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Defining the Reversible Limit of Anionic Redox via Interlayer Li Ordering.

Yuansheng Shi1, Pengfeng Jiang2, Fushan Geng3

  • 1School of Materials Science and Engineering, Nanyang Technological University, 50 Nanyang Avenue, Singapore 639798, Singapore.

Journal of the American Chemical Society
|May 15, 2026
PubMed
Summary
This summary is machine-generated.

Achieving ordered lithium stacking in sodium-ion batteries unlocks lattice oxygen

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Battery Technology

Background:

  • High-energy sodium-ion batteries require unlocking latent capacity from lattice oxygen.
  • Anionic redox chemistry (ARC) is hindered by structural irreversibility and voltage hysteresis.
  • Current research focuses on in-plane lithium topology, neglecting long-range interlayer ordering.

Purpose of the Study:

  • To define the reversible limit of anionic redox by correlating structure and performance with c-axis lithium ordering.
  • To investigate the impact of interlayer lithium stacking on oxygen activity in P2-Na0.7Li0.1Cu0.2Mn0.7O2 (NLCM).
  • To establish a protocol for controlling ARC through 3D crystallographic regulation.

Main Methods:

  • Utilized P2-Na0.7Li0.1Cu0.2Mn0.7O2 (NLCM) as a model system.
  • Employed advanced operando diagnostic analyses to study interlayer Li stacking effects.
  • Decoupled interlayer Li stacking from in-plane structures to isolate their influence.

Main Results:

  • Turbostratic lithium disorder triggers uncontrolled Li migration, causing excess capacity and degradation.
  • A highly ordered lithium stacking framework acts as a structural lock, defining the reversible boundary of ARC.
  • Interlayer Li ordering suppressed cation migration and over-activation of anionic capacity, achieving reversible ARC.

Conclusions:

  • Ordered interlayer lithium stacking is critical for reversible anionic redox in high-energy sodium-ion batteries.
  • This approach significantly reduces voltage hysteresis and improves capacity retention (86% over 200 cycles).
  • The study offers a 3D crystallographic regulation strategy to tame ARC, moving beyond 2D design limitations.