• Resources Recycling
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• v.33 no.5
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• pp.28-40
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• 2024

This paper provides a comprehensive review of the latest research trends in wet processing methods for recycling LiFePO₄ batteries. In particular, it analyzes various chemical leaching methods for the selective recovery of lithium from these batteries, evaluating their efficiency. The study covers lithium recovery techniques using strong and weak acids, leaching processes utilizing strong oxidants, and lithium recovery through isomorphic substitution reactions involving salts. Additionally, this research explores optimal leaching conditions to maximize lithium recovery, discusses various chemical reactions for the selective recovery of lithium, iron, and phosphorus, and offers insights into their potential. Ultimately, the paper aims to serve as a valuable reference for the advancement and practical application of LiFePO₄ battery recycling technologies.

• Clean Technology
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• v.29 no.2
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• pp.87-94
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• 2023

The recovery of valuable metals from waste lithium-based secondary batteries is very important in terms of efficiently utilizing earth's limited number of resources. Currently, the cathode material of a LiFePO₄ battery, a type of battery which is widely used in automobiles, contains approximately 5% lithium. After use, the lithium in these batteries can be used again as a raw material for new batteries through lithium recycling. In this study, low-concentration sulfuric acid, a commonly used type of inorganic acid, was used to selectively leach the lithium contained in a waste LiFePO₄ cathode material powder. In addition, in order to compare and analyze the leaching efficiency and separation efficiency of each component, the optimalleaching conditions were derived by applying a two-step leaching process with pulp density being used as a variable during leaching. When leaching with pulp density as a variable, it was confirmed that at a pulp density of 200 g/L, the separation efficiency was approximately 200 times higher than at other pulp densities because the iron and phosphorus components were hardly leached at this pulp density. Accordingly, the pulp density of 200 g/L was used tooptimize the leaching conditions for the selective leaching and recovery of lithium.

• Clean Technology
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• v.30 no.1
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• pp.28-36
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• 2024

As demand for electric vehicles increases, the market for lithium-ion batteries is also rapidly increasing. The battery life of lithium-ion batteries is limited, so waste lithium-ion batteries are inevitably generated. Accordingly, lithium was selectively preleached from waste lithium iron phosphate (LiFePO₄, hereafter referred to as the LFP) cathode material powder among lithium ion batteries, and iron phosphate (FePO₄) powder was recovered. The recovered iron phosphate powder was mixed with alkaline sodium carbonate (Na₂CO₃) powder and heat treated to confirm its crystalline phase. The heat treatment temperature was set as a variable, and then the leaching rate and powder characteristics of each ingredient were compared after water leaching using Di-water. In this study, lithium showed a leaching rate of approximately 100%, and in the case of powder heat-treated at 800 ℃, phosphorus was leached by approximately 99%, and the leaching residue was confirmed to be a single crystal phase of Fe₂O₃. Therefore, in this study, lithium, phosphorus, and iron components were individually separated and recovered from waste LFP powder.

• Clean Technology
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• v.30 no.2
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• pp.105-112
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• 2024

Globally, the demand for electric vehicles has surged due to greenhouse gas regulations related to climate change, leading to an increase in the production of used batteries as a consequence of the battery life issue. This study aims to selectively leach and recover valuable metal lithium from the cathode material of spent LFP (LiFePO₄) batteries among lithium-ion batteries. Generally, the use of inorganic acids results in the emission of toxic gases or the generation of large quantities of wastewater, causing environmental issues. To address this, research is being conducted to leach lithium using organic acids and other leaching agents. In this study, selective leaching was performed using the organic acid methane sulfonic acid (MSA, CH₃SO₃H). Experiments were conducted to determine the optimal conditions for selectively leaching lithium by varying the MSA concentration, pulp density, and hydrogen peroxide dosage. The results of this study showed that lithium was leached at approximately 100%, while iron and phosphorus components were leached at about 1%, verifying the leaching efficiency and the leaching rates of the main components under different variables.

• Resources Recycling
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• v.11 no.3
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• pp.10-16
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• 2002

In the leaching of $LiCoO_2$with a strong acid such as sulfuric and nitric acid, an additional step was needed to recover cobalt and lithium separately from spent lithium ion batteries (LIBs). The leaching of $LiCoO_2$in an oxalic acid solution was investigated to recover cobalt selectively using a low solubility of cobalt oxalate at low pH. Leaching efficiency of 95% of lithium and less than 1% of cobalt were obtained when pure $LiCoO_2$powder was leached in 3M oxalic acid at $80^{\circ}C$ and 50 g/L pulpdensity. Under the above leaching conditions, complete dissolution of lithium was accomplished with mere 0.25% of cobalt in the solution when the cathodic active material collected from spent LIBs was employed. The lithium in the leaching solution can be recovered as a form of carbonate or hydroxide depending on the addition of $Na_2$$CO_3$or LiOH.

• Resources Recycling
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• v.24 no.3
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• pp.44-50
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• 2015

Recycling technologies would be required in consideration of increasing demand in lithium ion batteries (LIBs). In this study, the leaching behavior of Ni, Co and Mn is investigated with ammoniacal medium for spent cathode active materials, which are separated from a commercial LIB pack in hybrid electric vehicles. The leaching behavior of each metal is analyzed in the presence of reducing agent and pH buffering agent. The existence of reducing agent is necessary to increase the leaching efficiency of Ni and Co. The leaching of Mn is insignificant even with the existence of reducing agent in contrast to Ni and Co. The most conspicuous difference between acid and ammoniacal leaching would be the selective leaching behavior between Ni/Co and Mn. The ammoniacal leaching can reduce the cost of basic reagent that makes the pH of leachate higher for the precipitation of leached metals in the acid leaching.

• Resources Recycling
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• v.33 no.3
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• pp.21-29
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• 2024

Globally, the demand for electric vehicles (EVs) is surging due to carbon-neutral strategies aimed at decarbonization. Consequently, the demand for lithium-ion batteries, which are essential components of EVs, is also rising, leading to an increase in the generation of spent batteries. This has prompted research into the recycling of spent batteries to recover valuable metals. In this study, we aimed to selectively leach and recover lithium from the cathode material of spent LFP batteries. To enhance the reaction surface area and reactivity, the binder in the cathode material powder was removed, and the material was subjected to heat treatment in both atmospheric and nitrogen environments across various temperature ranges. This was followed by a mechanochemical process for aqueous leaching. Initially, after heat treatment, the powder was converted into a soluble lithium compound using sodium persulfate (Na₂S₂O₈) in a mechanochemical reaction. Subsequently, aqueous leaching was performed using distilled water. This study confirmed the changes in the characteristics of the cathode material powder due to heat treatment. The final heat treatment in a nitrogen atmosphere resulted in a lithium leaching efficiency of approximately 100% across all temperature ranges.

• Resources Recycling
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• v.31 no.1
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• pp.21-28
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• 2022

The smelting reduction of spent lithium-ion batteries results in metallic alloys of cobalt, nickel, and copper. To develop a process to separate the metallic alloys, leaching of the metallic mixtures of these three metals with H₂SO₄ solution containing 3% H₂O₂ dissolved all the cobalt and nickel, together with 9.6% of the copper. Cyanex 301 selectively extracted Cu(II) from the leaching solution, and copper ions were completely stripped with 30% aqua regia. Selective extraction of Co(II) from a Cu(II)-free raffinate was possible using the ionic liquid ALi-SCN. Three-stage cross-current stripping of the loaded ALi-SCN by a 15% NH₃ solution resulted in the complete stripping of Co(II). A process was proposed to separate the three metal ions from the sulfuric acid leaching solutions of metallic mixtures by employing solvent extraction.

• Resources Recycling
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• v.30 no.2
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• pp.53-60
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• 2021

Leaching experiments from single metal and metallic mixtures were conducted to develop a process for the recovery of cobalt, copper, and nickel in spent lithium ion batteries. Inorganic and organic acid solutions without oxidizing agents were employed. No copper was dissolved in the absence of an oxidizing agent in the leaching solutions. The leaching condition to completely dissolve single metal of cobalt and nickel was determined based on acid concentration, reaction temperature and time, and pulp density. The leaching condition to dissolve all of cobalt and nickel from the metallic mixtures was also obtained. Leaching of the metallic mixture with methanesulfonic acid led to selective dissolution of cobalt at low temperatures.

• Resources Recycling
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• v.30 no.6
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• pp.36-42
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• 2021

Spent lithium-ion batteries are treated by reduction-smelting at high temperatures to recover valuable metals. Solvent extraction and precipitation of the HCl leaching solution of reduction-smelted metallic alloys resulted in a filtrate containing Ni(II) and a small amount of Si(IV). Adsorption and precipitation experiments were conducted to recover pure Ni(II) compounds from the filtrate. Si(IV) was selectively loaded onto polyacrylamide, but this method did not efficiently filter the solution due to an increase in viscosity. The addition of Na₂CO₃ as a precipitant to the filtrate led to the simultaneous precipitation of Ni(II) and Si(IV). However, it was possible to recover nickel oxalate with a purity higher than 99.99% by selectively precipitating Ni(II) with the addition of Na₂C₂O₄ as a precipitant.