With the successive retirement of lithium-ion batteries (LIBs) approaching, there has been an upsurge of spent LIBs, posing significant challenges to energy, resources, and environment, which has led to the...

A systematic review of efficient recycling for cathode materials of spent lithium-ion batteries: process intensification technologies beyond traditional methods

A clear understanding of the anodic dissolution behavior of zirconium in molten LiCl–KCl salt plays an essential role in developing the electrometallurgical recycling of spent nuclear-fuel cladding. In this study,...

Optical monitoring of the anodic dissolution of zirconium and the agglomeration of potassium hexachlorozirconate during transpassive dissolution in molten LiCl–KCl salt

Simultaneously achieving high Li leaching efficiency and Li/Co selectivity from lithium-ion batteries cathode by using natural low-melting mixture solvents (LoMMSs) as green solvents

All-solid-state lithium-ion batteries (ASSLIBs) are attracting significant attention due to their high energy density, conductivity and safety. However, they are expected to generate substantial waste in the near future, leading to resource depletion and environmental pollution. Therefore, it is crucial to achieve green, mild and safe recovery of ASSLIBs. Here, we for the first time to use green deep eutectic solvents (DESs) to effectively recover solid-state electrolytes (SSEs) from ASSLIBs at mild temperature. Results show that Li leaching efficiency can reach up to 87.5% with a superhigh Li/La selectivity of 1902 at a low temperature of 80 oC. Furthermore, 70 anti-solvents are screened to recycle the dissolved SSEs from leachate and 12 anti-solvents could precipitate SSEs from leachate at room temperature. This research opens new possibilities for recovering SSEs from ASSLIBs using the sustainable, cost-effective and safe solvents. 

Recycling Solid Electrolytes from All‐Solid‐State Lithium‐Ion Batteries by Using Deep Eutectic Solvents as Green Extractants

Different approaches for sustainable recovery of precious metals from electronic wastes: Techno-economic evaluation and future perspectives

To research Zr‐Dy alloy dissolution behavior at anode, the electrode process of LiCl‐KCl‐K2ZrF6‐DyCl3 on an inert W electrode was firstly explored through a group of electrochemical techniques. The depolarization phenomenon was observed owing to the formation of Zr‐Dy solid solution, and the redox potentials of Dy(III)/Dy, Zr(II)/Zr‐Dy solid solution, Zr(IV)/Zr(II) and Zr(II)/Zr(0) were determined. Then, Zr and Zr‐Dy alloy dissolution behaviors at anode were explored by cyclic voltammetry and linear sweep voltammetry. It was confirmed that the rapid dissolution potentials of Zr and Zr‐Dy solid solution were observed at −0.86 V and − 1.90 V, and the passivation phenomena of Zr and Zr‐Dy solid solution were also observed. Zr‐Dy alloy dissolution at anode was conducted employing constant potential (CP) and current (CC) electrolysis. It was found that both Dy and Zr could be dissolved by CC electrolysis. However, Zr dissolution could be controlled by CP electrolysis. Furthermore, Zr‐Dy alloy dissolution process was monitored online at different current densities, the dissolution rate increased with the increase of the applied current density.

Anodic dissolution behavior of Zr‐Dy alloy in LiCl‐KCl molten salt

Water, supercritical fluids, ionic liquids and deep eutectic solvents (DESs) have been considered as green solvents for many years. The demand of green and sustainable development requires the search of novel green solvents. Some of the reported DESs might be not be the real DESs because we observe that these so-called reported liquid DESs become solid after exposure to the room temperature for many hours or days. Here, we for the first time propose a new concept of green solvents, superlong supercooling solvents (SSSs), as the green alternatives to water, supercritical fluids, ionic liquids and DESs. SSSs are the metastable liquid solvents either single component or multiple components due to the superlong supercooling effect at the temperature around or a little higher than room temperature. SSSs should condense after a superlong time; however, SSSs could be used as the green solvents before the condensation due to the superlong supercooling. Typical application example of SSSs is that SSSs could leach nearly 100% valuable metals from lithium-ion batteries cathode at low temperature, which is much higher than that by reported DESs and ILs at the same conditions. The new concept of SSSs would be very helpful for expanding the area of green solvents and green chemistry for building a greener world. 

Superlong supercooling solvents (SSSs): Alternative green solvents to ionic liquids and deep eutectic solvents for lithium-ion batteries recycling

Polyethylene glycol:acetamide (PEG:acetamide) are deemed as one of typical deep eutectic solvents (DESs) with low cost, high biodegradability and easy-synthesizing procedure in previous reports. However, there is no clear evidence validating that PEG:acetamide are DESs. The reliable evidence of DESs is phase-diagram. Here, contrary to the previous reports, we found that PEG:acetamide are not deep and not eutectic but just solvents according to the phase diagram. Acetamide owns melting point while there is no melting point for PEG. It gives us a hint that the widely-used so-called DESs (e.g., polyethylene glycol-acetamide) might not be really deep and eutectic; sometimes, they might be just common solvents. 

So-called deep eutectic solvents polyethylene glycol-acetamide are not deep and not eutectic but just solvents via phase diagram

A soluble uranium oxycarbide (UC0.4O0.6) anode was synthesized by a carbothermal reduction process, using U3O8, UO2, and graphite as raw materials, in a vacuum environment of 0.1 MPa at 1750 °C. The sintered UC0.4O0.6 exhibited excellent conductivity and stability in LiCl–KCl molten salt. The dissolution process of UC0.4O0.6 in molten salt was analyzed by linear sweep voltammetry (LSV), and the initial dissolution potential, rapid dissolution potential, and passivation potential were determined. The oxidation/reduction process of dissolved uranium ions in LiCl–KCl molten salt was studied by cyclic voltammetry (CV) and square wave voltammetry (SWV). The experimental results showed that the addition of Li2O significantly reduced the volatilization of U(VI) and increased the concentration of UO22+ in molten salt. Finally, the product was conducted by electrolysis at 1.0 V and was confirmed to be UO2 by XRD and SEM-EDS analysis. 

Preparation and Electrochemical Dissolution of a Soluble Uranium Oxycarbide Anode.

Water, supercritical fluids, ionic liquids, and deep eutectic solvents have been deemed as traditional green solvents. The increasing demand for sustainable development necessitates the exploration of innovative green solvents due to some disadvantages of the traditional green solvents. In this regard, a novel concept of “natural biomass soups (NBSs)” is introduced to be eco-friendly alternatives to traditional green solvents. NBSs represent the solvents directly prepared from natural biomass without any additional industrial purification, rendering the advantages of being cheap, simple, green, biocompatible, natural, tunable, and task-specific and avoiding the usage of any additional solvents/catalysts/additives. An exemplary application of NBSs involves their exceptional ability to efficiently extract metals from lithium-ion battery cathodes at mild temperatures. NBSs have the potential to replace ionic liquids and deep eutectic solvents and significantly expand the realm of green solvents and green chemistry. 

Natural Biomass Soups (NBSs): New Green Solvents Replacing Ionic Liquids and Deep Eutectic Solvents for Lithium-Ion Batteries Recovery

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