石油炼制与化工 ›› 2025, Vol. 56 ›› Issue (6): 28-35.

• 催化剂 • 上一篇    下一篇

蒸汽辅助晶化法制备高骨架钛含量纳米TS-1分子筛及其催化1-己烯环氧化性能

朱婷婷1,邓青桃1,董鹏2,李铁森1,2,崔勍焱1,施杰2,周林裕2,岳源源1,2   

  1. 1. 福州大学化工学院
    2. 清源创新实验室
  • 收稿日期:2024-11-22 修回日期:2025-01-03 出版日期:2025-06-12 发布日期:2025-05-30
  • 通讯作者: 岳源源 E-mail:yueyy@fzu.edu.cn
  • 基金资助:
    国家自然科学基金项目;国家自然科学基金项目;清源创新实验室贵重仪器设备开放测试基金;清源创新实验室贵重仪器设备开放测试基金;清源创新实验室贵重仪器设备开放测试基金

STEAM-ASSISTED SYNTHESIS OF NANO TS-1 ZEOLITE WITH HIGH FRAMEWORK TITANIUM CONTENT FOR CATALYTIC EPOXIDATION OF 1-HEXENE

  • Received:2024-11-22 Revised:2025-01-03 Online:2025-06-12 Published:2025-05-30

摘要: 常规TS-1分子筛存在反应活性位点(骨架钛物种)数量有限和可及性差的问题,降低了其催化烯烃环氧化的性能。基于此,采用溶剂络合钛源与硅源预水解相结合的策略,以蒸汽辅助晶化法合成出具有高骨架钛含量的纳米TS-1分子筛,并与利用水热晶化法制备出的具有高骨架钛含量的常规TS-1分子筛样品进行对比。结果表明:所制备的纳米TS-1分子筛比商业TS-1分子筛和所合成的常规TS-1分子筛具有更小的晶粒尺寸和更高的外比表面积;与对比样品相比,所制备的纳米TS-1分子筛具有更高的骨架钛含量,因此在被应用于1-己烯环氧化反应时,其表现出比对比催化剂更优异的催化性能,1-己烯转化率为70.4%,1,2-环氧己烷选择性和收率分别为94.0%和66.2%。

关键词: 纳米TS-1分子筛, 溶剂络合, 蒸汽辅助晶化, 高骨架钛含量, 1-己烯环氧化

Abstract: Conventional TS-1 zeolite has the problems of limited number and poor accessibility of active sites (framework titanium species), reducing its catalytic performance for olefin epoxidation. To address these issues, a nano TS-1 zeolite with high framework titanium content was synthesized using a combination of solvent-complexed titanium source and pre-hydrolyzed silicon source via steam-assisted crystallization, and compared with conventional TS-1 zeolite with high framework titanium contentprepared using hydrothermal crystallization. The results show that compared with commercial and synthesized conventional TS-1 zeolites, the resultant nano TS-1 zeolite owns smaller crystal size, abundant external specific surface and higher framework titanium content. As a result,when applied to the 1-hexene epoxidation reaction, the resultant nano TS-1 zeolite demonstrates superior catalytic performance compared to the reference catalysts, reflected by a 1-hexene conversion of 70.4%, with selectivity and yield of 1,2-epoxyhexane at 94.0% and 66.2%, respectively.

Key words: nano TS-1 zeolite, solvent complexation, steam-assisted crystallization, high framework titanium content, 1-hexene epoxidation