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Solid-state Graft Copolymer Electrolytes for Lithium Battery Applications
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High Capacity Garnet-Based All-Solid-State Lithium Batteries: Fabrication and 3D-Microstructure Resolved Modeling.

Martin Finsterbusch1,2, Timo Danner3,4, Chih-Long Tsai1

  • 1Forschungszentrum Juelich GmbH , Wilhelm-Johnen Str. , 52425 Juelich , Germany.

ACS Applied Materials & Interfaces
|June 12, 2018
PubMed
Summary

Researchers developed a novel all-inorganic solid-state battery cathode using LiCoO2 and LLZ:Ta. Microstructure simulations revealed interface phenomena limit room temperature performance, offering insights for future solid-state battery design.

Keywords:
Li batteryall-solid-stateceramiccontinuummicrostructuremodeling

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Battery Technology

Background:

  • Developing high-performance all-solid-state batteries (ASSBs) is crucial for next-generation energy storage.
  • Optimization of the positive electrode is a key challenge in ASSB development.

Purpose of the Study:

  • To create and characterize a novel, fully inorganic mixed positive electrode for ASSBs.
  • To investigate the electrochemical performance limitations of this new electrode design using advanced simulations.

Main Methods:

  • Fabrication of a mixed positive electrode using LiCoO2 and Ta-substituted Li7La3Zr2O12 (LLZ:Ta).
  • Assembly and electrochemical testing of a complete ASSB cell with a Li metal anode and LLZ:Ta electrolyte.
  • 3D reconstruction and microstructure-resolved continuum simulations of the positive electrode.

Main Results:

  • A novel LiCoO2 + LLZ:Ta mixed cathode was successfully produced without sintering aids or conductive additives.
  • The ASSB cell demonstrated 81% theoretical capacity utilization at elevated temperatures and 0.1 C discharge rate.
  • Simulations accurately predicted high-temperature performance but failed to capture room-temperature performance loss.

Conclusions:

  • Interface phenomena at the cathode active material/solid-electrolyte interface are identified as the primary cause of poor room-temperature performance.
  • Microstructure-resolved simulations provide valuable insights into performance limitations and optimization potential for oxide-based ASSBs.
  • This research offers critical guidelines for the future development and fabrication of advanced ASSBs.