The broad applications of rechargeable batteries urge people to develop alternative energy storage devices with sustainable resources, high capacity, long cycling life, and wide-temperature operability. Aqueous proton batteries are considered as a state-of-the-art energy storage system due to their intrinsic safety and low cost. However, aqueous electrolytes have a low boiling point and narrow electrochemical stability window, limiting their applications in wide-temperature and high-energy batteries. Herein, a hybrid organic ionic liquid electrolyte with organic alkali 1-methyl-1,2,4-triazole (MTA) protonated by organic acid bis(trifluoromethysulfonyl)imide (HTFSI) as proton carriers and tetramethylene sulfone (TMS) as the solvent, noted as HTFSI-MTA-TMS, exhibited the stable electrochemical windows exceeding 5V at -20°C and 3.5V at 80°C. Benefiting from this electrolyte, the assembled MnO2-S//MoO3 button proton full battery can display an operation voltage up to 1.8V, energy density of 44.8Wh kg-1, and good cycling stability at room temperature when bis(trifluoromethanesulfonyl)imide manganese (II) salt (Mn(TFSI)2) is introduced into the electrolyte, and run well in a wide-temperature range (-20°C-60°C). The work reveals the potential of organic acid-alkali coregulated electrolytes to meet the need of energy storage in a wide-temperature range and will advance the development of high-energy proton batteries.
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