High-Entropy Layered Oxide Cathode Enabling High-Rate for Solid-State Sodium-Ion Batteries

Abstract Na-ion O3-type layered oxides are prospective cathodes for Na-ion batteries due to high energy density and low-cost. Nevertheless, such cathodes usually suffer from phase transitions, sluggish kinetics and air instability, making it difficult to achieve high performance solid-state sodium-ion batteries. Herein, the high-entropy design and Li doping strategy alleviate lattice stress and enhance ionic conductivity, achieving high-rate performance, air stability and electrochemically thermal stability for Na 0.95 Li 0.06 Ni 0.25 Cu 0.05 Fe 0.15 Mn 0.49 O 2 . This cathode delivers a high reversible capacity (141 mAh g −1 at 0.2C), excellent rate capability (111 mAh g −1 at 8C, 85 mAh g −1 even at 20C), and long-term stability (over 85% capacity retention after 1000 cycles), which is attributed to a rapid and reversible O3–P3 phase transition in regions of low voltage and suppresses phase transition. Moreover, the compound remains unchanged over seven days and keeps thermal stability until 279 ℃. Remarkably, the polymer solid-state sodium battery assembled by this cathode provides a capacity of 92 mAh g −1 at 5C and keeps retention of 96% after 400 cycles. This strategy inspires more rational designs and could be applied to a series of O3 cathodes to improve the performance of solid-state Na-ion batteries.