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Recently, the Institute of Physics of the Chinese Academy of Sciences and others have made progress in the stability research of sodium ion high entropy layered oxides. This achievement points out the direction for the element composition design of high entropy oxide cathode materials and provides a potential solution for the development of long-life layered oxide cathode materials suitable for sodium ion batteries.
The performance of positive electrode materials in sodium ion batteries directly affects the cycling life of the battery. In traditional ternary sodium ion layered oxide cathode materials, variable valence elements tend to be uniformly distributed to reduce the energy of the system. This is because once the material undergoes a change in oxidation state, the local structure will change, leading to a phase transition. In previous studies, high entropy layered oxide cathode materials have shown many advantages, but there are still some unresolved issues. The most prominent issue among them is that the transition metal layer contains different transition metal ions, and different ion masses, radius sizes, and valence electron configurations may lead to lattice strain inside the material. This lattice strain not only affects the structural integrity of the material, but may also lead to degradation of its electrochemical performance. Therefore, it is urgent to develop design strategies that can effectively suppress lattice strain and maximize the use of high entropy effects to stabilize material structures.
Researchers and collaborators from the Institute of Physics of the Chinese Academy of Sciences/National Research Center for Condensed Matter Physics in Beijing designed two types of O3 type high entropy oxides: NaNi0.3Cu0.1Fe0.2Mn0.3Ti0.1O2 (NCFMT), an oxide containing only 3d transition metals in the transition metal layer, and NaNi0.3Cu0.1Fe0.2Mn0.3Ti0.1O2 (NCFMS), an oxide of partial 3d transition metals with Sn replacing Ti, and discussed the structural characteristics and electrochemical properties of the two materials. Research has found that both materials exhibit uniform element distribution in their original state, but the mismatch in size, mass, and valence electron configuration of transition metal ions in NCFMS results in lattice distortion, exhibiting significant lattice strain within the transition metal layer. The study analyzed the samples after cycling using aberration corrected high angle annular dark field scanning transmission electron microscopy and atomic level energy dispersive X-ray spectroscopy. Research has found that during the cycling process, the intrinsic strain and cumulative lattice strain in the transition metal layer promote the migration of metal ions, leading to element segregation and crack formation inside and on the surface of NCFMS positive electrode particles. In contrast, the NCFMT all 3D transition metal composition has better structural electrochemical compatibility, enhances structural stability during cycling, reduces lattice stress accumulation, ion migration, and mechanochemical fatigue damage of electrode materials. Therefore, NCFMT has relatively excellent half cell and full cell cycling stability.
This achievement provides direction for the elemental composition design of high entropy oxide cathode materials and offers potential solutions for the development of long-life layered oxide cathode materials suitable for sodium ion batteries.
Recently, the related research results were published in Nature Energy under the title of Tailoring planar strain for robust structural stability in high-end layered sodium oxide cathode materials. The research work has been supported by the National Natural Science Foundation of China, the National Key R&D Program, the Chinese Academy of Sciences strategic pilot science and technology project, the Chinese Academy of Sciences Youth Innovation Promotion Association member project and relevant projects in Jiangsu Province.

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