高稳定的Zr(IV) 基金属有机框架与酸用于催化不对称的双重反应
Wei Gong1, Xu Chen1, Hong Jiang1
1School of Chemistry and Chemical Engineering and State Key Laboratory of Metal Matrix Composites , Shanghai Jiao Tong University , Shanghai 200240 , China.
Journal of the American Chemical Society
|April 16, 2019
概括
在稳定的金属有机框架 (Zr-MOFs) 中使用连接体设计策略成功固定化了酸. 这些异质催化剂在各种不对称反应中表现出增强的酸性和选择性,为绿色化学提供了有前途的途径.
科学领域:
- 材料科学
- 催化剂
- 有机化学
背景情况:
- 不同质的布伦斯特酸催化剂对于化学合成至关重要,但具有高孔隙性,结晶性和稳定性而具有挑战性.
- 现有的方法往往难以有效地整合催化站点,同时保持结构完整性.
研究的目的:
- 在坚固的基金属有机框架 (Zr-MOF) 中开发一种用于固定酸催化剂的新型联体设计策略.
- 研究这些异质催化剂在不对称的双重反应中的催化性能.
主要方法:
- 使用基于enantiopure spirobiindane的配体合成有毛孔的Zr(IV) -MOFs.
- MOF结构,多孔性和稳定性的特征.
- 在不对称的乙化,Friedel-Crafts和iso-Pictet-Spengler反应中对催化活性和酶选择性的评估.
主要成果:
- 成功制备了两个具有相同拓但不同通道大小的合式Zr-MOF,具有出色的水,酸和耐受性.
- 与同类药物相比,固定酸显著提高了布伦斯特德酸度.
- 在两组分和三组分不对称的协奏反应中实现高反应性和反选择性,结果与同质系统相比或更高.
结论:
- 联体设计策略有效地将酸安装到Zr-MOF中,防止金属协调并增强稳定性.
- 由此产生的异质催化剂具有高活性,选择性,稳定性和可回收性,使其成为环保精细化学合成的前景.
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