Xu Lei, Zhou Li, Li Yan-Xiang, Gao Run-Tan, Chen Zheng, Liu Na, Wu Zong-Quan
State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, 130012, Changchun, China.
Key Laboratory of Green and Precise Synthetic Chemistry and Applications, Ministry of Education, Huaibei Normal University, 235000, Huaibei, Anhui, China.
Nat Commun. 2023 Nov 10;14(1):7287. doi: 10.1038/s41467-023-43092-7.
Developing eco-friendly chiral organocatalysts with the combined advantages of homogeneous catalysis and heterogeneous processes is greatly desired. In this work, a family of amphiphilic one-handed helical polyisocyanides bearing phosphine pendants is prepared, which self-assembles into well-defined chiral micelles in water and showed thermo-responsiveness with a cloud point of approximately 38.4 °C. The micelles with abundant phosphine moieties at the interior efficiently catalyze asymmetric cross Rauhut-Currier reaction in water. Various water-insoluble substrates are transferred to target products in high yield with excellent enantioselectivity. The yield and enantiomeric excess (ee) of the product generated in water are up to 90% and 96%, respectively. Meanwhile, the yields of the same R-C reaction catalyzed by the polymer itself in organic solvents is <16%, with an ee < 72%. The homogeneous reaction of the chiral micelles in water turns to heterogeneous at temperatures higher than the cloud point, and the catalyst precipitation facilitates product isolation and catalyst recovery. The polymer catalyst is recycled 10 times while maintaining activity and enantioselectivity.
开发具有均相催化和多相过程综合优势的环保型手性有机催化剂是非常必要的。在这项工作中,制备了一系列带有膦侧基的两亲性单手螺旋聚异腈,它们在水中自组装成明确的手性胶束,并表现出约38.4 °C的浊点的热响应性。内部含有大量膦部分的胶束在水中有效地催化不对称交叉Rauhut-Currier反应。各种水不溶性底物以高收率和优异的对映选择性转化为目标产物。在水中生成的产物的收率和对映体过量(ee)分别高达90%和96%。同时,聚合物本身在有机溶剂中催化的相同R-C反应的收率<16%,ee<72%。手性胶束在水中的均相反应在高于浊点的温度下转变为多相反应,催化剂沉淀有利于产物分离和催化剂回收。聚合物催化剂可循环使用10次,同时保持活性和对映选择性。