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Tailoring Intergranular Interfaces through Zirconium Solubility-Controlled Segregation for Optimized LiNiO2 Cathodes.

Baoyu Han1, Xinhai Li1, Zhiliang Yan1,2

  • 1National Energy Metal Resources and New Materials Key Laboratory, Engineering Research Center of the Ministry of Education for Advanced Battery Materials, Hunan Provincial Key Laboratory of Nonferrous Value-Added Metallurgy, School of Metallurgy and Environment, Central South University, Changsha, 410083, P. R. China.

Small Methods
|November 3, 2025
PubMed
Summary
This summary is machine-generated.

Interface engineering using zirconium doping in nickel-rich layered cathodes (LiNi0.996Zr0.004O2) enhances stability and performance for high energy density lithium-ion batteries.

Keywords:
Li+ diffusion kineticshigh nickel layered cathodeintergranular interfaces regulationmicrocrack suppressionprecursor engineering

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Battery Technology

Background:

  • Ni-rich layered cathodes face structural instability and interfacial degradation, limiting lithium-ion battery energy density.
  • Developing stable, high-performance cathode materials is crucial for advanced energy storage.

Purpose of the Study:

  • To engineer the intergranular interfaces of nickel-rich layered cathodes via in situ doping with zirconium.
  • To improve the structural integrity, electrochemical performance, and cycle life of LiNiO2-based cathodes.

Main Methods:

  • In situ doping of LiNi0.996Zr0.004O2 (LNO-Zr) precursors with Zr4+ to guide crystal growth.
  • Kilogram-scale synthesis and characterization of the engineered cathode material.
  • Analysis of interfacial properties, Li+ pathways, and electrochemical performance.

Main Results:

  • Zr doping promoted preferential {010}/{101} facet growth and formed ultrafine primary particles.
  • A conformal Li2ZrO3 nanolayer at intergranular interfaces inhibited grain growth and preserved structure.
  • The LNO-Zr cathode achieved 239.1 mAh g-1 capacity, 78.3% retention after 200 cycles, and improved kinetics.

Conclusions:

  • Scalable intergranular interface engineering via Zr doping enhances structural stability and electrochemical performance of Ni-rich cathodes.
  • The engineered architecture mitigates lattice strain, microcracking, and parasitic reactions.
  • This strategy offers insights into defect chemistry and mechanical stabilization for next-generation lithium-ion batteries.