It
is desired to develop self-healing gel electrolytes for flexible
electrochromic devices (ECDs) due to the demand of healing damages
caused during operations. We here report a hydrogel electrolyte with
remarkable self-healing capability, excellent stretchability, and
ionic conductivity. The hydrogel electrolyte was synthesized via one-step
copolymerization of glycerol monomethacrylate (GMA) and acrylamide
(AAm) in the presence of borate. Within the hydrogel electrolyte,
dynamic cross-linking is expected to be formed due to the borate-didiol
complexation and hydrogen-bonding interactions. As a result, the hydrogel
electrolyte demonstrates an excellent self-healing efficiency of up
to 97%, a fracture strain of 1155%, a fracture toughness of 136.6
kJ m–3, and a fracture stress of 13.0 kPa. Additionally,
a flexible ECD based on the hydrogel electrolyte and an electrochromic
layer of poly(3,4-(2,2-dimethyl-propylenedioxy)thiophene) (PProDOT-Me2) was assembled and evaluated. The device is found to be stable
in both mechanical and optical properties over 1000 operation cycles.
This study may provide a promising way for self-healing electrolyte
gels to be utilized in a variety of flexible electrochemical devices,
including ECDs, supercapacitors, and batteries.