Selective and Closed-Loop Recycling of Different Metals from Spent Lithium-Ion Batteries Through Phosphoric Acid Leaching: Parameter Optimization and Regulation of Reaction Kinetics

Abstract

The sustainable recycling of valuable metals from spent lithium-ion batteries (LIBs) is critical for resource conservation and environmental protection but remains challenging due to the complex coexistence of target and impurity metals. This study systematically investigates the selective leaching behaviors of metals (Co, Li, Cu, Fe, Al) in phosphoric acid media, revealing that lithium could be preferentially extracted in mild acidic conditions (0.8 mol/L H3PO4), while complete dissolution of both Li and Co was achieved in concentrated acid (2.0 mol/L H3PO4). Kinetic analysis demonstrated that metal leaching followed a chemically controlled mechanism, with distinct extraction sequences: Li > Cu~Co > Fe > Al in dilute acid and Cu > Al~Li > Fe > Co in concentrated acid. Furthermore, we developed a closed-loop process wherein oxalic acid simultaneously precipitates Co/Li while regenerating H3PO4, enabling acid reuse with minimal efficiency loss during cyclic leaching. These findings establish a single-step phosphoric acid leaching strategy for selective metal recovery, governed by tunable acid concentration and reaction kinetics, offering a sustainable pathway for LIBs recycling.