Vanadium Doping Enables Partially Disordered Li-Rich Spinel Cathodes with High Reversible Capacity and Low Migration Barriers

High-capacity cathode materials for lithium-ion batteries (LIBs) are urgently needed to meet the demands of electric vehicles and grid storage. To address the limitations of conventional cathode materials in lithium-ion batteries, we report a novel Li-rich partially disordered spinel (PDS) cathode Li1.5Mn0.7V0.9O3.7F0.3 that synergistically combines Mn/V dual-redox activity with controlled cation disorder to achieve exceptional electrochemical performance. First-principles calculations demonstrate a high reversible capacity of 263 mAh g–1 through reversible Mn3+/Mn4+ and V3+/V5+ redox processes while effectively suppressing oxygen activity. Molecular dynamics simulations reveal ultrafast Li+ migration with a remarkably low activation barrier of 62.6 meV/mol, enabled by 3D diffusion pathways. The stability of the Li1.5Mn0.7V0.9O3.7F0.3 material is further enhanced by fluorine doping and partial cation disorder, which collectively mitigate phase transitions and oxygen loss. This work establishes a new design paradigm for high-performance cathode materials that simultaneously achieve high energy density, rapid ion transport, and structural stability in lithium-ion batteries.