Recovering valuable metals from LiNixCoyMn1-x-yO2 cathode materials of spent lithium ion batteries via a combination of reduction roasting and stepwise leaching

Liu, Pengcheng; Xiao, Li; Chen, Yifeng; Tang, Yiwei; Wu, Jian; Chen, Han

doi:10.1016/j.jallcom.2018.12.226

Cited by 107 publications

(20 citation statements)

References 41 publications

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“…Hence, the process´s bottleneck lies in lithium extraction as a solid product instead of lithium leachability (leaching efficiency). A wide range of hydrometallurgical studies shows high leaching efficiencies using different solvents [29][30][31][32][33][34], for example, by using H2SO4, a lithium leaching efficiency of 96.7% [35], and by HCl 99.2% [36]. In [37], leaching in citric acid and precipitating lithium by sodium phosphate leads to a leaching efficiency of 99% Li and a recovery as Li3PO4 of 89%.…”

Section: Lithium Behavior In Pyro-and Hydrometallurgical Recycling Steps and Need For Early-stage Li-separationmentioning

confidence: 99%

Early-Stage Recovery of Lithium from Tailored Thermal Conditioned Black Mass Part I: Mobilizing Lithium via Supercritical CO2-Carbonation

Schwich

Schubert

Friedrich

2021

Metals

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In the frame of global demand for electrical storage based on lithium-ion batteries (LIBs), their recycling with a focus on the circular economy is a critical topic. In terms of political incentives, the European legislative is currently under revision. Most industrial recycling processes target valuable battery components, such as nickel and cobalt, but do not focus on lithium recovery. Especially in the context of reduced cobalt shares in the battery cathodes, it is important to investigate environmentally friendly and economic and robust recycling processes to ensure lithium mobilization. In this study, the method early-stage lithium recovery (“ESLR”) is studied in detail. Its concept comprises the shifting of lithium recovery to the beginning of the chemo-metallurgical part of the recycling process chain in comparison to the state-of-the-art. In detail, full NCM (Lithium Nickel Manganese Cobalt Oxide)-based electric vehicle cells are thermally treated to recover heat-treated black mass. Then, the heat-treated black mass is subjected to an H2O-leaching step to examine the share of water-soluble lithium phases. This is compared to a carbonation treatment with supercritical CO2, where a higher extent of lithium from the heat-treated black mass can be transferred to an aqueous solution than just by H2O-leaching. Key influencing factors on the lithium yield are the filter cake purification, the lithium separation method, the solid/liquid ratio, the pyrolysis temperature and atmosphere, and the setup of autoclave carbonation, which can be performed in an H2O-environment or in a dry autoclave environment. The carbonation treatments in this study are reached by an autoclave reactor working with CO2 in a supercritical state. This enables selective leaching of lithium in H2O followed by a subsequent thermally induced precipitation as lithium carbonate. In this approach, treatment with supercritical CO2 in an autoclave reactor leads to lithium yields of up to 79%.

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Section: Lithium Behavior In Pyro-and Hydrometallurgical Recycling Steps and Need For Early-stage Li-separationmentioning

confidence: 99%

Early-Stage Recovery of Lithium from Tailored Thermal Conditioned Black Mass Part I: Mobilizing Lithium via Supercritical CO2-Carbonation

Schwich

Schubert

Friedrich

2021

Metals

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“…They subsequently demonstrated how Ni, Co, and MnO can easily be leached in H 2 SO 4 where more than 96% efficiency was achieved at a low liquid/solid ratio (3.5 mL/g) and without requiring a reducing agent, as the metals already exist at low valence states. Through a similar concept, Liu et al ball‐milled NMC with carbon black (10 wt% dosage) and calcined the powder at 550°C for 0.5 hours under Ar flow, producing Li 2 CO 3 , Ni, Co, NiO, and MnO. Due to the low solubility of Li 2 CO 3 , 93% of Li was selectively leached with water at a relatively high liquid/solid ratio of 30 mL/g at 25°C for 1.5 hours.…”

Section: Leaching Developments and Unconventional Approachesmentioning

confidence: 99%

Recycling of mixed cathode lithium‐ion batteries for electric vehicles: Current status and future outlook

et al. 2020

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Worldwide trends in mobile electrification, largely driven by the popularity of electric vehicles (EVs) will skyrocket demands for lithium‐ion battery (LIB) production. As such, up to four million metric tons of LIB waste from EV battery packs could be generated from 2015 to 2040. LIB recycling directly addresses concerns over long‐term economic strains due to the uneven geographic distribution of resources (especially for Co and Li) and environmental issues associated with both landfilling and raw material extraction. However, LIB recycling infrastructure has not been widely adopted, and current facilities are mostly focused on Co recovery for economic gains. This incentive will decline due to shifting market trends from LiCoO2 toward cobalt‐deficient and mixed‐metal cathodes (eg, LiNi1/3Mn1/3Co1/3O2). Thus, this review covers recycling strategies to recover metals in mixed‐metal LIB cathodes and comingled scrap comprising different chemistries. As such, hydrometallurgical processes can meet this criterion, while also requiring a low environmental footprint and energy consumption compared to pyrometallurgy. Following pretreatment to separate the cathode from other battery components, the active material is dissolved entirely by reductive acid leaching. A complex leachate is generated, comprising cathode metals (Li+, Ni2+, Mn2+, and Co2+) and impurities (Fe3+, Al3+, and Cu2+) from the current collectors and battery casing, which can be separated and purified using a series of selective precipitation and/or solvent extraction steps. Alternatively, the cathode can be resynthesized directly from the leachate.

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“…After filtration and washed in deionized water, the cathode material was dried under ambient conditions for 24 h. The final product was dissolved in 10 mL of 6 mol/L H 2 SO 4 , 8 mL of 36% v/v H 2 O 2 and 200 mL of distilled water. The solution was kept under stirring and heating at 80 • C for 2 h [41,[45][46][47][48][49]. After cooling to room temperature, the solutions were filtered and the pH adjusted to 3.0 [27,29,[50][51][52] with the addition of sodium acetate.…”

Section: Recycled Electrolyte Solutions: Hydrometallurgical Routementioning

confidence: 99%

Obtaining Mn-Co Alloys in AISI 430 Steel from Lithium-Ion Battery Recycling: Application in SOFC Interconnectors

et al. 2020

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The recycling of exhausted lithium-ion batteries from mobile phones originate five solutions with different Co and Mn proportions that were used as electrolytic solutions to obtain Mn-Co spinel coatings on the surface of AISI430 stainless steel. The coatings are intended to contain chromium volatility in the working conditions of Solid Oxide Fuel Cells (SOFC) metallic interconnectors. Potentiostatic electrodeposition was the technique used to obtain Mn-Co coatings from low concentration electrolytes at pH = 3.0 and potential applied −1.3 V. Charge efficiency data were used for sample optimization. Three optimized samples were subjected to oxidation heat treatment at 800 °C for 300 h and then characterized by XRD, SEM and EDS. The results showed that the addition of manganese ions instead of cobalt ions in the electrolytic bath produces more stable and well-distributed deposits as the ratio of the two ions becomes equal in the electrolytic bath. Thin, homogeneous and stable spinel coatings (Mn, Co)3O4 2.8 μm and 3.9 μm thick were able to block chromium volatility when exposed to SOFC operating temperature.

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Recovering valuable metals from LiNixCoyMn1-x-yO2 cathode materials of spent lithium ion batteries via a combination of reduction roasting and stepwise leaching

Cited by 107 publications

References 41 publications

Early-Stage Recovery of Lithium from Tailored Thermal Conditioned Black Mass Part I: Mobilizing Lithium via Supercritical CO2-Carbonation

Early-Stage Recovery of Lithium from Tailored Thermal Conditioned Black Mass Part I: Mobilizing Lithium via Supercritical CO2-Carbonation

Recycling of mixed cathode lithium‐ion batteries for electric vehicles: Current status and future outlook

Obtaining Mn-Co Alloys in AISI 430 Steel from Lithium-Ion Battery Recycling: Application in SOFC Interconnectors

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