The zinc-copper redox couple exhibits several merits, which motivated us to reconstruct the rechargeable Daniell cell by combining chloride shuttle chemistry in a zinc chloride-based aqueous/organic biphasic electrolyte. An ion-selective interface was established to restrict the copper ions in the aqueous phase while ensuring chloride transfer. We demonstrated that the copper-water-chloro solvation complexes are the descriptors, which are predominant in aqueous solutions with optimized concentrations of zinc chloride; thus, copper crossover is prevented. Without this prevention, the copper ions are mostly in the hydration state and exhibit high spontaneity to be solvated in the organic phase. The zinc-copper cell delivers a highly reversible capacity of 395 mAh g-1 with nearly 100% coulombic efficiency, affording a high energy density of 380 Wh kg-1 based on the copper chloride mass. The proposed battery chemistry is expandable to other metal chlorides, which widens the cathode materials available for aqueous chloride ion batteries.
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