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Notably, the physicochemical properties of component elements fundamentally determine the material structure of cathodes. Herein, a diffusion\u2010controlled incubation mechanism of intragranular cracking is unraveled, and an underlying correlation model with Co element is established. Multi\u2010dimensional analysis reveals that oxygen vacancies appear due to the charge compensation from highly oxidizing Co ions in the deeply charged state, driving the transition metal migration to Li layer and layered to rock\u2010salt phase transition. The local accumulation of two accompanying tensile strains collaborates to promote the nucleation and growth of intragranular cracks along the fragile rock\u2010salt phase domain on (003) plane. This study focuses on the potential risks posed by Co to the architectural and thermal stability of Ni\u2010rich cathodes and is dedicated to the compositional design and performance optimization of Ni\u2010rich cathodes.<\/jats:p>","DOI":"10.1002\/smll.202310321","type":"journal-article","created":{"date-parts":[[2024,1,5]],"date-time":"2024-01-05T11:56:50Z","timestamp":1704455810000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":30,"title":["Oxygen Vacancies Driven by Co in the Deeply Charged State Inducing Intragranular Cracking of Ni\u2010Rich Cathodes"],"prefix":"10.1002","volume":"20","author":[{"given":"Fuqiren","family":"Guo","sequence":"first","affiliation":[{"name":"School of Chemical Engineering Sichuan University  Chengdu 610065 P. R. 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