Solvent-Free Synthesis of Self-Healable and Recyclable Crosslinked Polyurethane Based on Dynamic Oxime-Urethane Bonds

Polyurethane is widely used for its versatility in design and range of performance. Self-healing and recyclable dynamic polyurethane networks have attracted extensive attention due to their potential to extend service life and ensure safety in use, as well as to promote sustainable use of resources. Developing green and environment-friendly methods to obtain this material is an interesting and challenging task, as the majority of current dynamic polyurethane networks utilize the solution polymerization method. The use of solvents makes the processes complicated, harmful to environment, and increase the cost. Poly(oxime-urethanes) (POUs) are emerging dynamic polyurethanes and show great potential in diverse fields, such as biomaterials, hot melt adhesives, and flexible electronics. In this study, we utilized the solubility properties of dimethylglyoxime in raw material poly(ethylene glycol) to prepare POUs through bulk polymerization for the first time. This method is simple, convenient and cost-efficient. Simultaneously, copper ion coordination improves POUs strength and dynamic properties, with mechanical strength up from 0.54 MPa to 1.03 MPa and self-healing recovery rate up from 85.5% to 91.8%, and activation energy down from 119.6 kJ/mol to 95.4 kJ/mol. To demonstrate the application of this technology, self-healing and stretchable circuits are constructed from this dynamic polyurethane network.