Polyelectrolyte Complex-Covalent Interpenetrating Polymer Network Hydrogels

Polyelectrolyte Complex-Covalent Interpenetrating Polymer Network Hydrogels
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DOI:
10.1021/acs.macromol.2c00590
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发表时间:
2022-06-14
期刊:
影响因子:
5.5
通讯作者:
Srivastava, Samanvaya
Srivastava, Samanvaya
中科院分区:
化学1区
文献类型:
--
作者:
Li, Defu;Goeckler, Tobias;Srivastava, Samanvaya

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聚电解质复合物(PEC)水凝胶具有丰富的微观结构多样性和剪切响应、自修复属性以及pH和盐响应性的可调谐性。然而,由于其机械强度弱和不受控制的膨胀,它们在生物技术和生物医学中的用途受到限制。她;我们介绍了一种克服PEC水凝胶的这些缺点的策略,其通过将静电交联的PEC网络与共价交联的聚合物网络交织,从而产生双络合物-共价互穿聚合物网络(PEC-IPN)水凝胶。由带相反电荷的阿坝三嵌段共聚物和可光交联的4臂聚(环氧乙烷)(PEO)组成的模型PEC-IPN水凝胶的结构和材料表征突出了我们的方法的关键优势。在三种组分的初始混合后,PEC网络在水性环境中迅速自组装,提供结构刚性并作为共价可交联的PEO前体的保护支架。PEO链的光交联产生共价网络,为PEC网络提供结构增强。所得的PEC-IPN水凝胶具有显着改善的剪切和拉伸强度,溶胀特性,并在盐水环境中的机械稳定性,同时保持固有的介观结构的PEC网络和其盐响应性。我们设想,我们制造基于PEC的IPN水凝胶的方法将为创建利用静电自组装途径的独特属性的自组装混合材料铺平道路,在生物医学中具有广泛的应用。
Polyelectrolyte complex (PEC) hydrogels possess rich microstructural diversity and tunability of the shear response, self-healing attributes, and pH- and salt-responsiveness. Yet, their utility in biotechnology and biomedicine has been limited, owing to their weak mechanical strength and uncontrolled swelling. Her; we introduce a strategy to overcome these drawbacks of PEC hydrogels by interlacing the electrostatically crosslinked PEC network with a covalently crosslinked polymer network, creating polyelectrolyte complex-covalent interpenetrating polymer network (PEC-IPN) hydrogels. Structural and material characterizations of model PEC-IPN hydrogels composed of oppositely charged ABA triblock copolymers and photocrosslinkable 4-arm poly(ethylene oxide) (PEO) highlight the key advantages of our approach. Upon initial mixing of the three constituents, the PEC network selfassembles swiftly in aqueous environs, providing structural rigidity and serving as protective scaffoldings for the covalently crosslinkable PEO precursors. Photocrosslinking of the PEO chains creates a covalent network, providing structural reinforcement to the PEC network. The resulting PEC-IPN hydrogels possess significantly improved shear and tensile strengths, swelling characteristics, and mechanical stability in saline environments while preserving the intrinsic mesoscale structure of the PEC network and its salt-responsiveness. We envision that our approach to fabricating PEC-based IPN hydrogels will pave the way for the creation of self-assembled hybrid materials that harness the unique attributes of electrostatic self-assembly pathways, with broad applications in biomedicine.