Designing Antifreezing Hydrogels with Enhanced Mechanical Properties Using a Simple Crosslinker
Designing Antifreezing Hydrogels with Enhanced Mechanical Properties Using a Simple Crosslinker
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DOI：
10.1016/j.giant.2023.100203
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发表时间：
2023-10
期刊：
影响因子：
7
通讯作者：
Dong Zhang;Yonglan Liu;William Gross;Yijing Tang;Jie Zheng
中科院分区：
文献类型：
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作者：
Dong Zhang;Yonglan Liu;William Gross;Yijing Tang;Jie Zheng
防冻水凝胶对于材料设计和实际应用是必不可少的，但由于其高含水率，其开发和理解一直是具有挑战性的。目前的防冻水凝胶通常依赖于有机溶剂或防冻剂的添加。在这项研究中，我们提出了一种新的交联策略来制备防冻水凝胶，而不需要额外的防冻剂。我们介绍了一种新的交联剂，PEGn-Egina，它将高度亲水的Egina与不同分子量的聚乙二醇组分结合在一起。以聚乙二醇乙二醇酯(PEGn-Egina)为交联剂，合成了琼脂/聚丙烯酰胺(琼脂/PAAM)双网络水凝胶，并与传统的MBAA交联型水凝胶进行了比较。得到的PEGn-Egina交联型水凝胶具有固有的防冻性能，即使在零下温度下也能长时间保持其机械完整性。分子动力学(MD)模拟进一步表明，PEGn-Egina交联水凝胶的抗冻性能可以归因于其高度亲水和紧密交联的双网络结构。这些结构使水和水凝胶网络之间能够牢固地结合，从而有效地防止水凝胶内冰晶的形成。值得注意的是，与MBAA交联型水凝胶相比，PEGn-Egina交联型水凝胶不仅表现出优异的机械性能，而且即使在冷冻条件下也能保持其机械性能，使其适用于广泛的应用。这项研究提出了一种简单而有效的设计概念，以突出新型交联剂在提高防冻和机械性能方面的作用，展示了它们在各种需要防冻能力和坚固机械性能的应用中的潜力。
Antifreezing hydrogels are essential for materials design and practical applications, but their development and understanding have been challenging due to their high-water content. Current antifreezing hydrogels typically rely on organic solvents or the addition of antifreezing agents. In this study, we present a novel crosslinking strategy to fabricate antifreezing hydrogels without the need for additional antifreezing agents. We introduce a new crosslinker, PEGn-EGINA, which combines highly hydrophilic EGINA with polyethylene glycol (PEG) of varying molecular weights. Utilizing PEGn-EGINA as the crosslinker, we synthesize Agar/Polyacrylamide (Agar/PAAm) double-network hydrogels, alongside conventional MBAA-crosslinked hydrogels for comparison. The resulting PEGn-EGINA-crosslinked hydrogels exhibit inherent antifreezing properties and retain their mechanical integrity even at subzero temperatures for extended periods. Molecular dynamics (MD) simulations further reveal that the antifreezing behavior observed in the PEGn-EGINA-crosslinked hydrogels can be attributed to their highly hydrophilic and tightly crosslinked double-network structures. These structures enable strong bindings between water and the hydrogel network, thus effectively preventing the formation of ice crystals within the hydrogels. Notably, PEGn-EGINA-crosslinked hydrogels not only demonstrate superior mechanical performance compared to MBAA-crosslinked hydrogels, but also maintain their mechanical properties even in frozen conditions, making them suitable for a wide range of applications. This study presents a simple yet effective design concept for highlighting the role of novel crosslinker in enhancing antifreezing and mechanical properties, showcasing their potential for various applications that require both antifreezing capabilities and robust mechanical performance.