High‐Entropy Co‐Free O3‐Type Layered Oxyfluoride: A Promising Air‐Stable Cathode for Sodium‐Ion Batteries

Sodium-ion batteries have recently emerged as a promising alternative to lithium-based batteries, driven by an ever-growing demand for electricity storage systems. The present workproposes a cobalt-free high-capacity cathode for sodium-ion batteries, synthesized using a high-entropy approach. The high-entropy approach entails mixing more than five elements in a single phase; hence, obtaining the desired properties is a challenge since this involves the interplay between different elements. Here, instead of oxide, oxyfluoride is chosen to suppress oxygen loss during long-term cycling. Supplement to this, lithium is introduced in the composition to obtain high configurational entropy and sodium vacant sites, thus stabilizing the crystal structure, accelerating the kinetics of intercalation/deintercalation, and improving the air stability of the material. With the optimization of the cathode composition, a reversible capacity of 109 mAh g-1 (2-4 V) and 144 mAh g-1 (2-4.3 V) is observed in the first few cycles, along with a significant improvement in stability during prolonged cycling. Furthermore, in situ and ex situ diffraction studies during charging/discharging reveal that the high-entropy strategy successfully suppresses the complex phase transition. The impressive outcomes of the present work strongly motivate the pursuit of the high-entropy approach to develop efficient cathodes for sodium-ion batteries.