Co3O4 phase in the Ca-doped or Sr-doped samples was beneficial for the reduction of the active Co component, while Sr-doped or Ce-doped samples showed good activity and stability. The sample incorporating Sr demonstrated better catalytic performance than those of other samples.

Key words: Citric acid-complexing method, Perovskite, Cobalt, Composite catalyst, Ethanol steam reforming, Hydrogen