A cost-effective water-in-salt electrolyte enables highly stable operation of a 2.15-V aqueous lithium-ion battery

Extensive efforts are currently underway to develop safe and cost-effective electrolytes for large-scale energy storage. In this regard, water-based electrolytes may be an attractive option, but their narrow electrochemical stability window hinders their realization. Although highly concentrated fluorinated electrolytes have been shown to be highly effective in suppression of water splitting, enabling significant widening of the applied potential range, they utilize expensive salts (e.g., lithium bis(trifluoromethane sulfonyl) imide [LiTFSI] or lithium trifluoromethane sulfonate [LiOTf]); hence, they cannot be considered for practical applications. Here, we demonstrate a cost-effective aqueous electrolyte solution combining 14 M LiCl and 4 M CsCl that allows stable operation of a 2.15-V battery comprising a TiO₂ anode and LiMn₂O₄ cathode. Addition of CsCl to the electrolyte plays a double role in system stabilization: the added chloride anions interact with the free water molecules, whereas the chaotropic cesium cations adsorb at the electrified interface, preventing hydrogen formation.