通过有机催化循环的三级类立体中心的酶选择性构造
Qiang Wang1, Marvin Lübcke1, Maria Biosca1
1Department of Organic Chemistry, Stockholm University, SE-106 91 Stockholm, Sweden.
Journal of the American Chemical Society
|November 16, 2020
概括
化 (III) 催化剂使新的氧化循环反应成为可能. 这种方法通过控制的三级碳-立体中心产生四和罗利丁,从而达到高反选择性.
科学领域:
- 有机化学
- 催化剂
- 化化学
背景情况:
- 氧化环化是合成化异环的关键转化.
- 控制立体化学,特别是在三级碳中心,仍然是合成化学的一个重大挑战.
研究的目的:
- 开发一种新的氧化循环化方法.
- 在四二和二支架中形成三级碳立体中心的高反控制.
主要方法:
- 在氧化循环过程中使用*in situ*生成的催化剂.
- 采用甲基乳酸衍生的 (III) 催化剂来诱导立体选择性.
- 进行密度函数理论 (DFT) 计算以阐明反应机制和立体选择性.
主要成果:
- 成功合成含有三级碳-立体中心的化四和.
- 使用新开发的酸催化剂,达到高达96%的酸过量 (ee).
- DFT计算提供了对反应途径和影响立体化学结果的因素的见解.
结论:
- 开发的氧化循环化提供了一个有效的途径,以化异环.
- 性 (III) 催化剂系统显示了控制三级碳立体中心的显著潜力.
- 来自DFT计算的机制理解有助于合理设计未来的催化系统.
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