具有多刺激响应行为和自修复能力的纤维素纳米晶增强聚乙烯醇水凝胶

赵姣; 孙少妮; 姜春胜; 孙丽丽; 曹学飞

doi:10.12171/j.1000-1522.20250104

具有多刺激响应行为和自修复能力的纤维素纳米晶增强聚乙烯醇水凝胶

Cellulose nanocrystal reinforced polyvinyl alcohol hydrogels with multi-stimulus responsive behavior and self-healing properties

摘要

摘要:
目的水凝胶在生物传感器、伤口敷料、组织工程、药物控释和超级电容器等领域具有广泛应用前景。然而，传统聚乙烯醇（PVA）水凝胶功能较为单一且缺乏自修复能力，这在一定程度上限制了其应用范围。因此，赋予PVA水凝胶多刺激响应性和自修复能力，对于拓展其应用领域至关重要。
方法通过在PVA中引入纤维素纳米晶（CNC）和硼酸酯键，并结合冻融处理，制备一种具有优异力学性能和多刺激响应行为的自修复PVA/CNC/四硼酸钠水凝胶（PCBs）。
结果（1）CNC和四硼酸钠的加入可显著提高PCBs的力学性能。当PVA/CNC/四硼酸钠的质量比为10∶1.5∶1（PCB_0.1）时，PCB_0.1的抗拉强度是纯PVA水凝胶的4.4倍，且该凝胶具有良好的自修复能力，PCB_0.1的自修复效率达90%以上。（2）PCB_0.1具有多刺激响应行为。在温度、pH等外部环境刺激下，PCB_0.1表现出良好的可逆凝胶−溶胶转化特性。（3）当PCB_0.1的拉伸率从60%提高到220%时，PCB_0.1的光学性质发生显著变化，偏光下该凝胶的干涉色从蓝色逐渐变为绿色、黄色、红色和紫色。（4）PCB_0.1具有良好的离子响应性，对\textSO_4^2 - 、Ca²⁺ 表现出敏感性。
结论通过简单共混PVA、纤维素纳米晶（CNC）和四硼酸钠，并结合冻融处理，成功制备了一种具有多刺激响应行为和自修复能力的PVA/CNC/四硼酸钠水凝胶。该水凝胶具有制备工艺简便、成本低廉、力学强度高和响应性能优异等优点，在多功能传感器和防伪材料领域展现出广阔的应用前景。

Abstract:
Objective Hydrogels have a wide range of applications in areas such as biosensors, wound dressings, tissue engineering, controlled drug release and supercapacitors. Traditional polyvinyl alcohol (PVA) hydrogels have relatively single functions and lack self-healing ability, which limits their applications to a certain extent. Therefore, it is essential to endow PVA hydrogels with multi-stimulus responsiveness and self-healing ability to broaden their potential applications.
Method In this study, self-healing PVA/CNC/sodium tetraborate hydrogels (PCBs) with excellent mechanical properties and multi-stimulus responsive behaviors were prepared by introducing cellulose nanocrystal (CNC) and borate bonds into PVA and combining them with freeze-thaw treatment.
Result (1) The addition of CNC and sodium tetraborate significantly enhanced the mechanical properties of PCBs. When the mass ratio of PVA/CNC/ sodium tetraborate was 10∶1.5∶1 (PCB_0.1), the tensile strength of PCB_0.1 was 4.4 times higher than PVA hydrogel. Moreover, the hydrogel PCB_0.1 exhibited excellent self-healing properties, which showed a self-healing efficiency higher than 90%. (2) The PCB_0.1 exhibited multi-stimulus response behavior. PCB_0.1 showed excellent reversible gel-sol transition behaviors under external environmental stimuli such as temperature and pH. (3) When the tensile strain of PCB_0.1 increased from 60% to 220%, significant changes in its optical properties were observed. Under polarized light, the interference color of hydrogel gradually shifted from blue to green, yellow, red, and purple. (4) PCB_0.1 exhibited ionic responsiveness and showed sensitivity to \textSO_4^2 - and Ca²⁺.
Conclusion The PVA/CNC/sodium tetraborate composite hydrogels with multi-stimulus responsive behavior and self-healing ability can be prepared successfully by simply mixing PVA, CNC, and sodium tetraborate and then subjecting them to freeze-thaw treatment. These hydrogels are easy to prepare and have the advantages of low cost, high strength, and good responsiveness, which show certain application potential in the fields of multi-functional sensors and anti-counterfeiting.

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