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While eutectic molten salt systems have emerged as a promising liquid\u2013solid medium for direct regeneration, the selection of salts has been largely empirical, and the critical role of anions in governing the relithiation efficacy and interface chemistry remains underappreciated. Herein, we demonstrate that the strategic choice of anions in a binary molten salt flux is paramount to achieving structural repair and performance enhancement. We identify that anions with high adsorption energy to the CoO\n                    <jats:sub>6<\/jats:sub>\n                    slabs and low dissociation energy for Li\n                    <jats:sup>+<\/jats:sup>\n                    , such as Cl\n                    <jats:sup>\u2212<\/jats:sup>\n                    , are optimal. This anion\u2010mediated process directs a preferential crystallographic reconstruction along the\n                    <jats:italic>c<\/jats:italic>\n                    \u2010axis and fosters the development of a Li\u2212O enriched, (104)\u2010facetted surface. Consequently, the upcycled LCO cathode retained over 95% of its original capacity after 1000 cycles at 4.2\u00a0V. Even at an elevated voltage of 4.6\u00a0V, the upcycled LCO retains 85.5% of its capacity after 100 cycles at 0.5 C. This work underscores that understanding and engineering the anion in molten salts could be a powerful step toward the rational design of advanced upcycling protocols.\n                  <\/jats:p>","DOI":"10.1002\/advs.77656","type":"journal-article","created":{"date-parts":[[2026,9,27]],"date-time":"2026-09-27T18:00:31Z","timestamp":1790532031000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Anion\u2010Driven Surface Reconstruction Enables Direct Regeneration of LiCoO\n                    <sub>2<\/sub>\n                    Cathode Material"],"prefix":"10.1002","author":[{"given":"Mengting","family":"Zheng","sequence":"first","affiliation":[{"name":"College of Chemical and Biological Engineering Zhejiang University  Hangzhou China"},{"name":"Centre For Clean Environment and Energy School of Environment and Science Gold Coast Campus Griffith University  Gold Coast Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shangshu","family":"Qian","sequence":"additional","affiliation":[{"name":"College of Chemical and Biological Engineering Zhejiang University  Hangzhou China"},{"name":"Centre For Clean Environment and Energy School of Environment and Science Gold Coast Campus Griffith University  Gold Coast Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Meng","family":"Li","sequence":"additional","affiliation":[{"name":"Institute For Sustainable Transformation School of Chemical Engineering and Light Industry Guangdong University of Technology  Guangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5192-1844","authenticated-orcid":false,"given":"Shanqing","family":"Zhang","sequence":"additional","affiliation":[{"name":"Centre For Clean Environment and Energy School of Environment and Science Gold Coast Campus Griffith University  Gold Coast 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