Graphite-Mediated Selective Li Recovery from Spent Ternary Cathodes toward Battery-Grade Li ₂ CO ₃

Conventional recycling of spent cathode materials typically involves complete dissolution, prioritizing the recovery of Ni, Co, and Mn while leaving Li extraction to the final step. This approach results in low Li recovery and significant resource loss. Here, we report a short, high-efficiency process for selective Li extraction. Graphite anode reduction coupled with CO2-assisted pyrolysis enables simultaneous reduction of cathode oxides and release of Li2O, which reacts with CO2 to form Li2CO3. Meanwhile, transition metals (Ni, Co, Mn) convert into insoluble metals or low-valent oxides, disrupting the layered structure. Systematic investigation of graphite reduction and Li carbonization-water leaching identifies a streamlined pathway for efficient Li recovery. Under optimized conditions (graphite 40%, 750 °C, 4 h roasting, liquid–solid ratio 15 mL g–1, 2 h leaching, CO2 300 mL min–1), Li leaching reaches 95.57%, yielding 99.61% pure battery-grade Li2CO3. The regenerated Li2CO3 enables cathode resynthesis with electrochemical performance comparable to commercial materials. This work demonstrates a sustainable, closed-loop strategy for battery recycling with high Li recovery efficiency.