催化学报 ›› 2011, Vol. 32 ›› Issue (9): 1537-1544.DOI: 10.3724/SP.J.1088.2011.10508

• 研究论文 • 上一篇    下一篇

载体焙烧温度对 Ru/MgAl2O4 催化剂液相苯部分加氢性能的影响

周功兵, 刘建良, 许可, 裴燕a, 乔明华b, 范康年   

  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:2011-05-28 修回日期:2011-07-21 出版日期:2011-09-09 发布日期:2015-01-24

Liquid-Phase Partial Hydrogenation of Benzene over Ru/MgAl2O4 Catalyst: Effect of Calcination Temperature of MgAl2O4

ZHOU Gongbing, LIU Jianliang, XU Ke, PEI Yana, QIAO Minghuab, FAN Kangnian   

  1. Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200433, China
  • Received:2011-05-28 Revised:2011-07-21 Online:2011-09-09 Published:2015-01-24

摘要: 采用水热合成法制备了镁铝尖晶石 (MgAl2O4) 材料, 制备了其负载的 Ru 催化剂, 研究了 MgAl2O4 焙烧温度对 Ru/MgAl2O4 催化剂上液相苯部分加氢催化性能的影响. 采用 X 射线粉末衍射、27Al 固体核磁共振、傅里叶变换红外光谱、H2-程序升温还原、H2-程序升温脱附、N2 物理吸附、透射电子显微镜和 X 射线光电子能谱等手段对催化剂进行了系统的表征. 结果表明, 在较低的焙烧温度 (773 K) 下即可制得很好尖晶石晶型的 MgAl2O4 材料. 载体焙烧温度对催化剂结构和 Ru 粒径等有显著的影响. 1023 K 焙烧的 MgAl2O4负载的 Ru 催化剂上环己烯选择性及收率最高, 分别可达 52.4% 和 38.5%. 结合催化剂的表征和反应结果, 对载体焙烧温度影响催化剂活性和选择性的原因进行了讨论.

关键词: 钌, 镁铝尖晶石, 焙烧温度, 苯, 部分加氢, 环己烯

Abstract: The MgAl2O4 material was synthesized by the hydrothermal method. A series of Ru/MgAl2O4 catalyst samples were prepared using this MgAl2O4 calcined at different temperatures. The catalyst samples were characterized by powder X-ray diffraction, 27Al solid-state nuclear magnetic resonance spectroscopy, Fourier transform infrared spectroscopy, temperature-programmed reduction, temperature-programmed desorption, N2 physisorption, transmission electron microscopy, and X-ray photoelectron spectroscopy. It was found that the spinel phase readily formed at calcination temperature as low as 773 K. The calcination temperature of MgAl2O4 strongly influenced the structural properties of the catalyst. In the liquid-phase partial hydrogenation of benzene, the Ru/MgAl2O4 catalyst sample calcined at 1023 K exhibited the highest cyclohexene selectivity and yield. The maximum cyclohexene yield was 38.5% and the corresponding selectivity was 52.4%. Based on the characterization results, the effect of the calcination temperature of MgAl2O4 on the activity and selectivity of Ru/MgAl2O4 catalyst samples was discussed.

Key words: ruthenium, magnesium aluminum spinel, calcination temperature, benzene, partial hydrogenation, cyclohexene