强烈的易斯酸性金属有机框架用于连续流催化
Pengfei Ji1, Xuanyu Feng1, Pau Oliveres1
1Department of Chemistry , The University of Chicago , 929 East 57th Street , Chicago , Illinois 60637 , United States.
Journal of the American Chemical Society
|September 5, 2019
概括
为催化合成了高度酸性的金属有机框架 (MOF). 与传统催化剂相比,一种新的ZrOTf-BTC MOF显示出更高的易斯酸度和催化活性,使得有效的连续流反应成为可能.
科学领域:
- 材料科学:新型多孔材料的合成和特征.
- 催化:用于有机转换的异质易斯酸催化剂的开发.
背景情况:
- 高酸性金属有机框架 (MOF) 对催化应用具有重大研究兴趣.
- 现有的MOF通常需要严苛的条件或缺乏足够的易斯酸度以实现广泛的应用.
研究的目的:
- 设计和合成一个强烈的易斯酸性MOF,ZrOTf-BTC,具有增强的催化性能.
- 开发一种复合材料 (ZrOTf-BTC@SiO2),用于高效的连续流催化.
- 量化测量易斯酸度并将催化性能与均基准进行比较.
主要方法:
- 使用盐酸和三甲基三酸 (Me3SiOTf) 的MOF-808 (Zr-BTC) 的两步转化.
- 使用电子磁共振 (EPR) 和光光谱学的定量易斯酸度测量.
- 准备ZrOTf-BTC@SiO2复合物用于连续流反应器研究.
主要成果:
- 成功合成了具有强易斯酸度的ZrOTf-BTC (ΔE = 0.99 eV),与Sc(OTf) 3相比.
- 在各种有机反应中ZrOTf-BTC表现出高的催化活性和稳定性 (Diels-Alder,环氧化开放,Friedel-Crafts化,基化).
- 在连续流催化中,ZrOTf-BTC@SiO2复合物表现出异常的周转率 (TON).
结论:
- 化是一种有效的策略,可以在MOF中创建强烈的易斯酸性位点.
- ZrOTf-BTC及其SiO2复合物是高度活性和稳定的固体易斯酸催化剂.
- 研发的MOF@SiO2复合物可为重要的有机转化提供高效的连续流催化.
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