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Highly conductive Li garnets by a multielement doping strategy.

Xia Tong1, Venkataraman Thangadurai1, Eric D Wachsman2

  • 1†Department of Chemistry, University of Calgary, 2500 University Dr. NW, Calgary, Alberta T2N 1N4, Canada.

Inorganic Chemistry
|March 21, 2015
PubMed
Summary

Optimizing lithium-ion solid electrolytes by doping Li7La3Zr2O12 (LLZ) with Ba, Ta, and Nb enhanced conductivity. An Al-free composition achieved a bulk Li-ion conductivity of 0.72 mS cm(-1), significantly higher than the parent LLZ.

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Area of Science:

  • Materials Science
  • Solid-State Chemistry
  • Electrochemistry

Background:

  • Lithium-ion batteries require highly conductive solid electrolytes for improved safety and performance.
  • Garnet-type Li7La3Zr2O12 (LLZ) is a promising solid electrolyte material, but its ionic conductivity needs further enhancement.
  • Multielement doping offers a strategy to optimize the structure and properties of LLZ.

Purpose of the Study:

  • To optimize Li-ion conduction in LLZ by substituting La(3+) sites with Ba(2+) and Zr(4+) sites with Ta(5+) and Nb(5+).
  • To investigate the effect of multielement doping on the ionic conductivity of garnet-structured metal oxides.
  • To study the influence of potential Al doping on the properties of these multielement doped LLZ materials.

Main Methods:

  • Synthesis of garnet-structured metal oxides via conventional solid-state reaction.
  • Characterization using powder X-ray diffraction (PXRD) for phase formation, scanning electron microscopy (SEM) for morphology, and alternating current (AC) impedance spectroscopy for Li-ion conductivity.
  • Solid-state (27)Al and (7)Li magic-angle spinning (MAS) Nuclear Magnetic Resonance (NMR) spectroscopy to probe Al content and its effects.

Main Results:

  • All prepared samples exhibited the cubic garnet-type structure (space group: Ia3̅d) at 1150 °C, similar to the parent LLZ.
  • An Al-free composition, Li6.4La3Zr1.4Ta0.6O12, demonstrated a significantly higher bulk Li-ion conductivity of 0.72 mS cm(-1) at 25 °C.
  • This optimized composition also showed a low apparent activation energy of 0.26 eV, indicating efficient Li-ion transport.

Conclusions:

  • Multielement doping with Ba, Ta, and Nb effectively enhances the Li-ion conductivity of LLZ-based solid electrolytes.
  • The "Al-free" Li6.4La3Zr1.4Ta0.6O12 composition represents a highly conductive garnet-type solid electrolyte.
  • These findings contribute to the development of advanced solid electrolytes for next-generation lithium-ion batteries.