Boosting Zinc Storage Performance of Li3VO4 Cathode Material for Aqueous Zinc Ion Batteries via Carbon‐Incorporation: A Study Combining Theory and Experiment

Abstract

AbstractIn the search for sustainable cathode materials for aqueous zinc ion batteries (AZIBs), vanadium (V)‐based materials have garnered interest, primarily due to their abundance and multiple oxidation states. Among the contenders, Li3VO4 (LiVO) stands out for its affordability, high specific capacity, and elevated ionic conductivity. However, its limited electrical conductivity results in significant resistance polarization, limiting its rate capability, especially under high currents. Through density functional theory (DFT) calculations, this study evaluates the electrochemical implications of carbon (C) incorporation within the LiVO matrix. The findings indicate that C integration significantly ameliorates the conductivity of LiVO. Moreover, C serves as a barrier, mitigating direct interactions between Zn2+ and LiVO, which in turn expedites Zn2+ diffusion. When considering various C materials for this role, glucose is emerged as the optimal candidate. The LiVO/C‐glucose composite (LiVO/C‐G) is observed to undergo dual phase transitions during charge–discharge cycles, resulting in an amorphous vanadium‐oxygen (VO) derivative, paving the way for subsequent electrochemical reactions. Collectively, the insights pave a promising avenue for refining AZIB cathode design and performance.