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However, severe Li\u2212Ni antisite defects and their undetermined dynamic evolutions during high\u2010voltage cycling limit the further development of these ultrahigh\u2010Ni cathodes. In this study, we quantify the dynamic evolutions of the Li\u2212Ni antisite defect using operando neutron diffraction and reveal its coupling relationship with anionic redox, another critical challenge restricting ultrahigh\u2010Ni cathodes. We detect a clear Ni migration coupled with an unstable oxygen lattice, which accompanies the oxidation of oxygen anions at high voltages. Based on these findings, we propose that minimized Li\u2212Ni antisite defects and controlled Ni migrations are essential for achieving stable high\u2010voltage cycling structures in ultrahigh\u2010Ni cathodes. This is further demonstrated by the optimized ultrahigh\u2010Ni cathode, where reduced dynamic evolutions of the Li\u2212Ni antisite defect effectively inhibit the anionic redox, enhancing the 4.5\u2005V cycling stability.<\/jats:p>","DOI":"10.1002\/anie.202410326","type":"journal-article","created":{"date-parts":[[2024,7,26]],"date-time":"2024-07-26T05:31:10Z","timestamp":1721971870000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":26,"title":["Dynamic Evolution of Antisite Defect and Coupling Anionic Redox in High\u2010Voltage Ultrahigh\u2010Ni Cathode"],"prefix":"10.1002","author":[{"given":"Kang","family":"Wu","sequence":"first","affiliation":[{"name":"Songshan Lake Materials Laboratory  Dongguan 523808 China"},{"name":"Beijing National Laboratory for Condensed Matter Physics, Institute of Physics Chinese Academy of Sciences  Beijing 100190 China"},{"name":"College of Chemical Engineering and Safety Shandong university of aeronautics  Binzhou, Shandong 256600 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Peilin","family":"Ran","sequence":"additional","affiliation":[{"name":"Songshan Lake Materials Laboratory  Dongguan 523808 China"},{"name":"Beijing National Laboratory for Condensed Matter Physics, Institute of Physics Chinese Academy of Sciences  Beijing 100190 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wen","family":"Yin","sequence":"additional","affiliation":[{"name":"Spallation Neutron Source Science Center  Dongguan 523803, Guangdong China"},{"name":"Institute of High Energy Physics Chinese Academy of Sciences  Beijing 100049 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lunhua","family":"He","sequence":"additional","affiliation":[{"name":"Songshan Lake Materials Laboratory  Dongguan 523808 China"},{"name":"Beijing National Laboratory for Condensed Matter Physics, Institute of Physics Chinese Academy of Sciences  Beijing 100190 China"},{"name":"Spallation Neutron Source Science Center  Dongguan 523803, Guangdong China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Baotian","family":"Wang","sequence":"additional","affiliation":[{"name":"Spallation Neutron Source Science Center  Dongguan 523803, Guangdong China"},{"name":"Institute of High Energy Physics Chinese Academy of Sciences  Beijing 100049 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fangwei","family":"Wang","sequence":"additional","affiliation":[{"name":"Songshan Lake Materials Laboratory  Dongguan 523808 China"},{"name":"Beijing National Laboratory for Condensed Matter Physics, Institute of Physics Chinese Academy of Sciences  Beijing 100190 China"},{"name":"Spallation Neutron Source Science Center  Dongguan 523803, Guangdong China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4170-7427","authenticated-orcid":false,"given":"Enyue","family":"Zhao","sequence":"additional","affiliation":[{"name":"Songshan Lake Materials Laboratory  Dongguan 523808 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jinkui","family":"Zhao","sequence":"additional","affiliation":[{"name":"Songshan Lake Materials Laboratory  Dongguan 523808 China"},{"name":"Beijing National Laboratory for Condensed Matter Physics, Institute of Physics Chinese Academy of Sciences  Beijing 100190 China"},{"name":"School of Physical Sciences Great Bay University  Dongguan 523808 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2024,9,13]]},"reference":[{"key":"e_1_2_7_1_1","unstructured":"\u00a0"},{"key":"e_1_2_7_2_2","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.abm6624"},{"key":"e_1_2_7_3_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41560-023-01355-z"},{"key":"e_1_2_7_4_2","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.2c13151"},{"key":"e_1_2_7_5_2","doi-asserted-by":"publisher","DOI":"10.1002\/advs.202304425"},{"key":"e_1_2_7_6_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41586-024-07045-4"},{"key":"e_1_2_7_7_2","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.ado4472"},{"key":"e_1_2_7_8_1","unstructured":"\u00a0"},{"key":"e_1_2_7_9_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202307243"},{"key":"e_1_2_7_10_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-023-43792-0"},{"key":"e_1_2_7_11_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202216155"},{"key":"e_1_2_7_12_2","doi-asserted-by":"publisher","DOI":"10.1002\/smll.202106719"},{"key":"e_1_2_7_13_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.jpowsour.2022.231035"},{"key":"e_1_2_7_14_1","unstructured":"\u00a0"},{"key":"e_1_2_7_15_2","author":"Lee S.","year":"2024","journal-title":"Adv. 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