Abstract

Utilization of secondary spherical structures derived from metal hydroxides as precursor materials is one of the most promising approaches in terms of energy density and industrial viability for sodium-ion batteries. However, the understanding of how the particle size and arrangement of these secondary spherical structures influence electrochemical performance remains limited. Herein, a series of O3-type layered oxide cathode materials with various sizes (6, 8, 10, and 12 μm) and internal structures (hollow and radial arrangements) were tailored based on precursor-based structural control and particle sizing strategies. The relation in precursor size/structure, cathode characteristics, crystal microstress, structural stability, and electrochemical performance was established through a combination of structure, morphology, and electrochemical characterization. Notably, the size of secondary spherical particles exerted influence on microstress, leading to consequential changes in the c-axis. Elevated microstress levels induced compression of the unit cell along the c-axis, hampering sodium ion migration and undermining the stability of secondary spherical particles during cyclic charge-discharge processes. The optimized NaNi1/3Fe1/3Mn1/3O2-10 material exhibits the least micro stress and significant layer distance, delivers a capacity of 110 mAh g−1, and maintains an impressive capacity retention rate of 91.8% after 100 cycles at 10 C. This work offers valuable insights in energy-density cathode materials in sodium ion batteries.

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