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Recycling and Direct-Regeneration of Cathode Materials from Spent Ternary Lithium-Ion Batteries by Hydrometallurgy: Status Quo and Developing
Abstract
The cathodes of spent ternary lithium-ion batteries (LIBs) are rich in non-ferrous metals, such as lithium (Li), nickel (Ni), cobalt (Co)and manganese (Mn), which are important strategic raw materials and also potential sources of environmental pollution. How to extract these valuable metals cleanly and efficiently from spent cathodes is of great significance for sustainable development of LIBs industry. In the light of low energy consumption, green and high recovery efficiency, this paper provides an overview on different recovery technologies to recycle valuable metals in cathode materials of spent ternary LIBs. And the development trend and application prospects on recovery strategies for cathode materials in spent ternary LIBs are simply predicted also. It is proved that the high economic recovery system of “alkaline solution dissolution/calcination pre-treatment → H2SO4 leaching → H2O2 reduction → co-precipitation regeneration NCM” will be the dominant stream for recycling retired NCM batteries soon. Furthermore, the emerging advanced technologies, such as deep eutectic solvents (DESs) extraction and one–step direct regeneration/recovery of NCM cathode materials are preferred methods to substitute conventional regeneration system in the future.
... Today, LIB recycling e.g. based on the Batrec, and Duesenfeld process, respectively, which combine mechanical and thermal treatments with hydrometallurgical methods, mainly acidic leaching in the presence of reductants [6,7]. After leaching, Ni and Co normally exist as Ni(II) and Co(II) in an acidic aqueous phase, from which they are subsequently recovered by solvent extraction, and precipitation, respectively. ...
... After leaching, Ni and Co normally exist as Ni(II) and Co(II) in an acidic aqueous phase, from which they are subsequently recovered by solvent extraction, and precipitation, respectively. Depending on the leaching agent employed, the recovery rates for Co(II) and Ni(II) range from approximately 80 to 99% [6,8,9]. Thus, considerable amounts of up to 20% of these valuable metals get lost via wastewater. ...
... Ultrapure water of type 1 was utilized in all experiments and generated with the water purification system B30 Integrity (AQUAlab, Höhr-Grenzhausen, Germany). Cobalt(II) nitrate hexahydrate (Co(NO 3 ) 2 · (H 2 O) 6 , purity > 98%), purchased from Carl Roth (Karlsruhe, Germany), and Nickel(II) nitrate hexahydrate (Ni(NO 3 ) 2 · (H 2 O) 6 , purity 99%) as well as 65 wt% Suprapur® nitric acid, delivered from Merck (Darmstadt, Germany), were applied for sample preparation. ...
Effective and sustainable separation processes for critical metals, especially for the physicochemically similar elements nickel and cobalt in battery recycling, are of great interest in the future. Selective adsorption represents a highly potential process for this purpose. In this publication, a silica adsorbent functionalized with an amino-polycarboxylate derivate (HSU331) was investigated regarding the selective adsorption of Ni(II) in the presence of Co(II) in acidic solution (pH range at equilibrium 1.8–2.3) at elevated temperature. Comparable maximum equilibrium loadings ( q max ) for Ni(II) and Co(II) of 0.59 μmol(Ni(II)) · μmol(Ligand)-1 (18.3 mg(Ni(II)) · g(Adsorbent)-1), and 0.52 μmol(Co(II)) · μmol(Ligand)-1 (16.0 mg(Co(II)) · g(Adsorbent)-1), respectively, were achieved at T = 50°C in single-component experiments. Under competitive conditions, the Ni(II) loading remained constant at 0.60 μmol(Ni(II)) · μmol(Ligand)-1 (18.4 mg(Ni(II)) · g(Adsorbent)-1), while the Co(II) loading drastically decreased to 0.09 μmol(Co(II)) · μmol(Ligand)-1 (2.7 mg(Co(II)) · g(Adsorbent)-1) in an equimolar dual-component system. Calculated stability constants of 3 · 103 and 0.7 · 103 L · mol-1, respectively, for the formed metal ion complexes of Ni(II) and Co(II) onto the adsorbent HSU331, clarify the clear selectivity of the adsorbent towards Ni(II) in the presence of Co(II) even at elevated temperature (T = 50°C).
... For example, the metal precursors for NCM are mixed (e.g., sol-gel or co-precipitation) and subject to some preprocessing, further mixed with a lithium source, and then typically undergo a two-step synthesis to generate new cathode material. For standard synthesis procedures, the first step is around 400-550 • C for 4-6 h, and the second step is around 800-1,000 • C for 12 h (Xia et al., 2009;Hua et al., 2014;Duan et al., 2021). Table 3 outlines some example re-synthesis methods. ...
... Table 3 outlines some example re-synthesis methods. Some recent hydrometallurgical methods also have proposed direct coprecipitation of the various cathode elemental compounds after dissolution and purification to produce mixed precursor that is ready to be mixed with a Li source to undergo re-synthesis (Duan et al., 2021;Ascend Elements, 2022). These processes are able to bypass the additional steps of precipitating precursor and then undergoing an additional mixing process. ...
As the global consumption of lithium-ion batteries (LIBs) continues to accelerate, the need to advance LIB recycling technologies and create a more robust recycling infrastructure has become an important consideration to improve LIB sustainability and recover critical materials to reuse in new LIB production. Battery collection, sorting, diagnostics, and second-life usage all contribute to the LIB logistics network, and developments in each of these areas can improve the ultimate recycling and recovery rate. Recent progress in LIB recycling technology seeks to increase the amount of valuable metal compounds, electrode materials, and other LIB components that are recoverable and that can be redeployed in new LIB production or other markets. This review establishes an overview of these developments and discusses the strengths and weaknesses of each major recycling technology. Of particular note are the differences in recycling technology and infrastructure requirements created by various LIB markets, as well as the techno-economic considerations for different recycling methods based on the evolving LIB formats and component compositions.
... higher in the next 30 years (Deetman et al. 2018). China is the world's largest producer of lithium-ion batteries, and its production is still increasing (Duan et al. 2020). China's grip on global battery production will reach 70% by 2021 (Prevete 2019), using a large quantity of cobalt (Zeng and Li 2015). ...
... The technology selected in this study is hydrometallurgical refining, which is consistent with all the five projects listed in Table S2. This technology has been mentioned in many papers as an international mainstream cobalt refining technology (Cerdas et al. 2018;Duan et al. 2020;Farjana et al. 2019). Consistent data sources are used in Sect. ...
Purpose
In the booming electric vehicle market, the demand for refined cobalt is showing a blowout growth. China is the largest cobalt-refiner and cobalt-importer in the world. However, the life cycle inventory and potential environmental impact from cobalt refining in China have not been clearly illustrated. This paper builds a comprehensive inventory to support the data needs of downstream users of cobalt sulfate. A “cradle-to-gate” life cycle assessment was conducted to provide theoretical support to stakeholders.
Methods
A life cycle assessment was performed based on ISO 14040 to evaluate the potential environmental impact and recognize the key processes. The system boundary of this study contains four stages of cobalt sulfate production: mining, beneficiation, primary extraction, and refining. Except for the experimental data used in the primary extraction stage, all relevant data are actual operating data. The normalization value was calculated based on the latest released global emission and extraction data.
Results and discussion
Normalization results show that the potential impacts of cobalt refining were mainly concentrated in the fossil depletion and freshwater ecotoxicity categories. The beneficiation stage and the refining stage account for 72% and 26% of the total normalization value, respectively. The beneficiation stage needs to consume a lot of chemicals and energy to increase the cobalt content, due to the low grade of cobalt ore in China. Compared with cobalt concentrate, the use of cobalt-containing waste (e.g., cobalt waste from EV batteries) can ease endpoint impact by up to 73%. With the application of the target electricity structure in 2050, the potential impact of China’s cobalt sulfate production on global warming, fossil depletion, and particulates formation can be reduced by 24%, 22%, and 26%, respectively.
Conclusion
Findings indicate that the chemical inputs and electricity consumption are primary sources of potential environmental impact in China’s cobalt sulfate production. Promoting the development of urban mines can reduce excessive consumption of chemicals and energy in the beneficiation stage. The environmental benefits of transforming the electricity structure and using more renewable energy to reduce dependence on coal-based power in the cobalt refining industry were revealed.
... Compared with the above methods, hydrometallurgy has been used in many factories to recycle worthy metals. Because it is highly efficient, has low energy consumption, and has low toxic emissions [22,23]. The hydrometallurgy processes typically use inorganic acids, such as H 2 SO 4 , HCl, and HNO 3, and organic acids, such as DL-malic acid, formic acid, and citric acid, for leaching [24][25][26][27]. ...
With the goal of carbon neutrality, increasing end-of-life spent lithium-ion batteries (LIBs) is inevitable owing to the rapidly growing number of electric vehicles worldwide, which brings management and environmental problems. Nevertheless, the scarcity of valuable metals used in LIBs and the potential value of recycling them have attracted increased interest in recovering spent LIBs. The traditional methods for recycling spent LIBs, pyrometallurgy, and hydrometallurgy cause energy waste and environmental problems. Herein, green reagents, ascorbic acid, is introduced to reduce the amount of strong acid and help in-site precipitate the ternary precursor in this novel process for the recovery of spent LiNi0.5Co0.2Mn0.3O2 (NCM523). A reduction reaction caused by ascorbic acid occurs on the surface of the material, determining the chemical reaction that controls the leaching process and enhances leaching efficiency. The ternary precursor is formed in-site by oxidative precipitation in the leaching solution, which exists ascorbic acid. The regenerated NCM523 shows a high discharge capacity (158.5 mAh g−1 at 0.1C), and the capacity retention rate is 83.7% after 100 cycles. This ascorbic acid coordinated leaching in the sulfuric acid system following in-site precipitation is an environmentally friendly treatment for spent LIBs, which has the potential to be applied in the industry.
... [50,51] Surprisingly, DESs not only show the advantages of high selectivity, low cost and recyclability in metal leaching process, [52] but also reflect the characteristics of green chemistry, that is, they can efficiently extract metal elements without producing harmful substances (Figure 2), so it is considered as the preferred method to replace the traditional battery regeneration scheme. [53,54] ...
The Lithium‐ion battery (LIB) is one of the main energy storage equipment. Its cathode material contains Li, Co, and other valuable metals. Therefore, recycling spent LIBs can reduce environmental pollution and resource waste, which is significant for sustainable development. However, traditional metallurgical methods are not environmentally friendly, with high cost and environmental toxicity. Recently, the concept of green chemistry gives rise to environmental and efficient recycling technology, which promotes the transition of recycling solvents from organic solvents to green solvents represented by deep eutectic solvents (DESs). DESs are considered as ideal alternative solvents in extraction processes, attracting great attention due to their low cost, low toxicity, good biodegradability, and high extraction capacity. It is very important to develop the DESs system for LIBs recycling for sustainable development of energy and green economic development of recycling technology. In this work, the applications and research progress of DESs in LIBs recovery are reviewed, and the physicochemical properties such as viscosity, toxicity and regulatory properties are summarized and discussed. In particular, the toxicity data of DESs are collected and analyzed. Finally, the guidance and prospects for future research are put forward, aiming to explore more suitable DESs for recycling valuable metals in batteries.
... By the year 2027, the goal is to achieve a 50% recovery rate, which is expected to further increase to 80% by 2031 [156,157]. The recovery of nickel, cobalt, and lithium will also be fully commercially viable in future [158,159]. Nickel-based batteries have a long life and are very reliable. Recycling efficiency should increase from the current 79% (active materials at 50%) to 80-85% (active materials at 55-60%) by 2030 to reach a break-even business model [160]. ...
Battery technologies have recently undergone significant advancements in design and manufacturing to meet the performance requirements of a wide range of applications, including electromobility and stationary domains. For e-mobility, batteries are essential components in various types of electric vehicles (EVs), including battery electric vehicles (BEVs), plug-in hybrid electric vehicles (PHEVs), and fuel cell electric vehicles (FCEVs). These EVs rely on diverse charging systems, including conventional charging, fast-charging, and vehicle-to-everything (V2X) systems. In stationary applications, batteries are increasingly being employed for the electrical management of micro/smart grids as transient buffer energy storage. Batteries are commonly used in conjunction with power electronic interfaces to adapt to the specific requirements of various applications. Furthermore, power electronic interfaces to batteries themselves have evolved technologically, resulting in more efficient, thermally efficient, compact, and robust power converter architectures. This article offers a comprehensive review of new-generation battery technologies. The topic is approached from the perspective of applications, emerging trends, and future directions. The article explores new battery technologies utilizing innovative electrode and electrolyte materials, their application domains, and technological limitations. In conclusion, a discussion and analysis are provided, synthesizing the technological evolution of batteries while highlighting new trends, directions, and prospects.
... The existing research on recycling lithium-ion batteries is mainly focused on the recovery of high-valuable metals like cobalt, nickel, manganese, and lithium in the cathode materials [5][6][7][8][9][10][11]. Although extensive investigations have been carried out on the typical • They have many complicated separation steps and overall, recycling routes are often complex; • Secondary pollution occurs due to the elimination of impurities and precipitation of metal ions using different solvents, acids, and alkalis in the conventional recycling process; • Some valuable materials lost in the recycling process; • High intake of chemicals, the low recovery efficiency of valuable metallic elements from spent cathode materials, costly solvents, and intricate recycling routes in the techniques of chemical precipitation, solvent extraction, or ion-exchange method are hindering the large-scale application of the hydrometallurgical technique in the industry; • Traditional approaches to recycling cathode materials (pyrometallurgical or hydrometallurgical processes) cannot handle the complex system of LIBs (i.e., the mixture of cathodes such as LCO, LMO, NMC, and LFP); • ...
Research on the regeneration of cathode materials of spent lithium-ion batteries for resource reclamation and environmental protection is attracting more and more attention today. However, the majority of studies on recycling lithium-ion batteries (LIBs) placed the emphasis only on recovering target metals, such as Co, Ni, and Li, from the cathode materials, or how to recycle spent LIBs by conventional means. Effective reclamation strategies (e.g., pyrometallurgical technologies, hydrometallurgy techniques, and biological strategies) have been used in research on recycling used LIBs. Nevertheless, none of the existing reviews of regenerating cathode materials from waste LIBs elucidated the strategies to regenerate lithium nickel manganese cobalt oxide (NCM or LiNixCoyMnzO2) cathode materials directly from spent LIBs containing other than NCM cathodes but, at the same time, frequently used commercial cathode materials such as LiCoO2 (LCO), LiFePO4 (LFP), LiMn2O4 (LMO), etc. or from spent mixed cathode materials. This review showcases the strategies and techniques for regenerating LiNixCoyMnzO2 cathode active materials directly from some commonly used and different types of mixed-cathode materials. The article summarizes the various technologies and processes of regenerating LiNixCoyMnzO2 cathode active materials directly from some individual cathode materials and the mixed-cathode scraps of spent LIBs without their preliminary separation. In the meantime, the economic benefits and diverse synthetic routes of regenerating LiNixCoyMnzO2 cathode materials reported in the literature are analyzed systematically. This minireview can lay guidance and a theoretical basis for restoring LiNixCoyMnzO2 cathode materials.
Waste recycling as secondary source has become important from the environmental perspective and the circular economy. In this context, any waste can become raw material to manufacture other products, such as nanoparticles. Thus, this study aims to provide a descriptive and critical view of metal recovery techniques and later use them as raw materials for nanoparticle synthesis. After scoping searches, an investigation was carried out and found a gap in the research on synthesizing nanoparticles from secondary sources. The possible technologies to recover metals are hydrometallurgical processes, pyrolysis, and bioleaching followed by purification processes. The advantages and disadvantages were discussed. Based on this analysis, hydrometallurgical processing was identified as the most suitable method and, consequently, the most used method for synthesizing nanoparticles. There is a difference in the size and shapes of nanoparticles synthesized by secondary sources and commercial salts.
The huge amount of degraded NCM (LiNi0.5Co0.2Mn0.3O2) cathode materials from spent lithium-ion batteries is arising as a serious environmental issue as well as a severe waste of metal resources, and therefore, direct recycling of them toward usable electrode materials again is environmentally and economically more attractive in contrast to present metallurgical treatments. In this work, we design a robust two-step method for direct recycling of degraded NCM materials, which uses the aluminum impurity from the attached current collector to supplement the transition metal vacancies for simultaneous elemental compensation and structural restoration. This single-element compensation strategy leads to the regeneration of high-quality NCM material with depressed cation disordering and stabilized layered structure. Moreover, the regenerated NCM material with controllable Al doping delivered an outstanding electrochemical performance; specifically, the capacity (158.6 mAh g-1), rate capability (91.6 mAh g-1 at 5 C), and cycling stability (89.6% capacity retention after 200 cycles) of the regenerated NCM material are even comparable with those of fresh materials. The as-established regeneration protocol has its chance in simplifying the industrial recycling process of degraded NCM materials.
Fluoride contained in the leaching solution of spent lithium-ion batteries (LIBs) not only decreased product quality, but also led to severe equipment corrosion and potential environmental hazards. Therefore, a coordination extraction system using di-(2-ethylhexyl) phosphoric acid (D2EHPA) loaded with aluminum ions (Al³⁺) as extractant was designed to deeply remove fluoride from the sulfate leaching solution of spent LIBs that combined the excellent binding affinity of Al³⁺ to fluoride and the perfect chemical efficiency of solvent extraction. The effects of D2EHPA concentration, loaded Al³⁺ concentration, equilibrium pH and shaking time on the extraction efficiency of fluoride were investigated. Experimental results indicated that over 99% of fluoride was selectively extracted and the fluoride concentration in the leaching solution of spent LIBs was reduced from 210 mg/L to 2 mg/L by single-stage extraction, meeting the requirement of fluoride content in the battery grade Ni/Co/Mn sulfate solution and the wastewater discharge standards. The loaded organic phase was scrubbed and stripped by diluted H2SO4, and fluoride could be fully stripped into the stripping solution. Further characterization studies revealed that Al³⁺ and D2EHPA may mainly coordinate in the form of AlL3·HL in the Al-loaded organic phase (HL denotes D2EHPA). After the Al-loaded organic phase was contacted with solution containing fluoride, a structure of AlFL2·HL coordinated with F⁻ was formed. This study provides a novel technical approach to improve product quality and reduce fluoride wastewater pollution for the recycling process of spent LIBs.
This study provides a method for selective recovery of manganese after acid leaching from NCM-based cathode active material of spent lithium-ion secondary batteries (LIBs). The mechanism of this method involves Mn(II) generated in the NCM material as an reducing agent in sulfate media, so that nickel and cobalt are reduced and dissolved in a solution by Mn(II), in which Mn(II) is oxidized as MnO2 precipitate. The effect of leaching time, leaching temperature, and acid concentration on the leaching behavior of valuable metals were investigated. After the primary and secondary leaching, the leaching of Co and Ni were improved to 99% and 100%, respectively, while leaching of Mn was 15.5% (167 mg/L in the leachate). The residue after leaching was analyzed by XRD indicates that it mainly consists of manganese (hydr)oxide which contain Mn 40%. After roasting of the Mn-rich residue at 650°C, the phase was converted to Mn2O3 and Mn3O4 in which Mn contents enhanced about 70%.
Unlike common solvent extraction and chemical precipitation, a novel extraction-precipitation process for the separation of Li and transition metals using p-tertylphenoxyacetic acid (POAA) is developed. Extraction-precipitation method refers to a method in which the extraction-precipitant can quantitatively extract the metal ions to form precipitate without the requirement of organic solvent or carrier, and the extraction-precipitant can be stripped and recycled. In this study, the extraction-precipitation mechanism and thermodynamic parameters between POAA and manganese (Mn), cobalt (Co), nickel (Ni) were analyzed. Subsequently, the equilibrium time and pH value of the separation process were optimized. Finally, the leach solution of LIB having Li, Ni, Co, Mn with concentration of 3.52 g/L, 7.93 g/L, 5.72 g/L, and 14.16 g/L, respectively, was studied for the separation at pH 4.5. The results indicate that efficient separation of Li and transition metals was possible by one-step precipitation using 0.2 mol/L POAA solution (degree of saponification = 100%) when the ratio of nPOAA/nMn+Co+Ni was 2. The separation factor for the transition metals over lithium (βCoNiMn/βLi) reached as high as 133,014. After the transition metal-loaded POAA was stripped with 2 mol/L sulfuric acid, the stripped solution could be used for the production of ternary material precursor, and the regenerated POAA could be recycled for the extraction-precipitation process. The lithium in the solution was recovered in the form of lithium carbonate (Li2CO3) with a purity level of 97.7%. This high efficiency and sustainable process based on extraction-precipitation has shown potential application for spent LIB recovery.
To control the power hierarchy design of lithium-ion battery (LIB) built-up sets for electric vehicles (EVs), we offer intensive theoretical and experimental sets of choice anode/cathode architectonics that can be modulated in full-scale LIB built-up models. As primary structural tectonics, heterogeneous composite superstructures of full-cell-LIB (anode//cathode) electrodes were designed in closely packed flower agave rosettes TiO 2 @C (FRTO@C anode) and vertical-star-tower LiFePO 4 @C (VST@C cathode) building blocks to regulate the electron/ion movement in the three-dimensional axes and orientation pathways. The superpower hierarchy surfaces and multi-directional orientation components may create isosurface potential electrodes with mobile electron movements, in-to-out interplay electron dominances, and electron/charge cloud distributions. This study is the first to evaluate the hotkeys of choice anode/cathode architectonics to assemble different LIB–electrode platforms with high-mobility electron/ion flows and high-performance capacity functionalities. Density functional theory calculation revealed that the FRTO@C anode and VST-(i)@C cathode architectonics are a superior choice for the configuration of full-scale LIB built-up models. The integrated FRTO@C//VST-(i)@C full-scale LIB retains a huge discharge capacity (~ 94.2%), an average Coulombic efficiency of 99.85% after 2000 cycles at 1 C, and a high energy density of 127 Wh kg ⁻¹ , thereby satisfying scale-up commercial EV requirements.
With the rapid growth of the lithium‐ion battery (LIBs) market, recycling and re‐use of end‐of‐life LIBs to reclaim lithium (Li) and transition metal (TM) resources (e.g., Co, Ni), as well as eliminating pollution from disposal of waste batteries, has become an urgent task. Here, for the first time the ambient‐pressure relithiation of degraded LiNi0.5Co0.2Mn0.3O2 (NCM523) cathodes via eutectic Li⁺ molten‐salt solutions is successfully demonstrated. Combining such a low‐temperature relithiation process with a well‐designed thermal annealing step, NCM523 cathode particles with significant Li loss (≈40%) and capacity degradation (≈50%) can be successfully regenerated to achieve their original composition and crystal structures, leading to effective recovery of their capacity, cycling stability, and rate capability to the levels of the pristine materials. Advanced characterization tools including atomic resolution electron microscopy imaging and electron energy loss spectroscopy are combined to demonstrate that NCM523's original layered crystal structure is recovered. For the first time, it is shown that layer‐to‐rock salt phase change on the surfaces and subsurfaces of the cathode materials can be reversed if lithium can be incorporated back to the material. The result suggests the great promise of using eutectic Li⁺ molten–salt solutions for ambient‐pressure relithiation to recycle and remanufacture degraded LIB cathode materials.
As the consumption of lithium-ion batteries (LIBs) for the transportation and consumer electronic sectors continues to grow, so does the pile of battery waste, with no successful recycling model, as exists for the lead–acid battery. Here, we exhibit a method to recycle LIBs using deep eutectic solvents to extract valuable metals from various chemistries, including lithium cobalt (iii) oxide and lithium nickel manganese cobalt oxide. For the metal extraction from lithium cobalt (iii) oxide, leaching efficiencies of ≥90% were obtained for both cobalt and lithium. It was also found that other battery components, such as aluminium foil and polyvinylidene fluoride binder, can be recovered separately. Deep eutectic solvents could provide a green alternative to conventional methods of LIB recycling and reclaiming strategically important metals, which remain crucial to meet the demand of the exponentially increasing LIB production.
Nickel–manganese–cobalt oxides, with LiNi0.33Mn0.33Co0.33O2 (NMC) as the most prominent compound, are state-of-the-art cathode materials for lithium-ion batteries in electric vehicles. The growing market for electro mobility has led to a growing global demand for Li, Co, Ni, and Mn, making spent lithium-ion batteries a valuable secondary resource. Going forward, energy- and resource-inefficient pyrometallurgical and hydrometallurgical recycling strategies must be avoided. We presented an approach to recover NMC particles from spent lithium-ion battery cathodes while preserving their chemical and morphological properties, with a minimal use of chemicals. The key task was the separation of the cathode coating layer consisting of NMC, an organic binder, and carbon black, from the Al substrate foil. This can be performed in water under strong agitation to support the slow detachment process. However, the contact of the NMC cathode with water leads to a release of Li+ ions and a fast increase in the pH. Unwanted side reactions may occur as the Al substrate foil starts to dissolve and Al(OH)3 precipitates on the NMC. These side reactions are avoided using pH-adjusted solutions with sufficiently high buffer capacities to separate the coating layer from the Al substrate, without precipitations and without degradation of the NMC particles.
Li-rich manganese-based layered cathode Li1.2Mn0.54Ni0.13Co0.13O2 (LMNCO) nanotubes are synthesized by electrospinning and surface coated with different amounts of amorphous Al2O3. The effects of the coating content of Al2O3 on the structural and electrochemical performances of LMNCO nanotubes are investigated systematically. The results show that the morphologies and structures of the samples exhibit no apparent changes after being coated with Al2O3. Electrochemical tests indicate that the Al2O3-coated LMNCO nanotubes exhibit obviously enhanced electrochemical performances. The initial coulombic efficiency of surface modified LMNCO nanotubes increased from 74.9% to 85.2%, and the modified LMNCO nanotubes have a high capacity retention of 97.6% after 90 cycles at 1C. The improved electrochemical performances of the coated samples are attributed to the protective function of the uniform Al2O3 coating and the three-dimensional Li⁺ diffusion channel in the spinel interface layer.
Traction batteries are a key factor in the environmental sustainability of electric mobility and, therefore, it is necessary to evaluate their environmental performance to allow a comprehensive sustainability assessment of electric mobility. This article presents an environmental assessment of a lithium-ion traction battery for plug-in hybrid electric vehicles, characterized by a composite cathode material of lithium manganese oxide (LiMn2O4) and lithium nickel manganese cobalt oxide Li(NixCoyMn1-x-y)O2. Composite cathode material is an emerging technology that promises to combine the merits of several active materials into a hybrid electrode to optimize performance and reduce costs. In this study, the environmental assessment of one battery pack (with a nominal capacity of 11.4 kWh able to be used for about 140,000 km of driving) is carried out by using the Life Cycle Assessment methodology consistent with ISO 14040. The system boundaries are the battery production, the operation phase and recycling at the end of life, including the recovery of various material fractions. The composite cathode technology examined besides a good compromise between the higher and the lower performance of NMC and LMO cathodes, can present good environmental performances.
The results of the analysis show that the manufacturing phase is relevant to all assessed impact categories (contribution higher than 60%). With regard to electricity losses due to battery efficiency and battery transport, the contribution to the use phase impact of battery efficiency is larger than that of battery transport. Recycling the battery pack contributes less than 11% to all of the assessed impact categories, with the exception of freshwater ecotoxicity (60% of the life cycle impact). The environmental credits related to the recovery of valuable materials (e.g. cobalt and nickel sulphates) and other metal fractions (e.g. aluminium and steel) are particularly relevant to impact categories such as marine eutrophication, human toxicity and abiotic resource depletion.
The main innovations of this article are that (1) it presents the first bill of materials of a lithium-ion battery cell for plug-in hybrid electric vehicles with a composite cathode active material; (2) it describes one of the first applications of the life cycle assessment to a lithium-ion battery pack for plug-in hybrid electric vehicles with a composite cathode active material with the aim of identifying the “hot spots” of this technology and providing useful information to battery manufacturers on potentially improving its environmental sustainability; (3) it evaluates the impacts associated with the use phase based on primary data about the battery pack's lifetime, in terms of kilometres driven; and (4) it models the end-of-life phase of the battery components through processes specifically created for or adapted to the case study.
The rapid growth of lithium ion batteries (LIBs) for portable electronic devices and electric vehicles has resulted in an increased number of spent LIBs. Spent LIBs contain not only dangerous heavy metals but also toxic chemicals that pose a serious threat to ecosystems and human health. Therefore, a great deal of attention has been paid to the development of an efficient process to recycle spent LIBs for both economic aspects and environmental protection. In this paper, we review the state-of-the-art processes for metal recycling from spent LIBs, introduce the structure of a LIB, and summarize all available technologies that are used in different recovery processes. It is notable that metal extraction and pretreatment play important roles in the whole recovery process, based on one or more of the principles of pyrometallurgy, hydrometallurgy, biometallurgy, and so forth. By further comparing different recycling methods, existing challenges are identified and suggestions for improving the recycling effectiveness can be proposed.
The paper focuses on the improved process of metal recovery from lithium-ion batteries (LIBs) lithium nickel manganese cobalt oxide (NMC) cathode waste materials by using hydrometallurgical methods. In the acid leaching step, the essential effects of acidity concentration, H2O2 concentration, leaching time, liquid-solid mass ratio, and reaction temperature with the leaching percentage were investigated in detail. The cathode material was leached with 2M H2SO4 and 10 vol. % H2O2 at 70 °C and 300 rpm using a liquid-solid mass ratio of 30 mL/g. In order to complete the recovery process, this paper designs the proper separation process to recover valuable metals. The leach liquor in the recovery process uses Cyanex 272 to first extract Co and Mn to the organic phase. Secondly, Co and Mn are separated by using D2EHPA, and a high purity of Co is obtained. Thirdly, Ni is selectively precipitated by using DMG, and Ni is completely formed as a solid complex. Finally, in the chemical precipitation process, the remaining Li in the leach liquor is recovered as Li2CO3 precipitated by saturated Na2CO3, and Co, Mn, and Ni are recovered as hydroxides by NaOH. This hydrometallurgical process may provide an effective separation and recovery of valuable metals from LIBs waste cathode materials.
Tremendous efforts are being made to develop electrode materials, electrolytes, and separators for energy storage devices to meet the needs of emerging technologies such as electric vehicles, decarbonized electricity, and electrochemical energy storage. However, the sustainability concerns of lithium-ion batteries (LIBs) and next-generation rechargeable batteries have received little attention. Recycling plays an important role in the overall sustainability of future batteries and is affected by battery attributes including environmental hazards and the value of their constituent resources. Therefore, recycling should be considered when developing battery systems. Herein, we provide a systematic overview of rechargeable battery sustainability. With a particular focus on electric vehicles, we analyze the market competitiveness of batteries in terms of economy, environment, and policy. Considering the large volumes of batteries soon to be retired, we comprehensively evaluate battery utilization and recycling from the perspectives of economic feasibility, environmental impact, technology, and safety. Battery sustainability is discussed with respect to life-cycle assessment and analyzed from the perspectives of strategic resources and economic demand. Finally, we propose a 4H strategy for battery recycling with the aims of high efficiency, high economic return, high environmental benefit, and high safety. New challenges and future prospects for battery sustainability are also highlighted.
Spent lithium ion battery (LIB) recovery is becoming quite urgent for environmental protection and social needs due to the rapid progress in LIB industries. However, recycling technologies cannot keep up with the exaltation of the LIB market. Technological improvement of processing spent batteries is necessary for industrial application. In this paper, spent LIB recovery processes are classified into three steps for discussion: gathering electrode materials, separating metal elements, and recycling separated metals. Detailed discussion and analysis are conducted in every step to provide beneficial advice for environmental protection and technology improvement of spent LIB recovery. Besides, the practical industrial recycling processes are introduced according to their advantages and disadvantages. And some recommendations are provided for existing problems. Based on current recycling technologies, the challenges for spent LIB recovery are summarized and discussed from technological and environmental perspectives. Furthermore, great effort should be made to promote the development of spent LIB recovery in future research as follows: (1) gathering high-purity electrode materials by mechanical pretreatment; (2) green metals leaching from electrode materials; (3) targeted extraction of metals from electrode materials.
Given exceptional specific discharge capacity, excellent energy density, high rate capability, fast charge capacity, and long-term cycling stability, large-scale giant porous complex super-architectonics (GPS) integrated into anode/cathode complex geometrics improve the full-model lithium ion batteries (LIBs). We examine the integration of a series of anode and cathode (GPS) super-architectonics into half- and full-cell LIB models to allow non-prescriptive charge/discharge cycles, and to achieve spatial rate performance capabilities. As a distinguishable GPS model, the super-architectonics included multi-directional orientation geometrics, building-blocks egress/ingress pathways, and giant loophole-on-surface topographies of ripples, irregular bumps, undulations, and anticlines offer a set of fully functional multi-axial/dimension GPS cathode- and anode-electrode geometrics and multi-gate-in-transports of electron/Li⁺ ions in diverse pathways. Our precisely defined GPS-modulated LIB models generate high-power and volumetric-energy density, excellent long-term cycling durability without deterioration in its capacity under a high energy density, and a comparable high tap density. GPS-integrated LIB modules provide superior durability (i.e., maintaining high specific capacity ~77.5% within long-term life period of 2000 cycles) and average Coulombic efficacy of ~99.6% at 1 C. Powerful and robust super-architectonic GPS building-blocks-in full-scale LIB designs offer outstanding specific energy density of ≈179 Wh kg–1 for a future market of LIB-EVs with longest driving range. The key leap super-surface topographies of LIB-GPS modules are critical in creating ever-changing charge/discharge cycle, “fully cycled dynamics,” affordable on-/off-site storage, and super-large door-in transport of Li⁺-ion/electron, thereby highlighting its promising storage modules and rechargeable lithium batteries.
Inspired by the desert terrain, three-dimensional (3D) hierarchical LiNi0.5Mn1.5O4 desert-waves (LNMO-DW) composed of primary two-dimensional (2D) nanodiscs is synthesized via a template-free route. The 3D hierarchical LNMO-DW reveals good structural interconnectivity and extends infinitely in a wide area similar to the desert, thus triggering fast electrode kinetics and abundant electroactive zones by enabling multi-directional ionic/electronic transmissions. The rate capability and cycling stability of LNMO-DW are improved to a superior level compared to the control groups and other reported works, which proves that 3D hierarchical desert-waves-like structure is one of the optimal structures for LNMO cathodes. Its specific capacity reaches 130 mAh g⁻¹ at 10 C after 200 cycles, together with capacity retention of 91%. Noticeably, even when cycling at the high rates of 15 and 20 C after 200 cycles, the discharge capacities are still up to 117 and 108 mAh g⁻¹, respectively. The corresponding structural formation mechanisms and electrochemical principles have also been unraveled.
Ni-rich layered LiNi1-x-yMnxCoyO2 (NMC, x+y<0.5) oxides have been demonstrated to be dominant cathode materials for high-energy lithium ion batteries. However, NMC cathode materials with high Ni contents usually show unsatisfied capacity decay and voltage fading cycled at high voltages, owing to aggravated side reactions and electrochemical irreversibility during prolonged lithiation/delithiation cycles. Here, we report the Mn-rich Li0.65Mn0.59Ni0.12Co0.13Oδ (marked as LMNCO) material that is integrated of layered Li2MnO3 and spinel LiMn1.5Ni0.5O4-type components as a desired shell for improving high-voltage cycling stability of the Ni-rich LiNi0.8Mn0.1Co0.1O2 (marked as NMC811) cathode material. The core-shell-structured NMC811@x% LMNCO materials have been fabricated in satisfied structural conformality by using an initial sonofragmentation, followed by the solvent evaporation-induced self-assembly (EISA) and post-annealing processes. The optimized NMC811@5% LMNCO cathode material can deliver an initial discharge capacity of 150.0 mAh g-1 at 5 C (1 C=200 mA g-1) in a voltage range of 2.7-4.6 V vs. Li+/Li with 83.4 % retention up to 500 cycles, significantly superior to that (75.6 %) of the bare NMC811 material. The Mn-rich shell also enables to effectively stabilize Ni-rich cathode materials for long-term cycles in such a high voltage range at 55 °C. In addition, this work offers a synthetic prototype for the conformal core-shell-structured fabrications, which could be adopted for the surface modification of various functional materials to achieve enhanced performance in device applications.
The recovery of waste lithium-ion batteries (LIBs) is an intensively studied worldwide because of environmental pollution and the risk of undersupply of a strategic raw material. Traditional technologies have poor selectivity for lithium recovery from waste LIBs. Metallic Ni, Co, and Mn are usually recovered by leaching, precipitation, and solvent extraction. These recycling methods are costly and have a long recycling route and high potential for secondary waste generation. In this paper, a mechanochemical activation approach was proposed for the selective recycling of lithium and recovery of Ni0.5Mn0.3Co0.2(OH)2 from spent LiNi0.5Mn0.3Co0.2O2 batteries. The leaching efficiency and Li selectivity were found to be 95.10% and 100%, respectively. The structure of Ni0.5Mn0.3Co0.2(OH)2 was investigated using various characterisation techniques. The selective reaction mechanism of mechanochemical activation was identified. High-purity Li2CO3 (99.96 wt%) was obtained. Electrochemical tests showed that the performance of Ni0.5Mn0.3Co0.2(OH)2 was comparable to that of a commercial oxygen evolution reaction catalyst (IrO2). This research demonstrates an effective and shorter route from waste to a functional material during recycling spent LIBs that incorporates the principles of green chemistry and shows great potential for practical application.
The separation of cathode materials from aluminum (Al) foil is a key issue worthy of attention in the process of resource utilization of spent lithium-ion batteries (LIBs). Traditional technologies for the Al foil and cathode materials separation have the disadvantages of the use of corrosive acid/alkali, release of HF hazards, and environment and healthy risks of the toxicity reagent. In this study, a low-toxicity, high-efficiency, and low-cost deep eutectic solvent (DES), choline chloride-glycerol, was synthesized and applied to solving the separation dilemma of Al foil and cathode materials in spent LIBs. The experimental results show that separation of the Al foil and cathode materials can be achieved under optimal conditions designed by the response surface method: heating temperature 190 ℃, choline chloride: glycerol molar ratio 2.3:1, and heating time 15.0 min; the peeling percentage of cathode material can reach 99.86 wt%. Mechanism analysis results confirm that the separation of Al foil and cathode materials was the result of the deactivation of the organic binder polyvinylidene fluoride (PVDF), which can be attributed to an alkali degradation process caused by the attack of the hydroxide of choline chloride on the acidic hydrogen atom in PVDF.
Li-rich Mn-based layered oxide Li1.2Mn0.54Ni0.13Co0.13O2 (LMNCO) has received great interest due to its high discharge capacity. However, the fast capacity attenuation seriously hinders its wide application. LMNCO particles are synthesized via a co-precipitation method. To enhance the cycle stability, (Ni0.4Co0.2Mn0.4)1-xTix(OH)2+2x surface layer is deposited on LMNCO precursor particles by a second co-precipitation process. Due to the mutual diffusion of elements during sintering, Ti is distributed in the 2–3 μm shell of particles. The cells are cycled in a voltage window of 2.0–4.8 V at 0.5C. After 200 cycles, LMNCO exhibits a capacity retention of 43%, and LMNCO particles have been pulverized by the cycle process. In contrast, the structural integrity of coated particles is maintained, and therefore the cycle stability is evidently improved.
The present work focuses on simultaneous recycling of Li and
Co from crushed products of mixed electrode materials using mixed
organic acids, in which benzenesulfonic acid and formic acid were
cooperatively used as the leaching reagents. Results show that the optimal leaching efficiency of 97% Co and 99% Li were obtained under the conditions of 1.3mol/L benzenesulfonic acid, 1.5 mol/L formic acid, a solid to liquid (S/L) ratio of 30g/L, and 40 min reaction time at 50°C. Meanwhile, the leaching of Li and Co fits well to logarithmic rate model with apparent activation energy of 32.7 and 47.0 kJ/mol in this given leaching system, respectively. Besides, cobalt was directly recovered from the leach liquor as pure cobalt benzene sulfonic with the recovery efficiency of 99%, and lithium can be entirely precipitated by adding phosphoric acid. Further, the reaction mechanism involves the leachinghydrating-complexing model of LiCoO2 particles was proposed based on the dissolution behavior of metals and then verified by morphological and phase characterization (i.e. FT-IR, XRD and SEM-EDS) of the recycling product. The whole process is found to be effective and sustainable for recovery of Li, Co and graphite from mixed industrial crushing product of spent LIBs.
The technology for recycling the spent coin cells is pressing needed due to a large amount of generated spent coin cells. However, there is little information about the recycling technology of spent coin cells. In this work, a two-step bioleaching method for recovery of metals from spent coin cells by Acidithiobacillus thiooxidans is performed for the first time. In this regard, the growth characteristics of A. thiooxidans was investigated in pure culture and during the two-step bioleaching approach. The highest recovery of Li, Co and Mn was achieved at a pulp density of 30 g L-1, in values of 99%, 60%, and 20%, respectively. The structural analyzes confirmed the progress of bioleaching process. In addition, the kinetics models showed that the chemical reaction was the rate-controlling step of the two-step bioleaching of spent coin cells. The comparative results between bioleaching and chemical leaching showed that Acidithiobacillus thiooxidans can enhance the leaching of metals. Toxicity characteristic leaching procedure of the spent coin cells powder demonstrated that the bioleached residue met the environmental limitations for safe disposal. In fact, bioleaching is an effective and promising route to reduce the environmental hazard of spent coin cells.
The valuable metals in the cathode of spent lithium-ion batteries (LIBs) have been recovered by a more simple and efficient process. The cathode was leached directly by citric acid without pretreatment such as immersed in N-methyl-pyrrolidone (NMP) or calcined. The leaching conditions of the concentration of citric acid, H2O2 dosage, reaction temperature, reaction time and solid-to-liquid ratio on the leaching efficiency have been discussed. Results show that under the condition of 1.0 M citric acid, 8% (Vhydrogen peroxide/Vcitric acid) hydrogen peroxide, reaction temperature of 70 °C, leaching time of 70 min and solid-to-liquid ratio of 40 g/L, the leaching rate reached 99%. The leaching solution could be used to prepare new cathode materials of LIBs, and the detached aluminum foil and residue were recycled. The leaching solution has been dried and detected, and the result shows that the product is the mixture of citrate and citric acid. The chelating of the cobalt and lithium ions with the citrate plays an important role in improving the leaching efficiency.
In this work, an excellent ionic conductor Li3PO4 was deposited on the surface of LiNi0.8Mn0.1Co0.1O2 by a hydrothermal treatment method. This method avoided contact between the active material and water, and required only one step of calcination to obtain the product. The X-ray photoelectron spectroscopy (XPS) results indicated that the Li3PO4 coating layer had a protective effect which can greatly suppress the reaction of active material with the air and the electrolyte. Besides that, the Li3PO4 layer provided fast channels for lithium ions migration, and effectively inhibited the growth of SEI film and decreased the charge transfer resistance at the interface between the electrode and electrolyte. Therefore, the coated materials had excellent rate capability and cycle performance. The lithium ions diffusion (DLi+) of H-LPO&NMC was enhanced to the range of 10⁻¹³-10⁻¹² cm² s⁻¹, while that of the bared material was only about 10⁻¹⁵-10⁻¹³ cm² s⁻¹.
A novel hydrometallurgical process for recycling LiNi0.5Co0.2Mn0.3O2 cathode materials harvested from spent Li-ion batteries (LIBs) is established in this work. The cathode material LiNi0.5Co0.2Mn0.3O2 is dissolved in a mixed acid containing phosphoric acid (leaching agent) and citric acid (leaching agent and reductant). Using 0.2 M phosphoric acid and 0.4 M citric acid with a solid to liquid (S/L) ratio of 20 g/L at 90 °C for 30 min, the proposed method results in a leaching efficiency of ca. 100% for Li, 93.38% for Ni, 91.63% for Co, and 92.00% for Mn, respectively. Kinetics of the leaching process is well described by the Avrami equation. It is found that the leaching process is controlled by surface chemical reactions, and the apparent activation energies (kJ/mol) are 45.83 for Li, 83.01 for Ni, 81.38 for Co and 92.35 for Mn, respectively. With aids of various advanced characterizations methods, including UV–Vis, FT-IR and TOC, we find that there are a great deal of citrates and a small amount of dihydrogen phosphates in the mixed acid leachate. This leaching method enjoys advantages of low acid consumption, short leaching time and no need to add extra reductant.
Cobalt (Co) recycling from the spent LIBs not only favors the ecological protection also meets the supply chain of Co in the international market. In this research, a three-dimensional microbial-fuel-cell (3D-MFC) two-chamber system with granular activated carbon (GAC) microelectrodes was constructed to remove and recover Co from the stripping cobalt sulfate solution. The 3D bio-electrochemical (BE) system exhibited the largest voltage output and power production at 12th day during the acclimation, achieving the maximum power densities (W/m³) of 6.24, 10.29, 14.52, 12.59, and 8.78, respectively. The GAC prepared at 500 °C achieved highest removal and recovery efficiencies of Co in the 3D-MFC system. The maximum removal efficiency of 98.47%, the recovery efficiency of 96.35%, the power density of 11.34 W/m³, and the columbic efficiency of 28.74% were obtained in the orthogonal experiments. The influence of the operating time on the removal and recovery of Co was more obvious than the electro-output of the system. The addition of ammonium carbonate to the 3D-MFC systems clearly increased the precipitation of Co. The stacking of GAC particles in MFC had strengthened the adsorption of Co ions by intensifying the acidic-alkaline pathways during the 3D BE process. The removal and recovery of Co ions from the stripping solution in the 3D-MFC experiments were mainly achieved by the electromigration, electrostatic adsorption of GAC, and chemical precipitations of cobalt hydroxide and cobalt carbonate. A continuous process was suggested for the 3D-MFC application integrating to the traditional recovery procedure of Co from the spent LIBs at the pilot scale.
This work focuses on the recovery of valuable metal from the cathode materials of spent lithium ion batteries to ensure resource recycling and environmental protection. An environmentally friendly process involving reduction roasting and stepwise leaching is proposed to recover Li and Ni, Co, and Mn from spent LiNixCoyMn1-x-yO2 materials. Suitable leaching conditions are obtained from thermodynamic analysis (Eh-pH diagram). The effects of several factors, such as acid concentration, temperature, leaching time and liquid‒solid ratio, on the leaching efficiency of valuable metals are investigated. Under optimum conditions, the leaching efficiency of Li, Ni, Co, and Mn are as high as 93.68%, 99.56%, 99.87%, and 99.9%, respectively. The kinetic aspect of the acid leaching process is analyzed by shrinking the core model, which suggests a residue layer diffusion process. The reaction activation energies of Ni, Co, and Mn are 29.35 kJ mol⁻¹, 24.00 kJ mol⁻¹, and 23.29 kJ mol⁻¹, respectively. This metallurgic method contributes to environmentally friendly and economical recovery of valuable metals from spent lithium-ion batteries.
With declining ore grades and increasing waste volumes, lithium-ion battery (LIB) wastes are increasingly considered valuable for urban mining for metal recovery and re-use. In Australia, LIB is not classified as hazardous, despite having significant human and environmental health risks if handled and disposed of improperly. Unlike in Europe and Asia, regulations or policies to enforce or encourage product stewardship are lacking, with small recycling schemes targeting only consumer behaviour, and voluntary actions of manufacturers and distributors. Although manual sorting and dismantling of LIB waste occur onshore, the valuable components are shipped overseas for processing due to limited onshore capacity to recover the inherent metal values. In this paper, LIB recycling in Australia is reviewed, considering the projections of LIB waste generation, identification of future trends, opportunities and potential for innovation for LIB recycling in Australia. Key gaps surrounding materials tracking, waste generation and fate and technology design need to be addressed to support the development of the industry and to support the use of primary minerals and materials in Australia.
Fluorine (F)-doped carbon modified lithium rich layered oxides Li1.2Mn0.54Ni0.13Co0.13O2 (LMCNO@C-F) are synthesized by a facile sol-gel process. In this constructed architecture, the F-doped carbon surface modification layers can not only enhance the electronic conductivity of overall electrode but also avoid the direct exposure of LNMCO to the electrolyte. As a result, The LMNCO@C-F sample exhibits a high reversible capacity (289.5 mA h g-1 at 0.1 C), excellent rate capability (263.6, 218.9, 182.9, and 108.6 mA h g-1 at 0.5, 1, 5 and 10 C, respectively) and superior cycling stability (with a high capacity retention of 88.5% at 5 C after 500 cycles). The enhanced performance is ascribed to the formed metal fluorides (Mn-F bond) and a strong electronic coupling between F-doped carbon and bulk LMNCO, while can greatly enhance the structure stability and electronic conductivity of LMNCO cathode materials.
A combined process was presented to recover valuable metals from lithium nickel cobalt manganese (NCM) cathodes of spent lithium-ion batteries. In this process, the cathode scrap was first roasted with carbonaceous reductant, and then carbonation water leaching was employed to selectively extract Li from the roasted cathodes. Finally, the obtained residue was leached in sulfuric acid solution to recover Co, Ni and Mn. A systematic investigation combining thermodynamic analysis, leaching experiments and characterization was conducted to explore the effect of operating conditions and leaching mechanism. The results indicate that the leaching of Li is significantly improved by injecting of CO2 into the leaching system, and more than 80% of Li can be leached within 10 min at a low liquid-solid ratio. High-quality Li2CO3 can be prepared from the leachate by direct evaporation. More than 96% of Ni, Co and Mn are extracted without adding reductant under the conditions of a H2SO4 dosage of 1.15 times the theoretical value, a time of 2.5 h, a temperature of 55 °C and a liquid-solid ratio of 3.5 mL g⁻¹. The acid leaching process is more efficient and economical, which is ascribed to the transformation of the low-valence states of metals with high activity after reduction roasting.
Controlled design of low-cost, eco-friendly, and efficient metal recycling process of waste printed circuit boards (PCBs) is essential for sustainable industries. In this study, a metal extractor (ME) design was fabricated by anchoring organic chromophore chelate [(E)-4-((3-amino-4-hydroxyphenyl)diazenyl)naphthalen-1-ol (AHPDN)] into three-dimensional (3D), and vertical platelets of ZnO platforms to continuously extract and sensitively and selectively detect ultra-trace Co2+ concentration (approximately 95.7%) in real e-waste leach liquor. Results reveal that the microscopic ZnO platelet hierarchy is successfully fabricated with non-stacked 3D platelet morphology through hydrothermal-assisted methodology. The 3D non-stacked ZnO platelets are oriented in horizontal and vertical domains, thereby enabling fabrication of potential ME for multi-directional diffusion and efficient adsorptivity of Co2+ ions. Multi-diffusible, intermingled platelets and numerous active sites decorated the ME hierarchy promote the ultra-trace separation and recovery of Co2+ ions from PCBs. This scalable immobilization and accommodation of AHPDN along ZnO platelet surfaces control effectively the Co2+ ion-recovery/extraction process. The selective adsorption of Co2+ ions in the presence of other competitive ions strongly depends on pH control assay. The consumed MEs can be repeatedly recycled, their platelet hierarchy and surface features are retained, and their selective adsorption functionalities are negligibly altered. Hierarchical MEs are suitable for the extraction of Co2+ from the waste PCBs.
Ever-growing global energy needs and environmental damage have motivated the pursuit of sustainable energy sources and storage technologies. As attractive energy storage technologies to integrate renewable resources and electric transportation, rechargeable batteries, including lead–acid, nickel–metal hydride, nickel–cadmium, and lithium-ion batteries, are undergoing unprecedented rapid development. However, the intrinsic toxicity of rechargeable batteries arising from their use of toxic materials is potentially environmentally hazardous. Additionally, the massive production of batteries consumes numerous resources, some of which are scarce. It is therefore essential to consider battery recycling when developing battery systems. Here, we provide a systematic overview of rechargeable battery recycling from a sustainable perspective. We present state-of-the-art fundamental research and industrial technologies related to battery recycling, with a special focus on lithium-ion battery recycling. We introduce the concept of sustainability through a discussion of the life-cycle assessment of battery recycling. Considering the forecasted trend of a massive number of retired power batteries from the forecasted surge in electric vehicles, their repurposing and reuse are considered from economic, technical, environmental, and market perspectives. New opportunities, challenges, and future prospects for battery recycling are then summarized. A reinterpreted 3R strategy entailing redesign, reuse, and recycling is recommended for the future development of battery recycling.
With the ever-growing need for lithium-ion batteries, particularly from the electric transportation industry, a large amount of lithium-ion batteries is bound to retire in the near future, thereby leading to serious disposal problems and detrimental impacts on environment and energy conservation. Currently, commercial lithium-ion batteries are composed of transition metal oxides or phosphates, aluminum, copper, graphite, organic electrolytes with harmful lithium salts, polymer separators, and plastic or metallic cases. The lack of proper disposal of spent lithium-ion batteries probably results in grave consequences, such as environmental pollution and waste of resources. Thus, recycling of spent lithium-ion batteries starts to receive attentions in recent years. However, owing to the pursuit of lithium-ion batteries with higher energy density, higher safety and more affordable price, the materials used in lithium-ion batteries are of a wide diversity and ever-evolving, consequently bringing difficulties to the recycling of spent lithium-ion batteries. To address this issue, both technological innovations and the participation of governments are required. This article provides a review of recent advances in recycling technologies of spent lithium-ion batteries, including the development of recycling processes, the products obtained from recycling, and the effects of recycling on environmental burdens. In addition, the remaining challenges and future perspectives are also highlighted.
LiNi0.5Co0.2Mn0.3O2 (LNCM) was resynthesized by a novel metallurgical approach coupled with solid-state sintering using cathode materials from spent lithium-ion batteries (LIBs) as starting materials. A combination of reduction roasting, two-step leaching, co-precipitation, and solid-state reaction was applied to recover valuable metals and regenerate cathode materials. The prepared LNCM was characterized by a series of physical and electrochemical measurements for comparison with commercial LNCM. X-ray diffraction and scanning electron microscopy results indicate that the resynthesized LNCM exhibits good layered structure and a sphere of approximately 6 μm. The electrochemical tests indicate that the resynthesized LNCM has an initial discharge capacity of 172.9 mA h g⁻¹ (0.2 C) between 2.5 and 4.3 V; the discharge capacity is 160.9 mA h g⁻¹ (0.2 C) after 50 cycles, in which the capacity retention is 93.8%. Cyclic voltammograms and electrochemical impedance spectra detected that resynthesized LNCM has good structural reversibility and conductivity, similar to commercial LNCM. This method is feasible for regenerating the spent cathode material of LIBs, which can contribute to both resource recycling and environmental protection.
Spent Li-ion batteries (LIB) are highly rich in Cobalt and Lithium that need to be recovered to reduce shortage of these valuable metals and decrease of their potential environmental risks. This study applied bioleaching using Aspergillus niger strains MM1 and SG1, and Acidithiobacillus thiooxidans 80191 for removal of Co and Li from spent LIB under type 1 and type 2 conditions. Moreover, metal recovery was attempted from the fungal leaching solution by sodium sulfide, sodium hydroxide and sodium oxalate for Co, then Li using sodium carbonate. The findings of this work show that metal removal in fungal bioleaching under type 2 system was highly comparable or even better than bacterial or acid leaching. Significant quantity of Co (82 %) and Li (100 %) dissolution observed in strain MM1, however metal solubilisation was poor in strain 80191 since only 22 % Co and 66 % Li solubilized. High amount of Co precipitated potentially as cobalt sulphide (100 %), cobalt hydroxide (100 %) or cobalt oxalate (88 %), and Li as lithium carbonate (73.6 %). Finally, results of this study suggest that fungal bioleaching could be an environmental friendly approach for solubilisation and recovery of considerable quantity of metals from spent LIB.
Spent lithium-ion batteries have caused global concern owing to their rich resource metal content and high potential for polluting the environment. In the present study, a green, efficient, and simple process was developed to recycle and detoxify Li, Mn, Cu, Al, Co, and Ni from spent lithium-ion mobile phone batteries using adapted Aspergillus niger. The adaptation of Aspergillus niger to heavy metals improved the production of organic acids and the leaching efficiency of metals compared to unadapted fungi. Moreover, it decreased the time required to enter the logarithmic phase and increased the speed of acid production. In the presence of spent lithium-ion battery powder, gluconic acid was the main lixiviant produced by the adapted fungi. At a pulp density of 1% (w/v), the adapted Aspergillus niger leached 100% Li, 94% Cu, 72% Mn, 62% Al, 45% Ni, and 38% Co. The results of SEM, FTIR, XRD, EDX, and mapping analyses of the original spent battery powder and bioleached residue confirmed the effectiveness of fungal metabolites to leach the metals of spent lithium-ion mobile phone batteries.
Over the past 30 years, significant commercial and academic progress has been made on Li‐based battery technologies. From the early Li‐metal anode iterations to the current commercial Li‐ion batteries (LIBs), the story of the Li‐based battery is full of breakthroughs and back tracing steps. This review will discuss the main roles of material science in the development of LIBs. As LIB research progresses and the materials of interest change, different emphases on the different subdisciplines of material science are placed. Early works on LIBs focus more on solid state physics whereas near the end of the 20th century, researchers began to focus more on the morphological aspects (surface coating, porosity, size, and shape) of electrode materials. While it is easy to point out which specific cathode and anode materials are currently good candidates for the next‐generation of batteries, it is difficult to explain exactly why those are chosen. In this review, for the reader a complete developmental story of LIB should be clearly drawn, along with an explanation of the reasons responsible for the various technological shifts. The review will end with a statement of caution for the current modern battery research along with a brief discussion on beyond lithium‐ion battery chemistries. This review presents the major development events in the history of lithium‐ion batteries and discusses in detail the driving forces responsible for the various technological shifts.
Waste streams containing heavy metals are always of concerns from both environmental and resource depleting points of view. The challenges are in most cases related to the effectiveness for high-added value materials recovery from such waste, with which the environmental impacts during recycling shall be low. In this research, two typical heavy metals containing waste streams, i.e. spent lithium ion battery and vanadium-bearing slag were simultaneously treated, and it enables regeneration of the LiNi1/3Co1/3Mn1/3O2 cathode materials which was considered difficult due to the dislocation of nickel and lithium ions during electrochemical performance. By using the intermediate product during vanadium-bearing slag treatment, vanadium embedded cathode material can be prepared which delivers excellent electrochemical performances with a specific capacity of 156.3mAhg-1 after 100 cycles at 0.1C with the capacity retention of 90.6%, even the additive amount is only 5%. A thin layer of vanadium oxide is found to be effective to promote electrochemical performance of the cathode material. Using the principles of green chemistry, this process enables high performance cathode materials regeneration without introducing extraction chemicals and with much lower environmental impacts comparing traditional metallurgical technologies.
Visual extraction, detection, and recovery of Co2+ ions from spent lithium-ion batteries (SLIBs) via a one-step process become a new attractive simple route for management of urban electronic wastes (e-wastes), which in turn lead to exploit of the accumulated e-waste ideally and protect the green environment. The Co2+ ion-capture system was achieved by selective binding with synthesized chelating agents, namely, (E)-4-((2-mercaptophenyl)diazenyl)-2-nitrosonaphthalen-1-ol (MPDN) and (E)-5-((1,3,4-thiadiazol-2-yl)diazenyl)benzene-1,3-diol (TDDB), at controlled pH solution. The dense dressing assembly of MPDN and TDDB into microscopic, mesospongy γ-Al2O3 monoliths enabled the design of solid/sponge Co2+ ion extractor (IE) from SLIB leach liquor. Our recycling process of Co2+ ions from SLIBs showed evidence of (i) Co2+ ion waste management, (ii) low-cost collection/recovery of Co2+ ions, (iii) sensitive and selective extraction of ultra-trace Co2+ ion, and (iv) reduction of e-waste volume through multiple reusability or recyclability. Furthermore, our sponge IE design with large surface area-to-volume ratios, macro/mesopores, and grooves along the micrometric, hierarchal monolith structures results in a facile, naked eye monitoring of the ultra-trace Co2+ ion collection/binding to a detection limit of approximately 3.05 × 10−8 M during multifunction extraction steps from SLIBs. Our result also showed evidence of the extraction of Co2+ ions (196 mg/g) from SLIBs by a one-step process. This finding provides a basis for the control of multifunction processes (i.e., extraction, detection, and recovery) and the high performance for selective extraction and recovery of Co2+ ions from SLIBs in a one-step process.
It is significant to recover metal values from spent lithium ion batteries (LIBs) for the alleviation or prevention of potential risks towards environmental pollution and public health, as well as for the conservation of valuable metals. Herein a hydrometallurgical process was proposed to explore the possibility for the leaching of different metals from waste cathodic materials (LiCoO2) of spent LIBs using organics as reductant in sulfuric acid medium. According to the leaching results, about 98% Co and 96% Li can be leached under the optimal experimental conditions of reaction temperature - 95 °C, reaction time - 120 min, reductive agent dosage - 0.4 g/g, slurry density - 25 g/L, concentration of sulfuric acid-3 mol/L in H2SO4 + glucose leaching system. Similar results (96% Co and 100% Li) can be obtained in H2SO4 + sucrose leaching system under optimized leaching conditions. Despite a complete leaching of Li (∼100%), only 54% Co can be dissolved in the H2SO4 + cellulose leaching system under optimized leaching conditions. Finally, different characterization methods, including UV-Vis, FT-IR, SEM and XRD, were employed for the tentative exploration of reductive leaching reactions using organic as reductant in sulfuric acid medium. All the leaching and characterization results confirm that both glucose and sucrose are effective reductants during leaching, while cellulose should be further degraded to organics with low molecular weights to achieve a satisfactory leaching performance.
Recovery of valuable metals from spent lithium-ion battery (LIB) is of both environmental and economic importance. Acidic leaching usually encounters issues of low selectivity or slow kinetics with considerable secondary waste generation during further purification. In this research, a closed-loop process with improved leaching selectivity for recycling of spent LiNixCoyMn1-x-yO2 battery using weak acidic leachant was demonstrated. To obtain optimal conditions of the leaching process, the effects of acid concentration, solid to liquid (S/L) ratio, temperature and reductant content were systematically investigated. Almost all Co, Li, Mn and Ni could be effectively recovered into the solution while Al remained in the residue as metallic form, after one-step leaching. The role of reductant during leaching was further evaluated which was found to be critical for the leaching kinetics. It is clear that the addition of reductant could alter the rate-controlling step of leaching from the ion diffusion in the residue layer to the surface chemical reactions. With high selectivity against impurities, this research proposed and verified a process to recover high purity Li2CO3 from the cathode scrap of LIBs, and more than 90% of the global recovery rate of valuable metals can be achieved.
Lithium ion battery (LIB) waste contains significant valuable resources that could be recovered and reused to manufacture new products. This study aimed to develop an alternative process for extracting metals from LIB waste using acidic solutions generated by electrolysis for leaching. Results showed that solutions generated by electrolysis of 0.5 M NaCl at 8 V with graphite or mixed metal oxide (MMO) electrodes were weakly acidic and leach yields obtained under single stage (batch) leaching were poor (<10%). This was due to the highly acid-consuming nature of the battery waste. Multistage leaching with the graphite electrolyte solution improved leach yields overall, but the electrodes corroded over time. Though yields obtained with both electrolyte leach solutions were low when compared to the 4 M HCl control, there still remains potential to optimise the conditions for the generation of the acidic anolyte solution and the solubilisation of valuable metals from the LIB waste. A preliminary value proposition indicated that the process has the potential to be economically feasible if leach yields can be improved, especially based on the value of recoverable cobalt and lithium.
The rapid increase in the production of electrical and electronic equipment, along with higher consumption of these products, has caused defective and obsolete equipment to accumulate in the environment. In this research, bioleaching of spent lithium-ion batteries (LIBs) used in laptops is carried out under two-step condition based on the bacterial activities of a mixture of Acidithiobacillus ferrooxidans and Acidithiobacillus thiooxidans. First, the best inoculum ratio of two acidophilic bacteria for the mixed culture is obtained. Next, adaptation is carried out successfully and the solid-to-liquid ratio reaches 40 g L⁻¹. Response surface methodology is utilized to optimize the effective variables of initial pH, iron sulfate and sulfur concentrations. The maximum recovery of metal is about 99.2% for Li, 50.4% for Co and 89.4% for Ni under optimum conditions of 36.7 g L⁻¹ iron sulfate concentration, 5.0 g L⁻¹ sulfur concentration and initial pH of 1.5 for the best inoculum ratio of 3/2. Results of FE-SEM, XRD and FTIR analysis before and after bioleaching confirm that bacterial activity is a promising and effective route for metal recovery from spent LIBs. Toxicity assessment tests demonstrate the suitability of the bioleached residual as a nonhazardous material that meets environmental limitations for safe disposal.
Recycling of spent lithium-ion-batteries (LIBs) has attracted significant attentions in recent years due to the increasing demand on corresponding critical metals/materials and growing pressure on environmental impact from solid waste disposal. A range of investigations have been carried out for recycling spent LIBs to obtain either battery materials or individual compounds. In order to enhance effective recovery of materials, physical pretreatment is usually applied to obtain different streams of waste materials ensuring efficient separation for further processing. Subsequently, a metallurgical process is used to extract metals or separate impurities from a specific waste stream so that the recycled materials or compounds can be further prepared by incorporating principles of materials engineering. In this review, the current status of spent LIBs recycling is summarized in view of the whole recycling process, especially focusing on the hydrometallurgy. In addition to understanding different hydrometallurgical technologies including acidic leaching, alkaline leaching, chemical precipitation and solvent extraction, the existing challenges for process optimization during the recycling are critically analyzed. Besides, the energy consumption of different processes is evaluated and discussed. It is expected that this research could provide a guideline for improvement of the spent LIBs recycling and this topic can be further stimulated for industrial realization.
An eco-friendly and benign process has been investigated for the dissolution of Li, Co, Ni, and Mn from the cathode materials of spent LiNi1/3Co1/3Mn1/3O2 batteries, using DL-malic acid as the leaching agent in this study. The leaching efficiencies of Li, Co, Ni, and Mn can reach about 98.9%, 94.3%, 95.1%, and 96.4%, respectively, under the leaching conditions of DL-malic acid concentration of 1.2 M, hydrogen peroxide content of 1.5 vol.%, solid-to-liquid ratio of 40 g l⁻¹, leaching temperature of 80°C, and leaching time of 30 min. In addition, the leaching kinetic was investigated based on the shrinking model and the results reveal that the leaching reaction is controlled by chemical reactions within 10 min with activation energies (Ea) of 21.3 kJ·mol⁻¹, 30.4 kJ·mol⁻¹, 27.9 kJ·mol⁻¹, and 26.2 kJ·mol⁻¹ for Li, Co, Ni, and Mn, respectively. Diffusion process becomes the controlled step with a prolonged leaching time from 15 to 30 min, and the activation energies (Ea) are 20.2 kJ·mol⁻¹, 28.9 kJ·mol⁻¹, 26.3 kJ·mol⁻¹, and 25.0 kJ·mol⁻¹ for Li, Co, Ni, and Mn, respectively. This hydrometallurgical route was found to be effective and environmentally friendly for leaching metals from spent lithium batteries.
Due to the low recovery of valuable metals and the great loss of Co in the smelting process, the traditional pyrometallurgical process suffers to treat low nickel-copper matte efficiently. This work focused on a novel and controllable two-stage chlorinating roasting followed by a water leaching process to synchronously extract valuable metals from low-grade nickel-copper matte. The effects of first stage roasting temperature, roasting atmosphere, dosage of ammonium chloride, particle size of matte, first stage roasting time and second stage roasting temperature were studied. More than 99% of Ni, 99% of Cu and 96% of Co, whereas only 1.02% of Fe, were extracted under optimum conditions in which the first roasting temperature was 450 °C, the proportion of O2 was 10%, the dosage of ammonium chloride was 200%, the first roasting time was 1.5 h, and the second roasting temperature was 400 °C. The chlorination mechanism and phase transformation during the two-stage roasting process were revealed using X-ray diffraction (XRD), scanning electron microscopy (SEM) and differential thermal and thermogravimetric analysis (DTA-TG). Thermal analysis kinetics method was used to analyze the kinetics in the chlorinating process, and the results showed that the first-stage roasting process has three stages to chloridize the metals in matte. Their apparent activation energies are 88.13 kJ mol⁻¹, 338.61 kJ mol⁻¹, and 252.27 kJ mol⁻¹, respectively.
A Donnan Dialysis based process utilizing cation exchange membranes to separate and recover lithium, nickel, cobalt, and manganese during hydrometallurgical recycling of lithium ion battery cathodes is proposed. Compared to conventional processes, the process has the potential to achieve higher lithium recoveries and to recycle lixiviant. The present work introduces the process, develops mathematical equations to describe it, presents experimentally found cation mass transfer coefficients through cation exchange membranes, and uses the experimental data and equations to predict theoretical kinetics and recoveries achievable by the process.
The simulation predicts that in two days, utilizing 5000 dm² of CMS C-1805 Neosepta monovalent CEM and 2000 dm² of CMX C-1586 Neosepta polyvalent CEM, the proposed process is capable of processing 1000 L of leachate containing 285 mol of lithium, 95 mol each of cobalt, nickel, and manganese. 94.1% of the lithium can be recovered as high purity lithium carbonate and 99.4% of the transition metals as mixed sulphates ready for solvent extraction. At a minimum 422.6 mol of pure sulphuric acid and 268 mol of potassium bicarbonate are needed.
Spherical LiNi1/3Co1/3Mn1/3O2 cathode particles were resynthesized by a carbonate co-precipitation method using spent lithium-ion batteries (LIBs) as a raw material. The physical characteristics of the Ni1/3Co1/3Mn1/3CO3 precursor, the (Ni1/3Co1/3Mn1/3)3O4 intermediate, and the regenerated LiNi1/3Co1/3Mn1/3O2 cathode material were investigated by laser particle-size analysis, scanning electron microscopy–energy-dispersive spectroscopy (SEM-EDS), thermogravimetry–differential scanning calorimetry (TG-DSC), X-ray diffraction (XRD), inductively coupled plasma–atomic emission spectroscopy (ICP-AES), and X-ray photoelectron spectroscopy (XPS). The electrochemical performance of the regenerated LiNi1/3Co1/3Mn1/3O2 was studied by continuous charge–discharge cycling and cyclic voltammetry. The results indicate that the regenerated Ni1/3Co1/3Mn1/3CO3 precursor comprises uniform spherical particles with a narrow particle-size distribution. The regenerated LiNi1/3Co1/3Mn1/3O2 comprises spherical particles similar to those of the Ni1/3Co1/3Mn1/3CO3 precursor, but with a narrower particle-size distribution. Moreover, it has a well-ordered layered structure and a low degree of cation mixing. The regenerated LiNi1/3Co1/3Mn1/3O2 shows an initial discharge capacity of 163.5 mA h g⁻¹ at 0.1 C, between 2.7 and 4.3 V; the discharge capacity at 1 C is 135.1 mA h g⁻¹, and the capacity retention ratio is 94.1% after 50 cycles. Even at the high rate of 5 C, LiNi1/3Co1/3Mn1/3O2 delivers the high capacity of 112.6 mA h g⁻¹. These results demonstrate that the electrochemical performance of the regenerated LiNi1/3Co1/3Mn1/3O2 is comparable to that of a cathode synthesized from fresh materials by carbonate co-precipitation.
In this paper, an effective recycling process from spent LIBs has been developed. The aluminum residual commonly exists in hydrometallurgy, and also aluminum is considered as a resultant additive in LIB modification, therefore, the tolerability of aluminum was studied in this work. Li[(Ni1/3Co1/3Mn1/3)1-xAlx]O2 (0.01 ≤ x ≤ 0.05) cathode materials were regenerated from spent ternary LIBs. X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS) and electrochemical measurements were carried out to characterize the performances of all of the samples. XRD and XPS results indicate that Mn and Ni are possibly replaced by Al. When x ≤ 0.03, the initial discharge capacity is up to 170 mA h g⁻¹ at 0.05C between 2.5 and 4.5 V, and more than 100 mA h g⁻¹ at 2C. The results showed that the existence of aluminum of up to x = 0.03 has no significant impact on the cathode materials of Li[(Ni1/3Co1/3Mn1/3)1-xAlx]O2, and the content surpasses the conventional limitations. © The Royal Society of Chemistry and the Centre National de la Recherche Scientifique 2017.
A selective leaching process is proposed to recover Li, Fe and P from the cathode materials of spent lithium iron phosphate (LiFePO4) batteries. It was found that using stoichiometric H2SO4 at low concentration as leachant and H2O2 as oxidant, Li could be selectively leached into solution while Fe and P could remain in leaching residue as FePO4, which is different from the traditional process of using excess mineral acid to leach all the elements into solution. Under the optimized conditions (0.3 M H2SO4, H2O2/Li molar ratio 2.07, H2SO4/Li molar ratio 0.57, 60 oC and 120 min), the leaching rates of 96.85 % for Li, 0.027 % for Fe and 1.95 % for P were recorded. The Li contained in solution was then recovered by introducing Na3PO4 as precipitant., Around 95.56 % Li was precipitated and recovered in the form of Li3PO4 under the experimental conditions. In addition, the FePO4 in the leaching residue was directly recovered by burning at 600 oC for 4 h to remove carbon slag. This study illustrates an effective process for the recycling of spent LiFePO4 batteries in a simple, efficient and cost-effective way, which makes it potential to be industrially applied.
Production of lithium from primary resources is lagging behind demand (12% versus 16% in 2016), cost of lithium is increasing (was increased between 40-60% in 2016), battery energy density rapidly increasing versus declined cost, and estimated lithium ion battery (LIB) markets size ($77.42 billion by 2024) driven by projected demands for plugged in electric vehicle (PEV) clearly justifies recycling. Wake of PEV technology and projected demand raising several challenges, including, lithium demand/scarcity and futuristic technology to recover lithium from all those LIB wastes. To address the circular economy, steady supply chain security, self-reliance, environment safety, environment directive, energy security, resources conservation, futuristic carbon footprint, WEEE directives and waste crime recycling of LIB is at absolute essential. During last decade, LIB recycling research and industrial recycling of LIB have attracted the interest of researcher, industrialist, and environmentalist significantly. All those reported progress are with interest to the recovery of valuable metals like Co, but rarely lithium recovery has been focused. Hence, this paper address logical hypothesis and application of available technology in a fashion where lithium recycling from LIB can be addressed.