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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Chemistry

Background:

  • Conventional Li-M-X6 frameworks face conductivity limitations in solid electrolytes (SEs).
  • Halide-based SEs are crucial for solid-state battery (ASSB) development but often suffer from poor ionic conductivity.
  • Overcoming conductivity limitations is key to advancing high-performance ASSBs.

Purpose of the Study:

  • To develop a novel Li-M-X5 oxyhalide chemistry to overcome the conductivity limitations of halide-based SEs.
  • To investigate the structural and ionic transport properties of the new oxyhalide material.
  • To evaluate the performance of the developed SE in all-solid-state batteries (ASSBs).

Main Methods:

  • Synthesis of Li-M-X5 oxyhalide compounds (Li3xTaO3xCl5-3x).
  • Comprehensive characterization using X-ray diffraction (XRD), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), and X-ray absorption spectroscopy (XAS).
  • Ionic conductivity measurements at various temperatures and electrochemical performance testing in full ASSBs.

Main Results:

  • Achieved record ionic conductivities of 9 mS cm⁻¹ at 30 °C and 0.59 mS cm⁻¹ at -35 °C, surpassing most reported halides.
  • Confirmed that oxygen incorporation induces structural distortions and enhances ion migration pathways.
  • Demonstrated excellent stable cycling in full ASSBs with 100% capacity retention after 3200 cycles at a 4 C rate.

Conclusions:

  • The novel Li-M-X5 oxyhalide chemistry offers a promising alternative to conventional SEs.
  • Oxygen incorporation is an effective strategy to enhance ionic conductivity in halide-based SEs.
  • The developed material enables high-performance and stable operation of ASSBs.