Healable, Recyclable, and Ultra-Tough Waterborne Polyurethane Elastomer Achieved through High-Density Hydrogen Bonding Cross-Linking Strategy

With the increasing popularity of elastomers in industry and daily life, their high performance and functionality have attracted widespread attention. However, it is a great challenge for them to possess both high mechanical properties and excellent healing and recovery capabilities due to the limitations of the preparation methods and the intrinsic microstructure of the elastomers. In this study, a strategy of ice-controlled interfacial stepwise cross-linking was proposed to prepare the waterborne polyurethane-based elastomers with ultrahigh-density hydrogen bonding interaction achieved by enhancing the utilization rate of phenol hydroxyl groups of tannic acid to the maximum extent. The elastomers have incredible mechanical properties, including ultrahigh toughness of 1.03 GJ m^–3 (which represents the highest level among polyurethane elastomers prepared through common processing techniques to date), extremely high true fracture stress of ∼1.9 GPa, world-record fracture energy of 520 kJ m^–2, and exciting multiple functional characteristics, such as highly efficient self-healing ability of 10 min, high resistance to physical damage and chemical corrosion, broad temperature and frequency damping effects, good shape memory effect, and excellent melt-processing recyclability and solvent recyclability. These robust multifunctional elastomers represent considerable potential in various fields, from defense and military industry and civil transportation to precision manufacturing, etc.