高等学校化学学报 ›› 2019, Vol. 40 ›› Issue (6): 1222-1228.doi: 10.7503/cjcu20180844

• 物理化学 • 上一篇    下一篇

Ti-Beta分子筛的控制合成及高效催化环己烯环氧化

刘新超, 赵亚榕, 袁珍闫, 周丹(), 鲁新环, 夏清华()   

  1. 湖北大学有机化工新材料湖北省协同创新中心, 有机功能分子合成与应用教育部重点实验室, 武汉 430062
  • 收稿日期:2018-12-17 出版日期:2019-06-10 发布日期:2019-04-04
  • 作者简介:

    联系人简介: 周丹, 女, 博士, 教授, 博士生导师, 主要从事分子筛类孔材料的合成、 表征及应用研究. E-mail: d.zhou@hubu.edu.cn;夏清华, 男, 博士, 教授, 博士生导师, 主要从事多孔催化材料的开发及催化性能研究. E-mail: xiaqh518@aliyun.com

  • 基金资助:
    国家自然科学基金(批准号: 21571055, 21673069, 21503074)和湖北省自然科学基金杰青项目(批准号: 2016CFA040)资助.

Controllable Synthesis of Ti-Beta Zeolite and Efficiently Catalytic Epoxidation of Cyclohexene

LIU Xinchao, ZHAO Yarong, YUAN Zhenyan, ZHOU Dan(), LU Xinhuan, XIA Qinghua()   

  1. Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials, Ministry-of-Education Key Laboratory for the Synthesis and Application of Organic Functional Molecules, Hubei University, Wuhan 430062, China
  • Received:2018-12-17 Online:2019-06-10 Published:2019-04-04
  • Supported by:
    † Supported by the National Natural Science Foundation of China(Nos.21571055, 21673069, 21503074) and the Outstanding Youth Foundation of Hubei Province, China(No.2016CFA040).

摘要:

构建了以H2O2为氧化剂催化环己烯合成环氧环己烷的高效、 绿色催化反应体系. 在不加入铝源的情况下, 以四乙基氢氧化铵(TEAOH)为模板剂, 通过改进的干胶转化法控制H2O/SiO2摩尔比为1.5合成出Ti-Beta分子筛. 实验结果表明, 适宜的酸碱性、 含水量以及模板剂用量显著影响分子筛的结晶度, 同时影响晶粒尺寸和晶粒尺寸的均一性. 通过对Ti-Beta分子筛原粉进行焙烧处理制得Ti-Beta分子筛催化剂, 再通过对反应溶剂、 反应温度和反应时间的筛选和优化, 获得最优催化反应条件, 在该条件下, 环己烯转化率可达33.5%, 环氧环己烷选择性可达99.6%. 实验结果表明该催化剂是一种高效的多相催化剂.

关键词: 过氧化氢, 干胶转化, Ti-Beta分子筛, 催化环氧化, 环己烯

Abstract:

The construction of a green catalytic reaction system with characteristic of high efficiency for the synthesis of epoxycyclohexane by catalytic epoxidation of cyclohexene with H2O2 was focused. We succeeded in synthesizing Ti-Beta zeolites in the absence of Al by the dry-gel conversion method using tetraethylammonium hydroxide(TEAOH) as the structure directing agent with n(H2O)/n(Si) of about 1.5. We found that the crystallization, the uniformity of crystal and size of Ti-Beta were significantly affected by proper acidity and basicity, the amount of water and template dosage. Then, highly efficient Ti-Beta catalyst was prepared by calcination treatment of the raw powder. Under the optimal catalytic reaction conditions, the cyclohexene conversion of 33.5% and the epoxidation selectivity of 99.6% were achieved. The results indicate that Ti-Beta is an excellent heterogeneous catalyst.

Key words: H2O2, Dry-gel conversion, Ti-Beta zeolite, Catalytic epoxidation, Cyclohexene

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