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Mechanochemically Robust LiCoO2 with Ultrahigh Capacity and Prolonged Cyclability.

Weiyuan Huang1,2, Jianyuan Li1, Qinghe Zhao1

  • 1School of Advanced Materials, Peking University Shenzhen Graduate School, Shenzhen, 518055, China.

Advanced Materials (Deerfield Beach, Fla.)
|May 27, 2024
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Summary

Researchers developed a gradient disordered structure to enhance lithium cobalt oxide (LCO) cathodes, improving battery capacity and stability. This breakthrough addresses mechanical failures in high-energy batteries.

Keywords:
Li‐ion battery cathodefatigue resistancegradient disorderingprolonged cyclabilityultrahigh capacity

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Chemistry

Background:

  • Intercalation cathodes face capacity fading due to fragile Li-deficient frameworks and lattice strain.
  • Layered oxide cathodes are particularly susceptible to structural degradation from excessive lithium extraction.
  • Existing strategies like doping and surface coatings have not fully resolved these issues.

Purpose of the Study:

  • To develop a mechanochemical strengthening strategy for LiCoO2 (LCO) cathodes.
  • To enable LCO cathodes to approach their theoretical capacity limit while maintaining structural integrity.
  • To improve the cyclability and rate capability of high-energy-density battery materials.

Main Methods:

  • Development of a gradient disordered structure using a mechanochemical strengthening strategy.
  • Comprehensive characterization using multiscale X-ray, electron diffraction, and imaging techniques.
  • Validation in practical Ah-level pouch full cells under demanding operating conditions.

Main Results:

  • Achieved 93% lithium utilization, reaching 256 mAh g⁻¹ capacity in LCO cathodes.
  • Demonstrated exceptional cyclability and rate capability, surpassing current performance benchmarks.
  • Gradient disordered structure significantly reduced anisotropic lattice strain and enhanced fatigue resistance.

Conclusions:

  • The gradient disordered structure effectively impedes particle crack propagation and irreversible phase transitions.
  • This approach successfully mitigates mechanical failures in Li-deficient frameworks.
  • The study offers a promising direction for designing next-generation high-energy-density battery materials.