High-Strength, Tough, and Self-Healing Nanocomposite Physical Hydrogels Based on the Synergistic Effects of Dynamic Hydrogen Bond and Dual Coordination Bonds,ACS Applied Materials & Interfaces

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High-Strength, Tough, and Self-Healing Nanocomposite Physical Hydrogels Based on the Synergistic Effects of Dynamic Hydrogen Bond and Dual Coordination Bonds
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2017-08-16 00:00:00 , DOI: 10.1021/acsami.7b09614
Changyou Shao ₁ , Huanliang Chang ₁ , Meng Wang ₁ , Feng Xu ₁ , Jun Yang ₁

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Dynamic noncovalent interactions with reversible nature are critical for the integral synthesis of self-healing biological materials. In this work, we developed a simple one-pot strategy to prepare a fully physically cross-linked nanocomposite hydrogel through the formation of the hydrogen bonds and dual metal-carboxylate coordination bonds within supramolecular networks, in which iron ions (Fe³⁺) and TEMPO oxidized cellulose nanofibrils (CNFs) acted as cross-linkers and led to the improved mechanical strength, toughness, time-dependent self-recovery capability and self-healing property. The spectroscopic analysis and rheological measurements corroborated the existence of hydrogen bonds and dual coordination bonds. The mechanical tests and microscopic morphology were explored to elucidate the recovery properties and toughening mechanisms. The hydrogen bonds tend to preferentially break prior to the coordination bonds associated complexes that act as skeleton to maintain primary structure integrity, and the survived coordination bonds with dynamic feature also serve as sacrificial bonds to dissipate another amount of energy after the rupture of hydrogen bonds, which collectively maximize the contribution of sacrificial bonds to energy dissipation while affording elasticity. Additionally, the multiple noncovalent interactions in diverse types synergistically serve as dynamic but highly stable associations, leading to the effective self-healing efficiency over 90% after damage. We expect that this facile strategy of incorporating the biocompatible and biodegradable CNFs as building blocks may enrich the avenue in exploration of dynamic and tunable cellulosic hydrogels to expand their potential applications in the biomedical field.

中文翻译：

基于动态氢键和双配位键协同效应的高强度，高韧性，自修复纳米复合物理水凝胶

具有可逆性质的动态非共价相互作用对于自我修复生物材料的整体合成至关重要。在这项工作中，我们开发了一种简单的一锅策略，通过在超分子网络中形成铁离子（Fe ³⁺）和TEMPO氧化纤维素纳米原纤维（CNF）充当交联剂，并提高了机械强度，韧性，随时间变化的自我恢复能力和自我修复性能。光谱分析和流变学测量证实了氢键和双配位键的存在。探索了机械测试和微观形态，以阐明其恢复性能和增韧机理。氢键往往优先于配位键相关的配合物先断裂，这些配合物起骨架作用，以维持一级结构的完整性，而存活下来的具有动态特征的配位键也可以作为牺牲键，在氢键断裂后消散另一量的能量，它在赋予弹性的同时，使牺牲键对能量耗散的贡献最大化。另外，多种类型的多种非共价相互作用协同地充当动态但高度稳定的缔合，导致损伤后超过90％的有效自我修复效率。我们预计，这种将生物相容性和可生物降解的CNF用作构建单元的简便策略可能会丰富探索动态和可调纤维素水凝胶的途径，以扩大其在生物医学领域的潜在应用。

更新日期：2017-08-16

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