Design of Slidable Polymer Networks: A Rational Strategy to Stretchable, Rapid Self-Healing Hydrogel Electrolytes for Flexible Supercapacitors

Hydrogel electrolytes are of particular interest in the fabrication of flexible supercapacitors that are able to withstand deformation and physical damage. Nevertheless, there still exists a huge space in the design of hydrogel electrolytes with comprehensive performances including high processability, conductivity, mechanical strength, and self-healability. Herein, a slidable polymer network is constructed through the cross-linking reaction among commercially available polyethyleneimine (PEI), polyvinyl alcohol (PVA), and 4-formylphenylboronic acid (Bn) to generate PEI–PVA–Bn hydrogels, which have high adaptability to various electrolytes such as LiCl, NaCl, KCl, and ionic liquids. The as formed hydrogel electrolytes not only show excellent mechanical property (elongation at break up to 1223%, strength of 34.6 kPa) and self-healability (highest strain self-healing efficiency reaches 94.3% within 2 min) but also exhibit high conductivity (up to 21.49 mS cm–1). Flexible supercapacitors constructed by sandwiching the PEI–PVA–Bn-LiCl hydrogel electrolyte between two multiwalled carbon nanotube electrodes demonstrate a broadened operating potential window of 1.4 V, specific capacitance of 16.7 mF cm–2, high cycling stability up to 10 000 charge/discharge cycles, and excellent mechanical stability.