高等学校化学学报 ›› 2009, Vol. 30 ›› Issue (6): 1162.

• 研究论文 • 上一篇    下一篇

Ga2O3/HZSM-5催化剂上丙烷脱氢反应

任英杰, 华伟明, 乐英红, 高滋   

  1. 复旦大学化学系, 上海市分子催化和功能材料重点实验室, 上海 200433
  • 收稿日期:2009-01-07 出版日期:2009-06-10 发布日期:2009-06-10
  • 通讯作者: 乐英红, 男, 博士, 教授, 博士生导师, 主要从事多相催化剂研究. E-mail: yhyue@fudan.edu.cn
  • 基金资助:

    国家自然科学基金(批准号: 20633030, 20773027和20773028)、国家“九七三”计划项目(批准号: 2006CB806103)和上海市科学技术委员会(批准号: 08DZ2270500)资助.

Dehydrogenation of Propane to Propene over Ga2O3/HZSM-5 Catalysts

REN Ying-Jie, HUA Wei-Ming, YUE Ying-Hong*, GAO Zi   

  1. Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200433, China
  • Received:2009-01-07 Online:2009-06-10 Published:2009-06-10
  • Contact: YUE Ying-Hong, E-mail: yhyue@fudan.edu.cn
  • Supported by:

    国家自然科学基金(批准号: 20633030, 20773027和20773028)、国家“九七三”计划项目(批准号: 2006CB806103)和上海市科学技术委员会(批准号: 08DZ2270500)资助.

摘要:

以直接水热合成和低硅沸石高温水蒸气脱铝两种方法制备了不同Si/Al摩尔比的HZSM-5载体, 考察了Ga2O3/HZSM-5催化剂上丙烷脱氢制丙烯的反应性能. 结合XRD, N2气吸附, 27Al MAS NMR和NH3-TPD等表征方法, 讨论了催化剂酸性质和孔性质与性能的关系. 实验结果表明, 减少催化剂表面的中强酸量可以显著提高反应的稳定性和丙烯的选择性; 水蒸气脱铝所增加的介孔有同样的效果, 这可能是由于介孔的存在有利于丙烯的脱附和扩散而抑制了寡聚、环化等副反应的发生, 减少了表面积炭的可能性.

关键词: Ga2O3/HZSM-5, 丙烷, 脱氢, 二氧化碳, 稳定性

Abstract:

Dehydrogenation of propane to propene in the presence of CO2 was carried out over Ga2O3 catalysts supported on HZSM-5 with different Si/Al molar ratios. The structural and acidic properties were characterized by XRD, XRF, N2 adsorption, 27Al MAS NMR, NH3-TPD and model acid-catalyzed reaction. It is found that the stability of supported Ga2O3 catalysts for the reaction improves with increasing Si/Al molar ratio of HZSM-5 support, which is thought to be caused by the decrease of the acidity of the catalysts, resulting in the suppression of the side reactions. The stability can also be enhanced by the mesopores generated by steaming, due to the promotion of the diffusion and desorption of the propene.

Key words: Ga2O3/HZSM-5, Propane, Dehydrogenation, Carbon dioxide, Stability

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