Unraveling the Ultrafast Deposition Kinetics Within Zincphilic and Hydrophobic Organic Interphases for Dendrite‐Free and Long Lifespan Zinc Anodes

Abstract Aqueous zinc (Zn) batteries (AZBs) have garnered significant attention due to their inherent safety, environmental benignity, and low cost. However, their practical application is hampered by inevitable dendrite growth and an unstable anode/electrolyte interface. In this study, a dual regulation mechanism is proposed through the development of a Zn tetrafluoroterephthalate (ZTFA) interphase layer on the Zn anode (Zn@ZTFA). Theoretical calculations reveal that the ZTFA actively participates in the Zn ²⁺ ‐solvation structure, while its hydrophobic organic matrix effectively inhibits water‐induced side reactions. Additionally, ZTFA is rich in zincophilic functional groups, such as –COO ⁻ and C–F, which promote uniform Zn deposition, modulate the Zn ²⁺ desolvation and nucleation processes, and thereby enhance the Zn anode's reversibility and stability. As a result, the Zn@ZTFA anode delivers a highly reversible cycle lifespan of over 3100 h in symmetric cells and maintains an ultrahigh coulombic efficiency of 99.91% for 3000 cycles. Notably, the Zn@ZTFA||V ₂ O ₅ full cell exhibits excellent cycling stability, sustaining 1000 cycles at 5 A g ⁻¹ . This work presents a promising organic acid‐etching strategy for robust Zn anodes.