Effective recycling of spent lithium-ion batteries via radiolytic radical reactions

The rapidly growing volume of spent lithium-ion batteries (LIBs) poses an urgent recycling challenge, as conventional pyro-/hydro-metallurgical methods remain inefficient and require harsh operating conditions. Herein, we develop an efficient, pilot-scale radiation-driven leaching strategy for processing kilogram quantities of spent ternary cathode material dispersed in aqueous citric acid. In minutes, ambient and controllable electron beam irradiation achieves near-complete (>99%) leaching of valuable transition metals and lithium. Mechanistic studies reveal that the hydrated electrons and citric acid-derived radicals generated jointly during water radiolysis drive rapid cathode amorphization by reducing high-valence metal centers and cleaving metal-oxygen bonds. Concurrently, direct irradiation induces lattice defects and oxygen vacancies, synergistically enhancing amorphization and strengthening radical-metal site coupling, thereby accelerating dissolution. Furthermore, the leachate is repurposed into effective cathode materials and oxygen evolution reaction catalysts, enabling an economically viable closed-loop recycling process. Energy efficiency and techno-economic analyses indicate that industrial-scale radiation technology offers a practical solution for scalable spent LIB recycling. The study presents a radiation-based method that rapidly recovers valuable metals from spent lithium-ion batteries under mild conditions and converts them into new battery materials and catalysts, supporting scalable closed-loop recycling.