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Stacking Order Induced Anion Redox Regulation for Layer-Structured Na0.75 Li0.2 Mn0.7 Cu0.1 O2 Cathode Materials.

Cui Ma1, Aierxiding Abulikemu2, Jian Bao1

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Small (Weinheim an Der Bergstrasse, Germany)
|May 4, 2023
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The P3 stacking order in layered cathode materials enhances oxygen redox reversibility and structural stability for sodium-ion batteries (SIBs), leading to improved electrochemical performance.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Chemistry

Background:

  • Layer-structured cathode materials are crucial for sodium-ion batteries (SIBs).
  • Stacking order significantly influences electrochemical behavior and structural stability.
  • The specific impact of stacking order on anionic redox remains largely uninvestigated.

Purpose of the Study:

  • To compare the electrochemical and structural properties of two layered cathodes with different stacking orders: P2-Na0.75Li0.2Mn0.7Cu0.1O2 (P2-LMC) and P3-Na0.75Li0.2Mn0.7Cu0.1O2 (P3-LMC).
  • To elucidate the role of stacking order in anionic redox mechanisms within these materials.
  • To provide insights into designing advanced cathode materials for SIBs.

Main Methods:

  • Synthesis and characterization of P2-LMC and P3-LMC materials.
  • Synchrotron hard and soft X-ray absorption spectroscopies to analyze redox couples.
  • In situ X-ray diffraction to study structural evolution during cycling.
  • Electrochemical testing (capacity, retention, rate capability).

Main Results:

  • P3 stacking order demonstrates superior oxygen redox reversibility compared to the P2 stacking order.
  • P3-LMC exhibits simultaneous contributions from Cu2+/Cu3+, Mn3.5+/Mn4+, and O2-/O- redox couples.
  • Enhanced electronic densities in Cu 3d and O 2p orbitals in P3-LMC contribute to more reversible redox reactions.
  • P3-LMC shows higher structural reversibility during charge/discharge, even at a 5C rate.
  • P3-LMC achieves a high reversible capacity of 190.3 mAh g-1 and capacity retention of 125.7 mAh g-1 over 100 cycles.

Conclusions:

  • The P3 stacking order is beneficial for improving oxygen redox reversibility in layered cathode materials for SIBs.
  • Understanding the influence of stacking order on anionic redox provides critical insights for developing high-performance SIB cathodes.
  • P3-LMC represents a promising cathode material for advanced sodium-ion battery applications.