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Herein, we report an atom\u2010economical one\u2010pot tandem conversion (OTC) strategy for the rapid recovery of critical metals from spent layered oxide cathodes (i.e., LiNi\n                    <jats:sub>0.5<\/jats:sub>\n                    Co\n                    <jats:sub>0.2<\/jats:sub>\n                    Mn\n                    <jats:sub>0.3<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    ). This approach completely converts cathode powder into transition metal oxalates and a lithium\u2010rich solution in a single reactor at 80\u00a0\u00b0C within 20 min, achieving &gt; 98% recovery for Ni\/Co\/Mn and 99.4% for Li. Crucially, near\u2010quantitative (\u2248100%) utilization of stoichiometrically dosed K\n                    <jats:sub>2<\/jats:sub>\n                    SO\n                    <jats:sub>3<\/jats:sub>\n                    , ascorbic acid (AA), and oxalic acid (Ox) is confirmed by ion chromatography and pH tracking, leaving negligible reagent waste. Mechanistic investigations combining experimental evidence and theoretical calculations reveal that the OTC strategy proceeds through a uniquely orchestrated, pH\u2010modulated sequence, where the reductive activation, coordinative dissolution, and spontaneous precipitation are decoupled and activated in a sequential manner to avoid the competitive interactions that plague conventional one\u2010pot systems. The OTC strategy demonstrates broad applicability across various layered oxide cathodes, establishing a green and efficient paradigm for spent LIB recycling that significantly enhances both leaching kinetics and atom economy compared to existing hydrometallurgical routes.\n                  <\/jats:p>","DOI":"10.1002\/anie.4600564","type":"journal-article","created":{"date-parts":[[2026,6,4]],"date-time":"2026-06-04T16:17:24Z","timestamp":1780589844000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["One\u2010Pot Tandem Conversion Strategy Enables Atom\u2010Economical Recovery of Spent Layered Oxide Cathodes"],"prefix":"10.1002","volume":"65","author":[{"given":"Xinlei","family":"Zhang","sequence":"first","affiliation":[{"name":"Faculty of Materials Science and Chemistry China University of Geosciences  Wuhan 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