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The increasing demand for lithium, alongside concerns over resource scarcity and supply chain risks, has driven the need for alternative lithium sources, particularly from spent lithium-ion batteries (LIBs). Here, we introduce a redox-active crown ether copolymer designed for highly selective and electrochemically reversible lithium recovery from organic LIB leachates. A lithium-selective moiety, (12-crown-4) methyl methacrylate (12C4MA), is combined with a redox-active moiety, ferrocenylpropyl methacrylamide (FPMAm), into a redox copolymer electrosorbent to replace acid-based regeneration with electrostatic repulsion. The redox response enhances lithium ingress into the polymer, doubling lithium uptake (0. 58 mol Li /mol CrE) and enabling electrochemical regeneration upon the FPMAm oxidation. Our system exhibits exclusive lithium uptake, even in complex leachates containing competing metals (e. g. , iron, nickel, and cobalt) and organic degradants. Techno-economic analysis highlights high energy efficiency and competitive lithium pricing to the market value (∼12. 7 per kg Li). Overall, our work demonstrates a scalable, electrified adsorbent platform for sustainable and chemical-free critical metal recovery.
Kim et al. (Mon,) studied this question.