An Organic Acid-Alkali Coregulated Ionic Liquid Electrolyte Enabling Wide-Temperature-Range Proton Battery

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 5 V at −20 °C and 3.5 V at 80 °C. Benefiting from this electrolyte, the assembled MnO₂-S//MoO₃ button proton full battery can display an operation voltage up to 1.8 V, energy density of 44.8 Wh 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.