Spin State Modulation via Magnetic Fields in Fe Single Atom Catalysts for High-Performance Aqueous Zinc–Sulfur Batteries

Aqueous zinc-sulfur battery has garnered significant attention as a high-energy, low-cost, and safe energy storage system. However, the multielectron transfer kinetics of sulfur cathodes are relatively slow, presenting challenges such as limited sulfur utilization and lower discharge voltage, which significantly hinder their practical applications. In this study, we explored a comprehensive design approach for high-performance, long-cycle aqueous zinc-sulfur batteries. The simultaneous introduction of ZnI2 and Fe single atoms (Fe-SAs) as catalytically active agents decouples the redox reactions, effectively facilitating ZnS oxidation and S reduction separately. The application of an external magnetic field regulates the spin state of Fe-SAs, further enhancing their catalytic activity and electron transfer capability. Electrochemical tests demonstrate that the S@Fe-NC HS/ZnI2 cathode assembled under a magnetic field exhibits excellent rate performance, achieving an impressive specific capacity of 1399 mAh g-1 at a high current density of 5 A g-1 and good cycling stability over 300 cycles, representing the highest reported high-current discharge capacity to date. This study provides a comprehensive design framework for optimizing zinc-sulfur (Zn-S) battery performance and elucidates the influence of magnetic field-induced spin state modulation on catalytic behavior.