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Construction and Testing of Coin Cells of Lithium Ion Batteries
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Surface Vacancy Engineering Re-Routes First-Cycle Redox for Stabilized Li-Rich Layered Cathodes.

Seongkoo Kang1, Dayeon Choi1, Suwon Lee1

  • 1Department of Materials Science and Engineering, Korea University, Seoul, 02841, Republic of Korea.

Angewandte Chemie (International Ed. in English)
|November 5, 2025
PubMed
Summary
This summary is machine-generated.

Engineered surface disorder in lithium-rich layered oxides prevents oxygen release and lattice collapse. This improves first-cycle efficiency and durability for high-energy-density cathodes.

Keywords:
DisorderLi‐ion batteryLi‐rich layered cathodesOxygen redoxVacancy engineering

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Surface Chemistry

Background:

  • Lithium-rich layered oxides (LRLO) are promising for high-energy-density batteries.
  • First-cycle performance degradation, including oxygen release and lattice collapse, limits LRLO application.
  • Controlling surface chemistry is crucial for mitigating these degradation pathways.

Purpose of the Study:

  • To investigate how atomic-scale surface disorder influences the redox sequence in LRLO.
  • To develop a strategy for enhancing the electrochemical performance and stability of Li1.14Ni0.32Mn0.54O2 (LNMO) cathodes.
  • To establish a general design principle for durable LRLO cathodes.

Main Methods:

  • Chemical treatment to introduce surface oxygen and transition metal vacancies in LNMO.
  • Multi-modal synchrotron analyses (e.g., X-ray diffraction, X-ray absorption spectroscopy) to characterize surface structure and oxidation states.
  • Electrochemical testing to evaluate first-cycle Coulombic efficiency, voltage fade, and capacity retention.

Main Results:

  • Surface vacancies were successfully introduced in LNMO, confined to the particle surface.
  • The treated LNMO exhibited an early oxygen oxidation below 4.4 V and delayed nickel oxidation.
  • Suppression of detrimental Ni4+─O covalent states, irreversible oxygen release, and manganese dissolution was observed.
  • The modified redox pathway maintained metal-oxygen coordination at high voltages.

Conclusions:

  • Atomic-scale surface disorder effectively controls the first-cycle redox sequence in LRLO.
  • Engineered surface vacancies prevent oxygen release and lattice collapse, enhancing electrochemical performance.
  • This work provides a general design strategy for developing stable, high-energy-density LRLO cathodes.