Pre-removing partial ammonium ion induces vanadium vacancy assist NH4V4O10 as a high-performance aqueous zinc ion battery cathode.

The increased interlayer spacing and vanadium vacancies enhance the diffusivity of Zn2+ ions in V d -NVO, endowing it with excellent cyclic stability and a capacity retention of 81.76 % after 1000 cycles at 5 A g−1. [Display omitted] • Pre-removing some ammonium ions from NH 4 V 4 O 10 expands the interlayer spacing. • The vanadium vacancy accelerates the diffusion kinetics of Zn2+. • The V d -NVO electrode demonstrates a reversible capacity of 131 mAh g−1 even after 1000 cycles at 5 A g−1. Ammonium vanadate (NH 4 V 4 O 10) is regarded as a promising cathode material for aqueous zinc-ion batteries, given its considerable theoretical capacity and tunable interlayer spacing. However, due to its inherent low electrical conductivity and the excessive presence of ammonium ions between layers, NH 4 V 4 O 10 exhibits unsatisfactory electrochemical performance. In this study, it is proposed that the electrochemical performance of NH 4 V 4 O 10 can be significantly enhanced by removing part of the ammonium cation and increasing the vanadium vacancy. The decrease of ammonium further increases the layer spacing, reduces the irreversible deamination and accelerates the diffusion of Zn2+. Density functional theory (DFT) calculations reveal that increasing vanadium vacancies significantly diminishes the strong electrostatic interactions between the V-O layers and Zn2+, enhances the material's electrical conductivity, and stabilizes the crystal structure during zinc ion (de)intercalation, thus obtaining excellent electrochemical properties. As a result, the V d -NVO cathode demonstrates a high reversible capacity of 371 mAh g−1, excellent rate performance, and remarkable cyclic stability, maintaining a reversible capacity of 131 mAh g−1 even after 1000 cycles at 5 A g−1. [ABSTRACT FROM AUTHOR]