Surface Forces and Structure in a Water-in-Salt Electrolyte

Water-in-salt electrolytes are a fascinating new class of highly concentrated aqueous solutions with wide electrochemical stability windows that make them viable as aqueous battery electrolytes. However, the high ion concentration of water-in-salt electrolytes means that these systems are poorly understood when compared to more dilute electrolyte solutions. Here, we present direct surface force measurements across thin films of a water-in-salt electrolyte at several concentrations. We find that the electrolyte adopts a layered structure at charged interfaces composed of a nanostructure of a hydrated cation and nonaqueous anion-rich domains. These observations will aid in the interpretation of capacitance and double-layer behavior of water-in-salt electrolytes with consequences for their use in energy storage devices.