A Design Strategy for Durable Anionic Redox via Fluorine-Induced Electronic Structure Modulation in In Situ Formed Disordered Phases.
basic_science · Level V
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- Record sourced from PubMed, PMID 41645879.
- Also identified by DOI 10.1002/adma.202518963.
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Abstract
Disordered cathode materials are attractive candidates for next-generation lithium-ion batteries (LIBs), but the intrinsic instability of anionic redox hinders their commercialization. Unlike conventional Li-excess disordered systems limited by compositional constraints of Li<sub>1+x</sub>M<sub>1-x</sub>O<sub>2</sub>, Immm-Li<sub>2</sub>NiO<sub>2</sub> offers a platform to access highly lithiated chemistries that enable in situ disorder formation during electrochemical cycling. This allows lattice O to contribute to charge compensation; however, O<sub>2</sub> release at high voltages compromises reversibility and cycling stability. To address this, fluorination generates a quadrupolar Li-O-M-F configuration that lowers the Li─O─Li band energy level and delays the onset of anionic redox. This electronic structure modification suppresses O<sub>2</sub> evolution, enhances structural stability, and improves cycling performance. By coupling electrochemically induced disorder with stabilization through Li-O-M-F units, this work establishes a new framework for engineering durable, high-capacity cathodes, offering a blueprint for material design strategies that transcend stoichiometric restrictions and unlock stable anion redox functionality.