Mechanically Robust and Electrically Conductive Hybrid Hydrogel Electrolyte Enabled by Simultaneous Dual In Situ Sol-Gel Technique and Free Radical Copolymerization

Mechanically robust and ionically conductive hydrogels poly(acrylamide-co-2-acrylamido-2-methylpropanesulfonate-lithium)/TiO2/SiO2 (P(AM-co-AMPSLi)/TiO2/SiO2) with inorganic hybrid crosslinking are fabricated through dual in situ sol-gel reaction of vinyltriethoxysilane (VTES) and tetrabutyl titanate (TBOT), and in situ radical copolymerization of acrylamide (AM), 2-acrylamide-2-methylpropanesulfonate-lithium (AMPSLi), and vinyl-SiO2. Due to the introduction of the sulfonic acid groups and Li+ by the reaction of AMPS with Li2CO3, the conductivity of the ionic hydrogel can reach 0.19 S m(-1). Vinyl-SiO2 and nano-TiO2 are used in this hybrid hydrogel as both multifunctional hybrid crosslinkers and fillers. The hybrid hydrogels demonstrate high tensile strength (0.11-0.33 MPa) and elongation at break (98-1867%), ultrahigh compression strength (0.28-1.36 MPa), certain fatigue resistance, self-healing, and self-adhesive properties, which are due to covalent bonds between TiO2 and SiO2, as well as P(AM-co-AMPSLi) chains and SiO2, and noncovalent bonds between TiO2 and P(AM-co-AMPSLi) chains, as well as the organic frameworks. Furthermore, the specific capacitance, energy density, and power density of the supercapacitors based on ionic hybrid hydrogel electrolytes are 2.88 F g(-1), 0.09 Wh kg(-1), and 3.07 kW kg(-1) at a current density of 0.05 A g(-1), respectively. Consequently, the ionic hybrid hydrogels show great promise as flexible energy storage devices.