在离子结合催化剂和氨基催化剂之间使用Rotaxane双功能催化剂
Katarzyna Eichstaedt1, Javier Jaramillo-Garcia1, David A Leigh1
1School of Chemistry, University of Manchester , Oxford Road, Manchester M13 9PL, U.K.
Journal of the American Chemical Society
|June 20, 2017
概括
这项研究揭示了一种可切换的轮催化剂,可以在氨基催化和离子结合催化之间切换. 一个反应的"关闭"状态是另一个反应的"开启"状态,由宏观循环位置控制.
科学领域:
- 超分子化学
- 催化剂
- 有机化学
背景情况:
- 可切换的催化剂为复杂的化学转化提供可调节的反应性.
- 基于罗塔的分子机器为受控的催化活动提供平台.
研究的目的:
- 演示具有可切换氨基催化和离子结合能力的双功能罗塔催化剂.
- 根据宏观循环位置阐明催化状态之间的切换机制.
主要方法:
- 一种可切换的 [2]rotaxane的合成和特征.
- 研究氨基催化和离子结合反应中的催化活性.
- 使用刺激诱导的宏循环运动来控制催化功能.
主要成果:
- 在氨基催化和离子结合催化中,罗塔表现出相互排斥的"开启"和"关闭"状态.
- 阴离子结合催化涉及三团的合作CH-结合以稳定中间体.
- 催化部位的顺序激活使得协同反应过程成为可能.
结论:
- 可切换的罗塔克桑可以设计为具有直角功能的复杂分子催化剂.
- 对宏循环定位的控制是调节催化活性并使序列催化成为可能的关键.
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