Thermoresponsive Hydrogels Based on Telechelic Polyelectrolytes: From Dynamic to "Frozen" Networks
Thermoresponsive Hydrogels Based on Telechelic Polyelectrolytes: From Dynamic to "Frozen" Networks
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DOI：
10.1021/acs.macromol.8b00193
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发表时间：
2018-03-27
期刊：
影响因子：
5.5
通讯作者：
Chassenieux, Christophe
中科院分区：
文献类型：
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作者：
Tsitsilianis, Constantinos;Serras, George;Chassenieux, Christophe
设计并探索了一种新型的温敏性(B-co-C)-b-A-b(B-co-C)拓扑结构，以聚(2-二甲氨基)甲基丙烯酸乙酯(PDMAEMA)弱聚电解质为中心嵌段，末端封端为热敏性聚甲基丙烯酸三乙二醇甲醚/甲基丙烯酸丁酯[P(Tegma-co-nBuMA)]无规共聚物。本设计的主要目标是通过温度控制胶粘剂的动态，从而创造出一种在低温下表现为弱凝胶，在生理温度下表现为强凝胶的可注射水凝胶。事实上，在低温下，体系表现为粘弹性复杂流体(动态网络)，而在较高温度下，形成弹性水凝胶(冻结网络)。粘度在加热时呈指数增加，从5到45摄氏度大约增加5个数量级，这归因于自组装贴纸寿命的指数增加。凝胶剂的热响应和剪切响应特性的集成使凝胶具有可注射性。此外，在37摄氏度停止施加应力后，凝胶可以迅速恢复，模拟类似于通过28号注射器针头注射的条件。所有这些水凝胶特性使其成为通过注射策略在细胞移植中潜在应用的良好候选者。
A novel thermoresponsive gelator of (B-co-C)-b-A-b (B-co-C) topology, comprising a poly(2-(dimethylamino)ethyl methacrylate) (PDMAEMA) weak polyelectrolyte as central block, end-capped by thermosensitive poly(triethylene glycol methyl ether methacrylate/n-butyl methacrylate) [P(TEGMA-co-nBuMA)] random copolymers, was designed and explored in aqueous media. The main target of this design was to control the dynamics of the stickers by temperature as to create an injectable hydrogel that behaves as a weak gel at low temperature and as a strong gel at physiological temperature. Indeed, at low temperatures, the system behaves like a viscoelastic complex fluid (dynamic network), while at higher temperatures, an elastic hydrogel is formed ("frozen" network). The viscosity increases exponentially upon heating, about 5 orders of magnitude from 5 to 45 degrees C, which is attributed to the exponential increase of the lifetime of the self-assembled stickers. The integration of thermo- and shear responsive properties in the gelator endows the gel with injectability. Moreover, the gel can be rapidly recovered upon cessation of the applied stress at 37 degrees C, simulating conditions similar to those of injection through a 28-gauge syringe needle. All these hydrogel properties render it a good candidate for potential applications in cell transplantation through injection strategies.