I−/I3− Conversion‐Activated and Stabilized Bipedal‐Redox Bis(dimethylthiocarbamyl) Sulfide Cathode for High‐Performance Zinc‐Organosulfide Batteries

Abstract Organosulfides are considered promising cathode materials for zinc batteries due to their merits of high‐density active sites and multielectron reactions, but often suffer from sluggish kinetics and limited electrochemical stability. Here organic iodide‐catalyzed is reported and stabilized multielectron‐redox bis(dimethylthiocarbamyl) sulfide (BS) cathode for superior zinc‐organosulfide batteries. Activated by 2e − I − /I 3 − conversion in 1‐methyl‐3‐propylimidazolium iodide (MPII)‐modulated electrolyte, the electron‐deficient structure of BS can stretch the electron cloud of two adjacent C═S bonds to form bipedal C─S bonds, affording high‐kinetics and stable 2e − Zn─S storage electrochemistry. This allows high accessibility of zincophilic dual C = S sites with a low activation energy, and stabilizes BS to fulfil anti‐dissolution in electrolyte. Consequently, Zn||BS battery with 4e − conversion‐coordination harvests high‐rate capacities (452 mAh g −1 at 1 A g −1 ; 255 mAh g −1 at 10 A g −1 ), high energy density (312 Wh kg −1 ) and ultralong life (30000 cycles), becoming the state‐of‐the‐art zinc batteries in all‐round metrics. This work constitutes a significant advance in developing high‐redox‐activity organosulfide materials and stand for a good starting point for advanced zinc batteries.