催化学报 ›› 2007, Vol. 28 ›› Issue (8): 715-719.

• 研究论文 • 上一篇    下一篇

多孔Pd/α-Al2O3活性膜上1,5-环辛二烯选择加氢

周永华1,叶红齐1,Reinhard SCHOMACKER2   

  1. 1 中南大学化学化工学院粉体技术研究所, 湖南长沙 410083; 2 柏林工业大学化学研究所, 柏林 10623, 德国
  • 收稿日期:2007-08-25 出版日期:2007-08-25 发布日期:2011-08-19

Selective Hydrogenation of1,5-Cyclo-octadiene over Porous Pd/α-Al2O3 Active Membrane

ZHOU Yonghua1, YE Hongqi1, Reinhard SCHOMACKER2   

  1. 1 Institute of Powder Technology, College of Chemistry and Chemical Engineering, Central South University, Changsha 410083, Hunan, China; 2 Institute of Chemistry, Technical University of Berlin, Berlin 10623, Germany
  • Received:2007-08-25 Online:2007-08-25 Published:2011-08-19

摘要: 利用微乳液及浸渍技术制备了多孔Pd/α-Al2O3催化活性膜. 利用透射电镜、扫描电镜和X射线衍射对微乳液中及α-Al2O3陶瓷膜孔结构中纳米Pd颗粒的形貌和分布进行了表征. 分析结果表明,通过浸渍技术,微乳液中的纳米Pd颗粒以几百纳米大小的晶体形态均匀负载于陶瓷膜孔中. 在“催化接触器”型膜反应器中,以1,5-环辛二烯催化加氢为模型反应,考察了多孔Pd/α-Al2O3膜的活性与选择性,并与Pd-聚丙烯酸(PAA)有机催化膜反应器、悬浮床反应器和固定床反应器中的催化性能进行了比较. 结果表明, Pd/α-Al2O3膜反应器的催化活性与目的产物1-环辛烯的选择性远高于Pd-PAA有机膜反应器和固定床反应器. Pd/α-Al2O3膜反应器在强化传质和消除孔内扩散方面效果显著,这与Pd在陶瓷膜孔中的分布及反应物在膜反应器中的高速流动有关.

关键词: 钯, 氧化铝, 催化活性膜, 膜反应器, 5-环辛二烯, 选择加氢, 微乳液

Abstract: Porous Pd/α-Al2O3 catalytically active membrane was prepared by microemulsion and impregnation techniques. Palladium nanoparticles in the microemulsion and in the pore structure of α-Al2O3 membrane were characterized by transmission electron microscopy, scanning electron microscopy, andX-raydiffraction. The results show that the palladium nanoparticles dispersed in microemulsion are evenly immobilized in the pore structure of the membrane in the form of palladium crystalline particles with several hundred nanometers by impregnation. The catalytic activity and selectivity of porous Pd/α-Al2O3 active membranes were investigated for the hydrogenation of1,5-cyclo-octadiene (COD) in a catalytic membrane contactor and were compared with the Pd-polyacrylic acid (PAA) membrane reactor (MR), slurry reactor, and fixed-bed reactor (FBR). The results show that both reaction rate of COD and selectivity for 1-cyclo-octene in Pd/α-Al2O3 MR are considerably improved compared with Pd-PAA MR and FBR. The effects of Pd/α-Al2O3 MR in facilitating mass transfer and in eliminating diffusion inside the pores are remarkable. This can be attributed to the distribution of palladium in the membrane structure and the high flow rate of reactants in the membrane pores.

Key words: palladium, alumina, catalytically active membrane, membrane reactor, 5-cyclo-octadiene, selective hydrogenation, microemulsion