Multiarm Star‐Crosslinked Hydrogel: Polymer Network with Thermoresponsive Free‐End Chains Densely Connected to Crosslinking Points,Macromolecular Rapid Communications

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Multiarm Star‐Crosslinked Hydrogel: Polymer Network with Thermoresponsive Free‐End Chains Densely Connected to Crosslinking Points
Macromolecular Rapid Communications ( IF 4.2 ) Pub Date : 2020-11-26 , DOI: 10.1002/marc.202000558
Shohei Ida ₁ , Shogo Toda ₁ , Masatoshi Oyama ₂ , Hiroki Takeshita ₁ , Shokyoku Kanaoka ₁

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Soft tissue in biological system is a hydrogel with elaborate structure exhibiting repeatable dynamic function. In order to approach such sophisticated system, precise construction of a designed network with multi‐components is desired. This communication presents a novel hydrogel having highly dense stimuli‐responsive free‐end chains around crosslinking structure. A key molecule is a core‐crosslinked star‐shaped polymer with multiple thermoresponsive arms, which can be prepared by reversible addition–fragmentation chain transfer polymerization of divinyl crosslinker with poly(N‐isopropylacrylamide) (PNIPAAm) macro‐chain transfer agent and have a number of unreacted carbon–carbon double bonds in the core. These unreacted double bonds can be utilized as a crosslinker for poly(acrylamide) (PAAm) gel synthesis by free radical polymerization. The obtained gel contains homogeneously dispersed star PNIPAAms as crosslinking points and exhibits thermoresponsive swelling behavior in water depending on the star contents. In particular, the gel with low content of the star crosslinker shows localized responsive behavior with expansion and shrinkage of the star in one molecule. The mechanical properties of the star‐crosslinked gel are significantly high compared to the conventional PAAm gels particularly in compressive strength (≈9 MPa). Moreover, the star‐crosslinked gel has thermoresponsive mechanical toughening property.

中文翻译：

多臂星状交联水凝胶：具有热响应性自由端链的聚合物网络紧密连接至交联点

生物系统中的软组织是具有精细结构的水凝胶，具有可重复的动态功能。为了处理这种复杂的系统，需要精确构建具有多组件的设计网络。这种交流提出了一种新型的水凝胶，在交联结构周围具有高度致密的刺激响应自由端链。关键分子是具有多个热响应臂的核交联星形聚合物，可以通过二乙烯基交联剂与聚（N异丙基丙烯酰胺（PNIPAAm）大链转移剂，其核心中有许多未反应的碳-碳双键。这些未反应的双键可以用作通过自由基聚合的聚（丙烯酰胺）（PAAm）凝胶合成的交联剂。所获得的凝胶包含均匀分散的星形PNIPAAms作为交联点，并根据星形含量在水中表现出热响应性溶胀行为。特别是，星形交联剂含量低的凝胶在一个分子中具有星形扩展和收缩的局部响应行为。与传统的PAAm凝胶相比，星形交联凝胶的机械性能非常高，特别是在抗压强度（≈9MPa）方面。此外，星形交联凝胶具有热响应性机械增韧性能。

更新日期：2020-11-26

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