Li Zhikang, Wang Bin, Lu Jijian, Xue Yumeng, Wang Jiaxiang, Jia Boqing, Han Gengyu, Zhao Yihe, Qureshi Muhammad Afzal Khan, Yu Lan, Zhao Kang, Li Min, Yang Ping, Lu Dejiang, Zhao Libo
State Key Laboratory for Manufacturing System Engineering, International Joint Laboratory for Micro/Nano Manufacturing and Measurement Technologies, State Industry-Education Integration Center for Medical Innovations, Xi'an Jiaotong University (Yantai) Research Institute for Intelligent Sensing Technology and System, Xi'an Jiaotong University, Xi'an, 710049, China.
Shandong Laboratory of Yantai Advanced Materials and Green Manufacturing, Yantai, 264000, China.
Adv Sci (Weinh). 2025 Aug;12(30):e02678. doi: 10.1002/advs.202502678. Epub 2025 May 29.
Constructing hydrogels with both remarkable mechanical and self-healing properties is highly desirable for soft electronics, yet remains challenging due to conflicting demands on chemical bonds and polymer chain mobility. Herein, a highly stretchable, self-healing, and conductive gelatin methacryloyl (GelMA) hydrogel is developed by incorporating polyvinyl alcohol, N-(2-amino-2-oxoethyl)-2-propenamide, sodium tetraborate, and sodium chloride into GelMA, followed by a two-step polymerization process. The introduced novel interpenetrating networks, hierarchical hydrogen bonds (weak and strong H-bonds), and borate ester bonds (BEBs) synergistically improve the mechanical strength, and concurrently function as sacrificial bonds for energy dissipation under deformation. Moreover, the constructed reversible BEBs and weak H-bonds enable autonomous self-healing at room temperature. The resulting hydrogel achieves remarkable stretchability (≈160%), tensile strength (≈130 kPa), and self-healing efficiency (86%), surpassing previously reported GelMA hydrogels. Importantly, a self-healing GelMA hydrogel strain sensor is demonstrated, featuring a high gauge factor (≈3.28), ultra-low detection limit (0.1%), and excellent recovery of sensitivity (≈100%) and detection range (≈75%) after damage. Successful monitoring of subtle and large-scale human motions with both original and healed sensors highlights the device's durability and longevity. This study provides a promising approach for the rational design and practical application of GelMA hydrogels in wearable bioelectronics.
构建具有卓越机械性能和自愈性能的水凝胶对于软电子学来说是非常理想的，但由于对化学键和聚合物链流动性的要求相互冲突，这仍然具有挑战性。在此，通过将聚乙烯醇、N-(2-氨基-2-氧代乙基)-2-丙烯酰胺、硼酸钠和氯化钠加入到甲基丙烯酰化明胶（GelMA）中，然后进行两步聚合过程，开发出了一种高度可拉伸、自愈且导电的GelMA水凝胶。引入的新型互穿网络、分级氢键（弱氢键和强氢键）和硼酸酯键（BEB）协同提高了机械强度，并在变形时同时作为能量耗散的牺牲键发挥作用。此外，构建的可逆BEB和弱氢键能够在室温下实现自主自愈。所得水凝胶具有显著的拉伸性（约160%）、拉伸强度（约130 kPa）和自愈效率（86%），超过了先前报道的GelMA水凝胶。重要的是，展示了一种自愈的GelMA水凝胶应变传感器，其具有高应变系数（约3.28）、超低检测限（0.1%）以及在受损后灵敏度（约100%）和检测范围（约75%）的出色恢复能力。用原始传感器和愈合后的传感器成功监测细微和大规模人体运动突出了该器件的耐用性和寿命。这项研究为GelMA水凝胶在可穿戴生物电子学中的合理设计和实际应用提供了一种有前景的方法。
