催化学报

催化学报 ›› 2007, Vol. 28 ›› Issue (9): 817-822.

• 研究论文 • 上一篇    下一篇

ZSM-34分子筛的合成及其催化甲醇转化制烯烃反应性能

周帆1,2,田鹏1,刘中民1,刘广宇1,常福祥1,2,李金哲1,2   

  1. 1 中国科学院大连化学物理研究所, 辽宁大连 116023; 2 中国科学院研究生院, 北京 100049
  • 收稿日期:2007-09-25 出版日期:2007-09-25 发布日期:2011-09-28

Synthesis of ZSM-34 and Its Catalytic Properties in Methanol-to-Olefins Reaction

ZHOU Fan1,2, TIAN Peng1, LIU Zhongmin1*, LIU Guangyu1, CHANG Fuxiang1,2, LI Jinzhe1,2   

  1. 1 Dalian Institute of Chemical Physics, The Chinese Academy of Sciences, Dalian 116023, Liaoning, China; 2 Graduate University of Chinese Academy of Sciences, Beijing 100049, China
  • Received:2007-09-25 Online:2007-09-25 Published:2011-09-28

PDF

688

摘要： 以氯化胆碱为模板剂,采用水热合成法在较短的晶化时间内合成了OFF/ERI共晶体ZSM-34, 考察了各种合成条件对产物的影响. 通过调变合成参数可以获得不同ERI含量的ZSM-34. 用X射线衍射、扫描电子显微镜和X射线荧光分析等对合成产物进行了表征. 吸附实验显示,所合成的分子筛具有较大的孔容,其对正己烷的吸附容量为11.4%. HZSM-34分子筛对甲醇转化制烯烃(MTO)反应具有良好的催化活性和高的乙烯选择性,低碳烯烃(乙烯+丙烯)选择性高达86.0%, 并且在反应过程中始终维持在较高的水平,不受甲醇转化率降低的影响. 高温水蒸气处理后的分子筛酸性降低,大大抑制了MTO初始反应中丙烷的选择性,而初始低碳烯烃的选择性则明显提高.

关键词: ZSM-34, 分子筛, 水热合成, 甲醇转化制烯烃, 氯化胆碱

Abstract: ZSM-34 (OFF/ERI intergrowth) was synthesized using choline chloride as the template in a shorter crystallization time under hydrothermal conditions. Many factors that may influence the synthesis were investigated. The ERI content in ZSM-34 could be adjusted by selecting different synthesis conditions. The synthesized products were characterized byX-raydiffraction, scanning electron microscopy, andX-rayfluorescence spectroscopy. Adsorption experiments showed that ZSM-34 possessed high pore volume, and the adsorption amount of n-hexane reached 11.4%. In the methanol-to-olefins reaction, HZSM-34 exhibited high selectivity for ethylene. The maximum selectivity for total olefins (C2H4+C3H6) over HZSM-34 was 86.0%, and it nearly did not change even when the methanol conversion decreased. High-temperature steam treatment increased the framework Si/Al ratio and thus decreased the acidity of HZSM-34, which led to the obvious decrease in propane selectivity and the increase in initial olefins selectivity.

Key words: ZSM-34, molecular sieve, hydrothermal synthesis, methanol-to-olefins reaction, choline chloride