催化学报 ›› 2011, Vol. 32 ›› Issue (10): 1656-1661.DOI: 10.3724/SP.J.1088.2011.10653

• 研究论文 • 上一篇    

以阳离子聚合物为介孔模板合成多级孔 TS-1

王晓星, 李钢*, 刘丽萍, 刘海鸥   

  1. 大连理工大学化工学院精细化工国家重点实验室, 辽宁大连 116024
  • 收稿日期:2011-06-25 修回日期:2011-08-10 出版日期:2011-09-30 发布日期:2015-02-12

Synthesis of Hierarchical TS-1 Zeolite Using Cationic Polymer as Mesoporous Template

WANG Xiaoxing, LI Gang*, LIU Liping, LIU Hai’ou   

  1. State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, Liaoning, China
  • Received:2011-06-25 Revised:2011-08-10 Online:2011-09-30 Published:2015-02-12

摘要: 分别以阳离子聚季铵盐-7 和聚季铵盐-6 为介孔模板, 通过水热法合成了多级孔 TS-1 沸石, 采用 X 射线衍射、紫外可见光谱、扫描电镜、透射电镜及 N2 吸附-脱附等手段对所得样品进行了表征, 并考察了其催化苯并噻吩及噻吩氧化反应性能. 结果表明, 聚季铵盐-7 的加入对多级孔 TS-1 的晶化、钛物种的配位状态及晶粒形貌的影响不大; 而随着聚季铵盐-6 用量的增加, 多级孔 TS-1 的晶貌逐渐由立方状转变为长方状晶粒. 两种聚合物合成的多级孔 TS-1 都具有明显的介孔孔道, 而且具有明显高于 TS-1 的催化苯并噻吩氧化反应和相似的噻吩氧化反应性能.

关键词: 聚季铵盐-7, 聚季铵盐-6, 多级孔 TS-1 沸石, 水热合成, 苯并噻吩, 噻吩, 氧化反应

Abstract: Hierarchical TS-1 zeolites were synthesized successfully by the hydrothermal method using cationic polyquaternium-7 and polyquaternium-6 as mesoporous template, respectively. The obtained samples were characterized by X-ray diffraction, UV-Visible spectroscopy, scanning electron microscopy, transmission electron microscopy, and N2 adsorption-desorption. The catalytic performance of the materials was evaluated for the oxidation of bulky molecular benzothiophene and small molecular thiophene. The results show that the addition of polyquaternium-7 has a little effect on the crystallization, the state of titanium sites, and the crystal morphology of hierarchical TS-1. However, the crystal morphology of hierarchical TS-1 changes from small cubic crystals to large rectangular crystals with increasing content of polyquaternium-6. Hierarchical TS-1 zeolites synthesized from the two kinds of polymers possess obvious mesoporous channels. Moreover, they give much higher activity in benzothiophene oxidation than TS-1, which is attributed to the presence of additional mesopores for reducing the diffusion limitation. In addition, hierarchical TS-1 zeolites also exhibit the similar oxidative activity for thiophene to TS-1 and give the removal rate of 100% for 2 h.

Key words: polyquaternium-7, polyquaternium-6, hierarchical TS-1 zeolite, hydrothermal synthesis, benzothiophene, thiophene, oxidation