• A novel two-step chlorination roasting process achieves simultaneous recovery of Li and Co from spent LiCoO2 with leaching efficiencies of 99.43% and 99.05%, respectively.
• The activation energy for the chlorination reaction is 88.41 kJ/mol, with a kinetic model transition from first-order (F1) to second-order (F2) at a conversion rate of 0.5.
• Optimal conditions are low temperature (400°C), short time (20 min), and NH4Cl/LiCoO2 mass ratio of 3:1, offering energy-efficient and environmentally friendly recycling.
• The technology provides a crystal-structure-based mechanism, enabling high recovery efficiency and high added value, supporting the circular economy for LIBs.
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