催化学报 ›› 2014, Vol. 35 ›› Issue (10): 1676-1686.DOI: 10.1016/S1872-2067(14)60133-9

• 论文 • 上一篇    下一篇

SAPO-11/Beta 复合分子筛的合成及其异构化性能研究

朱数金a,b, 刘粟侥a,b, 张怀科a,c, 吕恩静c, 任杰a,c   

  1. a 中国科学院山西煤炭化学研究所煤转化国家重点实验室, 山西 太原 030001;
    b 中国科学院大学, 北京 100049;
    c 中科合成油技术有限公司煤液化国家能源中心, 北京 101407
  • 收稿日期:2014-03-07 修回日期:2014-04-10 出版日期:2014-09-28 发布日期:2014-09-30
  • 通讯作者: 任杰

Investigation of synthesis and hydroisomerization performance of SAPO-11/Beta composite molecular sieve

Shujin Zhua,b, Suyao Liua,b, Huaike Zhanga,c, Enjing Lüc, Jie Rena,c   

  1. a State key Laboratory of Coal Conversion, Shanxi Institute of Coal Chemistry, Chinese Academy of Science, Taiyuan 030001, Shanxi, China;
    b University of Chinese Academy of Sciences, Beijing 10049, China;
    c National Energy Center for Coal to Liquids, Synfuels China Co., Ltd, Beijing 101400, China
  • Received:2014-03-07 Revised:2014-04-10 Online:2014-09-28 Published:2014-09-30

摘要:

以Beta分子筛为硅源通过水热合成法合成了SAPO-11/Beta复合分子筛,采用X射线衍射、N2物理吸脱附、扫描电镜、透视电镜-能谱分析、固体核磁及吡啶红外等方法对单分子筛、复合分子筛和机械混合分子筛的物化性质进行了表征. 以正十二烷为模型化合物,在固定床反应器上考察了铂负载型分子筛催化剂的异构化性能. 结果表明,复合分子筛的物理化学性质明显不同于单分子筛和机械混合分子筛,其呈现核壳结构,SAPO-11和Beta间存在化学作用,使得复合分子筛具有适宜的B酸分布. 在正十二烷异构化反应中,复合分子筛催化剂的异构化性能优于单分子筛催化剂和机械混合分子筛催化剂,多支链异构体收率高.

关键词: SAPO-11, Beta分子筛, 复合分子筛, 核壳结构, 协同作用, 临氢异构化反应, 多支链异构体

Abstract:

The SAPO-11/Beta composite molecular sieve was synthesized by the hydrothermal method with zeolite Beta as the silicon source. The physicochemical properties of SAPO-11, Beta molecular sieve, the composite molecular sieve, and the mechanical mixture of SAPO-11 and Beta molecular sieve were characterized by X-ray diffraction, N2 adsorption-desorption, scanning electron microscopy, transmission electron microscopy-energy dispersive spectroscopy, magic-angle spinning nuclear magnetic resonance, and pyridine adsorption infrared spectroscopy. In addition, the catalytic performance of platinum-loaded zeolite samples in the hydroisomerization of n-dodecane was investigated. The results indicate that the properties and catalytic performance of the composite molecular sieve were quite different from those of the pure zeolites and the mechanical mixture. Compared with the mechanical mixture, the combination of SAPO-11 and Beta by chemical bonds was more tightly bound in the composite molecular sieve with a core-shell structure. The acidity and pore structure of the composite were favorable for catalytic performance in the hydroisomerization of n-dodecane. The composite catalyst was superior to the other catalysts, especially in the yield of multibranched isomers.

Key words: SAPO-11, Beta molecular sieve, Composite molecular sieve, Core-shell structure, Synergistic effect, Hydroisomerization, Multibranched isomers