Ultrastable Electrolytic Zn–I2 Batteries Based on Nanocarbon Wrapped by Highly Efficient Single‐Atom Fe‐NC Iodine Catalysts

Abstract Aqueous Zn–iodine (Zn–I 2 ) conversion batteries with iodine redox chemistry suffers the severe polyiodide shuttling and sluggish redox kinetics, which impede the battery lifespan and rate capability. Herein, an ultrastable Zn–I 2 battery is introduced based on single‐atom Fe–N–C encapsulated high‐surface‐area carbon (HC@FeNC) as the core–shell cathode materials, which accelerate the I − /I 3 − /I° conversion significantly. The robust chemical–physical interaction between polyiodides and Fe–N 4 sites tightly binds the polyiodide ions and suppresses the polyiodide shuttling, thereby significantly enhancing the coulombic efficiency. As a result, the core–shell HC@FeNC cathode endows the electrolytic Zn–I 2 battery with an excellent capacity, remarkable rate capability, and an ultralong lifespan over 60 000 cycles. More importantly, a practical 253 Wh kg −1 pouch cell shows good capacity retention of 84% after 100 cycles, underscoring its considerable potential for commercial Zn–I 2 batteries.