Strengthening‐Durable Trade‐Off and Self‐Healing, Recyclable Shape Memory Polyurethanes Enabled by Dynamic Boron–Urethane Bonds

Addressing the demand for integrating strength and durability reinforcement in shape memory polyurethane (SMPU) for diverse applications remains a significant challenge. Here a series of SMPUs with ultra‐high strength, self‐healing and recyclability, and excellent shape memory properties through introducing dynamic boron–urethane bonds are synthesized. The introducing of boric acid (BA) to polyurethane leading to the formation of dynamic covalent bonds (DCB) boron–urethane, that confer a robust cross‐linking structure on the SMPUs led to the formation of ordered stable hydrogen‐bonding network within the SMPUs. The flexible crosslinking with DCB represents a novel strategy for balancing the trade‐off between strength and durability, with their strengths reaching up to 82.2 MPa while also addressing the issue of durability in prolonged usage through the provision of self‐healing and recyclability. The self‐healing and recyclability of SMPU are demonstrated through rapid dynamic exchange reaction of boron–urethane bonds, systematically investigated by dynamic mechanical analysis (DMA). This study sheds light on the essential role of such PU with self‐healing and recyclability, contributing to the extension of the PU's service life. The findings of this work provide a general strategy for overcoming traditional trade‐offs in preparing SMPUs with both high strength and good durability. The incorporation of dynamic boron–urethane bonds effectively enhances the strength and toughness of polyurethanes, while imparting self‐healing, recyclable, and shape reconfigurable properties to shape‐memory polyurethane materials. Self‐healing and recycled samples maintain almost all of their original mechanical properties, which provide a new strategy to ensure that SMPUs balance high strength and durability.