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High Operating Potential Induces Conversion in Li-Rich Chalcogenides.

Abhiroop Mishra1, Victoria K Davis1, Nicholas V Dulock1

  • 1Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, California 91125, United States.

ACS Applied Materials & Interfaces
|July 6, 2026
PubMed
Summary
This summary is machine-generated.

Li-rich battery cathodes show promise for higher capacity but face challenges. Researchers found that conversion reactions above 3 V limit performance, suggesting potential-limited cycling below this threshold to avoid parasitic reactions and improve efficiency.

Keywords:
Li-ion batteryLi-rich chalcogenidesactive-material lossconversion reactionpolysulfides

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • Lithium-ion batteries are crucial for renewable energy, but current cathode capacities are limiting performance improvements.
  • Li-rich cathodes offer higher capacities through combined cationic and anionic redox, yet their full potential remains unrealized.
  • High operating potentials needed for anion redox in oxides cause electrolyte degradation, hindering the study of intrinsic cathode behavior.

Purpose of the Study:

  • To evaluate conditions for full delithiation of Li-rich materials, specifically Li-rich sulfide and selenide Li2FeCh2 (Ch = S, Se).
  • To investigate the electrochemical behavior of Li2FeCh2 at higher operating potentials (>3 V vs Li/Li+) and understand degradation mechanisms.
  • To determine strategies for avoiding parasitic side reactions and improving the performance of Li-rich cathodes.

Main Methods:

  • Galvanostatic measurements were performed on Li2FeS2 and Li2FeSe2 to assess their electrochemical performance.
  • Ex situ laser ablation inductively coupled plasma mass spectrometry (ICP-MS) and X-ray diffraction (XRD) were used to analyze material changes.
  • Electrochemical cycling was conducted under different voltage cutoffs to identify optimal operating conditions.

Main Results:

  • Both Li2FeS2 and Li2FeSe2 exhibited poor Coulombic efficiency and rapid capacity loss when cycled above 3 V vs Li/Li+ due to conversion reactions.
  • Li2FeS2 conversion to polysulfides led to material loss, but cycling below 3 V prevented sulfur dissolution.
  • Li2FeSe2 conversion to gamma-selenium was solid-state, but electrolyte decomposition and proton formation caused active material dissolution.

Conclusions:

  • Conversion reactions in Li2FeCh2 occur at potentials significantly higher than reversible anion redox, indicating these parasitic reactions can be avoided.
  • Potential-limited cycling below 3 V vs Li/Li+ is crucial for preventing detrimental conversion reactions and improving the stability of Li-rich sulfide and selenide cathodes.
  • Understanding and mitigating conversion reactions are key to unlocking the high-capacity potential of Li-rich materials for advanced energy storage.