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Single-chain chiral Ru-Cu star polymers for highly efficient catalytic aqueous asymmetric transfer hydrogenation
Journal of Catalysis ( IF 6.5 ) Pub Date : 2022-05-06 , DOI: 10.1016/j.jcat.2022.04.025
Xinjuan Li 1 , Jiaxin Dong 1 , Guanglei Ma 1 , NaNa Ma 1 , Xianbin Jia 1
Affiliation  

It is of great research value to design simulated enzyme catalysts with high catalytic activity, high selectivity and that are reusable in water. In this work, a star-shaped thermal responsive polymer-Ru/diamine functional intelligent chiral catalyst was synthesized by controlled atom transfer radical polymerization (ATRP). Polymerization can be controlled through self-catalysis of chiral monomers and polymers. Because of the complex that forms between the chiral polymer and Cu2+, the synthesized star polymer experiences a chiral amplification effect. At the same time, the star Ru-Cu catalyst can be assembled into single-chain polymers in water, which showed better catalytic activity and selectivity than the Ru catalyst for aqueous asymmetric reactions, and can be recycled up to six times. Our work provides a new method for controllable synthesis of chiral polymers without additional ligands and the need to remove Cu2+ at the end of the reaction, making the method green and more cost-effective. In summary, bimetallic nanocatalysts were controllably constructed by star chiral polymers through the ATRP pathway. This method significantly aids the development of helical chiral polymers and the preparation of high-efficiency enzyme catalysts.



中文翻译:

用于高效催化水性不对称转移氢化的单链手性 Ru-Cu 星形聚合物

设计具有高催化活性、高选择性、可在水中重复使用的模拟酶催化剂具有重要的研究价值。本工作通过可控原子转移自由基聚合(ATRP)合成了星形热响应聚合物-Ru/二胺功能智能手性催化剂。聚合可以通过手性单体和聚合物的自催化来控制。由于手性聚合物和Cu 2+之间形成的络合物,合成的星形聚合物经历手性放大效应。同时,星型Ru-Cu催化剂可以在水中组装成单链聚合物,在水性不对称反应中表现出比Ru催化剂更好的催化活性和选择性,最多可循环使用6次。我们的工作为手性聚合物的可控合成提供了一种新方法,无需额外的配体,也无需在反应结束时去除 Cu 2+ ,使该方法绿色环保且更具成本效益。总之,双金属纳米催化剂是由星形手性聚合物通过 ATRP 途径可控构建的。该方法显着有助于螺旋手性聚合物的开发和高效酶催化剂的制备。

更新日期:2022-05-06
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