波谱学杂志 ›› 1995, Vol. 12 ›› Issue (2): 147-154.

• 研究论文 • 上一篇    下一篇

晶化时间及硅源对SAPO-5分子筛的结构及模板剂状态的影响

肖天存1, 安立敦1, 王弘立1, 邓风2, 杨年华2, 裘鉴卿2   

  1. 1. 中国科学院兰州化学物理研究所, 兰州 730000;
    2. 中国科学院武汉物理研究所, 武汉 430071
  • 收稿日期:1994-06-21 修回日期:1994-08-08 出版日期:1995-04-05 发布日期:2018-01-17
  • 基金资助:
    甘肃省青年自然科学基金资助项目

EFFECT OF AGING TIME AND SILICON SOURCE ON THE STRUCTURE AND TEMPLATE STATES OF SAPO-5 MOLECULAR SIEVES

Xiao Tiancun1, An Lidun1, Wang Hongli1, Deng Feng2, Yang Nianhua2, Qiu Jianging2   

  1. 1. Lanzhou Institute of Chenucal Physics, Chinese Academy of Sciences, Lanzhou 730000;
    2. Wuhan Institute of Physics, Chinese Academy of Scienas, Wuhan 430071
  • Received:1994-06-21 Revised:1994-08-08 Online:1995-04-05 Published:2018-01-17

摘要: 通过改变硅源和晶化时间的方法,采用水热法合成了系列SAPO-5分子筛材料,用X光衍射(XRD)和27Al MAS NMR对产物的晶相结构进行表征,用13C CP MAS NMR研究了不同阶段的产物中模板剂的存在状态。结果可见:以SiO2凝胶为硅源时;薄水铝石反应物有较高的活性,在48h的晶化时间内,延长晶化时间有助于SAPO-5分子筛的完整结晶,当晶化时间超过48h时,其中已形成的SAPO-5的结构部分被破坏,并转化为SAPO-34.且SAPO-34的量随晶化时间的延长而增多。当以Si(OEt)4为硅源时,铝反应物的反应活性较低,在72h的晶化时间范围内,延长晶化时间有助于SAPO-5产物的形成,使其结构愈加完整,在SAPO-5分子筛的形成过程中,模板剂的状态随分子筛结构的变化而变化,由于三乙胺(Et3N)模板剂中的甲基和亚甲基所处位置不同,其弛豫时间受分子筛结构的影响较大,可用其中甲基的13C MAS NMR诺线的强度及化学位移来表示分子筛结构的完整性。

关键词: SAPO-5分子筛结构, 模板剂状态, 硅源, 晶化时间, MAS NMR

Abstract: A series of SAPO-5 molecular sieves have been synthesized by varying the aging time and silicon source, their structures have been characterlzed by XRD and 27Al MAS NMR spectra. The state of the template in molecular sieves were studied by 13C CP MAS NMR. The results reveal that when using silicon gel as silicon source, prolonging aging time can improve the structure of SMO-5 within a linlit of 48 h, when beyond this limit,the produced SAPO-5 is gradually decomposed and some of them is changed into SAPO-34 with a chabazite structure. However, when using Si(OEt)4 as silicon source, prolonging aging time can improve the structure of SAPO-5 and make Si occupy the framework in the crystallization time of 0 to 72 h. These differences may result from that SiO2 gel has a higher activity than Si(OEt)4.The results of 13C MAS NMR of the tcmplate in SAPO-5 show that SAPO-5 has some influence on the state of the template. Probably for the methyl group in Et3N existing at the gate of the pore,the framework can exert some effect on it,so its delay time is different from that of the methylene group connected with nitrogen. Its NMR line intensity decreases with the crystallinity of SAPO-5 and can be used as a pro be to study the crystallinity of SAPO-5.

Key words: Structure of SAPO-5 molecular sieve, Template state, Silicon souroc, Agingtime, MAS NMR