Decomposition of Deep Eutectic Solvent Aids Metals Extraction in Lithium‐Ion Batteries Recycling

Schiavi, Pier Giorgio; Altimari, Pietro; Sturabotti, Elisa; Marrani, Andrea Giacomo; Simonetti, Giulia; Pagnanelli, Francesca

doi:10.1002/cssc.202200966

Cited by 32 publications

(28 citation statements)

References 41 publications

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“…Furthermore, Schiavi et al. did not detect chlorine evolving upon metal oxide dissolution as Cl 3 − is formed in chloride‐rich DES [58] . In our reaction, chlorine evolution could also not be detected by conducting the reaction gases through an aqueous potassium iodide solution, as reported previously [3] .…”

Section: Resultssupporting

confidence: 71%

Cobalt Deposition from Ionothermally Dissolved Cobalt Oxides

2023

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Owing to the environmental problems of numerous metal production processes, there is a growing need for more energyefficient approaches. Cobalt is considered a strategic element that is extracted not only from ores but also from spent Li-ion batteries. One promising new approach is ionometallurgy, which is the extraction of metal oxides by ionic liquids (ILs). This study concerns new investigations into ionometallurgical processing of CoO, Co 3 O 4 , and LiCoO 2 in the IL betainium bis(trifluoromethylsulfonyl)imide, [Hbet][NTf 2 ]. Three crystal structures of cobaltÀ betaine complex compounds and combined spectroscopic and diffraction studies provide insights into the dissolution process. In addition, an optimized dissolution procedure for metal oxides is presented, avoiding the previously reported decomposition of the IL. Subsequent cobalt electrodeposition is only possible from cationic complex species, highlighting the importance of a thorough understanding of the complex equilibria. The presented method is also compared to other recently reported approaches.

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Section: Resultssupporting

confidence: 71%

Cobalt Deposition from Ionothermally Dissolved Cobalt Oxides

2023

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“…Schiavi et al. found that ChCl/EG at 180 °C for 72 h would thermally decompose into Cl 3 – , which is the key oxidant for the enhancement of metal oxide dissolution . Furthermore, Schiavi et al found that the decomposition products from ChCl/EG leaching at 180 °C for 24 h include trimethylamine .…”

Section: Resultsmentioning

confidence: 99%

“…However, mass loss of PEG/PHA (1:1) at 80 °C is , which is the key oxidant for the enhancement of metal oxide dissolution. 52 Furthermore, Schiavi et al found that the decomposition products from ChCl/EG leaching at 180 °C for 24 h include trimethylamine. 51 However, Mu et al concluded that PEG-based DESs are volatile at room temperature and atmospheric pressure.…”

Section: Comparison Of Metal-leachingmentioning

confidence: 99%

Efficient Recovery of Valuable Metals from Lithium-Ion Battery Cathodes Using Phytic Acid-Based Deep Eutectic Solvents at a Mild Temperature

et al. 2023

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Recycling of waste lithium-ion batteries (LIBs) requires metal leaching from the LIB cathode; however, the metal-leaching process is too challenging to be efficient, green, and mild simultaneously. Moreover, the leaching efficiency at mild conditions by green solvents is not high and needs to be improved urgently. Here, deep eutectic solvents (DESs) composed of poly(ethylene glycol) 200 (PEG) and phytic acid (PHA) are designed to leach Co from LIB cathodes with an ultrahigh metalleaching efficiency of 0.987 at a low temperature of 80 °C for 24 h, which is much higher (ca. 0.3) than the efficiency of previously reported DESs. Moreover, the constituents (PEG and PHA) in DESs are low-cost, sustainable, and biodegradable; particularly, PHA is naturally available in legumes, cereals, dried fruits, vegetables, and other fruits, which are also edible by human beings. This work provides a super highly efficient, sustainable, and mild route for metal leaching from LIB cathodes.

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“…The leaching process of Co from LCO mainly depended on the reduction of Co(III) by a hydrogen bond donor to form soluble [CoCl 4 ] 2– , which was also identified by Figure S2. , This caused the DES leachate to become increasingly bluish with an increased temperature. The existence of [CoCl 4 ] 2– proved the formation of Cl 3 – , which was proposed to play a pivotal role in the oxidative dissolution of LIB metal oxides . In previous studies using the conventional heating method, ChCl–OA could leach 85% of Co under the optimum conditions. ,, However, leaching Co using the microwave heating method made a difference.…”

Section: Resultsmentioning

confidence: 99%

“…The existence of [CoCl 4 ] 2− proved the formation of Cl 3 − , which was proposed to play a pivotal role in the oxidative dissolution of LIB metal oxides. 42 In previous studies using the conventional heating method, ChCl−OA could leach 85% of Co under the optimum conditions. 27,36,38 However, leaching Co using the microwave heating method made a difference.…”

Section: The Effect Of Different Leaching Temperatures On the Selecti...mentioning

confidence: 97%

An Efficient and Precipitant-Free Approach to Selectively Recover Lithium Cobalt Oxide Made for Cathode Materials Using a Microwave-Assisted Deep Eutectic Solvent

Liu

Zhang

et al. 2022

Energy Fuels

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The recovery of cathode materials using deep eutectic solvents (DESs) still requires a long leaching time and relatively high temperatures. The poor selectivity of the leaching process leads to the low purity of the precipitate. Herein, a microwave-assisted choline chlorine–oxalate–water system was designed to selectively leach Li and recover high-purity cobalt oxalate simultaneously, which could greatly shorten the extraction time and decrease the leaching temperature. Fourier transform infrared spectroscopy, X-ray diffraction, inductively coupled plasma–mass spectrometry, and X-ray photoelectron spectroscopy methods were used to explore the mechanism of microwave-assisted DES leaching of valuable metals from lithium cobalt oxide (LCO). It was found that 99.05% of Li could be selectively leached and 99.21% of Co could be precipitated as cobalt oxalate at 100 °C in 10 min simultaneously. The purity of cobalt oxalate precipitated was 95.36% without any purification procedures. A new polymer compound Co2+[(Ch+) x (Cl–) y (HC2O4 –) z ] was formed during the microwave-assisted leaching process. The compound could be hydrolyzed, and the cobalt oxalate precipitate appeared by increasing the water content in the DES. Finally, the DES for the recovery of LCO could be cycled four times with favorable selectivity. A low-pollution, efficient, process-simple, and precipitant-free technology using a microwave-assisted DES for selective recovery of LCO was proposed, which provided an important reference method for large-scale recovery of valuable metals from spent lithium-ion batteries.

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Decomposition of Deep Eutectic Solvent Aids Metals Extraction in Lithium‐Ion Batteries Recycling

Cited by 32 publications

References 41 publications

Cobalt Deposition from Ionothermally Dissolved Cobalt Oxides

Cobalt Deposition from Ionothermally Dissolved Cobalt Oxides

Efficient Recovery of Valuable Metals from Lithium-Ion Battery Cathodes Using Phytic Acid-Based Deep Eutectic Solvents at a Mild Temperature

An Efficient and Precipitant-Free Approach to Selectively Recover Lithium Cobalt Oxide Made for Cathode Materials Using a Microwave-Assisted Deep Eutectic Solvent

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