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Unlocking Reversible Anionic Redox in Layered Oxides via a Cationic-Pair-Mediated Stabilization.

Yizhou Fang1, Peng-Ji Wang1, Xiaohong Liu1

  • 1State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China.

ACS Applied Materials & Interfaces
|February 9, 2026
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Summary

This study stabilizes high-energy sodium-ion batteries using a cationic-pair strategy in P2-type layered oxides. This approach enhances anionic redox activity while preventing structural degradation for improved battery performance.

Keywords:
Li/Zn cationic-pair mediationP2-type layered oxidesphase transition suppressionreversible anionic redox reactionsodium-ion batteries

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • P2-type layered oxides offer high energy density for sodium-ion batteries (SIBs) via anionic redox.
  • Anionic redox in SIBs suffers from oxygen loss and structural degradation, limiting practical application.
  • Stabilizing oxygen redox activity is crucial for developing high-performance SIBs.

Purpose of the Study:

  • To introduce a cationic-pair-mediated strategy to stabilize anionic redox in P2-type layered oxides.
  • To investigate the synergistic effects of Li and Zn cosubstitution on the structure and electrochemical performance of P2-Na0.78Ni0.11Li0.12Zn0.1Mn0.67O2 (NNLZMO).
  • To demonstrate a method for concurrently unlocking and stabilizing anionic redox in high-energy layered cathodes.

Main Methods:

  • Cosubstitution of Li and Zn into the transition-metal layers of P2-Na0.78Ni0.11Mn0.67O2 to form NNLZMO.
  • Electrochemical characterization including cyclic voltammetry, galvanostatic cycling, and impedance spectroscopy.
  • In-situ/ex-situ characterization techniques to analyze structural evolution and phase transitions.

Main Results:

  • The Li-Zn cationic pair synergistically activates reversible anionic redox by stabilizing nonbonding O 2p states.
  • Structural confinement from the cationic pair suppresses Na+/vacancy ordering and prevents irreversible P2-O2 phase transition.
  • NNLZMO exhibits a minimal-strain P2-Z phase transition (1.59% volume change), achieving 174.62 mAh g-1 capacity and 90.8% retention after 100 cycles.

Conclusions:

  • Cationic-pair design is an effective strategy for stabilizing anionic redox in P2-type layered oxides.
  • The NNLZMO cathode demonstrates enhanced electrochemical performance and structural stability for SIBs.
  • This approach paves the way for developing stable, high-energy sodium-ion batteries.