高等学校化学学报 ›› 2018, Vol. 39 ›› Issue (5): 941.doi: 10.7503/cjcu20170756

• 物理化学 • 上一篇    下一篇

CoSAPO-5分子筛的快速合成及高效催化α-蒎烯与空气环氧化反应

夏坤, 王艺, 周丹, 黄哲, 伍忠汉, 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:2017-11-22 出版日期:2018-04-08 发布日期:2018-04-08
  • 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、 表征及应用方面的研究. E-mail: d.zhou@hubu.edu.cn;夏清华, 男, 博士, 教授, 博士生导师, 主要从事新材料的开发及催化方面的研究. E-mail: xiaqh518@aliyun.com

  • 基金资助:
    国家自然科学基金(批准号: 21571055, 21673069)和湖北省自然科学基金杰出青年项目(批准号: 2016CFA040)资助.

Rapid Synthesis of CoSAPO-5 Zeolite and Efficiently Catalytic Epoxidation of α-Pinene with Air

XIA Kun, WANG Yi, ZHOU Dan*, HUANG Zhe, WU Zhonghan, XIA Qinghua*   

  1. Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials,Key Laboratory for the Synthesis and Application of Organic Functional Molecules,Ministry of Education, Hubei University, Wuhan 430062, China
  • Received:2017-11-22 Online:2018-04-08 Published:2018-04-08
  • Contact: ZHOU Dan,XIA Qinghua
  • Supported by:
    Supported by the National Natural Science Foundation of China(Nos.21571055, 21673069) and the Outstanding Youth Project of Natural Science Foundation of Hubei Province, China(No.2016CFA040).

摘要:

构建了用于催化空气环氧化α-蒎烯合成α-环氧蒎烷的高效、 节能、 绿色催化反应体系. 首先, 采用转动水热晶化模式合成了SAPO-5分子筛前驱体. 相比于静态水热晶化模式, 转动水热晶化模式可以显著缩短分子筛成核时间和晶化时间, 同时可有效减小晶粒尺寸并显著提高晶粒尺寸的均一性. 进一步对SAPO-5分子筛前驱体进行改性制得CoSAPO-5分子筛催化剂, 并对反应溶剂、 催化剂用量、 反应温度和反应时间进行了优化. 在获得的最优催化反应条件下, α-蒎烯转化率可达96.5%, α-环氧蒎烷产率可达89.0%. 催化剂循环实验结果表明, 该催化剂是稳定的、 可多次循环使用的多相催化剂.

关键词: 水热转动晶化, 分子筛, 催化环氧化, α-蒎烯;, CoSAPO-5

Abstract:

A green catalytic reaction system with characteristic of high efficiency and energy saving for the synthesis of α-epoxy pinane by catalytic epoxidation of α-pinene with air was constructed. By using rotating hydrothermal route, the necessary time for crystal nucleation and growth of SAPO-5 was shortened distinctly, meanwhile the crystal size was decreased and the crystal size distribution became more uniform. Then, CoSAPO-5 catalyst was prepared by post treatment of SAPO-5 precursor. Under the investigation for various catalytic reaction conditions systematically, including solvent type, the amount of catalyst, reaction temperature, and reaction time, the optimal reaction system was established, under which the conversion of α-pinene can reach 96.5%, the yield of α-epoxy pinane can reach 89.0%, better than the best results reported. Moreover, CoSAPO-5 catalyst was also used in the catalytic epoxidation of other bulky alkene molecules. The recycling experiments indicate that CoSAPO-5 is an excellent heterogeneous recyclability catalyst.

Key words: Rotation hydrothermal synthesis, Zeolite, Catalytic epoxidation, α-Pinene;, CoSAPO-5

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