Tailoring the Interfacial Electric Field Using Silicon Nanoparticles for Stable Zinc‐ion Batteries

Abstract Aqueous zinc‐ion batteries (ZIBs) are among the most promising next‐generation energy storage systems due to their high level of safety, environmental friendliness, and low cost. However, the dendritic growth of Zn deposition leads to low Coulombic efficiency and severe capacity degradation, which limits their large‐scale application. In this study, silicon nanoparticles are used as electrolyte additives which can regulate the uniform electrodeposition of Zn by the formation of SiOZn bonds. Theoretical calculations and experimental investigations demonstrate that the silicon layer regulates the interfacial charge distribution, resulting in a lower nucleation energy barrier for the Zn anode. Consequently, Zn|Zn symmetric cells with nano‐Si electrolyte additives achieve remarkable cycling stability for 1250 cycles at 5 mA cm −2 . When coupled with NaV 3 O 8 cathodes, the resulting ZIBs deliver a high reversible capacity of 250 mAh g −1 and significantly improved capacity retention after long‐term cycles.