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Recently, direct regeneration has emerged as a novel recycling strategy but fails to repair the irreversible morphology and structure damage of the highly degraded polycrystalline layered oxide materials. Here, this work carries out a solid\u2010state upcycling study for the severely cracked LiNi\n                    <jats:sub>1\u2010x\u2010y<\/jats:sub>\n                    Co\n                    <jats:sub>x<\/jats:sub>\n                    Mn\n                    <jats:sub>y<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    cathodes. The specific single\u2010crystallization process during calcination is investigated and the surface rock salt phase is recognized as the intrinsic obstacle to the crystal growth of the degraded cathodes due to sluggish diffusion in the heterogeneous grain boundary. Accordingly, this work revives the fatigue rock salt phase by restoring a layered surface and successfully reshapes severely broken cathodes into the high\u2010performance single\u2010crystalline particles. Benefiting from morphological and structural integrity, the upcycled single\u2010crystalline cathode materials exhibit an enhanced capacity retention rate of 93.5% after 150 cycles at 1C compared with 61.7% of the regenerated polycrystalline materials. The performance is also beyond that of the commercial cathodes even under a high cut\u2010off voltage (4.5\u00a0V) or high operating temperature (45\u00a0\u00b0C). This work provides scientific insights for the upcycling of the highly degraded cathodes in spent LIBs.\n                  <\/jats:p>","DOI":"10.1002\/adma.202405238","type":"journal-article","created":{"date-parts":[[2024,6,25]],"date-time":"2024-06-25T09:40:55Z","timestamp":1719308455000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":75,"title":["Reviving Fatigue Surface for Solid\u2010State Upcycling of Highly Degraded Polycrystalline LiNi\n                    <sub>1\u2010x\u2010y<\/sub>\n                    Co\n                    <sub>x<\/sub>\n                    Mn\n                    <sub>y<\/sub>\n                    O\n                    <sub>2<\/sub>\n                    Cathodes"],"prefix":"10.1002","volume":"36","author":[{"given":"Min","family":"Fan","sequence":"first","affiliation":[{"name":"CAS Key Laboratory of Molecular Nanostructure and Nanotechnology Beijing National Laboratory for Molecular Sciences (BNLMS) Institute of Chemistry Chinese Academy of Sciences  Beijing 100190 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xin\u2010Hai","family":"Meng","sequence":"additional","affiliation":[{"name":"CAS Key Laboratory of Molecular Nanostructure and Nanotechnology Beijing National Laboratory for Molecular Sciences (BNLMS) Institute of Chemistry Chinese Academy of Sciences  Beijing 100190 P. R. China"},{"name":"University of Chinese Academy of Sciences  Beijing 100049 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hua","family":"Guo","sequence":"additional","affiliation":[{"name":"CAS Key Laboratory of Molecular Nanostructure and Nanotechnology Beijing National Laboratory for Molecular Sciences (BNLMS) Institute of Chemistry Chinese Academy of Sciences  Beijing 100190 P. R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ke\u2010Cheng","family":"Jiang","sequence":"additional","affiliation":[{"name":"Jiangsu Zenergy Battery Technologies Co., Ltd  Suzhou 215558 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ji\u2010Cheng","family":"Chen","sequence":"additional","affiliation":[{"name":"Jiangsu Zenergy Battery Technologies Co., Ltd  Suzhou 215558 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qinghai","family":"Meng","sequence":"additional","affiliation":[{"name":"CAS Key Laboratory of Molecular Nanostructure and Nanotechnology Beijing National Laboratory for Molecular Sciences (BNLMS) Institute of Chemistry Chinese Academy of Sciences  Beijing 100190 P. R. 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