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Introducing strong covalent Ni─O bonds stabilizes P2-type manganese-based layered oxides for sodium-ion batteries. This method enhances structural integrity and suppresses oxygen release, improving battery performance and durability.

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Mn‐based layered oxidescovalency modulationoxygen redox reactionphase transitionsodium‐ion batteries

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Inorganic Chemistry

Background:

  • P2-type manganese-based layered oxides are promising cathode materials for sodium-ion batteries due to their high capacity and ease of synthesis.
  • However, these materials suffer from structural instability, phase transitions, and irreversible oxygen release during cycling, leading to capacity fade.

Purpose of the Study:

  • To develop a stable P2-type manganese-based layered oxide cathode material for sodium-ion batteries.
  • To address structural distortion and irreversible oxygen release by employing a covalency modulation strategy.

Main Methods:

  • A covalency modulation strategy was implemented by introducing strong covalent nickel-oxygen (Ni─O) bonds into the P2-type manganese-based layered oxide structure.
  • The synthesized material, Na0.6Mg0.15Mn0.7Ni0.15O2, was characterized for its structural and electrochemical properties.

Main Results:

  • The introduction of Ni─O bonds significantly enhanced the structural rigidity of the transition metal layered framework, alleviating distortion and preserving local coordination environments.
  • The covalent Ni─O bonds effectively stabilized the oxygen environment, suppressing irreversible oxygen release during cycling.
  • The resulting Na0.6Mg0.15Mn{0.7}Ni{0.15}O2 cathode exhibited full solid-solution behavior, a low volume change of 0.9%, and enhanced reversibility of the lattice oxygen redox reaction.

Conclusions:

  • Covalency modulation is a crucial strategy for enhancing the structural integrity and electrochemical performance of P2-type manganese-based layered oxides.
  • The strong Ni─O bonds play a vital role in stabilizing the crystal structure and regulating oxygen redox chemistry, leading to durable and high-energy-density sodium-ion battery cathodes.