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Diverse reducing agents for Li supplements, such as quinone molecules, have been considered to homogenize the Li distribution in the cathode materials obtained after cycling; however, the detailed reaction mechanism is still unknown. Herein, the ideal electrochemical potential factor and reaction mechanism of the redox mediator 3,5\u2010di\u2010tert\u2010butyl\u2010o\u2010benzoquinone (DTBQ) for the chemical relithiation of high\u2010Ni\u2010layered cathodes are elucidated. Here, 100% efficiency of DTBQ\u2010assisted chemical relithiation is achieved by adjusting the direct immersion time of Li\u2010deficient cathode electrodes. The reversible reaction features of the physical and chemical structures of both the regenerated cathodes and the DTBQ molecules are investigated using advanced characterization and density functional theory calculations. These findings emphasize the potential of redox\u2010mediator\u2010assisted chemical relithiation for realizing direct recycling processes and offer a facile and sustainable solution for battery recycling.<\/jats:p>","DOI":"10.1002\/advs.202417094","type":"journal-article","created":{"date-parts":[[2025,1,22]],"date-time":"2025-01-22T08:25:31Z","timestamp":1737534331000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":19,"title":["Unraveling Redox Mediator\u2010Assisted Chemical Relithiation Mechanism for Direct Recycling of Spent Ni\u2010Rich Layered Cathode Materials"],"prefix":"10.1002","volume":"12","author":[{"given":"Suji","family":"Kim","sequence":"first","affiliation":[{"name":"Department of Chemical and Biological Engineering Sookmyung Women's University  100 Cheongpa\u2010ro 47\u2010gil, Yongsan\u2010gu Seoul 04310 Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ukseon","family":"Shin","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering Korea Advanced Institute of Science and Technology (KAIST)  291 Daehak\u2010ro Daejeon 34141 Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hyun Ju","family":"Yoon","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biological Engineering Sookmyung Women's University  100 Cheongpa\u2010ro 47\u2010gil, Yongsan\u2010gu Seoul 04310 Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Soo\u2010Ah","family":"Yoon","sequence":"additional","affiliation":[{"name":"Department of Energy &amp; Materials Engineering Dongguk University  Seoul 04620 Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jinju","family":"Song","sequence":"additional","affiliation":[{"name":"Gwangju Clean Energy Research Center Korea Institute of Energy Research (KIER)  270\u201025 Samso\u2010ro Gwangju 61003 Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiyoung","family":"Ma","sequence":"additional","affiliation":[{"name":"Gwangju Clean Energy Research Center Korea Institute of Energy Research (KIER)  270\u201025 Samso\u2010ro Gwangju 61003 Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jung\u2010Je","family":"Woo","sequence":"additional","affiliation":[{"name":"Gwangju Clean Energy Research Center Korea Institute of Energy Research (KIER)  270\u201025 Samso\u2010ro Gwangju 61003 Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kyung\u2010Wan","family":"Nam","sequence":"additional","affiliation":[{"name":"Department of Energy &amp; 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