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Efficient Synthesis of Asymmetric Miktoarm Star Polymers.
Macromolecules ( IF 5.1 ) Pub Date : 2020-01-08 , DOI: 10.1021/acs.macromol.9b02380
Adam E Levi 1 , Liangbing Fu 2 , Joshua Lequieu 3 , Jacob D Horne 4 , Jacob Blankenship 1 , Sanjoy Mukherjee 3 , Tianqi Zhang 2 , Glenn H Fredrickson 3, 4, 5 , Will R Gutekunst 2 , Christopher M Bates 1, 4, 5
Affiliation  

Asymmetric miktoarm star polymers produce unique material properties, yet existing synthetic strategies are beleaguered by complicated reaction schemes restricted in both the monomer scope and yield. Here, we introduce a new synthetic approach coined “μSTAR”, miktoarm synthesis by termination after ring-opening metathesis polymerization, that circumvents these traditional synthetic limitations by constructing the block–block junction in a scalable one-pot process involving (1) grafting-through polymerization of a macromonomer followed by (2) in situ enyne-mediated termination to install a single mikto-arm with exceptional efficiency. This modular μSTAR platform cleanly generates ABn and A(BA′)n miktoarm star polymers with unprecedented versatility in the selection of A and B chemistries as demonstrated using many common polymer building blocks. The average number of B or BA′ arms (n) is easily controlled by the equivalents of Grubbs catalyst. While these materials are characterized by dispersity in n that arises from the statistics of polymerization, they self-assemble into mesophases that are identical to those predicted for precise miktoarm stars. In summary, the μSTAR technique provides a significant boost in design flexibility and synthetic simplicity while retaining the salient phase behavior of precise miktoarm star materials.

中文翻译:


不对称 Miktoarm 星形聚合物的高效合成。



不对称米克托臂星形聚合物产生独特的材料性能,但现有的合成策略受到单体范围和产量限制的复杂反应方案的困扰。在这里,我们介绍了一种新的合成方法,称为“μSTAR”,通过开环复分解聚合后终止进行 miktoarm 合成,该方法通过在可扩展的一锅法中构建块-块连接来规避这些传统的合成限制,涉及(1)接枝-通过大分子单体的聚合,然后进行 (2) 原位烯炔介导的终止,从而以卓越的效率安装单个 mikto 臂。该模块化 μSTAR 平台可干净地生成 AB n和 A(BA') n miktoarm 星形聚合物,在选择 A 和 B 化学物质方面具有前所未有的多功能性,正如使用许多常见聚合物构建块所证明的那样。 B 或 BA' 臂的平均数量 ( n ) 很容易通过 Grubbs 催化剂的当量来控制。虽然这些材料的特征是聚合统计产生的n分散性,但它们自组装成中间相,与精确的米克托臂星预测的中间相相同。总之,μSTAR技术显着提高了设计灵活性和合成简单性,同时保留了精确miktoarm星材料的显着相行为。
更新日期:2020-01-08
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