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Energies 2022, 15, 1611 16 of 23 spent metal lithium batteries, showing a higher leaching curve for the cathode materials LiNi0.5Co0.2Mn0.3O2 (NCM523) and LiMn2O4. Heydarian et al. [75] performed bioleaching of spent LIBs for laptop computers under two-step conditions on the basis of the bacterial activity of a mixture of Thiobacillus ferrous oxide and Thiobacillus sulfate oxide strains. Maximum metal recoveries of 99.2%, 50.4%, and 89.4% for lithium, cobalt, and nickel, respectively, are achieved at an optimum inoculum level of 3/2, optimal conditions of 36.7 g/L iron sulfate, 5.0 g/L sulfur, and an initial pH of 1.5. Dolker et al. [76] used a combination of Bacillus lysine-citric acid for the recovery of spent LIBs. The citric acid method is used to separate copper and aluminum foils from the black powder. It leaves lithium and cobalt in a synthetic extractant, and the lithium is further separated by leaching and the cobalt is further separated by biosorption with the proposed hybrid combination. A 25% increase in lithium leaching and a 98% increase in cobalt biosorption can be achieved using this hybrid treatment. The reactions involved are as follows: C2H4O4 → C2HO4− + H+ (13) C2HO− → C2HO2− + H+ (14) 44 Xin et al. [77] first explored the release of valuable Li, Co, Mn, and Ni from three typical spent electric LIB cathodes, LFP, LiMn2O4, and NCM, by bioleaching at a slurry concentration of 1%. The cultures are inoculated with pure A.T (oxysulfate bacilli), pure L.F (iron screw bacilli), or mixed (A.T and L.F). Accordingly, three bioleaching systems, the sulfur–A.T system, the pyrite–L.F system, and the mixed energy–mixed culture system (MS-MC), are established. The results show that the highest extraction efficiency of Li is achieved by the sulfide–A.T system, indicating that the release of Li is due to the acid solubilization of bio-H2SO4. The mixed energy–mixed culture system shows the highest solubilization of Co, Ni, and Mn, indicating that the activation of these metals is the result of the combined effect of Fe2+ reduction and acid solubilization. Lithium extraction occurs because of a noncontact mechanism, which is necessary for the activation of Co, Ni, and Mn between the cathode and the cell. pH adjustment greatly improves the leaching performance of the bacteria due to the promotion of bacterial growth, with Li and Mn extractions reaching 95% and Co and Ni release rates increasing from 43.5% and 38.3% to 96% and 97%, respectively. 6. Other Recycling Treatments 6.1. Closed-Loop LIBs Recycling Process Strategies for the direct recovery of the cathode by the process exist and have attracted increasing interest in recent years. Many researchers have aimed to recycle spent LIBs by directly generating electrode materials to build a closed-loop industrial chain and reduce the pressure of spent liquid disposal. Zhao et al. [78] used ultrasonic cavitation to fully separate lithium cobalt oxide (LCO) and aluminum foil. The lithium in the negative elec- trode material is directly used as a lithium-leaching solution and applied to the ultrasonic repair of spent LCO. Peng et al. [79] effectively separated aluminum foil, lithium-containing compounds, and high-purity FePO4 using a one-step oxidative leaching reaction at room temperature. LFP with good chemical properties is successfully synthesized by using the resulting FePO4 and LiCO3 precipitated in the leachate, with a lithium leaching rate of up to 98%. Ribeiro et al. [80] used citric acid and nitric acid as leaching agents for the cathode and anode materials, respectively. Graphene oxide (GO) is prepared from the recovered graphite using a modified Hummers method. The GO and recovered CoO are mixed and heat-treated at 450 ◦C for 2 h using the sol-gel method, and the resulting hybrid material is used as the electrode material. Fan et al. [81] used DMC to clean the obtained ternary LIB cathode material to remove the electrolyte. It is then calcined at 600 ◦C for 2 h to remove PVDF and carbon black, with the HF and CO2 generated during the process being absorbed by the NaOH solution. The cathode material is separated from the aluminum foil to obtain the failed NCM523, which was dissolved in deionized water with LiOH, NiO, MnO2,PDF Image | Recycling of Lithium Batteries
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