Abstract

The application of sodium-based batteries in grid-scale energy storage requires electrode materials that facilitate fast and stable charge storage at various temperatures. However, this goal is not entirely achievable in the case of P2-type layered transition-metal oxides because of the sluggish kinetics and unfavorable electrode|electrolyte interphase formation. To circumvent these issues, we propose a P2-type Na0.78Ni0.31Mn0.67Nb0.02O2 (P2-NaMNNb) cathode active material where the niobium doping enables reduction in the electronic band gap and ionic diffusion energy barrier while favoring the Na-ion mobility. Via physicochemical characterizations and theoretical calculations, we demonstrate that the niobium induces atomic scale surface reorganization, hindering metal dissolution from the cathode into the electrolyte. We also report the testing of the cathode material in coin cell configuration using Na metal or hard carbon as anode active materials and ether-based electrolyte solutions. Interestingly, the Na||P2-NaMNNb cell can be cycled up to 9.2 A g−1 (50 C), showing a discharge capacity of approximately 65 mAh g−1 at 25 °C. Furthermore, the Na||P2-NaMNNb cell can also be charged/discharged for 1800 cycles at 368 mA g−1 and −40 °C, demonstrating a capacity retention of approximately 76% and a final discharge capacity of approximately 70 mAh g−1.

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