Huang Xiaowei, Zhang Mengya, Ming Jinfa, Ning Xin, Bai Shumeng
Industrial Research Institute of Nonwovens and Technical Textiles, College of Textiles and Clothing, Qingdao University, Qingdao 266071, People's Republic of China.
College of Biological Science and Engineering, Fuzhou University, Fuzhou 350108, People's Republic of China.
ACS Appl Bio Mater. 2020 Oct 19;3(10):7103-7112. doi: 10.1021/acsabm.0c00933. Epub 2020 Sep 28.
Natural polymer-based hydrogels attract great attention because of their inherent biocompatibility and controllable biodegradability. However, the broad applications of these hydrogels require a combination of high mechanical strength, high toughness, fatigue resistance, as well as self-healing. The integration of this combination into one natural polymer-based hydrogel remains challenging. Here, a molecular design strategy was proposed to fabricate mechanically robust silk fibroin-based hydrogels using host-guest interactions. Silk fibroin molecules was chemically modified with cholesterol (Chol, guest) or β-cyclodextrin (β-CD, host), and host-guest interaction between Chol and β-CD moieties drove the supramolecular assemblies of hydrogels. The dissociation/reassociation behavior of host-guest complexation, serving as sacrificial bonds, endowed hydrogels with effective energy dissipation and rapid self-healing ability. The prepared silk fibroin-based hydrogels exhibited high mechanical strength, high toughness, and remarkable fatigue resistance, superior to conventional silk fibroin hydrogels. Moreover, due to reversible host-guest interactions, hydrogels achieved facile functional recovery after damage without any external stimuli. This design strategy provides an avenue to develop natural polymer-based materials with robust mechanical properties, thus broadening current hydrogel applications.
基于天然聚合物的水凝胶因其固有的生物相容性和可控的生物降解性而备受关注。然而，这些水凝胶的广泛应用需要具备高机械强度、高韧性、抗疲劳性以及自我修复能力。将这些特性整合到一种基于天然聚合物的水凝胶中仍然具有挑战性。在此，提出了一种分子设计策略，利用主客体相互作用制备机械性能强大的丝素蛋白基水凝胶。丝素蛋白分子用胆固醇（Chol，客体）或β-环糊精（β-CD，主体）进行化学修饰，Chol与β-CD部分之间的主客体相互作用驱动了水凝胶的超分子组装。作为牺牲键的主客体络合的解离/重新缔合行为赋予了水凝胶有效的能量耗散和快速的自我修复能力。所制备的丝素蛋白基水凝胶表现出高机械强度、高韧性和显著的抗疲劳性，优于传统的丝素蛋白水凝胶。此外，由于主客体相互作用的可逆性，水凝胶在受损后无需任何外部刺激即可轻松实现功能恢复。这种设计策略为开发具有强大机械性能的天然聚合物基材料提供了一条途径，从而拓宽了当前水凝胶的应用范围。
