Electrochemistry‐Driven Complete Reconstruction of Spent Lithium–Ion Battery Cathodes for Matter Recycling

The rapid expansion of lithium–ion batteries (LIBs) applications has created urgent recycling challenges. To tackle these issues, this study proposes a novel electrochemistry‐driven complete reconstruction (EDCR) strategy for effective recycling of cathode materials. The well‐designed electrochemical cell is based on a used aluminum foil anode and spent cathodes in a tamed chloroaluminate molten salt electrolyte. During the discharge process, the spent cathodes undergo a reduction reaction, converting high‐valence transition metals into their elemental forms. After deep discharge, the spent LiCoO 2 cathode completely decomposes into Co, LiCl, and Al 2 O 3 . Subsequent treatment involving washing and calcination produces a pure LiCl solution and a mixed solid of Co 3 O 4 and Al 2 O 3 , which can be used to synthesize new cathode materials directly. Experimental results demonstrate the versatility of this method, achieving high recovery rates for LiCoO 2 , ternary cathodes (including NCM811 and NCA), as well as lithium–iron phosphate (LiFePO 4 ). When compared to traditional pyrometallurgical and hydrometallurgical methods, the EDCR strategy notably lowers energy consumption by 23% and reduces greenhouse gas emissions, all while ensuring a streamlined workflow, reduced operational costs, and a competitive profit margin of $1.96 per kilogram of batteries processed. This work paves the way for a sustainable closed‐loop LIB resource recovery.