化学学报 ›› 2010, Vol. 68 ›› Issue (21): 2161-2166. 上一篇    下一篇

研究论文

有机-无机骨架杂化酸碱双功能高硅Y型沸石的制备和结构表征

陈筱诚,余辉,郭娟,贺鹤勇,傅正文*,龙英才*   

  1. (复旦大学化学系 上海市分子催化与新材料重点实验室 上海 200433)
  • 投稿日期:2010-03-02 修回日期:2010-06-17 发布日期:2010-07-09
  • 通讯作者: 郭娟 E-mail:guojuan@fudan.edu.cn
  • 基金资助:

    国家科委973 计划项目(2003CB615801)资助。

Preparation and Structural Characterization on Organic-inorganic Hybrid Acid-base Bifunctional High Silica Y Zeolite

CHEN Xiao-Cheng, YU Hui, GUO Juan, HE He-Yong, FU Zheng-Wen, LONG Ying-Cai   

  1. (Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Fudan University, Shanghai 200433)
  • Received:2010-03-02 Revised:2010-06-17 Published:2010-07-09

以甲胺水溶液为改性剂, 高硅Y型沸石可在常温下吸附甲胺(MA)制备有机-无机杂化酸碱双功能高硅Y型沸石材料. X 射线粉末衍射(XRD), 固体29Si魔角核磁共振(13C及29Si MAS NMR)表征表明甲胺分子与高硅Y型沸石骨架相互作用导致沸石结构发生变化, 骨架上生成新的Si—N键及Si—OH. 以热重分析(TG/DTG), NH3, CO2程序升温脱附(NH3-TPD和CO2-TPD)研究杂化Y型沸石的酸碱性质及其经不同温度焙烧后的变化, 结果表明, 杂化后沸石的酸/碱量, 尤其是后者明显增大, 其原因是骨架上生成了新的Si—OH及Si—N键.

关键词: 高硅Y型沸石, 杂化, 酸碱双功能, 甲胺, 改性

An organic-inorganic hybrid acid-basic bifunctional HY zeolite has been prepared at room temperature with methylamine as a modifier. Characterized with X-ray powder diffraction (XRD), solid state 13C and 29Si magic angle spinning nuclear magnetic resonance (13C and 29Si MAS NMR), it has been observed that the obvious change of the framework and the appearance of new Si—N bonds and Si—OH in the framework. The acid-basic properties of the hybrid zeolite, investigated with TG/DTG and NH3-TPD or CO2-TPD, have been proved to be obviously enhanced. As pre-calcination at different temperature, the acid amount and basic amount of the modified zeolite increased obviously. It was confirmed that the enhanced acid and base properties mainly came from the structural defects, such as the species of Si—OH and the Si—N on the framework, respectively.

Key words: high silica Y zeolite, hybridation, acid-base bifunctional, methylamine, modification