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The role of crystallographic defects on structure evolution and performance degradation during electrochemical cycling is not yet fully understood. Here, we investigated the structural evolution of a Ni\u2010rich NMC cathode in a solid\u2010state cell by in\u2005situ transmission electron microscopy. Antiphase boundary (APB) and twin boundary (TB) separating layered phases played an important role on phase change. Upon Li depletion, the APB extended across the layered structure, while Li\/transition metal (TM) ion mixing in the layered phases was detected to induce the rock\u2010salt phase formation along the coherent TB. According to DFT calculations, Li\/TM mixing and phase transition were aided by the low diffusion barriers of TM ions at planar defects. This work reveals the dynamical scenario of secondary phase evolution, helping unveil the origin of performance fading in Ni\u2010rich NMC.\n                  <\/jats:p>","DOI":"10.1002\/anie.202008144","type":"journal-article","created":{"date-parts":[[2020,8,2]],"date-time":"2020-08-02T22:19:24Z","timestamp":1596406764000},"page":"22092-22099","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":157,"title":["Direct Observation of Defect\u2010Aided Structural Evolution in a Nickel\u2010Rich Layered Cathode"],"prefix":"10.1002","volume":"59","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-1141-8827","authenticated-orcid":false,"given":"Shuang","family":"Li","sequence":"first","affiliation":[{"name":"Key Laboratory of Carbon Materials of Zhejiang Province Institute of New Materials and Industrial Technologies Wenzhou University  Wenzhou Zhejiang 325027 China"},{"name":"Department of Chemical Engineering University of Waterloo  Waterloo Ontario N2L 3G1 Canada"},{"name":"Center for Functional Nanomaterials Brookhaven National Laboratory  Upton NY 11973 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8286-8257","authenticated-orcid":false,"given":"Zhenpeng","family":"Yao","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Chemical Biology Harvard University  12 Oxford Street Cambridge MA 02138 USA"},{"name":"Department of Chemistry and Department of Computer Science University of Toronto  Toronto Ontario M5S 3H6 Canada"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jianming","family":"Zheng","sequence":"additional","affiliation":[{"name":"Energy and Environment Directorate Pacific Northwest National Laboratory  902 Battelle Boulevard Richland WA 99352 USA"},{"name":"College of Chemistry and Chemical Engineering Xiamen University  Xiamen Fujian 361005 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