Remodeling Interfacial Electrical Field for Superhigh Capacity and Ultralong Lifespan Aqueous Zinc‐Ion Batteries
Yan Ran, Mengyao Li, Huaping Zhao, Jie Ren, Yonglong Sheng, Guosheng Shao, Yude Wang, Yong Lei
Abstract
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.