Oxygen Electronic Configuration Modulation Triggering Reversible Anionic Redox Chemistry toward High Voltage Tolerant Sodium Layered Oxide.
basic_science · Level V
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- Record sourced from PubMed, PMID 42383393.
- Also identified by DOI 10.1021/acs.nanolett.6c01916.
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Abstract
The O3-type NaNi<sub>1/3</sub>Fe<sub>1/3</sub>Mn<sub>1/3</sub>O<sub>2</sub> layered oxide cathode is appealing for building low-cost sodium-ion batteries (SIBs), but the insufficient specific capacity limits its practical application. Elevating the charging cutoff voltage to trigger the anionic redox reaction (ARR) effectively boosts capacity, yet balancing capacity and cycling stability remains challenging. Herein, we propose a Na-O-Mg/Ti electronic configuration modulation strategy to synergistically enhance capacity and cycling stability by activating reversible ARR. The tailored configuration weakens σ hybridization to activate more lattice oxygen for charge compensation, while enhancing π hybridization to regulate the oxygen oxidation depth and promote oxygen redox reversibility. The reversible anionic redox reaction drives electron transfer on oxygen, thus alleviating O-O repulsion during deep desodiation and fundamentally mitigating detrimental phase transition. Benefiting from the special electronic configuration, the modified material showcases a synergetic enhancement in both specific capacity and cycling stability, exhibiting great application potential.