Self‐Healing Waterborne Polyurethanes as a Sustainable Gel Electrolyte for Flexible Electrochromic Devices

Self‐healing polymers are promising for diverse applications in wearable technology and electronic skin. Polyurethanes are versatile polymers that can incorporate various monomer structures. Waterborne polyurethanes (WPUs) emerge as an environmentally conscious choice due to water usage instead of organic solvents, thereby minimizing the generation of volatile organic compounds. This study introduces a novel approach to enhance the self‐healing properties of WPUs by integrating disulfide bonds. These dynamic disulfide bonds undergo exchange reactions upon heating, facilitating the renewal of cross‐links on damaged film surfaces. Self‐healing WPUs with a low glass transition temperature achieve excellent self‐healing efficiency under mild conditions. Self‐healing adhesives applied to various flexible substrates retain stable peel strength, which confirms their potential as self‐healing solutions. Furthermore, the WPU hydrogel electrolyte is prepared with dihydroxyhexyl viologen (DHHV), and the prepared electrochromic gel exhibits good ionic conductivity while maintaining high transparency. The flexible electrochromic device exhibited excellent performances, including low coloration voltage, high coloration efficiency, and long‐term stability. The transmittance difference is exceptional, with over 99%, and no decay after repeated bending cycles is observed. The current results demonstrate the feasibility of self‐healing WPUs in improving the operation and durability of high‐performance flexible electrochromic devices.