Coordination Chemistry‐Driven One‐Step Selective Leaching‐Precipitation Strategy With Concomitant Fluorine Doping for Closed‐Loop Spent Cathode Regeneration

ABSTRACT The rapidly growing deployment of lithium (Li)‐ion batteries in electric vehicles has intensified the demand for efficient recycling of end‐of‐life cathode materials. However, existing recycling and regeneration strategies struggle to recover value from deeply degraded cathodes with severe structural disorder. Herein, we present a mechanism‐driven one‐step selective leaching‐precipitation strategy for spent cathodes, guided by coordination chemistry. Bidentate oxalate ligands selectively chelate transition metal (TM) ions to form an atomically homogeneous mixed TM oxalate precursor, while Li + remains soluble, enabling highly selective Li extraction with a selectivity of 99.23%. Residual fluoride species generated from binder pyrolysis are retained and utilized for in situ solid‐state fluorine doping during regeneration, which effectively suppresses cation disorder with a Li/Ni mixing to 1.4% and stabilizes the layered structure. This coordination chemistry‐enabled regeneration strategy points toward a new paradigm for upcycling deeply degraded cathode waste into structurally stable high‐performance materials, laying the foundation for scalable battery recycling technology.