A Universal Interfacial Reconstruction Strategy Based on Converting Residual Alkali for Sodium Layered Oxide Cathodes: Marvelous Air Stability, Reversible Anion Redox, and Practical Full Cell

Mn-based layered oxide cathodes have attracted widespread attention due to high capacity and low cost, however, poor air stability, irreversible phase transitions, and slow kinetics inhibit their practical application. Here, we propose a universal interfacial reconstruction strategy based on converting residual alkali to tunnel phase Na0.44MnO2 for addressing the above mentioned issue simultaneously, using O3 NaNi0.4Fe0.2Mn0.4O2@2 mol % Na0.44MnO2 (NaNFM@NMO) as the prototype material. The optimized material exhibits an initial capacity and energy density comparable with lithium-ion batteries. The reversible anionic redox behavior and charge compensation mechanism of NaNFM@NMO were analyzed and verified by soft X-ray absorption spectrum and in situ X-ray absorption spectrum. Due to the intrinsic stability of the tunnel structure, excellent air stability and highly reversible structure evolution of the NaNFM@NMO cathode material are achieved, which are confirmed by contact angle test, rigorous aging test, and in situ X-ray diffraction. More importantly, the NaNFM@NMO cathode demonstrates a great match with the nonpresodiated hard carbon anode and shows excellent electrochemical performance of the full cell. Additionally, such a strategy could be also applied to modify P2-type cathodes, showing superior universality and good prospects in industrialized production. Overall, the proposed strategy could improve air stability while remaining interfacial and bulk stable simultaneously and will open up a whole new field for the optimization of other electrode materials.