Cations‐Pillared and Polyaniline‐Encapsulated Vanadate Cathode for High‐Performance Aqueous Zinc‐Ion Batteries

Layered vanadium-based oxides have emerged as highly promising candidates for aqueous zinc-ion batteries (AZIBs) due to their open-framework layer structure and high theoretical capacity among the diverse cathode materials investigated. However, the susceptibility to structural collapse during charge-discharge cycling severely hampers their advancement. Herein, we propose an effective strategy to enhance the cycling stability of vanadium oxides. Initially, the structural integrity of the host material is significantly reinforced by incorporating bi-cations Na⁺ and NH₄ ⁺ as "pillars" between the V₂O₅ layers (NaNVO). Subsequently, surface coating with polyaniline (PA) is employed to further improve the conductivity of the active material. As anticipated, the assembled Zn//NaNVO@PA cell exhibits a remarkable discharge capacity of 492 mAh g^-1 at 0.1 A g^-1 and exceptional capacity retention up to 89.2 % after 1000 cycles at a current density of 5 A g^-1. Moreover, a series of in-situ and ex-situ characterization techniques were utilized to investigate both Zn ions insertion/extraction storage mechanism and the contribution of polyaniline protonation process towards enhancing capacity.