Air-stability is one of the most important considerations for the practical application of electrode materials in energy-harvesting/storage devices, ranging from solar cells to rechargeable batteries. The promising P2-layered sodium transition metal oxides (P2-Na_xTmO₂) often suffer from structural/chemical transformations when contacted with moist air. However, these elaborate transitions and the evaluation rules towards air-stable P2-Na_xTmO₂ have not yet been clearly elucidated. Herein, taking P2-Na_0.67MnO₂ and P2-Na_0.67Ni_0.33Mn_0.67O₂ as key examples, we unveil the comprehensive structural/chemical degradation mechanisms of P2-Na_xTmO₂ in different ambient atmospheres by using various microscopic/spectroscopic characterizations and first-principle calculations. The extent of bulk structural/chemical transformation of P2-Na_xTmO₂ is determined by the amount of extracted Na⁺, which is mainly compensated by Na⁺/H⁺ exchange. By expanding our study to a series of Mn-based oxides, we reveal that the air-stability of P2-Na_xTmO₂ is highly related to their oxidation features in the first charge process and further propose a practical evaluating rule associated with redox couples for air-stable Na_xTmO₂ cathodes.

Microspherical carbon particles were prepared from a mixture of resorcinol and formaldehyde. The resulting gel was annealed at 950°C under an Ar atmosphere. The carbon microparticles exhibit a highly disordered structure and low specific surface area. A maximum reversible capacity of has been achieved in sodium cells, which is mainly developed ( ) below 0.2 V. magic-angle spinning nuclear magnetic resonance results show the interaction between reversibly inserted sodium and carbon. Several electrolytes have been tested, and it has been concluded that tetrahydrofuran solvent improves the electrochemical performance of these carbon microspheres in sodium cells.

Layered transition metal oxides are the most important cathode materials for Li/Na/K ion batteries. Suppressing undesirable phase transformations during charge-discharge processes is a critical and fundamental challenge towards the rational design of high-performance layered oxide cathodes. Here we report a shale-like Na_xMnO₂ (S-NMO) electrode that is derived from a simple but effective water-mediated strategy. This strategy expands the Na⁺ layer spacings of P2-type Na_0.67MnO₂ and transforms the particles into accordion-like morphology. Therefore, the S-NMO electrode exhibits improved Na⁺ mobility and near-zero-strain property during charge-discharge processes, which leads to outstanding rate capability (100 mAh g⁻¹ at the operation time of 6 min) and cycling stability (>3000 cycles). In addition, the water-mediated strategy is feasible to other layered sodium oxides and the obtained S-NMO electrode has an excellent tolerance to humidity. This work demonstrates that engineering the spacings of alkali-metal layer is an effective strategy to stabilize the structure of layered transition metal oxides.

Na₃V_2-xFe_x(PO₄)₃/C (0 ≤ x ≤ 0.5) samples were prepared by a simple sol-gel method. X-ray diffraction patterns revealed high purity and crystalline phosphate indexed in the R-3c space group. On increasing the iron content, the cell volume increases due to the slightly higher radius of Fe³⁺. Cyclic voltammetry showed two signals at ca. 3.5 and 4.0 V, which evidence a linear dependence of potential on the level of substitution. The appearance of the short plateau at ca. 4.0 V is closely related to the higher iron substitution levels. The evaluation of XPS and ⁵⁷Fe Mössbauer spectra of charged and discharged electrodes allow ascribing the 4.0 V plateau to V⁴⁺/V⁵⁺ redox reaction and the extraction/insertion of extra sodium ions from octahedral M1 sites. Galvanostatic cycling showed capacity values as high as 115 mA h g⁻¹ for samples with x = 0.1, 0.2, 0.3 and exceptional cyclability.