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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Chemistry

Background:

  • Oxygen redox in metal oxides boosts rechargeable battery capacity but suffers from overoxidation and degradation.
  • Irreversible oxygen loss and structural instability limit high-voltage cathode performance.

Purpose of the Study:

  • To investigate the role of interlayer superstructure in oxygen redox reversibility.
  • To identify structural features that enhance electrochemical stability in metal oxide cathodes.

Main Methods:

  • Comprehensive characterization techniques.
  • Synthesis and electrochemical testing of P3-R-NMO and P2-R-NMO materials.
  • Analysis of interlayer stacking sequences and their impact on O-redox reactions.

Main Results:

  • P3-R-NMO with an -A-B-C- interlayered superstructure exhibits highly reversible oxygen redox.
  • The -A-B-C- superstructure spatially separates O-□Mn-O motifs, enhancing structural integrity and mitigating Mn migration.
  • P2-R-NMO with an -A-B- stacking sequence shows poor reversibility due to P2-to-O2 phase transition and Mn migration.

Conclusions:

  • Interlayer superstructure design is critical for stable oxygen redox in rechargeable batteries.
  • Optimized superstructures can reinforce lattice strength against gliding, preventing irreversible degradation.
  • This work provides a pathway for developing high-performance, stable metal oxide cathodes through structural engineering.