Edge-electron induced ferrimagnetic effect to accelerate interfacial desolvation kinetics toward dendrite-free Zn metal batteries

Rechargeable aqueous zinc metal batteries (AZMBs) have garnered significant attention for large-scale energy
storage. However, they are hindered by the sluggish Zn(H$_2$O)$_6$$^{2+}$ desolvation kinetics, leading to uneven Zn
deposition as well as side reactions of active water molecules for the formation of hydrogen evolution reaction
(HER). Herein, high spin-state ferrimagnetic interphase of spinel zinc ferrite (ZFO) has been pioneered to serve as
artificial interphase on metallic Zn anode (ZFO@Zn). Specifically, high-spin Fe$^{3+}$ center enhances electron
delocalization and the spinel crystal structure of ZFO layer facilitates the interfacial ion transfers, catalytically
reducing the barriers of Zn$^{2+}$ desolvation and atom diffusion. Meanwhile, the micro-magnetic field self-motivates
interfacial ion flux and separates the active molecules, enabling uniform Zn deposition without HER. The as-
fabricated cell employed with ZFO@Zn achieved an impressive cumulative capacity exceeding 3500 mAh
cm$^{-2}$at 30 mA cm$^{-2}$, demonstrating its remarkable kinetics and stability. The assembled vanadium-based full
cell exhibits superior performance of 411.1 mAh g$^{-1}$ at 10 A g$^{-1}$ and maintained the capacity-retention of 90.7%
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after 3000 cycles at 5 A g$^{-1}$. Impressively, the large-areal pouch cell with ZFO@Zn anode stabilizes for 150
cycles, underscoring the potential of magnetic spinel materials for the commercialization of AZMBs.