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Mitigating Sodium Ordering for Enhanced Solid Solution Behavior in Layered NaNiO2 Cathodes.

Krishnakanth Sada1, Steven Kmiec1, Arumugam Manthiram1

  • 1Materials Science and Engineering Program and Texas Materials Institute, The University of Texas at Austin, Austin, Texas, 78712, USA.

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|April 16, 2024
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Summary
This summary is machine-generated.

Magnesium substitution in nickel oxides enhances structural stability for sodium-ion batteries. This strategy alleviates Jahn-Teller distortion and improves capacity retention over 100 cycles.

Keywords:
cathodeselectrochemistrylayered oxidesoperando characterizationsodium-ion batteries

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Chemistry

Background:

  • O-type layered nickel oxides exhibit structural instability due to Jahn-Teller distortion from Ni3+ ions.
  • These materials undergo phase transformations during sodium-ion (Na+) insertion/extraction, limiting their performance in sodium-ion batteries.
  • Stabilizing the structural integrity is crucial for developing high-performance sodium-ion energy storage.

Purpose of the Study:

  • To investigate the effect of substituting 5% divalent (Mg2+) or trivalent (Al3+, Co3+) ions for Ni3+ in O-type layered nickel oxides.
  • To alleviate Na+ ordering and perturb the Jahn-Teller effect to enhance structural stability.
  • To understand the fundamental bonding interactions and their influence on structural and electrochemical properties.

Main Methods:

  • Systematic ion substitution (Mg2+, Al3+, Co3+) in nickel oxide structures.
  • Analysis of Mg-O and Na-O/Mg-O-Na bonding interactions.
  • Calculations of Van Vleck distortion modes.
  • Long-range structural analysis using operando X-ray diffraction.
  • Short-range structural analysis using magic angle spinning nuclear magnetic resonance.

Main Results:

  • Mg2+ substitution resulted in increased Mg-O bond ionicity, shielding oxygen from Na+ ions.
  • Calculations showed relaxation of NiO6 octahedra from Jahn-Teller distortion and reduced interlayer electron density with Mg2+.
  • Operando X-ray diffraction and magic angle spinning nuclear magnetic resonance revealed reduced ordering and a stable continuous solid solution.
  • Mg-substituted samples exhibited high capacity retention of ~96% after 100 cycles.

Conclusions:

  • Magnesium substitution effectively mitigates Jahn-Teller distortion and improves the structural stability of O-type layered nickel oxides.
  • The enhanced structural integrity leads to improved electrochemical performance and high capacity retention in sodium-ion batteries.
  • This strategy offers a promising pathway for developing robust and high-performance sodium-ion energy storage materials.