Current aqueous battery electrolytes, including conventional hydrogel electrolytes, exhibit unsatisfactory water retention capabilities. The sustained water loss will lead to subsequent polarization and increased internal resistance, ultimately resulting in battery failure. Herein, a double network (DN) organohydrogel electrolyte based on dimethyl sulfoxide (DMSO)/H2O binary solvent was proposed. Through directionally reconstructing hydrogen bonds and reducing active H2O molecules, the water retention ability and cathode/anode interfaces were synergistic enhanced. As a result, the synthesized DN organohydrogel demonstrates exceptional water retention capabilities, retaining approximately 75% of its original weight even after the exposure to air for 20 days. The Zn||MnO2 battery delivers an outstanding specific capacity of 275 mA h g−1 at 1 C, impressive rate performance with 85 mA h g−1 at 30 C, and excellent cyclic stability (95% retention after 6000 cycles at 5 C). Zn||Zn symmetric battery can cycle more than 5000 h at 1 mA cm−2 and 1 mA h cm−2 without short circuiting. This study will encourage the further development of functional organohydrogel electrolytes for advanced energy storage devices.
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