Crystalline‐Amorphous Phase and Oxygen Vacancies Synergistically Regulate Vanadium Electronic States for Unleashing Zinc‐Ion Storage Performance

Authors: Jingyu Sun, Li Zhang, Fengbo Li, Fajun Yang, Meiyu Liu, Shaobin Li, Deqing Zhang

Published: 2025-03-20

DOI: 10.1002/adfm.202501181

Source: Full article


Abstract

AbstractZinc‐ion capacitors (ZICs) are emerging as a compelling choice for energy storage in future, promising high power and energy densities coupled with eco‐friendly characteristics. This work presents a novel approach to enhance the performance of ZICs by employing a one‐step solvothermal synthesis to growth V‐MOF on the surface of V2CTX‐MXene, followed by annealing to fabricate a 3D cross‐linked VOX/V2CTX‐MXene‐x(VOX/MXene‐x) composite. The unique structure demonstrates excellent conductivity and high redox reaction activity, which significantly shortens the Zn2+ diffusion path. Moreover, the intertwined crystalline‐amorphous structure efficiently suppresses lattice volume expansion during Zn2+ (de)intercalation. Density functional theory (DFT) reveals that the amorphous V2O5 enhances conductivity, lowers the Zn2+ capture energy barrier, and improves charge transfer efficiency. The introduction of oxygen vacancies further enhances the electronic transport. The VOX/MXene‐4 composite exhibits a specific capacity of 336.39 mAh g−1 at 1 A g−1, maintaining 213.06 mAh g−1 at 10 A g−1, indicating outstanding rate performance, along with an energy density of 356.27 Wh kg−1 and a power density of 1280 W kg−1. This work offers novel insights for the design of electrode materials that feature intertwined crystalline‐amorphous phases, providing valuable insights into ion transport mechanisms and strategies to enhance Zn2+ diffusion kinetics.