Enabling Stable Zn Anode with PVDF/CNTs Nanocomposites Protective Layer Toward High‐Performance Aqueous Zinc‐Ion Batteries

Abstract Due to its abundance of natural resources, high theoretical capacity, and suitable redox potential (−0.76 V vs SHE), Zn anode has received extensive attention both from academy and industry. However, the coexistence of Zn and H2O, which is unfortunately thermodynamically unstable, always involves severe metal corrosion, H2 evolution, dendrite growth, resulting in low reversibility of Zn anode. Herein, a phase transfer method is adapted to design a porous conductive protective layer on the Zn anode, denoted as (PVDF (Polyvinylidene fluoride)/CNTs(Carbon Nanotubes)‐PT(phase transfer) @ Zn). Based on in situ characterization, COMSOL simulation, and migration energy barrier calculation, it can be demonstrated that PVDF/CNTs‐PT @ Zn effectively inhibited the production of Zn dendrites and the side reactions triggered by H2O, achieving uniform deposition. Especially, the full picture of Zn deposition is observed using in situ computed tomography (CT). The symmetrical cell using the PVDF/CNTs‐PT @ Zn demonstrates dendrite‐free plating/stripping and possesses much better cycle stability than the bare Zn. A stable rechargeable full battery is demoed through coupling the PVDF/CNTs‐PT @ Zn anode with commercial V2O5. The strategy showcases a feasible pathway to inhibit Zn dendrite and side reactions in aqueous Zn ion battery, opening a promising avenue for the construction of metal anode protection layer.