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Advanced High-Entropy Halide Solid Electrolytes Enabling High-Voltage, Long-Cycling All-Solid-State Batteries.

Yu Ye1,2, Zhi Gu1, Jiazhong Geng3

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|February 27, 2025
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Summary

This study introduces a novel high-entropy chloride solid electrolyte (HE-5) for safer, high-energy lithium batteries. It demonstrates excellent ionic conductivity and stability for advanced all-solid-state batteries.

Keywords:
All-Solid-State BatteriesHigh VoltageHigh-EntropySolid-State Electrolytes

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Chemistry

Background:

  • Stable solid electrolytes are crucial for enhancing the safety and energy density of lithium batteries, particularly for high-voltage applications.
  • Current solid electrolytes face challenges in balancing ionic conductivity with high-voltage stability.

Purpose of the Study:

  • To design and synthesize an innovative high-entropy chloride solid electrolyte (HE-5) for improved lithium battery performance.
  • To investigate the relationship between high-entropy engineering, ionic conductivity, and electrochemical stability in solid electrolytes.
  • To evaluate the performance of HE-5 in all-solid-state batteries (ASSBs) with high-voltage cathodes.

Main Methods:

  • Multielement doping was employed to create a high-entropy chloride solid electrolyte (HE-5) with the composition Li₂.₂In₀.₂Sc₀.₂Zr₀.₂Hf₀.₂Ta₀.₂Cl₆.
  • The ionic conductivity and activation energy of HE-5 were measured.
  • All-solid-state batteries (ASSBs) utilizing HE-5, NCM83 cathodes, and a Li-In anode were assembled and electrochemically tested.
  • Electrochemical performance, including capacity retention and cycling stability at high voltage, was evaluated.

Main Results:

  • The synthesized HE-5 exhibited a disordered lattice structure, facilitating lithium-ion mobility.
  • An ionic conductivity of 4.69 mS cm⁻¹ at 30 °C and an activation energy of 0.300 eV were achieved.
  • ASSBs with HE-5 demonstrated excellent electrochemical performance, retaining 70% capacity over 1600 cycles at a 4 C rate.
  • Stable operation at 5.0 V was achieved due to the high configurational entropy stabilizing the electrolyte structure.

Conclusions:

  • High-entropy engineering effectively enhances both ionic conductivity and high-voltage stability in chloride solid electrolytes.
  • HE-5 presents a promising material for next-generation energy-dense and safe all-solid-state lithium batteries.
  • This research provides a valuable roadmap for developing advanced solid electrolytes through compositional complexity.