A Self-Healing Elastomer with Extremely High Toughness Achieved by Acylsemicarbazide Hydrogen Bonding and Cu²⁺-Neocuproine Coordination Interactions

Elastomers with high mechanical toughness can guarantee their durability during service life. Self-healing ability, as well as recyclability, can also extend the life of materials and save the consuming cost of the materials. Many efforts have been dedicated to promoting the mechanical toughness as well as the self-healing capability of elastomers at the same time, while it remains a challenge to balance the trade-off between the above properties in one system. Herein we proposed a molecular design driven by dual interactions of acylsemicarbazide hydrogen bonding and Cu²⁺-neocuproine coordination simultaneously. By introducing the reversible multiple hydrogen bonds and strong coordination bonds, we successfully fabricated an extremely tough and self-healing elastomer. The elastomer can achieve an impressive top-notch toughness of 491 MJ/m³. Furthermore, it boasted rapid elastic restorability within 10 min and outstanding crack tolerance with high fracture energy (152.6 kJ/m²). Benefiting from the combination of dynamic interactions, the material was able to self-repair under 80 °C conveniently and could be reprocessed to restore the exceptional mechanical properties.