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催化不对称化和转移化为1,3-二极的二极

Liren Xu¹, Tilong Yang¹, Hao Sun¹

¹Department of Chemistry, the Grubbs Institute, and Medi-X Pingshan, Southern University of Science and Technology, Shenzhen, China.

Angewandte Chemie (International ed. in English)

|February 17, 2024

概括

这项研究引入了一种新型的 (III) 催化剂,用于不对称的化的子,产生具有高效率和选择性的性氧胺. 这一突破解决了合成化学中长期存在的挑战.

科学领域:

有机化学有机化学
催化剂是一种催化剂.
不对称的合成方法

背景情况:

由于它们的1,3-双极结构,子以氧胺的不对称化是一种具有挑战性的转化.
现有的方法面临着对抗控制的困难,并且容易发生N-O键裂变.

研究的目的:

为子开发一种高效的催化不对称化方法.
为了达到高产量和在合成性氧胺的enantioselectivity.

主要方法:

使用 TsDPEN 衍生型环二烯 (Cyclopentadienyl rhodium) 催化剂进行非对称化和转移化.
采用机理学研究和密度函数理论 (DFT) 计算来了解反应途径和酶选择性.
通过格拉姆尺度反应和随后的转换证明了实际可行性.

主要成果:

取得了成功的非对称化和转移化.
生产的性氧胺含量高达99%的产量和99%以上的反体过量 (ee).
确定了一种新型的7个成员循环过渡状态,该状态负责观察到的enantioselectivity.

结论:

开发的 (III) 催化系统有效地克服了中化中的挑战.
该方法提供了一种实用且高度酶选择性的途径,以获得有价值的性氧胺.
机理学研究提供了关于enantioselectivity的起源的见解,为未来的催化剂设计铺平了道路.

关键词:

1,3-二极二极子是什么意思有7个成员的周期性过渡状态.不对称的 (转移) 化.这是一种结相互作用.

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