Achieving Superior Cyclability Pouch Cells with Oxygen Vacancy-Moderated P'2/P3 Hybrid Layered Sodium Cathode Materials.

Layered P2-type sodium manganese oxide has emerged as a promising cathode candidate for sodium-ion batteries due to its appealing cost-effectiveness and high discharge voltage. However, its practical capacity within the voltage range of 2.0-4.0 V (vs Na/Na) is relatively low, and its rate capability is hampered by the adverse charge/vacancy ordering during charge/discharge. In this study, a layered P'2/P3 mixed-phase NaMnNiLiO cathode with high (003) crystal plane intensity was designed by introducing oxygen vacancies to P2-structured materials. Aided by these advantages, the hybrid cathode material demonstrates impressive structural and thermal stability and faster Na-ion diffusion kinetics compared to a regular P2 material. Half-cell shows an initial discharge capacity retention of 101 mA h/g at 12 mA/g and 92.25% retention after 500 cycles at 120 mA/g. In combination with a hard carbon anode, the 0.5 A h pouch cell achieved a prevailing capacity retention of 95.2% after 2600 cycles at 36 mA/g. This work opens new dimensions for layered cathode materials with the aim of achieving superior cyclabilities.