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Royal Society of Chemistry (RSC) Chemical Science 17(7)
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    초록·키워드

    Advancing the energy density of sodium-ion batteries requires layered oxide cathodes with higher specific capacity, necessitating redox chemistry beyond conventional cations. Oxygen anionic redox offers a pathway but presents inherent challenges, including irreversible structural degradation, such as Jahn-Teller distortion. Here, we report that cooperative Cu/Mg co-doping triggers an adaptive lattice respiration mechanism that concurrently suppresses structural distortion and unlocks highly reversible anionic redox. Through <i>in situ</i> spectroscopy, we visualize that this dynamic process involves the oxidation of Cu<sup>2+</sup> to Jahn-Teller inactive Cu<sup>3+</sup>, which induces a predictable lattice distortion, while Mg<sup>2+</sup> orchestrates a compensatory symmetric breathing of the oxygen framework. This respiration effectively mitigates structural strain and preserves the layered integrity. Consequently, the P3-Na<sub>0.67</sub>Mn<sub>0.9</sub>Mg<sub>0.05</sub>Cu<sub>0.05</sub>O<sub>2</sub> enables a remarkable reversible capacity of 258.1 mAh g<sup>-1</sup>. It retains 75.3% capacity after 80 cycles at 5.0C, demonstrating that adaptive lattice respiration is a viable strategy for achieving stable anionic redox chemistry.

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