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Full-Scale Regulation Enabled High-Performance Sodium O3-Type Layered Cathodes.

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Angewandte Chemie (International Ed. in English)
|February 12, 2025
PubMed
Summary
This summary is machine-generated.

This study introduces a modified O3-type sodium-ion battery cathode (NaNi1/3Fe1/3Mn1/3O2) with a CaZrO3 protective layer. This modification enhances structural stability and ion diffusion, significantly improving cycling performance and durability for energy storage applications.

Keywords:
Fe distortionO3-type layered cathodeTriple-lattice site dopingperovskite phase coating

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • O3-type cathodes offer high energy density for sodium-ion batteries but suffer from structural degradation and poor cycling stability.
  • Interfacial instability and kinetic limitations at elevated voltages lead to rapid capacity fading and safety concerns.

Purpose of the Study:

  • To develop a multifunctional surface-to-bulk modification strategy for O3-NaNi1/3Fe1/3Mn1/3O2 cathodes.
  • To enhance the structural integrity, interfacial stability, and sodium-ion diffusion kinetics of the cathode material.
  • To improve the overall state of health (SOH) and durability of sodium-ion batteries.

Main Methods:

  • In situ formation of a perovskite-type CaZrO3 protective layer on O3-NaNi1/3Fe1/3Mn1/3O2 primary particles.
  • Incorporation of Ca2+ and F- into the cathode's ternary lattice to reinforce the structure and facilitate Na+ diffusion.
  • Analysis of structural changes, including intergrowth phase transitions (P3-OP2) and mitigation of Jahn-Teller distortion.

Main Results:

  • The CaZrO3 layer successfully constructed a stable cathode-electrolyte-interphase, suppressing side reactions and transition metal dissolution.
  • Anchored Ca2+ pillars and Zr-O bonds reinforced the TMO6 octahedra, while F- doping facilitated Na+ diffusion.
  • Alleviation of lattice strain and restrained migration of Fe4+O6 due to an improved coordination environment.
  • The modified cathode (NFM-CZF) exhibited excellent rate capability and retained 83.8% of its capacity after 300 cycles at 2C.

Conclusions:

  • Synchronous surface and bulk modification effectively enhances the electrochemical performance and durability of O3-type cathodes.
  • The developed strategy provides valuable insights into regulating internal and external structures for high-performance sodium-ion batteries.
  • This approach offers a promising pathway for the commercialization of sodium-ion batteries with improved safety and longevity.