Remodeling Interfacial Electrical Field for Superhigh Capacity and Ultralong Lifespan Aqueous Zinc‐Ion Batteries

Abstract Although the electrochemical performance of electrode materials in aqueous zinc‐ion batteries (AZIBs) has been improved, a thorough investigation into the underlying modification mechanisms remains essential. Density functional theory (DFT) calculations are conducted to investigate the NH ₄ V ₄ O ₁₀ @carbon cloth (NVO@CC) as an efficient cathode material for AZIBs, with a particular focus on the heterostructure interface. The analysis of electronic structure, adsorption energy, and ion migration energy barrier reveals that the built‐in electric field at the NVO/CC interface induces additional active sites, thereby enhancing the conductivity and structural stability of the NVO@CC electrode. As a result, the optimized NVO@CC cathode demonstrates a high specific capacity of 607.1 mAh g ⁻¹ at 0.1 A g ⁻¹ , an outstanding energy density of 443.6 Wh kg ⁻¹ at 0.3 A g ⁻¹ , and excellent long‐term cycling stability, retaining 81.24% of its capacity after 10,000 cycles at 5 A g ⁻¹ . Furthermore, a series of ex situ characterization tests confirmed a reversible Zn ²⁺ insertion/extraction mechanism. This work reveals the mechanism of electrochemical performance regulation by building a built‐in electric field, which is another way to achieve high‐performance AZIBs.