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.

锌-铜氧化还原对具有多种优点，这促使我们通过在基于氯化锌的水性/有机双相电解质中结合氯化物穿梭化学来重建可充电 Daniell 电池。建立离子选择性界面以限制水相中的铜离子，同时确保氯离子转移。我们证明了铜-水-氯溶剂化络合物是描述符，它在具有最佳氯化锌浓度的水溶液中占主导地位；因此，防止了铜交叉。如果没有这种预防，铜离子大部分处于水合状态，并表现出在有机相中溶剂化的高度自发性。锌铜电池具有 395 mAh g ^{−1的高度可逆容量}具有接近 100% 的库仑效率，提供基于氯化铜质量的 380 Wh kg ^-1的高能量密度。拟议的电池化学可扩展到其他金属氯化物，这扩大了可用于含水氯离子电池的阴极材料。