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Tuning Oxide Properties by Oxygen Vacancy Control During Growth and Annealing
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Oxygen-deficient TiO

Yike Lei1, Yingchuan Zhang1, Yongkang Han1

  • 1School of Automotive Studies, Clean Energy Automotive Engineering Center, Tongji University (Jiading Campus) 4800 Cao'an Road Shanghai 201804 P. R. China xiaoqf@tongji.edu.cn.

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|June 7, 2023
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A novel TiO2-x interlayer coating significantly improves Li-rich Mn-based layered oxide (LMLO) cathodes by suppressing oxygen release, enhancing stability, and boosting electrochemical performance for better batteries.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • Li-rich Mn-based layered oxide (LMLO) cathodes offer high capacity due to anion redox.
  • Irreversible anion redox reactions in LMLO cathodes lead to structural degradation and poor performance.
  • Oxygen release during cycling is a key issue affecting LMLO cathode stability.

Purpose of the Study:

  • To enhance the electrochemical performance and stability of LMLO cathodes.
  • To mitigate issues associated with irreversible anion redox reactions and oxygen release.
  • To investigate the efficacy of a TiO2-x interlayer as a protective coating.

Main Methods:

  • Coating a commercial Celgard separator with a single-sided conductive oxygen-deficient TiO2-x interlayer.
  • Electrochemical testing including capacity retention and rate performance measurements.
  • Operando differential electrochemical mass spectroscopy (DEMS) and X-ray photoelectron spectroscopy (XPS) for analysis.

Main Results:

  • The TiO2-x interlayer improved initial coulombic efficiency from 92.1% to 95.8%.
  • Capacity retention after 100 cycles increased from 84.2% to 91.7%.
  • Rate performance at 5C significantly enhanced from 91.3 mA h g-1 to 203.9 mA h g-1.
  • DEMS confirmed oxygen release suppression, while XPS indicated reduced side reactions and improved cathode-electrolyte interphase.

Conclusions:

  • The oxygen-deficient TiO2-x interlayer effectively suppresses oxygen release from LMLO cathodes.
  • The interlayer enhances electrochemical kinetics, stability, and coulombic efficiency.
  • This approach offers a promising strategy to improve LMLO cathode performance for advanced batteries.