Water Radiolysis Enables CO₂-Activated Radical Recycling of Spent Lithium-Ion Cathodes

Conventional recycling of spent lithium-ion batteries (LIBs) relies on energy-intensive and complex processes that hinder sustainability. Here, we report a mild, efficient recycling strategy using programmable water radiolysis with CO₂ to establish an aqueous reductive radical platform. This radiolytic approach enables simultaneous cathode peeling, metal leaching, and component separation under ambient conditions, which is inaccessible to existing methods. Within minutes, high-dose-rate irradiation degrades the polymeric binder, enabling ∼99.5% active material recovery. Radiolytically generated CO₂ ^•- radicals reduce and leach transition metals (Co, Ni, Mn) and lithium with >96% efficiency. The dynamic pH evolution during irradiation precipitates transition metals in situ as carbonates while retaining Li⁺ in solution, accomplishing one-step separation. Regenerated cathodes deliver electrochemical performance comparable to commercial benchmarks. Techno-economic analysis indicates this CO₂-mediated radiolytic pathway offers a more sustainable, energy-efficient, and cost-effective route for battery recycling.