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Summary

Layered oxide cathodes suffer from oxygen release due to phase transitions. This study reveals metal segregation in defective cathodes precedes transitions, driven by oxygen vacancies and Mn migration, altering degradation pathways.

Keywords:
electron energy‐correlation spectroscopylayered cathodeoxygen vacanciesphase transition

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Chemistry

Background:

  • Irreversible lattice oxygen release is a key failure mechanism in layered oxide cathodes.
  • This degradation is typically linked to phase transitions and reduced oxygen content.

Purpose of the Study:

  • To investigate the early degradation mechanisms in oxygen vacancy defective layered oxide cathodes.
  • To understand the role of local oxygen vacancy heterogeneity in cathode degradation.

Main Methods:

  • Electron energy loss spectroscopy (EELS) to analyze elemental and electronic structure changes.
  • Density functional theory (DFT) simulations to model atomic migration and electronic interactions.
  • Investigation of oxygen vacancy defective layered cathodes.

Main Results:

  • An anomalous metal segregation pathway was observed in defective cathodes, occurring before phase transitions.
  • Early charge transfer from oxygen 2p to manganese (Mn) 3d orbitals was identified as the cause.
  • Local oxygen vacancy heterogeneity significantly reduces the migration barrier for Mn.
  • Oxygen release initiates from defective sites, not perfect crystal regions, changing the degradation pathway.

Conclusions:

  • Local oxygen vacancy heterogeneity plays a critical role in the phase degradation of layered cathodes.
  • The findings challenge the conventional understanding of cathode degradation pathways.
  • Early metal segregation due to vacancy-induced Mn migration is a crucial factor in layered cathode failure.