SAPO-11分子筛晶化过程研究

doi:10.1016/S1872-2067(12)60542-7

催化学报 ›› 2013, Vol. 34 ›› Issue (3): 593-603.DOI: 10.1016/S1872-2067(12)60542-7

SAPO-11分子筛晶化过程研究

李冰^a, 田鹏^a, 齐越^a, 张琳^a, 徐舒涛^a, 苏雄^a,b, 樊栋^a,b, 刘中民^a

a 中国科学院大连化学物理研究所洁净能源国家实验室(筹), 甲醇制烯烃国家工程实验室, 辽宁大连 116023;
b 中国科学院大学, 北京 100049

收稿日期:2012-11-21 修回日期:2012-12-30 出版日期:2013-04-02 发布日期:2013-04-03
通讯作者: 刘中民

Study of crystallization process of SAPO-11 molecular sieve

LI Bing^a, TIAN Peng^a, QI Yue^a, ZHANG Lin^a, XU Shutao^a, SU Xiong^a,b, FAN Dong^a,b, LIU Zhongmin^a

a Dalian National Laboratory for Clean Energy, National Engineering Laboratory for Methanol-to-Olefins, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
b University of Chinese Academy of Sciences, Beijing 100049, China

Received:2012-11-21 Revised:2012-12-30 Online:2013-04-02 Published:2013-04-03

摘要/Abstract

摘要：

采用X射线衍射、X射线荧光光谱、扫描电镜和固体核磁等方法研究了SAPO-11分子筛的水热晶化过程.结果表明,晶化初期,SAPO-11和一种具有磷硅铝组成的未知晶相同时生成;随着晶化的进行,中间相溶解,SAPO-11的生成速率大大增加,呈现快速晶化的特征;至2.33h后,SAPO-11的结晶度接近100%,并保持至晶化结束.硅从晶化初期即参与了SAPO-11的形成,它在晶体中的含量随晶化时间的延长而逐渐增加.硅原子主要以硅岛的形式分布于SAPO-11分子筛骨架中,从而导致多种硅配位环境的存在.分析显示,SAPO-11分子筛呈现外表面富硅的特点,结合晶化过程的分析可推测,硅在SAPO-11分子筛晶体中的分布不均匀,其含量从内向外递增.

关键词: SAPO-11分子筛, 表征, 晶化过程, 硅分布

Abstract:

The crystallization process of SAPO-11 was studied using a combination of X-ray diffraction, scanning electron microscopy, X-ray fluorescence, nuclear magnetic resonance, and X-ray photoelectron spectroscopy. In the initial stage of crystallization, SAPO-11 was formed along with an unknown crystalline material composed of Si-P-Al. As crystallization evolved, the crystalline material dissolved. The SAPO-11 formation rate increased greatly, which is characteristic of fast crystallization. After 2.33 h, the relative crystallinity of SAPO-11 reached ~100% and remained at a high level until crystallization was complete. Si was incorporated into the SAPO-11 framework from the initial stage of crystallization. The Si content of the solid samples increased with crystallization time. Most of the Si atoms existed as Si islands in the SAPO-11 framework, resulting in the presence of multiple coordination environments, i.e., Si(nAl, (4-n)Si), n=0-4. X-ray photoelectron spectroscopy analysis revealed Si enrichment on the external surfaces of the SAPO-11 crystals. Based on the experimental results, the distribution of Si in the crystals is not uniform, showing an increasing trend from the core to the surface.

Key words: SAPO-11 molecular sieve, Characterization, Crystallization process, Silicon distribution

李冰, 田鹏, 齐越, 张琳, 徐舒涛, 苏雄, 樊栋, 刘中民. SAPO-11分子筛晶化过程研究[J]. 催化学报, 2013, 34(3): 593-603.

LI Bing, TIAN Peng, QI Yue, ZHANG Lin, XU Shutao, SU Xiong, FAN Dong, LIU Zhongmin. Study of crystallization process of SAPO-11 molecular sieve[J]. Chinese Journal of Catalysis, 2013, 34(3): 593-603.

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SAPO-11分子筛晶化过程研究

Study of crystallization process of SAPO-11 molecular sieve

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