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Role of Ligand-to-Metal Charge Transfer in Anionic Redox Activity of the Layered Oxide Cathode for Na-Ion Batteries Abhinanda Sengupta (13249672) Amreen Bano (10324392) Kritika Thapliyal (25156983) Aakash Ahuja (8900993) Sri Harsha Akella (11835852) Malachi Noked (1300647) Dan T. Major (1484047) Sagar Mitra (1551556) Biophysics Biochemistry Medicine Microbiology Genetics Molecular Biology Neuroscience Evolutionary Biology Environmental Sciences not elsewhere classified Chemical Sciences not elsewhere classified Biological Sciences not elsewhere classified Developmental Biology Hematology synergistic redox landscape offering critical insights anionic redox process anionic redox activity rich layered oxides preventing oxygen undercoordination oxidized oxygen states ex situ </ design strategy enables 6 mah g strategic ru doping ru dopant stabilizes layered oxide cathode metal charge transfer performance cathode materials high discharge capacity metal charge capacity cathode oxygen holes rational design operando </ 6 v capacity retention layered na ∼ 93 type framework theoretical calculations structural integrity sibs ). scale sodium reversible formation material delivers ion batteries generation sibs fukui functions electronically stabilizing average voltage advancing grid advanced characterizations 1000 cycles Developing high-performance cathode materials is crucial for advancing grid-scale sodium-ion batteries (SIBs). Here, we introduce a P2-type layered oxide cathode material, Na_0·67Ni_0·33Mn_0·51Ru_0·16O₂, which demonstrates exceptional electrochemical performance through a robust dual cationic–anionic redox mechanism. This material delivers a high discharge capacity of 175.6 mAh g⁻¹ at an average voltage of 3.6 V and maintains remarkable cycling stability with ∼93% capacity retention after 1000 cycles. A key to this performance is the strategic Ru doping, which plays a pivotal role in electronically stabilizing the oxidized oxygen states. By mediating the reversible formation of oxygen holes and preventing oxygen undercoordination, the Ru dopant stabilizes the anionic redox process. Unlike Na-rich layered oxides, this ligand-to-metal charge-transfer mechanism effectively suppresses detrimental oxygen evolution and preserves the structural integrity of the layered Na-deficient P2-type framework. This design strategy enables a synergistic redox landscape, confirmed by <i>ex situ</i> and <i>operando</i> advanced characterizations and theoretical calculations such as Fukui functions, offering critical insights into the rational design of high-capacity cathode for next-generation SIBs. 2026-10-01T00:00:00Z Text Journal contribution 10.1021/acs.chemmater.6c00365.s001 https://figshare.com/articles/journal_contribution/Role_of_Ligand-to-Metal_Charge_Transfer_in_Anionic_Redox_Activity_of_the_Layered_Oxide_Cathode_for_Na-Ion_Batteries/34046331 CC BY-NC 4.0