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Uncovering the Network Modifier for Highly Disordered Amorphous Li-Garnet Glass-Ceramics.

Yuntong Zhu1, Ellis R Kennedy2, Bengisu Yasar2

  • 1Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA, 02139, USA.

Advanced Materials (Deerfield Beach, Fla.)
|January 30, 2024
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Summary
This summary is machine-generated.

Highly disordered amorphous Li7La3Zr2O12 (aLLZO) offers a grain-boundary-free pathway for lithium-ion (Li+) transport in solid-state batteries. Lanthanum acts as a network modifier, enhancing disorder and ionic conductivity in these promising battery materials.

Keywords:
Li garnetsLi7La3Zr2O12Li‐conducting glass‐ceramicsamorphous oxidessolid‐state batteries

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Area of Science:

  • Materials Science
  • Solid-State Chemistry
  • Electrochemistry

Background:

  • Amorphous Li7La3Zr2O12 (aLLZO) is a promising solid electrolyte for advanced batteries.
  • Its grain-boundary-free structure and wide electrochemical stability are advantageous.
  • Understanding structure-property relationships is key to optimizing Li+ transport.

Purpose of the Study:

  • To investigate the role of lanthanum (La) as a network modifier in amorphous Li7La3Zr2O12.
  • To elucidate how La concentration affects the local structure and Li+ transport.
  • To explore the potential of aLLZO for low-cost, sustainable solid-state batteries.

Main Methods:

  • Synthesis of amorphous Li7La3Zr2O12 phases with varying La concentrations.
  • Structural analysis to determine local building units (LBUs) and bonding environments.
  • Correlation of structural disorder with Li+ transport properties.

Main Results:

  • Lanthanum (La) identified as the primary network modifier, while Zr and Li act as network formers.
  • Increased La concentration leads to longer Zr-O and La-O bond distances, enhancing structural disorder.
  • This disorder promotes more efficient Li+ transport within the amorphous structure.
  • aLLZO exhibits wide electrochemical stability and is synthesizable at relatively low temperatures.

Conclusions:

  • Lanthanum concentration is a critical factor in tuning the disorder and Li+ conductivity of aLLZO.
  • These findings provide a pathway for designing novel amorphous Li+ electrolytes.
  • aLLZO presents a viable, cost-effective material for next-generation solid-state batteries.