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Alternating Edge- and Face-Sharing Octahedra with Partial Super-Exchange Enabling High-Voltage Layered Cathodes.

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Summary

A new edge-sharing coplanar (ESC) O2-type layered structure enhances the stability of high-voltage cathodes by suppressing cobalt migration. This novel structure improves lithium-ion diffusion and cycling stability for next-generation batteries.

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edge‐sharing coplanar layered cathodeslithium‐ion batteriesopen‐shell metalspartial super‐exchanges

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Chemistry

Background:

  • Traditional O3-type layered oxides exhibit poor structural stability during high-voltage operation due to edge-sharing octahedra.
  • Cobalt (Co) migration is a key factor limiting the performance and lifespan of these cathode materials.
  • Developing stable layered oxide structures is crucial for advancing high-energy-density batteries.

Purpose of the Study:

  • To design and synthesize a novel, structurally stable edge-sharing coplanar (ESC) O2-type layered oxide cathode.
  • To investigate the impact of the ESC configuration on suppressing transition metal migration and enhancing structural integrity.
  • To optimize Ni content for improved high-voltage cycling performance and lithium-ion diffusion.

Main Methods:

  • Synthesis of a novel ESC O2-type layered oxide structure.
  • Characterization of structural stability and Co migration suppression.
  • Electrochemical testing, including high-voltage cycling performance and capacity retention.
  • Analysis of Ni-O-TM super-exchange interactions and their effect on Li-ion diffusion.

Main Results:

  • The ESC configuration effectively suppresses Co migration and enhances intrinsic structural stability.
  • Modified ESC cathodes demonstrate high discharge capacity (247 mAh g⁻¹) and excellent capacity retention (79% at 1 C after 100 cycles).
  • Optimal Ni content expands unit-cell volume, reducing Li-ion diffusion activation energy, but excess Ni obstructs Li-ion pathways.

Conclusions:

  • The edge-sharing coplanar (ESC) O2-type layered structure offers a promising strategy for developing stable high-voltage cathode materials.
  • Regulating the local coordination environment is key to achieving high performance in layered oxide cathodes.
  • This work provides insights into the role of Ni content and its impact on electrochemical performance in ESC cathodes.