Strong, tough and mechanically self-recoverable poly(vinyl alcohol)/alginate dual-physical double-network hydrogels with large cross-link density contrast.
Strong, tough and mechanically self-recoverable poly(vinyl alcohol)/alginate dual-physical double-network hydrogels with large cross-link density contrast.
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强韧、机械可自恢复的聚（乙烯醇）/海藻酸盐双物理双网络水凝胶，具有大的交联密度对比
DOI：
10.1039/c8ra01302k
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发表时间：
2018-05-03
期刊：
影响因子：
3.9
通讯作者：
Wu, Chonggang
中科院分区：
文献类型：
--
作者：
Li, Xuefeng;Shu, Mengmeng;Li, Han;Gao, Xiang;Long, Shijun;Hu, Tao;Wu, Chonggang
通过简单的冻融（25-25-25 °C）循环，然后将聚乙烯醇（PVA）/海藻酸钠（SA）混合水溶液浸入浓（1.0 mol L−1）Ca 2+水溶液中，成功制备了强韧的PVA/海藻酸钠氢键离子双物理双网络（DN）水凝胶。发现，在PVA与SA重复单元的摩尔比为20/1至80/1时，DN凝胶可能演化出刚性藻酸盐网络分散在其中的半互穿聚合物网络（IPN）形态，同时与韧性PVA网络互锁以实现DN协同作用，这赋予它们高强度和韧性，其中藻酸盐的高刚性可能源自其致密的交联引起的脱水收缩和沿沿着交联缺陷空隙的分散，从而导致很小的内应力集中。从力学上看，随着20/1-80/1DN凝胶的稳定拉伸，它们的力学响应逐渐分化为不同的协同状态：稀疏氢键的PVA作为韧性基质，在其大的拉伸时承受小部分的既定应力;而密集离子（即Ca 2+）交联的藻酸盐起刚性骨架的作用，以在其较小的局部应变上维持剩余的较大应力。有希望的是，半IPN形态的这种韧性-刚性基质-骨架协同机制可以普遍地扩展到具有大的A-B刚性（或交联密度）对比度的所有A/B DN水凝胶，无论网络A或B的交联性质是共价的、离子的、氢键的还是货车范德华相互作用的。的强大和坚韧的DN凝胶也表现出令人满意的自恢复的粘弹性行为，因为它们的杨氏模量和耗散的能量在单轴拉伸模式和动态存储和损耗模量在振荡剪切模式都恢复显着从非线性粘弹性制度，尽管不同程度的失败恢复到（准）线性粘弹性。中间体组合物能够实现分散诱导的刚性、离子藻酸盐网络与全局延展性、氢键键合的聚（乙烯醇）网络互锁的协同的、坚韧的双物理双网络水凝胶。
Strong and tough poly(vinyl alcohol) (PVA)/alginate hydrogen-bonded-ionic dual-physical double-network (DN) hydrogels have been successfully prepared by a facile route of a freeze–thaw (25–25–25 °C) cycle followed by concentrated (1.0 mol L−1 of) aqueous-Ca2+ immersion of PVA/Na alginate (SA) mixed aqueous solutions. It was found that, at mole ratios of the PVA- to SA repeat units of 20/1 to 80/1, the DN gels likely evolved a semi-interpenetrating polymer network (IPN) morphology of rigid alginate networks dispersed in while interlocking with ductile PVA network to accomplish DN synergy that gave their high strength and toughness, where the high alginate rigidity originated probably from its dense cross-link induced syneresis and dispersion along crosslink-defective voids to result in little internal stress concentration. Tentatively mechanistically, as the 20/1–80/1 DN gels were stretched steadily, their mechanical response was gradually differentiated into distinct synergistic states: the sparsely hydrogen-bonded PVA served as a ductile matrix to bear small fractions of the established stresses at its large elongations; whereas the densely ionically (i.e. Ca2+) cross-linked alginate functioned as a rigid skeleton to sustain the remaining larger stresses upon its smaller local strains. Promisingly, this ductile-rigid matrix-skeleton synergistic mechanism of semi-IPN morphology may be universally extended to all A/B DN hydrogels of large A–B rigidity (or cross-link density) contrast, whether the cross-link nature of network(s) A or B is covalent, ionic, hydrogen bonded or van der Waals interacted. The strong and tough DN gels also displayed satisfactory self-recovery of viscoelastic behaviour, in that their Young's modulus and dissipated energy in the uniaxial tensile mode and dynamic storage and loss moduli in the oscillatory shear mode all recovered significantly from non-linear viscoelastic regimes despite different degrees of failure to revert to (quasi)linear viscoelasticity. Intermediate compositions enable synergised, strong-and-tough dual-physical double-network hydrogels of dispersion-induced rigid, ionic alginate-networks interlocking with global ductile, hydrogen-bonded poly(vinyl alcohol)-network.
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