Interfacial Regulation via Anionic Surfactant Electrolyte Additive Promotes Stable (002)‐Textured Zinc Anodes at High Depth of Discharge

Abstract Aqueous zinc‐ion batteries have been identified as a viable option for grid energy storage. However, their practical application is limited by the poor performances at a high use rate of zinc. A suitable strategy to improve the cycling stability at a high depth of discharge (DOD) is by realizing the (002)‐textured Zn plating to suppress dendrite growth and side reactions. Herein, a novel electrolyte additive sodium 3‐mercapto‐1‐propanesulfonate (MPS) is introduced to regulate the zinc/electrolyte interfacial structure. The MPS anions can form an adsorption layer on the anode surface, which induces Zn deposition in the (002) direction as indicated by first‐principles calculations. Additionally, the adsorption layer can facilitate the reduction of the energy barrier associated with zinc deposition. This modified interface effectively inhibits dendrite and side reactions, resulting in a remarkable cycling lifespan for Zn||Zn symmetric cells, exceeding 800 h at a high DOD of 50%, and over 4500 h at 1.0 mA cm −2 /1.0 mAh cm −2 . Moreover, the capacity stability of the full cells with V 2 O 5 ·H 2 O or polyaniline cathodes is substantially improved. A pouch‐type Zn||V 2 O 5 ·H 2 O full cell reveals a high capacity of 42 mAh and good capacity retention of 86.6% after 250 cycles, highlighting significant potential for practical applications.