Revealing Gliding-Induced\nStructural Distortion in\nHigh-Nickel Layered Oxide Cathodes for Lithium-Ion Batteries

After charging to a high state-of-charge (SoC), layered\noxide cathodes\nexhibit high capacities but suffer from gliding-induced structural\ndistortions caused by deep Li depletion within alkali metal (AM) layers,\nespecially for high-nickel candidates. In this study, we identify\nthe essential structure of the detrimental H3 phase formed at high\nSoC to be an intergrowth structure characterized by random sequences\nof the O3 and O1 slabs, where the O3 slabs represent Li-rich layers\nand the O1 slabs denote Li-depleted (or empty) layers that glide from\nthe O3 slabs. Moreover, we adopt two doping strategies targeting different\ndoping sites to eliminate the formation of Li-vacant O1 slabs. First,\nwe introduce direct transition metal (TM) pillars between TMO<sub>2</sub> slabs achieved through dopants (e.g., Nb) positioned within\nAM layers, significantly improving the cycling stability. Second,\nwe introduce indirect Li pillars achieved through dopants located\nat TM layers to adjust the Li–O bond strength. While this strategy\ncan regulate the uniformity of Li at the slab level, it results in\nan uneven Li distribution at the particle scale, ultimately failing\nto enhance the electrochemical performance. Our established research\nstrategy facilitates the realization of diverse pillars between TMO<sub>2</sub> slabs through doping, thereby offering guidance for stabilizing\nhigh-capacity layered oxide cathodes at high SoC.