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Energies 2022, 15, 1611 18 of 23 Although the direct regeneration process is relatively simple, impurities and damaged structures in the spent cathode material can affect the electrochemical performance of the resynthesized material [91]. 6.2. Electrochemical Methods Electrochemical methods are often used in the recycling of spent LIBs. Chu et al. [92] used aluminum foil and electrode active material obtained from spent LIBs as the anode and sulfuric acid solution as the electrolyte, and electrolysis resulted in complete separation of the aluminum foil and electrode active material. Copper enters the electrolyte as an impurity and is electrodeposited on the cathode, Ni, Co, and Mn remain undissolved in the active material, and Al is insoluble in the solution, where LiCO3 can be collected at high purity and enriched to a certain extent to be recycled. Meng et al. [93] investigated the leaching of LCO generated from spent LIBs by electrochemical cathodic reduction. A possible control mechanism for the leaching of cobalt from spent LCO is determined through thermodynamic, kinetic, and electrochemical impedance spectroscopy. When the malic acid concentration was 1.25 mol/L, the working voltage was 8 V, the temperature was 70 ◦C, and the time was 180 min, the leaching rate of cobalt is approximately 90%, and the leaching rate of lithium is approximately 94%. To save energy, some researchers have used a two-chamber electrolysis system. Lv et al. [94] used a hydrogen peroxide sulfate system to leach spent LIBs. Using 304 stainless-steel plates as cathodes and platinum or lead plates as anodes, the two chambers are separated by an anion exchange membrane, with the leaching solution as the cathode solution and (NH4)2SO4 as the anode solution. Electrolysis in a constructed two-chamber electrochemical reactor yields cobalt metal (>99% purity) and Li2CO3, with the simultaneous synthesis of sulfate. 7. Conclusions: Future Perspective of the Research As the mineral resources on earth are limited, the demand for mineral resources is growing rapidly with economic development, which will lead to a shortage of min- eral resources and soaring prices. The valuable metal content in spent LIBs is higher than the concentration in natural ores, and it is a good choice to replace natural ores as a high-concentration mineral source. At the same time, spent LIBs that are not treated and dis- carded can cause serious environmental safety problems. Thus, the recycling of used LIBs is imperative whether from the perspective of resource recovery or environmental protection. Among the existing methods to recover valuable metals from lithium batteries, py- rometallurgy is highly energy-intensive, generates large amounts of spent gas and slag, and can only produce alloy intermediate products with low recovery efficiency. Hydromet- allurgy requires large amounts of acids, such as hydrochloric acid (HCl), sulfuric acid (H2SO4), nitric acid (HNO3), phosphoric acid (H3PO4), formic acid (HCOOH), malic acid, ascorbic acid, lemon juice, citric acid, and iminodiacetic acid. Leaching with HCl may produce chlorine gas and leaching with HNO3 may produce NOx. Moreover, the separa- tion and purification steps of the resulting solution are tedious, and the solvent extraction method is mostly used in production practice. The current recovery of valuable metals focuses on Ni, Co, and Mn, and the resulting lithium-containing spent solution is under great pressure for treatment and has a great impact on the environment. Ammonia leaching enrichment can achieve preferential extraction of individual metals, but the metal leaching rate is inferior to that of acid-leaching enrichment. Biometallurgy has certain difficulties in the recovery of valuable metals from spent lithium batteries, specifically because spent lithium batteries contain large amounts of valuable metals and toxic electrolytes, which have a certain impact on microbial activity. The combined method of pyro roasting and hy- drometallurgy can destroy the structure of the positive active material at low temperatures and transform the valuable metals into a form that can be easily leached. In the subsequent water/acid leaching stage, the extraction of individual metals (e.g., Li) can be prioritized and the efficient leaching of valuable metals can be achieved without the use of reducing agents, which has good prospects for future applications.PDF Image | Recycling of Lithium Batteries
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