Artificial elastomers with self-healing functions are favored for their ability to repair damaged defects. However, balancing their mechanical strength, stretchability, and fast room temperature self-healing ability can be a significant challenge. Herein, this study presents a robust and highly stretchable self-healing elastomer with a spider-silk-like and inverse artificial nacre structure based on a nucleobase non-covalent assembly. Specifically, thymine-containing side chain hydrogen (H)-bonds and high-density sextuple H-bond arrays are introduced within polyurethanes to improve the kinematic activity of molecular chains and regulate the mechanical properties. Adenine-modified graphene oxide nanosheets are embedded into these elastomers to provide abundant interfacial non-covalent H-bonds. The multi-type H-bond synergy effectively resolved the abovementioned contradicting characteristics, creating an elastomer with the best reported mechanical properties (excellent strength of 46.60 MPa and stretchability of 1736.89%) within 2 h of room temperature self-healing (self-healing efficiency = 85.62%). Interestingly, the bionic polyurethane/graphene demonstrated anti-corrosion and crawling functions for rapid self-healing even in low-temperature and aqueous environments, providing a new strategy for the construction of tough self-healing flexible composites.

中文翻译：

---

由多类型氢键实现的超坚固、高拉伸性和环境温度快速自修复聚氨酯/石墨烯弹性体


具有自愈功能的人造弹性体因其修复受损缺陷的能力而受到青睐。然而，平衡它们的机械强度、拉伸性和快速室温自愈能力可能是一个重大挑战。在此，本研究提出了一种坚固且高度可拉伸的自修复弹性体，具有基于核碱基非共价组装的蜘蛛丝状和反向人工珍珠层结构。具体来说，在聚氨酯中引入含胸腺嘧啶的侧链氢（H）键和高密度六重氢键阵列，以改善分子链的运动活性并调节机械性能。将腺嘌呤改性的氧化石墨烯纳米片嵌入这些弹性体中，以提供丰富的界面非共价氢键。多型氢键协同作用有效解决了上述矛盾特性，创造了一种具有最佳力学性能的弹性体（优异的强度为46.60 MPa，拉伸率为1736.89%），在室温下2小时内自修复（自修复效率= 85.62%）。有趣的是，仿生聚氨酯/石墨烯即使在低温和水性环境下也表现出防腐蚀和爬行功能，可以快速自修复，为构建坚韧的自修复柔性复合材料提供了新策略。