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Nanoscale-Resolved STXM Reveals Shell π-Type Superexchange for Enhancing High-Voltage Stability in Surface Al-Doped

Hsiao-Tsu Wang1, Raneen Taha2,3, Yi-Hong Chang1

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PubMed
Summary

Surface modification of lithium- and manganese-rich (LMR) layered oxides with aluminum suppresses oxygen release and structural degradation. This orbital engineering enhances high-voltage stability and cycle life for advanced lithium-ion batteries.

Keywords:
Al-doped LMR cathodesX-ray absorption fine structure (XAFS)oxygen anionic redox (OAR)scanning transmission X-ray microscopy (STXM)shell π-type superexchange

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Battery Technology

Background:

  • Lithium- and manganese-rich (LMR) layered oxides offer high capacity for next-generation lithium-ion batteries.
  • Their practical application is limited by surface degradation and oxygen release at high voltages, impacting cycle life and structural integrity.

Purpose of the Study:

  • To investigate the surface-bulk electronic and atomic structural changes in LMR cathodes.
  • To establish the correlation between surface modification and improved electrochemical performance.
  • To demonstrate a strategy for enhancing the high-voltage stability of LMR cathodes.

Main Methods:

  • Synchrotron-based scanning transmission X-ray microscopy (STXM) for visualizing electronic reconstruction.
  • X-ray absorption fine structure (XAFS) for analyzing local atomic structures.
  • Surface aluminum incorporation as a modification strategy.

Main Results:

  • Surface Al incorporation creates oxygen vacancies, weakening TM-O covalency and activating Ni-O-Mn superexchange interactions.
  • Orbital reconfiguration stabilizes high-spin Ni4+ at high voltage, buffering oxygen redox reactions.
  • Al-modified LMR cathodes show suppressed irreversible oxygen evolution and lattice collapse, with shorter Ni-O bonds and reduced coordination loss.

Conclusions:

  • Nanoscale orbital engineering at the particle surface effectively mitigates oxygen anionic redox (OAR) driven degradation.
  • Surface Al modification offers a practical route to enhance cycling durability and high-voltage stability in LMR cathodes.
  • Stabilization is primarily driven by Ni-O interactions, with Mn valence remaining unchanged.