Stereochemical editing logic powered by the epimerization of unactivated tertiary stereocenters.
Stereochemical editing logic powered by the epimerization of unactivated tertiary stereocenters.
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DOI：
10.1126/science.add6852
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发表时间：
2022-10-28
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--
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复杂靶标的立体选择性合成需要精确协调化学转化，同时建立所需键的连接性和空间方向。在这项工作中，我们描述了手性分子及其异构体合成的补充范例，该范例在后期调整分子的三维结构。该策略成功的关键是开发一种由十钨酸聚阴离子和二硫化物助催化剂组成的温和且高度通用的光催化方法，该方法能够使先前构型固定的未活化的三级立体中心相互转化。我们通过快速构建手性支架（使用现有工具很难访问）以及复杂目标的后期立体编辑来展示这种方法的多功能性以及立体编辑逻辑的实现。
The stereoselective synthesis of complex targets requires the precise orchestration of chemical transformations that simultaneously establish the connectivity and spatial orientation of desired bonds. In this work, we describe a complementary paradigm for the synthesis of chiral molecules and their isomers, which tunes the three-dimensional structure of a molecule at a late stage. Key to the success of this strategy is the development of a mild and highly general photocatalytic method composed of decatungstate polyanion and disulfide cocatalysts, which enable the interconversion of unactivated tertiary stereogenic centers that were previously configurationally fixed. We showcase the versatility of this method—and the implementation of stereoediting logic—by the rapid construction of chiral scaffolds that would be challenging to access using existing tools and by the late-stage stereoediting of complex targets.
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影响因子：
8.4
作者：
Kuang Y;Cao H;Tang H;Chew J;Chen W;Shi X;Wu J
通讯作者：
Wu J
影响因子：
3.6
作者：
BREITHOLLE, EG;FALLIS, AG
通讯作者：
FALLIS, AG
影响因子：
1.8
作者：
Dang, HS;Roberts, BP
通讯作者：
Roberts, BP
影响因子：
4.9
作者：
Bhattarai, Khadga M.;del Amo, Vicente;Davis, Anthony P.
通讯作者：
Davis, Anthony P.
影响因子：
3.2
作者：
Mancino, Valentina;Ceccarelli, Giada;Gioiello, Antimo
通讯作者：
Gioiello, Antimo