Soft self-healing materials are promising candidates for flexible electronic devices due to their exceptional compatibility, extensibility, and self-restorability. Generally, these materials suffer from low tensile strength and susceptibility to fracture because of the restricted microstructure design. Herein, we propose a hydrothermal-freeze-thaw method to construct high-strength self-healing hydrogels with even interconnected networks and distinctive wrinkled surfaces. The integration of the wrinkled outer surface with the three-dimensional internal network confers the self-healing hydrogel with enhanced mechanical strength. This hydrogel achieves a tensile strength of 223 kPa, a breaking elongation of 442%, an adhesion strength of 57.6 kPa, and an adhesion energy of 237.2 J m^-2. Meanwhile, the hydrogel demonstrates impressive self-repair capability (repair efficiency: 93%). Moreover, the density functional theory (DFT) calculations are used to substantiate the stable existence of hydrogen bonding between the PPPBG hydrogel and water molecules which ensures the durability of the PPPBG hydrogel for long-term application. The measurements demonstrate that this multifunctional hydrogel possesses the requisite sensitivity and durability to serve as a strain sensor, which monitors a spectrum of motion signals including subtle vocalizations, pronounced facial expressions, and limb articulations. This work presents a viable strategy for healthcare monitoring, soft robotics, and interactive electronic skins.

中文翻译：

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通过水热冻融法制备具有蠕虫状表面的高强度自修复多功能水凝胶


软质自修复材料因其卓越的兼容性、可扩展性和自我恢复性而成为柔性电子设备的有前途的候选者。通常，由于微观结构设计受限，这些材料的抗拉强度低且易断裂。在此，我们提出了一种热液冻融方法来构建具有均匀互连网络和独特褶皱表面的高强度自修复水凝胶。起皱的外表面与三维内部网络的整合赋予了自修复水凝胶增强的机械强度。这种水凝胶的拉伸强度为 223 kPa，断裂伸长率为 442%，粘合强度为 57.6 kPa，粘合能为 237.2 J ^m-2。同时，水凝胶表现出令人印象深刻的自我修复能力（修复效率：93%）。此外，密度泛函理论 （DFT） 计算用于证实 PPPBG 水凝胶与水分子之间氢键的稳定存在，从而保证了 PPPBG 水凝胶长期应用的耐用性。测量表明，这种多功能水凝胶具有作为应变传感器所需的灵敏度和耐用性，该传感器可监测一系列运动信号，包括细微的发声、明显的面部表情和肢体关节。这项工作为医疗保健监测、软机器人和交互式电子皮肤提出了一种可行的策略。