Achieving severe damage restoration and the ideal combination of good mechanical properties and healing efficiency are two significant challenges for self-healing materials. In this study, a series of shape-memory, self-healing aqueous polyurethane (SMPU) were synthesized based on the molecular self-assembly design of 5-(2-hydroxyethyl)-6-methyl-2-aminuracil (HMA), 4-aminopyridine (4-APD) and polycaprolactone diol (PCL) moieties. The effects of HMA and 4-APD on mechanical properties, self-healing properties, and shape memory properties of SMPU were investigated. The dynamic crosslinking network generated by quadruple hydrogen bonds and multiple coordination bonds not only consumed strain energy but also promoted rapid re-formation after fracture, resulting in superior self-healing ability (healing efficiency 96.3%), excellent mechanical properties (tensile strength 39.1 MPa and elongation at break 908%) and recyclable capabilities of SMPU. Meanwhile, the SMPU showed a noteworthy shape memory effect; its shape fixation rate and recovery rate could reach 99% and 98%, respectively. The temperature and time dependence of the self-healing process were studied by molecular dynamics (MD), and the self-healing mechanism was clarified further. When SMPU was used for leather finishing, the finished and self-healing samples exhibited excellent wear resistance (wear rating: 4 ∼ 5). These advantageous properties endow SMPU with great potential applied value in leather and other regions.

实现严重损伤的修复以及良好机械性能和愈合效率的理想结合是自修复材料面临的两个重大挑战。本研究基于5-(2-羟乙基)-6-甲基-2-氨基尿嘧啶(HMA)、4-氨基吡啶(4-APD)和聚己内酯二醇(PCL)部分的分子自组装设计合成了一系列形状记忆、自修复水性聚氨酯(SMPU)。研究了HMA和4-APD对SMPU机械性能、自修复性能和形状记忆性能的影响。四重氢键和多重配位键生成的动态交联网络不仅消耗应变能，而且促进断裂后快速重新形成，从而产生优越的自修复能力（修复效率96.3%），SMPU 具有优异的机械性能（拉伸强度 39.1 MPa，断裂伸长率 908%）和可回收能力。同时，SMPU表现出值得注意的形状记忆效应；其形状固定率和恢复率分别可达99%和98%。通过分子动力学（MD）研究了自修复过程的温度和时间依赖性，进一步阐明了自修复机制。当SMPU用于皮革涂饰时，整理后的自修复样品表现出优异的耐磨性（磨损等级：4∼5）。这些优越的性能使得SMPU在皮革等领域具有巨大的潜在应用价值。SMPU表现出值得注意的形状记忆效应；其形状固定率和恢复率分别可达99%和98%。通过分子动力学（MD）研究了自修复过程的温度和时间依赖性，进一步阐明了自修复机制。当SMPU用于皮革涂饰时，整理后的自修复样品表现出优异的耐磨性（磨损等级：4∼5）。这些优越的性能使得SMPU在皮革等领域具有巨大的潜在应用价值。SMPU表现出值得注意的形状记忆效应；其形状固定率和恢复率分别可达99%和98%。通过分子动力学（MD）研究了自修复过程的温度和时间依赖性，进一步阐明了自修复机制。当SMPU用于皮革涂饰时，整理后的自修复样品表现出优异的耐磨性（磨损等级：4∼5）。这些优越的性能使得SMPU在皮革等领域具有巨大的潜在应用价值。成品和自修复样品表现出优异的耐磨性（磨损等级：4∼5）。这些优越的性能使得SMPU在皮革等领域具有巨大的潜在应用价值。成品和自修复样品表现出优异的耐磨性（磨损等级：4∼5）。这些优越的性能使得SMPU在皮革等领域具有巨大的潜在应用价值。