高等学校化学学报 ›› 2019, Vol. 40 ›› Issue (4): 755-762.doi: 10.7503/cjcu20180750

• 物理化学 • 上一篇    下一篇

MIL-101(Fe)高效催化β-蒎烯与甲醛的Prins缩合制备诺卜醇

景润, 鲁新环(), 张海福, 陶佩佩, 潘海军, 胡傲, 周丹, 夏清华()   

  1. 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, 湖北大学化学化工学院, 武汉 430062
  • 收稿日期:2018-11-07 出版日期:2019-04-03 发布日期:2019-01-09
  • 作者简介:

    联系人简介: 鲁新环, 女, 博士, 副教授, 主要从事新材料的开发及催化研究. E-mail: xinhuan003@hubu.edu.cn;夏清华, 男, 博士, 教授, 博士生导师, 主要从事多孔材料的开发及有机催化研究. E-mail: xiaqh518@aliyun.com

  • 基金资助:
    国家自然科学基金(批准号: 21503074, 21673069)和湖北省大学生创新创业训练计划项目(批准号: 201710512045)资助.

Highly Efficient MIL-101(Fe) Catalyst for the Preparation of Nopol by the Prins Condensation of β-Pinene and Formaldehyde

JING Run, LU Xinhuan*(), ZHANG Haifu, TAO Peipei, PAN Haijun, HU Ao, ZHOU Dan, 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, College of Chemistry Chemical Engineering, Hubei University, Wuhan 430062, China
  • Received:2018-11-07 Online:2019-04-03 Published:2019-01-09
  • Contact: LU Xinhuan,XIA Qinghua E-mail:xinhuan003@hubu.edu.cn;xiaqh518@aliyun.com
  • Supported by:
    † Supported by the National Natural Science Foundation of China(Nos.21503074, 21673069) and the Hubei Province Students Innovation and Entrepreneurship Training Foundation, China(No.201710512045).

摘要:

通过水热晶化法制备了MIL-101(Fe)金属有机骨架材料, 利用X射线衍射(XRD)、 傅里叶变换红外光谱(FTIR)、 热重分析(TG)、 扫描电子显微镜(SEM)、 透射电子显微镜(TEM)和X射线光电子能谱(XPS)对催化剂的结构和形貌进行了表征. 结果表明, 该材料用于催化β-蒎烯与甲醛的Prins缩合制备诺卜醇反应的效果优异; 催化剂合成温度、 合成时间、 催化剂用量、 反应溶剂、 反应温度和反应时间对β-蒎烯的反应结果均有一定影响. 在相似的反应条件下, 合成的MIL-101(Fe)催化β-蒎烯制备诺卜醇反应的最佳条件为使用150 ℃下反应15 h合成的催化剂MIL-101(Fe), 在90 ℃下反应8 h得到的β-蒎烯转化率高达97.3%, 诺卜醇选择性达到96.7%.

关键词: 金属有机骨架材料, MIL-101(Fe), β-蒎烯, 酸催化, 诺卜醇

Abstract:

Metal organic framework materials MIL-101(Fe) were prepared by hydrothermal synthesis method. All the catalysts were characterized by X-ray diffraction(XRD), Fourier transform infrared spectra(FTIR), thermogravimetric analysis(TG), scanning electron microscopy(SEM), transmission electron microscopy(TEM) and X-ray photoelectron spectroscopy(XPS). Those materials were applied for the catalytic condensation of β-pinene and formaldehyde, and achieved excellent catalytic result. The results indicated that the catalyst synthesis temperature, synthesis time, catalyst amount, solvent, reaction temperature and time have certain effects on the reaction results of condensation reaction. Under similar reaction conditions, MIL-101(Fe)-150-15 catalyst was found to be the most active in the Prins condensation of β-pinene and formaldehyde, for which 97.3% of conversion and 96.7% selectivity are achieved within 8 h at 90 ℃.

Key words: Metal organic framework material, MIL-101(Fe), β-Pinene, Acid catalysis, Nopol

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