Thiosulfate‐Mediated Polysulfide Redox for Energetic Aqueous Battery

Sulfur‐based aqueous batteries (SABs) are regarded as promising candidates for safe, low‐cost, and high‐energy storage. However, the sluggish redox kinetics of polysulfides pose a significant challenge to the practical performance of SABs. Herein, we report a unique redox regulation strategy that leverages thiosulfate‐mediated ligand‐chain interaction to accelerate the polysulfide redox process (S0/S2−). The S2O32− species in the electrolyte can induce the rapid reduction of polysulfide through a spontaneous chemical reaction with sulfur species, while facilitating the reversible oxidation of short‐chain sulfides. Moreover, the thiosulfate redox pair (S2O32−/S4O62−) within the K2S2O3 electrolyte contributes additional capacity at higher potential (E0 > 0 V vs SHE). Consequently, the elaborate SAB delivers an unprecedented K+ storage capacity of 2470 mAh gs−1, coupled with a long cycling life exceeding 1000 cycles. Remarkably, thiosulfate‐mediated SAB achieves an energy density of 616 Wh kgS+Zn−1, surpassing both organic K−S batteries and conventional aqueous battery systems. This work elucidates the mechanism underlying the thiosulfate‐mediated polysulfide redox process, thereby opening a pathway for the development of high‐energy aqueous batteries.