A universal strategy towards high–energy aqueous multivalent–ion batteries

Publication Type:
Journal Article
Nature Communications, 2021, 12, (1), pp. 2857
Issue Date:
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Rechargeable multivalent metal (e.g., Ca, Mg or, Al) batteries are ideal candidates for large-scale electrochemical energy storage due to their intrinsic low cost. However, their practical application is hampered by the low electrochemical reversibility, dendrite growth at the metal anodes, sluggish multivalent-ion kinetics in metal oxide cathodes and, poor electrode compatibility with non-aqueous organic-based electrolytes. To circumvent these issues, here we report various aqueous multivalent-ion batteries comprising of concentrated aqueous gel electrolytes, sulfur-containing anodes and, high-voltage metal oxide cathodes as alternative systems to the non-aqueous multivalent metal batteries. This rationally designed aqueous battery chemistry enables satisfactory specific energy, favorable reversibility and improved safety. As a demonstration model, we report a room-temperature calcium-ion/sulfur| |metal oxide full cell with a specific energy of 110 Wh kg-1 and remarkable cycling stability. Molecular dynamics modeling and experimental investigations reveal that the side reactions could be significantly restrained through the suppressed water activity and formation of a protective inorganic solid electrolyte interphase. The unique redox chemistry of the multivalent-ion system is also demonstrated for aqueous magnesium-ion/sulfur||metal oxide and aluminum-ion/sulfur||metal oxide full cells.
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