In-situ thermal reduction is a promising technology that realizes the reduction of high-valence metals in spent lithium-ion batteries (LIBs) through its reductive substances. However, the subsequent simple acid leaching cannot adapt to all thermal reduction products, especially elemental Ni and Co, resulting in low leaching efficiency and high acid consumption. In this work, in-situ thermal reduction combined with electrochemical-enhanced leaching technology was provided for extracting valuable metals from spent LIBs with minimum chemical consumption. Results show that after thermal reduction, the layered structure of LiNi1/3Co1/3Mn1/3O2 was fully broken, yielding acid-soluble components including Ni, Co, NiO, CoO, MnO, Li2CO3, and LiAlO2, all achieved without external reductants. During the electrochemical leaching, the acidic solution produced by water electrolysis and electrochemical oxidation synergistically promoted the leaching of valuable metals, and finally, 99.02 % Li, 96.34 % Ni, 98.28 % Co and 99.24 % Mn were leached from the roasted cathode product. Compared with traditional acid leaching, the proposed electrochemical method has advantages in the dissolution of elemental Ni and Co. Moreover, the whole process does not consume any external acids or bases, and there is no emission of waste acid. The findings of this work help to reduce reagent consumption in the spent LIBs recycling process and provide an effective, adaptable, and green method for leaching thermal reduction products.
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