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Breaking Capacity-Stability Trade-Off in Sodium Layered Oxide via Entropy-Mediated Dual-Site Engineering.

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Summary

This study introduces a novel dual-site modification for high-entropy oxide cathodes in sodium-ion batteries (SIBs). The optimized material achieves high capacity and excellent cycling stability, advancing SIB technology.

Keywords:
Ca2+ substitutionhigh rate capabilityhigh‐entropy cathodeshigh‐voltage phase transition suppressionsodium‐ion batteries

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • Layered high-entropy oxides are promising for sodium-ion batteries (SIBs) due to sodium's abundance.
  • Conventional designs face trade-offs between structural integrity and capacity.
  • A new approach is needed to enhance SIB cathode performance.

Purpose of the Study:

  • To develop an advanced high-entropy oxide cathode for SIBs.
  • To improve both specific capacity and long-term cycling stability.
  • To investigate the structural and electrochemical benefits of dual-site modification.

Main Methods:

  • Synthesized an O3-type Na0.91Ca0.02(Ni0.3Li0.05Fe0.1Mn0.4Ti0.1Mg0.05)O2 cathode.
  • Applied dual-site modification: Ca2+ pillars and high-entropy transition-metal slab.
  • Conducted electrochemical testing (capacity, rate, cycling) and in situ X-ray diffraction.

Main Results:

  • Achieved high reversible capacity (145.2 mAh g-1 at 0.1 C).
  • Demonstrated remarkable rate capability (81.3% retention at 2 C) and cycling stability (92.6% at 5 C after 800 cycles).
  • Suppressed detrimental P3-OP2 phase transition and enhanced Na+ transport.

Conclusions:

  • Synergistic entropy engineering and cationic substitution reconcile high capacity with cyclability.
  • The dual-site modification strategy offers a pathway to practical high-energy SIB cathodes.
  • This work advances the design principles for next-generation sodium-ion battery materials.