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A Design Strategy for Durable Anionic Redox via Fluorine-Induced Electronic Structure Modulation in In Situ Formed

Wontae Lee1,2,3, Yun Seong Byeon4, Kyeongkeun Kwon5

  • 1Department of Chemistry Education, Kyungpook National University, Daegu, Republic of Korea.

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

Fluorination stabilizes disordered cathode materials for next-generation lithium-ion batteries (LIBs) by suppressing oxygen release and enhancing cycling performance. This breakthrough enables durable, high-capacity LIB cathodes by engineering stable anionic redox functionality.

Keywords:
Li‐O‐M‐F quadrupolar environmentLi‐excess cathode materialsanionic redox reactionelectronic structure modulationin situ formed disordered phase

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Battery Technology

Background:

  • Disordered cathode materials offer potential for advanced lithium-ion batteries (LIBs).
  • Anionic redox in these materials is limited by instability and oxygen release, hindering commercialization.
  • Conventional Li-excess disordered systems face compositional constraints.

Purpose of the Study:

  • To overcome the instability and oxygen evolution issues in disordered cathode materials.
  • To develop a new framework for engineering durable, high-capacity LIB cathodes.
  • To unlock stable anionic redox functionality in next-generation LIBs.

Main Methods:

  • Utilized Immm-Li2NiO2 as a platform for highly lithiated chemistries.
  • Introduced fluorination to modify the electronic structure and create Li-O-M-F units.
  • Investigated the impact of fluorination on electrochemical cycling, oxygen release, and structural stability.

Main Results:

  • Fluorination suppressed oxygen evolution at high voltages by lowering Li─O─Li band energy.
  • The Li-O-M-F configuration enhanced structural stability and improved cycling performance.
  • Achieved in situ disorder formation with stable anionic redox functionality.

Conclusions:

  • Fluorination is a viable strategy to stabilize disordered cathode materials for LIBs.
  • The developed framework enables durable, high-capacity cathodes by transcending stoichiometric restrictions.
  • This approach offers a blueprint for designing next-generation LIB materials with enhanced performance.