Redox‐Ligand‐Coupled Chemical Reprogramming of Battery Waste Into Metal–Organic Electrodes for Closed‐Loop Energy Storage

ABSTRACT

Sustainable battery waste management requires moving beyond element recovery toward full‐component reutilization. Here, we report a redox‐ligand‐coupled chemical reprogramming strategy that transforms chemically distinct components of battery waste into functional energy storage materials. Using LiCoO ₂ and polyethylene terephthalate (PET) as a model system, terephthalate and ethylene glycol generated from PET depolymerization act synergistically as coordinating ligands, proton sources, and reductants, enabling the dissolution of cathode materials and their in situ reconstruction into a redox‐active metal–organic framework (cobalt terephthalate, CoTPA) under hydrothermal conditions without external leaching agents or reductants. This self‐reinforcing reaction network couples polymer depolymerization with cathode deconstruction, eliminating external reagents and complex separation processes. The resulting CoTPA anode delivers a reversible capacity of ≈1170 mAh g ⁻¹ at 0.1 A g ⁻¹ , and retains 92.1% of its initial capacity after 500 cycles at 1 A g ⁻¹ . When integrated with regenerated graphite (RG), CoTPA enables a battery‐level closed‐loop dual‐ion battery (DIB) with an energy density of 304 Wh kg ⁻¹ (based on total active material mass). The strategy is extended to layered oxide cathodes and diverse PET sources. Beyond conventional recycling, this work establishes a chemistry‐driven paradigm that reprograms waste components into value‐added functional materials, offering a scalable pathway toward circular energy storage.