Ultrahigh Mechanical Strength and Robust Room-Temperature Self-Healing Properties of a Polyurethane–Graphene Oxide Network Resulting from Multiple Dynamic Bonds

Addressing the conflict between achieving high mechanical properties and room-temperature self-healing ability is extremely significant to achieving a breakthrough in the application of self-healing materials. Therefore, inspired by natural spider silk and nacre, a room-temperature self-healing supramolecular material with ultrahigh strength and toughness is developed by synergistically incorporating flexible disulfide bonds and dynamic sextuple hydrogen bonds (H-bonds) into polyurethanes (PUs). Simultaneously, abundant H-bonds are introduced at the interface between graphene oxide nanosheets with dynamic multiple H-bonds and the PU matrix to afford strong interfacial interactions. The resulting urea-containing PU material with an inverse artificial nacre structure has a record mechanical strength (78.3 MPa) and toughness (505.7 MJ m^-3), superior tensile properties (1273.2% elongation at break), and rapid room-temperature self-healing abilities (88.6% at 25 °C for 24 h), forming the strongest room-temperature self-healing elastomer reported to date and thus upending the previous understanding of traditional self-healing materials. In addition, this bionic PU-graphene oxide network endows the fabricated flexible intelligent robot with functional repair and shape memory capabilities, thus providing prospects for the fabrication of flexible functional devices.