Characterization, modeling, and optimization of a single-step process for leaching metallic ions from LiNi1/3Co1/3Mn1/3O2 cathodes for the recycling of spent lithium-ion batteries

Cheng, Qian; Chirdon, William M.; Lin, Mu-Tu; Mishra, Kuber; Zhou, Xiao‐Dong

doi:10.1016/j.hydromet.2019.01.003

Cited by 46 publications

(13 citation statements)

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“…A similar rule can be observed in other studies. 27 − 30 When the reaction time was longer than 8 min, the separation rate of all samples except the sample in 0.3 mol/L oxalic acid solution changed slightly. In addition, the separation rates of 0.3 and 0.4 mol/L samples were 95.81 and 95.88 wt %, respectively.…”

Section: Resultsmentioning

confidence: 99%

Separating Sulfur from Fuel Gas Desulfurization Gypsum with an Oxalic Acid Solution

et al. 2020

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The separation of sulfur from the wet limestone fuel gas desulfurization (FGD) gypsum using oxalic acid solution was studied. Optimal separation conditions and a separation mechanism of sulfur were investigated. The obtained results indicate that the sulfur in FGD gypsum can be separated efficiently by oxalic acid solution. When separating under the optimal experimental conditions of 0.3 mol/L oxalic acid solution, 30 °C, and a 5/150 g/mL solid to liquid ratio for 8 min, the separation rate reached 97.0 wt %. Besides, the Avrami equation is more suitable for the kinetic analysis of the sulfur separation reaction than the unreacted shrinking core model. When the reaction temperature is less than or equal to 20 °C, the mechanism of the sulfur separation process is chemical-reaction-controlled; otherwise, it is diffusion-controlled. The activation energy E a of the sulfur separation reaction is 34.84 kJ/mol. During the separation process, the pH of the solution gradually decreased due to the conversion of oxalic acid to sulfuric acid, so the liquid obtained after the sulfur separation of FGD gypsum can be recycled as industrial sulfuric acid. Nearly 1 mol of sulfuric acid can be obtained for every mole of oxalic acid consumption.

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Section: Resultsmentioning

confidence: 99%

Separating Sulfur from Fuel Gas Desulfurization Gypsum with an Oxalic Acid Solution

et al. 2020

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“…Leaching includes reactive ion diffusion within the liquid film surface, then subsequent diffusion into the inner core through the particle product layer, and chemical reactions at the inner core surface. Following previous studies (Chen et al, 2019; Zhang et al, 2018), we employed surface chemical reaction, external diffusion control, and internal diffusion control models to analyze leaching mechanisms (Cheng et al, 2019)…”

Section: Resultsmentioning

confidence: 99%

“…The required amount of cathode material was added to a designated volume of diluted H 2 SO 4 solution at fixed temperature and the slurry was agitated with a magnetic stirrer for a specific time and subsequently filtered. Previous studies (Cheng et al, 2019) have shown that agitation speed has little effect on LR for metals, hence we selected agitation speed = 400 rpm for all experiments, and focused on investigating effects due to H 2 SO 4 concentration, solid–liquid (S/L) ratio, leaching time (LT) and temperature, and starch dosage during leaching.…”

Section: Methodsmentioning

confidence: 99%

Countercurrent leaching of Ni, Co, Mn, and Li from spent lithium-ion batteries

et al. 2020

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This study focuses on a countercurrent leaching process (CLP) for the dissolution of high-value metals from cathode active material of spent lithium-ion batteries (LIBs). Its main aim is to improve the effective utilization of acid during leaching and allow for the continuous operation of the entire CLP by adjusting the process parameters. The overall recovery of lithium (Li), cobalt (Co), nickel (Ni), and manganese (Mn) was 98%, 95%, 95%, and 92%, respectively; the acid utilization of the leaching process exceeded 95% under optimum conditions. The optimum conditions for first stage leaching were 70 g/L solid–liquid (S/L) ratio at 40°C for 30 minutes, and 2.0 M sulfuric acid, 100 g/L S/L ratio, 7 g/L starch, at 85°C for 120 minutes for second stage leaching. After five bouts of circulatory leaching, more than 98% Li, 95% Co, 95% Ni, and 92% Mn were leached under the same leaching conditions. Furthermore, we introduced the Avrami equation to describe metal leaching kinetics from spent LIBs, and determined that the second stage leaching process was controlled by the diffusion rate. In this way, Li, Ni, Co, and Mn can be recovered efficiently and the excess acid in the leachate can be reused in this hydrometallurgical process, potentially offering economic and environmental benefits.

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“…The main valuable metals contained in batteries exhibit high oxidation states, such as Ni(III), Co(III), and Mn(IV), thus leading to the essential introduction of reducing agents. Carbon, glucose, sulfites, Fe(II), and so on are the commonly used reductants for the recycling of spent Ni–Co–Mn-based lithium-ion batteries. − Additionally, the leaching agents can be classified into three types: inorganic acids − (H 2 SO 4 , H 3 PO 4 , and HCl), organic acids ,− (acetic acid, oxalic acid, tartaric acid, citric acid, benzenesulfonic acid, and formic acid), and ammoniacal leaching substances. , Among them, when the price of organic acids is very high and it is easy for the ammonia leaching agents with cathode materials containing Mn to form a double salt, ,, applying inorganic acids as leaching agents is most valuable for large-scale industrial production because of their high efficiency and low cost. However, inorganic acids show a strong corrosivity but no selectivity to the impurities in spent cathode materials, which makes actual production more costly.…”

Section: Introductionmentioning

confidence: 99%

Creative Method for Efficiently Leaching Ni, Co, Mn, and Li in a Mixture of LiFePO₄ and LiMO₂ Using Only Fe(III)

Xu¹,

Dai

Dong³

et al. 2021

ACS Sustainable Chem. Eng.

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Recycling end-of-life lithium-ion batteries has attracted widespread attention due to their potential environmental hazards and the importance of key metal supplies. However, the previously reported research methods are intended only for spent Ni–Co–Mn (NCM)-based lithium-ion batteries or spent lithium iron phosphate batteries. In this letter, a new method is proposed for recovering the mixed cathode materials of LiFePO4 and LiNi0.5Co0.2Mn0.3O2 from spent lithium-ion batteries by sole Fe2(SO4)3. According to our design, ferric iron itself acts as a Lewis acid and facilitates LiFePO4 to release the reducing agent of ferrous iron to reduce LiNi0.5Co0.2Mn0.3O2. Additionally, the environmentally friendly and efficient leaching process has been achieved for Ni, Co, Mn, and Li by reasonably adjusting the ratio of trivalent iron, LiFePO4, and LiNi0.5Co0.2Mn0.3O2. This method of processing mixed spent lithium-ion battery cathode materials significantly reduces the amount of reducing agent or oxidant usage. Also,it is effective at reducing time, energy consumption, and water consumption. It provides a new solution to recycling used lithium-ion batteries.

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Characterization, modeling, and optimization of a single-step process for leaching metallic ions from LiNi1/3Co1/3Mn1/3O2 cathodes for the recycling of spent lithium-ion batteries

Cited by 46 publications

References 47 publications

Separating Sulfur from Fuel Gas Desulfurization Gypsum with an Oxalic Acid Solution

Separating Sulfur from Fuel Gas Desulfurization Gypsum with an Oxalic Acid Solution

Countercurrent leaching of Ni, Co, Mn, and Li from spent lithium-ion batteries

Creative Method for Efficiently Leaching Ni, Co, Mn, and Li in a Mixture of LiFePO₄ and LiMO₂ Using Only Fe(III)

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Characterization, modeling, and optimization of a single-step process for leaching metallic ions from LiNi1/3Co1/3Mn1/3O2 cathodes for the recycling of spent lithium-ion batteries

Cited by 46 publications

References 47 publications

Separating Sulfur from Fuel Gas Desulfurization Gypsum with an Oxalic Acid Solution

Separating Sulfur from Fuel Gas Desulfurization Gypsum with an Oxalic Acid Solution

Countercurrent leaching of Ni, Co, Mn, and Li from spent lithium-ion batteries

Creative Method for Efficiently Leaching Ni, Co, Mn, and Li in a Mixture of LiFePO4 and LiMO2 Using Only Fe(III)

Contact Info

Product

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Creative Method for Efficiently Leaching Ni, Co, Mn, and Li in a Mixture of LiFePO₄ and LiMO₂ Using Only Fe(III)