催化学报

催化学报 ›› 2012, Vol. 33 ›› Issue (7): 1236-1241.DOI: 10.3724/SP.J.1088.2012.20226

• 研究论文 • 上一篇    

干胶法制备钛硅沸石及其催化性能

王维海, 李钢*, 刘丽萍, 陈永英   

  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:2012-02-13 修回日期:2012-05-02 出版日期:2012-06-21 发布日期:2012-06-21

Titanium Silicalite Synthesized by Dry Gel Conversion Method and Its Catalytic Performance

WANG Weihai, LI Gang*, LIU Liping, CHEN Yongying   

  1. State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, Liaoning, China
  • Received:2012-02-13 Revised:2012-05-02 Online:2012-06-21 Published:2012-06-21

PDF

778

被引次数

12

摘要： 以四丙基溴化铵为模板剂, 以乙二胺 (EDA) 为碱源, 采用干胶法制备了 TS-1, 并在此基础上引入介孔/大孔模板剂蔗糖而制备出多级孔道 TS-1. 采用 X 射线衍射、紫外-可见光谱及 N2 物理吸附-脱附等手段对所得样品进行了表征, 并考察了它们催化噻吩 (Th) 及苯并噻吩 (BT) 氧化反应的性能. 结果表明, 随着釜底部 n(EDA)/n(H2O) 比的降低, TS-1 结晶度、骨架 Ti 含量及其在 Th 氧化反应中的催化活性均升高. 而当以乙胺和正丁胺为碱源时, TS-1 难以晶化. 所制备的多级孔道 TS-1 样品具有介孔/大孔孔道, 在 Th 氧化反应中的催化活性高于 TS-1; 对于 BT 的氧化, 当 n(sucrose)/n(SiO2) 为 0.35 时,制备的多级孔道 TS-1 样品的催化活性最高, BT 脱除率可达 100%, 而 TS-1 则无催化活性.

关键词: 干胶法, TS-1 沸石, 多级孔道, 噻吩, 苯并噻吩, 催化氧化

Abstract: TS-1 zeolite was synthesized by dry gel conversion technique with ethylenediamine (EDA) as alkali source and tetrapropylammonium bromide as template. On this base, the hierarchical TS-1 was prepared with sucrose as meso/macropore template. The obtained samples were characterized by powder X-ray diffraction, UV-Vis spectroscopy, and N2 physical adsorption-desorption. The catalytic performance of the samples was evaluated using the oxidation of small molecular thiophene (Th) and bulky molecular benzothiophene (BT). With the decrease of the EDA/H2O molar ratio at the bottom of autoclave, TS-1 samples presented the trend of increase for the crystallinity, Ti content in framework, and the catalytic activity in Th oxidation. When the ethylamine and n-butylamine were used as the alkali source, it was difficult for TS-1 to crystallize. Hierarchical TS-1 possessed mesopore/macropore and exhibited higher catalytic performance than TS-1 in Th oxidation. For the oxidation of BT, hierarchical TS-1 synthesized with sucrose/SiO2 molar ratio of 0.35 presented the highest activity and the BT removal rate could reach almost 100%. However, the TS-1 had no catalytic activity in oxidation of BT.

Key words: dry gel conversion, TS-1 zeolite, hierarchical pore, thiophene, benzothiophene, catalytic oxidation