Xiao Yao, Zhao Zhi-Yuan, Irran Elisabeth, Oestreich Martin
Institut für Chemie, Technische Universität Berlin, Strasse des 17. Juni 115, 10623, Berlin, Germany.
Angew Chem Int Ed Engl. 2024 Dec 9;63(50):e202414005. doi: 10.1002/anie.202414005. Epub 2024 Oct 31.
A desymmetrizing 1,2-addition of silicon nucleophiles to biaryl derivatives containing an 2,6-dicarbaldehyde-1-yl unit is reported. The reaction is catalyzed by copper with a triazolium-ion-derived N-heterocyclic carbene as the chiral ligand and makes use of an Si-B reagent as the silicon pronucleophile. The practical methodology furnishes axially chiral aromatic carbaldehydes decorated with a centrally chiral α-hydroxysilane moiety in moderate to good yields and with high enantio- as well as excellent diastereoselectivities. The silicon nucleophile always attacks at the diastereotopic face of either carbonyl group away from the ortho substituent on the phenyl ring at C1 of the 2,6-dicarbaldehyde-1-yl fragment. The resulting axially and centrally chiral products can be further converted into valuable biaryl compounds with hardly any erosion of the enantiomeric excess.
据报道,含2,6 - 二甲醛 - 1 - 基单元的联芳基衍生物与硅亲核试剂发生不对称1,2 - 加成反应。该反应由铜催化,以三唑鎓离子衍生的N - 杂环卡宾作为手性配体,并使用Si - B试剂作为硅前体亲核试剂。该实用方法以中等至良好的产率、高对映选择性以及优异的非对映选择性提供了带有中心手性α - 羟基硅烷部分的轴向手性芳族甲醛。硅亲核试剂总是在2,6 - 二甲醛 - 1 - 基片段C1位苯环上邻位取代基远离的任一羰基的非对映异位面上进行进攻。所得的轴向和中心手性产物可进一步转化为有价值的联芳基化合物,且对映体过量几乎没有损失。