In Situ Formation of "Dimethyl Sulfoxide/Water-in-Salt"-Based Chitosan Hydrogel Electrolyte for Advanced All-Solid-State Supercapacitors.

Biodegradable hydrogel electrolytes are particularly attractive in the fabrication of all-solid-state supercapacitors due to environmental benignity and avoiding of leakage. The introduction of "water-in-salt" (WIS) electrolytes into hydrogels will further broaden the electrochemical stability window of aqueous supercapacitors significantly. Meanwhile, the addition of an organic co-solvent can effectively overcome the inevitable salt precipitation and extend the temperature adaptability. Herein, an in situ cross-linking approach was demonstrated without any extra binder to obtain a "dimethyl sulfoxide/water-in-salt"-based (DWIS) chitosan hydrogel electrolyte. Interestingly, the addition of 4-7 mol L-1 of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) salts not only conforms to the criterion of WIS, but also promoted the successful gelation through the supramolecular complexation between Li+ -solvated complexes and chitosan chains. A hydrogel-based all-solid-state supercapacitor was fabricated using the DWIS chitosan hydrogel as the electrolyte and separator while nitrogen-doped graphene hydrogel (NG) was used as the electrode. The optimized supercapacitor with a wide operating voltage of 2.1 V showed a high specific capacitance of 107.6 F g-1 at 1 A g-1 , remarkable capacitance retention of 80.1 % after 5000 cycles, a superior energy density of 62.9 Wh kg-1 at a power density of 1025.5 W kg-1 , and excellent temperature stability in the range of -20 to 70 °C. These findings suggest that the as-prepared hydrogel electrolyte holds great potential in the practical application of high-performance solid-state energy storage devices.