Inverse hydride shuttle catalysis enables the stereoselective one-step synthesis of complex frameworks
作者:Immo Klose、Giovanni Di Mauro、Dainis Kaldre、Nuno Maulide
DOI:10.1038/s41557-022-00991-4
日期:2022.11
into valuable azabicyclic scaffolds based on the concept of inverse hydride shuttle catalysis. The ternary complexes are readily constructed in situ from three simple precursors and enable a highly modular installation of various substitution patterns. Upon subjection to a unique dual-catalytic system, the transient intermediates undergo an unusual hydride shuttle process that is initiated by a hydride
从简单的前体一步一步快速组装复杂的支架被认为是效率和可持续性方面的理想反应。事实上,尽管该学科取得了巨大进步,但复杂生物碱框架的直接单步合成仍然是有机化学核心的一个未解决问题。在此,我们提出了一种广泛的策略,其中基于逆氢化物穿梭催化的概念,将动态组装的三元配合物转化为有价值的氮杂双环支架。三元复合物很容易从三个简单的前体原位构建,并能够高度模块化地安装各种替代模式。经受独特的双催化系统,瞬时中间体经历了一个不寻常的氢化物穿梭过程,该过程由氢化物捐赠事件引发。此外,我们表明,结合不对称有机催化,产物生物碱框架获得了优异的光学纯度。