Bioinspired Strategy to Reinforce Hydrogels via Cooperative Effect of Dual Physical Cross‐Linkers,Macromolecular Chemistry and Physics

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Bioinspired Strategy to Reinforce Hydrogels via Cooperative Effect of Dual Physical Cross‐Linkers
Macromolecular Chemistry and Physics ( IF 2.5 ) Pub Date : 2020-01-09 , DOI: 10.1002/macp.201900485
Xiuquan Ni ₁ , Dongran Liang ₁ , Guanbing Zhou ₁ , Chuanzhuang Zhao ₁ , Chongyi Chen _{1,

2}

Affiliation

Many biological tissues including cartilage and tendons are composed of polymeric hydrogels, which exhibit high toughness and rapid self‐recovery. However, developing hydrogels with both high toughness and rapid recovery remains a challenge. Inspired by the nacre of abalone shell, two non‐covalent cross‐linkers (Al³⁺ and diethylenetriamine [DETA]) with different relaxation times are introduced into a polyacrylic acid network. Compared with mono cross‐linked hydrogels, the dual physical cross‐linked hydrogel exhibits both high toughness (work of extension at fracture up to 8.0 MJ m⁻³) and rapid self‐recovery ability without loss of extensibility. Strong carboxylate‐DETA ionic cross‐links with longer relaxation time endow the hydrogels with high strength and help to localize the reformation of carboxylate‐Al³⁺ coordinate bonds; weak carboxylate‐Al³⁺ coordinate bonds with shorter relaxation time dissociate and reform to dissipate energy. Therefore, the hydrogels can dissipate massive energy effectively without any residual strain. More notably, the toughness and hysteresis of hydrogels can be completely recovered in 20 min. This finding unravels a new path to reinforce the hydrogels by the cooperation of different non‐covalent interactions, which can be applied in more material systems.

中文翻译：

通过双重物理交联剂的协同作用增强水凝胶的生物启发策略

包括软骨和肌腱在内的许多生物组织均由聚合物水凝胶组成，这些聚合物水凝胶具有很高的韧性和快速的自我恢复能力。然而，开发具有高韧性和快速恢复性的水凝胶仍然是一个挑战。受鲍鱼贝壳珍珠层的启发，将具有不同弛豫时间的两种非共价交联剂（Al ³⁺和二亚乙基三胺[DETA]）引入了聚丙烯酸网络。与单交联水凝胶相比，双物理交联水凝胶显示出高韧性（断裂时的延伸功高达8.0 MJ m ^-3））和快速的自我恢复能力，而不会失去可扩展性。较强的羧酸盐-DETA离子交联和更长的弛豫时间赋予水凝胶高强度，并有助于定位羧酸盐-Al ³⁺配位键的重整；较弱的羧酸盐-Al ³⁺配位键具有较短的弛豫时间，可以解离并重整以耗散能量。因此，水凝胶可以有效地耗散大量能量而没有任何残余应变。更值得注意的是，水凝胶的韧性和滞后性可以在20分钟内完全恢复。这一发现为通过不同的非共价相互作用的相互作用增强水凝胶开辟了一条新途径，该途径可以应用于更多的物质体系中。

更新日期：2020-01-09

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