Cathode and Plastic Corecycling from Spent Batteries via Paired Electrolysis

The escalating production of lithium-ion batteries (LIBs) poses serious challenges to metal resources sustainability and ecological environment stability, making the recycling of spent LIBs urgent. However, existing recycling methods suffer from high pollution and significant energy/chemical consumption and only focus on cathode metals while neglecting nonmetallic components like plastics, which account for approximately 10.9% of the battery’s weight. Here, we present a paired electrolysis corecycling (ECO) strategy that simultaneously recovers both critical metals and polymeric materials from spent LIBs. This method combines the electrochemical reduction of the cathode materials with the oxidative degradation of plastics, and the oxidation of plastic serves as a proton source, assisting complete metal extraction while reducing acid consumption, thereby enabling sustainable corecycling of both metals and plastics. Using lithium cobalt oxide (LCO) and polyethylene terephthalate (PET) as a proof of concept, we demonstrate near-complete metal recovery (∼100%) and the successful upcycling of plastics into valuable chemical products, such as potassium diformate and terephthalic acid. Compared to conventional electrochemical methods, the ECO strategy reduces cell voltage by ∼510 mV, achieving an energy-saving rate of 35%. And recycling one ton of spent batteries with this method generates a net revenue of $ 813.20, surpassing pyrometallurgy ($ 245.60), hydrometallurgy ($ 327.70), and conventional electrochemical methods ($ 709.60). It also decreases CO2 emissions by 1.10–2.80 tons. This corecycling strategy, applicable across various cathode chemistries, provides a scalable, economically viable, and environmentally sustainable solution for LIB recycling and beyond.