金属有机框架稳定了低坐标的复合物用于催化甲
Xuanyu Feng1, Yang Song1, Zhe Li1,2
1Department of Chemistry , The University of Chicago , 929 East 57th Street , Chicago , Illinois 60637 , United States.
Journal of the American Chemical Society
|July 3, 2019
概括
金属有机框架 (MOF) 稳定复合物以有效的甲化,将甲转化为有价值的化学物质. 这种新型的催化剂设计显著提高了涉及惰性基质的挑战反应的活性.
科学领域:
- 催化剂
- 材料科学
- 有机化学
背景情况:
- 甲通过催化化转化为精细化学物质是有前途的,但需要提高催化剂活性.
- 现有的 (Ir) 复合物与素和二素配体的效率有限.
研究的目的:
- 使用金属有机框架 (MOF) 开发高活性甲化催化剂.
- 稳定低坐标的复合物以提高催化性能.
主要方法:
- 合成和应用基于单的MOF (Zr-P1-Ir).
- 在110°C的甲化反应研究.
- 密度函数理论 (DFT) 的计算以阐明反应机制.
主要成果:
- Zr-P1-Ir MOF催化剂的转化率为127,产生了CH3Bpin.
- 由于稳定了四坐标的Ir复合体,DFT计算显示了甲氧化添加的激活屏障降低.
- 与其他IR催化剂不同,MOF策略避免了硬质阻碍的七坐标中间体.
结论:
- MOF有效地稳定低坐标的催化剂,使高度活跃的甲化成为可能.
- 这种方法提供了一个独特的策略来克服惰性基质的激活障碍.
- 基于MOF的催化剂设计显示出具有挑战性的催化转换的巨大潜力.
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