Abstract

Aqueous Zn-iodine (Zn-I2) 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-I2 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-/I3 -/I° conversion significantly. The robust chemical-physical interaction between polyiodides and Fe-N4 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-I2 battery with an excellent capacity, remarkable rate capability, and an ultralong lifespan over 60000 cycles. More importantly, a practical 253Wh kg-1 pouch cell shows good capacity retention of 84% after 100 cycles, underscoring its considerable potential for commercial Zn-I2 batteries.

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