Expanding Cyclic Topology-Based Biomedical Polymer Panel: Universal Synthesis of Hetero-“8”-Shaped Copolymers and Topological Modulation of Polymer Degradation,Macromolecular Rapid Communications

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Expanding Cyclic Topology-Based Biomedical Polymer Panel: Universal Synthesis of Hetero-“8”-Shaped Copolymers and Topological Modulation of Polymer Degradation
Macromolecular Rapid Communications ( IF 4.2 ) Pub Date : 2021-07-09 , DOI: 10.1002/marc.202100298
Gui-Ying Kang ₁ , Wei Ma ₁ , Ming-Zhu Liu ₂ , Hai-Xi Luo ₂ , Cui-Yun Yu ₁ , Hua Wei ₁

Affiliation

8-Shaped copolymers with two macrocycles connected together represent an interesting cyclic topology-derived polymer species due to the simultaneous incorporation of two cyclic moieties and the reported unique physical and chemical properties. To provide a proof-of-concept for a broad readership on biomedical polymers, a well-defined hetero-8-shaped amphiphilic copolymer, cyclic-poly(oligo(ethylene glycol)monomethyl ether methacrylate)-b-cyclic PCL (cPOEGMA-b-cPCL) is synthesized by an elegant integration of intrachain click cyclization and interchain click coupling. The potential of the self-assembled micelles of cPOEGMA-b-cPCL for controlled drug release is evaluated by in vitro drug loading and drug release, cellular uptake, cytotoxicity, and degradation studies. Most importantly, the micelles based on cPOEGMA-b-cPCL show much slower degradation profiles than the previously reported linear counterpart, POEGMA-b-PCL and tadpole-shaped analog, PEG-b-cPCL because of the presence of cyclic hydrophilic POEGMA segment. Therefore, this study not only develops a robust strategy for a universal precise synthesis of well-defined hetero-8-shaped copolymers based on diverse vinyl and ring-structured monomers, but also reveals the first modulation of polymer degradation property by topological control of the nondegradable moiety in the polymer construct through advanced macromolecular engineering.

中文翻译：

扩展基于环状拓扑的生物医学聚合物面板：异“8”形共聚物的通用合成和聚合物降解的拓扑调制

由于两个环状部分的同时结合和报道的独特的物理和化学性质，具有两个连接在一起的大环的 8 形共聚物代表了一种有趣的环状拓扑衍生聚合物种类。为了为生物医学聚合物的广大读者提供概念验证，这是一种明确定义的杂 8 形两亲共聚物，环状聚（低聚（乙二醇）单甲基醚甲基丙烯酸酯）- b -环状PCL ( c POEGMA- b - c PCL) 是通过链内点击环化和链间点击耦合的优雅整合合成的。c POEGMA- b - c自组装胶束的潜力用于控制药物释放的 PCL 通过体外药物装载和药物释放、细胞摄取、细胞毒性和降解研究进行评估。最重要的是，基于c POEGMA- b - c PCL的胶束显示出比先前报道的线性对应物 POEGMA- b - PCL 和蝌蚪形类似物 PEG- b - c慢得多的降解曲线PCL 因为存在环状亲水性 POEGMA 链段。因此，本研究不仅为基于多种乙烯基和环状结构单体的定义明确的异 8 形共聚物的通用精确合成开发了一种稳健的策略，而且还揭示了通过拓扑控制聚合物降解性能的首次调节。通过先进的大分子工程，聚合物结构中的不可降解部分。

更新日期：2021-09-07

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