A High‐Entropy Intergrowth Layered‐Oxide Cathode with Enhanced Stability for Sodium‐Ion Batteries

Abstract Layered transition metal oxides are widely considered as ideal cathode materials for SIBs. However, the existing P2 and O3 structures possess specific issues, which limit their practical applications. To address these issues, this work designed a novel intergrowth layered oxide cathode with P2 and O3 phases by implementing Cu and Ti into the structure with the formation of high‐entropy cathode materials with superior performance for SIBs. The electrochemical test results show that the optimized high‐entropy cathode with the P2/O3 intergrowth structure possesses a high initial discharge capacity of 157.85 mAh g −1 at 0.1 C, an excellent rate performance of 84.41 mAh g −1 at 10 C, and long‐term stability with capacity retention of 83.25 % after 500 cycles at 5 C. Furthermore, the analysis results of ex situ XRD and in situ XRD indicate that the adverse phase transition of P2‐O2 under high voltage is effectively suppressed. This work indicates that the integration of high‐entropy strategy with the two‐phase intergrowth structure can effectively stabilize the layered structure, suppress the slipping of transition metal layers, and improve electrochemical performance, which provides a new approach for designing high‐performance and practical layered transition metal oxide cathode materials for advanced SIBs.