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Bond Reformation, Self-Recovery, and Toughness in Hydrogen-Bonded Hydrogels
ACS Applied Polymer Materials ( IF 4.4 ) Pub Date : 2020-11-27 , DOI: 10.1021/acsapm.0c01009 Farshad Oveissi 1 , Geoffrey M. Spinks 2 , Sina Naficy 1
ACS Applied Polymer Materials ( IF 4.4 ) Pub Date : 2020-11-27 , DOI: 10.1021/acsapm.0c01009 Farshad Oveissi 1 , Geoffrey M. Spinks 2 , Sina Naficy 1
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Tough hydrogels have gained attention due to their potential applications in biomimetics and soft robotics. Among all proposed topologies, tough hydrogels comprising physical bonds (e.g., hydrogen bonds) are of particular interest because of the possibility of bond reformation and subsequent rapid recovery of the network damage responsible for energy dissipation during loading. We developed a model based on a sequential debonding and time-dependent reformation of physical bonds to explain the unexpectedly high toughness of hydrogels formed by single networks of hydrogen-bonded hydrogels. First, a series of mechanical testing experiments were performed on various polyether-based hydrophilic polyurethanes with different numbers of proton acceptor and donor sites to evaluate the correlation between toughness and mechanical recovery with physical cross-linking. Then, the parameters of the model were obtained using the experimental results from load-unload tensile cycles with different resting times between cycles to provide an estimate of the bond dissociation and bond reformation rates. Finally, the measured fractured energies were successfully and quantitatively predicted by our model. This model can be further adapted to describe and predict the toughness of other physically cross-linked polymer networks, linking their structural parameters (i.e., level of physical cross-linking, chain length, and rate of bond reformation) with their mechanical properties and load recovery.
中文翻译：
氢键水凝胶的键重整，自恢复和韧性
坚韧的水凝胶由于其在仿生和软机器人中的潜在应用而受到关注。在所有提议的拓扑结构中，由于包含物理键（例如氢键）的坚硬水凝胶特别重要，因为它们可能会发生键重整以及随后快速恢复造成负载过程中能量耗散的网络损坏。我们开发了基于物理键的顺序脱键和时间依赖的重整的模型，以解释由氢键合水凝胶的单个网络形成的水凝胶出乎意料的高韧性。第一，在具有不同数量的质子受体和施主位点的各种聚醚基亲水性聚氨酯上进行了一系列机械测试实验，以评估韧性与机械交联与物理交联之间的相关性。然后，使用实验结果从加载/卸载拉伸循环中获得模型的参数，循环之间具有不同的静置时间，以提供对键解离和键重整速率的估计。最终，我们的模型成功地定量预测了断裂能。该模型可以进一步适用于描述和预测其他物理交联的聚合物网络的韧性，并将其结构参数（例如，物理交联的水平，链长，
更新日期：2020-12-11
中文翻译：
氢键水凝胶的键重整，自恢复和韧性
坚韧的水凝胶由于其在仿生和软机器人中的潜在应用而受到关注。在所有提议的拓扑结构中，由于包含物理键（例如氢键）的坚硬水凝胶特别重要，因为它们可能会发生键重整以及随后快速恢复造成负载过程中能量耗散的网络损坏。我们开发了基于物理键的顺序脱键和时间依赖的重整的模型，以解释由氢键合水凝胶的单个网络形成的水凝胶出乎意料的高韧性。第一，在具有不同数量的质子受体和施主位点的各种聚醚基亲水性聚氨酯上进行了一系列机械测试实验，以评估韧性与机械交联与物理交联之间的相关性。然后，使用实验结果从加载/卸载拉伸循环中获得模型的参数，循环之间具有不同的静置时间，以提供对键解离和键重整速率的估计。最终，我们的模型成功地定量预测了断裂能。该模型可以进一步适用于描述和预测其他物理交联的聚合物网络的韧性，并将其结构参数（例如，物理交联的水平，链长，
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