动态水热法制备Silicalite-1分子筛膜包覆多孔缺陷Al2O3微球

doi:10.16085/j.issn.1000-6613.2017-2224

化工进展 ›› 2018, Vol. 37 ›› Issue (10): 3943-3948.DOI: 10.16085/j.issn.1000-6613.2017-2224

动态水热法制备Silicalite-1分子筛膜包覆多孔缺陷Al₂O₃微球

董道敏¹, 刘宾^1,2, 柴永明^1,2, 吴仪岚¹, 刘晨光^1,2

1 中国石油大学(华东)化学工程学院, 重质油国家重点实验室, 山东青岛 266580;
2 中国石油天然气集团公司催化重点实验室, 山东青岛 266580

收稿日期:2017-10-30 修回日期:2018-03-12 出版日期:2018-10-05 发布日期:2018-10-05
通讯作者: 刘晨光,教授,博士生导师,主要从事油品加氢精制和工业催化研究;柴永明,副教授,硕士生导师,主要从事超清洁油品加氢催化剂与工艺研究。
作者简介:董道敏(1992-),女,硕士研究生,研究方向为石油与天然气加工。
基金资助:
国家重点研发计划（2017YFB0306600）、国家自然科学基金（U1662119）及中央高校基本科研专项资金项目（17CX02061）。

Dynamic hydrothermal synthesis of Silicalite-1 zeolite membrane to encapsulate defective porous alumina spheres

DONG Daomin¹, LIU Bin^1,2, CHAI Yongming^1,2, WU Yilan¹, LIU Chenguang^1,2

1 State Key Laboratory of Heavy Oil Processing, School of Chemical Engineering, China University of Petroleum(East China), Qingdao 266580, Shandong, China;
2 Key Laboratory of Catalysis, China National Petroleum Corporation, Qingdao 266580, Shandong, China

Received:2017-10-30 Revised:2018-03-12 Online:2018-10-05 Published:2018-10-05

摘要/Abstract

摘要： 采用晶种涂覆-预晶化-晶化成膜的动态水热法成功在具有多孔缺陷的氧化铝微球上合成Silicalite-1分子筛膜。以乙醇作为润湿试剂在氧化铝表面涂覆一层晶种，将涂覆过晶种的载体加入到分子筛合成液中预晶化，一层分子筛完全覆盖载体并与载体结合牢固。预晶化后的载体在动态水热条件下处理3天，得到致密分子筛膜包覆的Al₂O₃微球。运用X射线衍射（XRD）和扫描电镜（SEM）对所得材料进行表征。结果表明，包覆的分子筛膜具有典型的MFI结构，晶粒交互生长，厚度约为3μm。考察了TPAOH用量和水量对分子筛膜微观结构的影响，结果发现TPAOH用量主要影响Silicalite-1分子筛膜的形貌，当TPAOH用量为0.17时，合成的Silicalite-1分子筛膜连续致密，而水量对分子筛膜微观结构的影响较小。这种晶种涂覆-预晶化-晶化成膜的方法有助于在多孔缺陷的Al₂O₃微球上制备高质量的分子筛膜。

关键词: 氧化铝, Silicalite-1分子筛膜, 复合材料, 动态水热法, 制备

Abstract: Silicalite-1 zeolite membranes were successfully prepared on defective porous alumina spheres by dynamic hydrothermal synthesis method through a seeding-pre-crystallizationcrystallization process. A layer of MFI zeolite seed was coated on the surface of alumina supports with ethanol as the wetting agent. Then the supports with the seeds were added into the zeolite synthesis solution for pre-crystallization. A layer of zeolite crystal covered the alumina support completely and had a strong bonding with the support. The pre-crystallized alumina supports were mixed with the synthesis solution for crystallization to obtain dense zeolite-membrane-coated alumina spheres. X-ray diffraction (XRD) and scanning electron microscopy (SEM) were used to characterize the samples. The results showed that the as-prepared membranes were polycrystalline with typical MFI zeolite structure and were well intergrown. The thickness of the Silicalite-1 zeolite membrane was about 3μm. In addition, the effects of tetrapropylammonium hydroxide (TPAOH) content and water (H₂O) content on the microstructure of zeolite membranes were investigated. The results indicated that TPAOH content affected the morphology of the Silicalite-1 zeolite membranes. The Silicalite-1 zeolite membranes were continuous and dense when the TPAOH content was 0.17. On the other hand, the H₂O content has small influence on the microstructure of the zeolite membranes. The seeding-pre-crystallization-crystallization method is an effective approach for the preparation of MFI zeolite membranes on defective porous alumina spheres.

Key words: alumina, Silicalite-1 zeolite membranes, composites, dynamic hydrothermal method, preparation

中图分类号:

O643

董道敏, 刘宾, 柴永明, 吴仪岚, 刘晨光. 动态水热法制备Silicalite-1分子筛膜包覆多孔缺陷Al₂O₃微球[J]. 化工进展, 2018, 37(10): 3943-3948.

DONG Daomin, LIU Bin, CHAI Yongming, WU Yilan, LIU Chenguang. Dynamic hydrothermal synthesis of Silicalite-1 zeolite membrane to encapsulate defective porous alumina spheres[J]. Chemical Industry and Engineering Progress, 2018, 37(10): 3943-3948.

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动态水热法制备Silicalite-1分子筛膜包覆多孔缺陷Al₂O₃微球

Dynamic hydrothermal synthesis of Silicalite-1 zeolite membrane to encapsulate defective porous alumina spheres

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