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The structure instability issues of the highly delithiated LiCoO2 have significantly hindered its high‐voltage applications (≥4.55 V vs Li/Li+). Herein, for the first time, multiple modifications of Li0.9Mg0.05CoO2 (L0.9M0.05CO) via a simple one‐step sintering synthesis are reported. A combination of the bulk Li/Co antisites, a Mg‐pillar enriched surface, and a thin MgO coating layer is achieved...
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