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Energies 2022, 15, 1611 17 of 23 and NH4H2PO4 and stirred vigorously. The NCM523 is directly regenerated by ion replen- ishment and ion-doping heat treatment. Xing et al. [82] used sulfuric acid as the leaching agent and 30% H2O2 as the reducing agent, with magnetic stirring at 400 r/min and an S/L ratio of 10 g/L for 2 h at 90 ◦C. The leachate is concentrated using a rotary evaporator and used as a precursor for the preparation of LiNi0.6Co0.2Mn0.2O2. It is prepared through calcination using a coprecipitation method with the addition of the appropriate sulfate. The lithium recovery is 81.2% in the closed-loop circuit process. Chu et al. [83] used sulfuric acid and H2O2 to leach mixed cathode powders with over 99% leaching of each metal. Li2CO3 is recovered from the residual solution by adding saturated Na2CO3. Ternary cath- ode precursors are prepared directly from the leach solution. The precursors were mixed with Li2CO3 and roasted to resynthesize the ternary cathode material LiNi0.6Co0.2Mn0.2O2. Fan et al. [84] NCM523 was cut into 2 × 2 cm squares. Then, these pieces were stirred in water for 15 min. In this way, the cathode material and the aluminum foil are separated by the shear force of the water flow. Since the aluminum foil remains intact, it can be re- moved from the water by clamping or filtering. Afterward, the cathode material is filtered and dried at 80 ◦C for 12 h. Finally, the degraded NCM523 (denoted as D-NCM523) is regenerated by quantitative mixing with LiOH, after which it is directly subjected to a solid-state sintering process (800 ◦C, 8 h). The powder obtained was regenerated NCM523. The electrochemical performance showed that the regenerated material was comparable to the original material in terms of cycling and multiplicative performance, maintaining capacity retention of 94.5% after 100 cycles and good capacity recovery after 1C cycles. Sa et al. [85] synthesized high-performance Ni1/3Mn1/3Co1/3(OH)2 precursors and NCM cathode materials. Ma et al. [86] cut, shredded, and sieved the discharged batteries. Steel cases, collectors (aluminum and copper), electronic circuits, plastic, and bag materials are removed and recycled. The remaining black material consists of graphite, carbon, cathode material, and some residues of Al, Cu, and Fe. Afterward, a hydrometallurgy process is implemented to dissolve the different anode materials and metals in the leach solution. At the same time, graphite, carbon, and undissolved materials are filtered out. First, impu- rities in the leachate, including copper, iron, and aluminum, are removed through a series of pH adjustments, leaving behind nickel, manganese, and cobalt ions. The leach solution contained some impurities, including Cu, Fe, and Al. The impurities were significantly removed after the impurity removal step. In addition, the concentration of Na increased due to the addition of NaOH to control the pH to remove the impurities. Furthermore, the concentration of Ni, Mn, Co, and Li decreased due to the volume change after the impurity removal step. The recoveries of Ni, Mn, and Co were above 90%. Next, various NMC were fabricated by adjusting the ratio of Ni, Mn, and Co to the desired ratio by adding pristine metal sulfates as needed. The recycled NCM was demonstrated to have excellent multiplicity and cycling performance, which was verified by various industry-grade tests. In addition to the preparation of electrode materials, they are recycled as energy storage materials, adsorbent materials, and supercapacitors. Ji et al. [87] used formic acid and hydrogen peroxide for the leaching of LFP and achieved a leaching rate of 98.84% for Li and less than 1% for Al and Fe, allowing the collection of a high-purity Li3PO4 product. The leached residue synthesizes Fe2P2O7/C. The simultaneous separation of Li, Fe, and Al is achieved, and the leached residue is converted into a new LIB energy storage material. Schiavi et al. [88] leached the spent cathode material. The dissolved metal is precipitated in the form of carbonate. The obtained precipitated carbonate is then dissolved to prepare an electrolyte and electrodeposited into nanoporous alumina templates to prepare nanowire battery cathodes for use as supercapacitors. Zou et al. [89] used the spent LFP battery cathode material as a raw material to generate mesoporous core–shell adsorbents using a simple alkali-leaching process. It has a good adsorption function for removing heavy metal ions from water. Suarez et al. [90] synthesized LiF using hydrofluoric acid to dissolve the spent LIB cathode material (LCO).PDF Image | Recycling of Lithium Batteries
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