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Artificial Post-Cycled Structure Modulation Towards Highly Stable Li-Rich Layered Cathode.

Xiao Han1, Ailin Liu1, Shihao Wang1

  • 1State Key Laboratory of Physical Chemistry of Solid Surface, Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials, College of Materials, Xiamen University, Xiamen, 361005, China.

Small (Weinheim an Der Bergstrasse, Germany)
|July 28, 2023
PubMed
Summary

Researchers stabilized high-capacity lithium-rich layered oxides (LLOs) by creating an artificial post-cycled structure. This shields against degradation, enhancing electrochemical performance and stability for advanced lithium-ion batteries.

Keywords:
Li-rich layered cathodesartificial post-cycled structurescation mixingcycling stabilityelectronic structure modulation

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Battery Technology

Background:

  • High-capacity lithium-rich layered oxides (LLOs) exhibit excellent potential for lithium-ion batteries.
  • However, LLOs suffer from structural degradation and poor cycling stability due to hybrid anion- and cation-redox activity.
  • The native post-cycled structure, characterized by a densified defective spinel layer (DSL) and cation mixing, impedes Li+ ion transport.

Purpose of the Study:

  • To engineer an artificial post-cycled structure in LLOs to mitigate degradation.
  • To suppress anion redox activity and modulate cation mixing for improved stability.
  • To enhance the electrochemical performance and cycling life of LLO cathodes.

Main Methods:

  • In situ construction of an artificial post-cycled structure comprising artificial DSL and modulated cation mixing.
  • Electrochemical characterization including cycling performance, rate capability, and stability at elevated temperatures.
  • Analysis of structural changes and redox mechanisms.

Main Results:

  • The modified DSL-2% LLO cathode achieved a high discharge capacity of 187 mAh g⁻¹ after 500 cycles at 2 C.
  • The artificial structure effectively suppressed oxygen emission and transition metal migration.
  • Excellent capacity retention (168 mAh g⁻¹ after 250 cycles at 50 °C) was observed, outperforming pristine LLOs.

Conclusions:

  • The artificial post-cycled structure acts as a protective shield, enhancing the stability of LLOs.
  • This approach offers a novel perspective on stabilizing lithium-depleted regions and mitigating degradation.
  • The study presents a universal design principle for developing highly stable intercalated materials with anionic redox activity.