Aerogel‐Driven Interface Rapid Self‐Gelation Enables Highly Stable Zn Anode

Abstract The practical application of Zn metal anodes is currently hindered by uncontrolled dendritic growth and water‐induced parasitic reactions that are closely related to the solvation structure and interfacial transport kinetics of Zn²⁺. Herein, a facile interface self‐gelation strategy is proposed to stabilize Zn anode by introducing ‐OH‐rich silica aerogel (HSA) on Zn anode surface. The unique interconnected network structure and strong hydrophilia of HSA made the aqueous electrolyte near Zn anode gel rapidly and spontaneously, resulting in the formation of a water‐poor gel interface layer. The interface layer can effectively accelerate the desolvation process and reduce water molecule activity near anode surface through hydrogen bonding interaction, thus achieving rapid Zn migration kinetics and alleviating side reactions. In addition, the well‐defined aerogel nanochannels can provide a fast Zn²⁺ migration path and homogenize Zn²⁺ flux, enabling rapid and uniform Zn deposition. As a result, the HSA‐modified Zn (HSA@Zn) anode exhibits excellent long‐term cycling stability (over 6000 h at 4 mA cm⁻²), and the feasibility for practical application of this HSA@Zn anode is further demonstrate in full cells. The aerogel‐driven interface self‐gelation strategy propose in this work provides new insights into the design of advanced Zn anode for aqueous zinc‐ion batteries.