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Porosity Development at Li-Rich Layered Cathodes in All-Solid-State Battery during In Situ Delithiation.

Shuang Li1, Yipeng Sun2, Ning Li3

  • 1Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, United States.

Nano Letters
|June 10, 2022
PubMed
Summary

Structural changes in high-voltage lithium, manganese-rich cathodes are key for performance. This study reveals nanopore and nanovoid evolution in Li1.2Ni0.2Mn0.6O2 cathodes, offering insights into battery design.

Keywords:
Lithium-ion batteryall-solid-state batteryin situ TEMlayered cathodenanovoid

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Batteries

Background:

  • High-voltage lithium, manganese-rich layered cathodes are critical for advanced energy storage.
  • The electrode-electrolyte interface significantly impacts ionic transport in all-solid-state batteries.

Purpose of the Study:

  • To investigate the structural evolution and porous structure formation in Li1.2Ni0.2Mn0.6O2 cathodes with LiPON solid-state electrolyte.
  • To understand the role of interfacial phenomena and nanovoid development on cathode performance.

Main Methods:

  • In situ characterization of Li1.2Ni0.2Mn0.6O2 cathode during Li+ extraction.
  • Analysis of interfacial layers and structural changes using advanced microscopy and spectroscopy techniques.

Main Results:

  • Two distinct porous structures, nanopores and nanovoids, were identified in the Li1.2Ni0.2Mn{0.6}O2 cathode.
  • Nanopores were observed at the pristine cathode/electrolyte interface, associated with cation mixing, phase transformation, oxygen loss, and Mn reduction.
  • In situ Li+ extraction led to the propagation of nanovoids from the interface into the bulk, while the layered structure remained conserved.

Conclusions:

  • The study reveals the dynamic formation of nanovoids within high-capacity layered cathodes.
  • Understanding the distinct nature and divergent impacts of nanopores and nanovoids is crucial for improving cathode performance and all-solid-state battery design.