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Purpose: The recycling of lithium-ion batteries is an emerging field faced with the challenge of recovering more than the most valuable elements from the batteries. While the literature presents many innovative approaches to the problem, an overview of the technical and environmental prospects of hydrometallurgical black mass recycling remains crucial. The goal was to analyze the impacts of a black mass process flowsheet and suggest ways to further reduce the impacts of battery recycling. Methods: The flowsheet was drafted from the literature by combining both state-of-the-art and experimentally demonstrated unit processes by starting with the leaching system, where reductive leaching is performed using only the copper and iron impurities already present in the black mass. The process targeted copper, manganese, cobalt, nickel, and lithium recovery, and three scenarios for manganese recovery were investigated. The flowsheet was simulated using HSC Sim software, and the mass and energy balances were adapted into internally consistent life cycle inventories. The scope was "gate-to-gate" in Europe and CML methodology was used for impact assessment. Results and discussion: Assuming that mechanical pre-treatment carries more environmental benefits than burdens, the results indicated that hydrometallurgical black mass recycling had a tentatively lower environmental footprint compared to virgin raw materials in all impact categories except ozone depletion, the results indicated that hydrometallurgical black mass recycling had a tentatively lower environmental footprint compared to virgin raw materials in all impact categories except ozone depletion. Sulfuric acid and neutralizing chemicals were among the most significant contributors to the impacts, and therefore further analysis was conducted based on an experimental study on low acid leaching with a low (< 0.5 M) initial sulfuric acid concentration instead of the baseline 2 M. This reduced the impacts by approximately 30–40% in all categories by decreasing downstream chemical consumption, and more significantly decreased ozone depletion. The challenges and opportunities for further process improvement were also considered. Conclusions: The study highlights the importance of process optimization to improve the environmental sustainability of battery chemical production, but also revealed critical research gaps in the experimental literature. Rather than focusing on a single unit process, experimental black mass recycling research should aim at finding solutions that are optimal for the up- and downstream units, such as minimization of aluminum in the black mass and acid consumption. [ABSTRACT FROM AUTHOR]

Battery recycling is a promising approach to mitigate the safety, environmental, and economic threats posed by numerous discarded lithium‐ion batteries (LIBs). However, the unclear atomic‐scale degradation of spent graphite complicates recycling, resulting in energy‐intensive impurity removal and graphitization, which hampers industrialization. This study uses Cryo‐transmission electron microscopy (Cryo‐TEM) to characterize spent graphite degradation and develop a scalable graphite self‐induced microwave plasma method for efficient regeneration. Cryo‐TEM images show graphite coated with a solid electrolyte interphase (SEI) layer, revealing lattice defects and structure expansion near the surface that impair electrochemical performance. The self‐induced microwave plasma method eradicates the SEI layer and restores the graphite lattice structure within 30 s. Multiphysics simulations indicate that the microwave field generates a strong electric field on the graphite surface, causing plasma discharge and rapid surface heating. Regenerated graphite demonstrates excellent electrochemical performance, with a specific charge capacity of 352.2 mAh g−1 at 0.2 C and ≈81% capacity retention after 400 cycles, matching commercially available materials. This efficient method offers a promising approach for recycling graphite anodes. [ABSTRACT FROM AUTHOR]

Discovering sources of transition metals, such as Ni, Co, and Mn, has become crucial due to their broad applicability, particularly as electrocatalysts for the oxygen evolution reaction (OER). Upcycled spent batteries have emerged as alternatives for transition metal sources for the OER electrocatalysts. In this work, Ni–Co–Mn oxalates were extracted from the spent LiNixCoyMnzO2 (NCM) cathode of lithium-ion batteries. The extracted oxalates were further processed via ball milling as a rapid and scalable mechanochemical route to engineer their structures. After calcination, Ni–Co–Mn oxides with nanosized granules on the surface that mainly consist of MnCo2O4 were obtained. With a correlation of morphology and trimetallic oxide formation with the OER catalytic performance, Ni–Co–Mn oxides exhibit OER overpotentials of 367 and 732 mV in alkaline and neutral media, respectively, showing OER catalytic activity in a wide pH range. The results indicate that ball milling can induce particle size reduction and bond formation between metals to facilitate mixed-metal oxide formation. Furthermore, the resulting material is also applicable as the catalyst in the air cathode of Zn-air batteries, where the battery achieved a power density of 85.42 mW cm–2 and 100 h of cycling stability, showing comparability with a battery with a Pt/C–Ir/C catalyst. [ABSTRACT FROM AUTHOR]

The surge in lithium‐ion batteries has heightened concerns regarding metal resource depletion and the environmental impact of spent batteries. Battery recycling has become paramount globally, but conventional techniques, while effective at extracting transition metals like cobalt and nickel from cathodes, often overlook widely used spent LiFePO4 due to its abundant and low‐cost iron content. Direct regeneration, a promising approach for restoring deteriorated cathodes, is hindered by practicality and cost issues despite successful methods like solid‐state sintering. Hence, a smart prelithiation separator based on surface‐engineered sacrificial lithium agents is proposed. Benefiting from the synergistic anionic and cationic redox, the prelithiation separator can intelligently release or intake active lithium via voltage regulation. The staged lithium replenishment strategy was implemented, successfully restoring spent LiFePO4's capacity to 163.7 mAh g−1 and a doubled life. Simultaneously, the separator can absorb excess active lithium up to approximately 600 mAh g−1 below 2.5 V to prevent over‐lithiation of the cathode This innovative, straightforward, and cost‐effective strategy paves the way for the direct regeneration of spent batteries, expanding the possibilities in the realm of lithium‐ion battery recycling. [ABSTRACT FROM AUTHOR]

Anthropogenic activities predominantly affect environmental Pb pollution, especially during waste lead-acid battery (LAB) recycling operations. In this study, the presence of Pb and nine other potentially toxic elements (PTEs) in the soil at an abandoned LAB recycling site was investigated. The focus was on spatial and vertical distributions and potential health issues related to PTEs. Average concentrations of Cd, As, Hg, Pb, Al, Zn, Cu, and Sb were elevated at all investigated soil depths, whereas the concentrations of Zn, Cu, and Sb were significant only on the soil surface. Positive matrix factorization, correlation and cluster analyses, as well as self-organizing maps, identified four primary pollution sources: recycling activities (Cd, Hg, Pb, and Sb), mixed anthropogenic sources (Zn and Cu), the soil parent material (As, Cr, and Ni), and surface runoff combined with sand application (Al and pH). While the non-carcinogenic risk results revealed a negligible risk for adults, the hazard index (HI) values for children were greater than one in 26% of the samples. For adults and children, the total carcinogenic risk (TCR) values were acceptable for 98% and 94% of the samples, respectively. Geospatial analysis identified the main hotspot in the battery disposal area. Source-specific non-carcinogenic and carcinogenic risks were most influenced by recycling activities. Monte Carlo simulation (MCS) of total HI for children showed that the risk value exceeded the threshold level (HI > 1) at the 10th percentile, whereas the maximum value of total HI for adults was 0.2. Regarding carcinogenic risk, the TCR values at the 95th percentile of all four sources for adults and children were below the limit value (1 × 10−4), indicating a low probability of cancer development. [ABSTRACT FROM AUTHOR]

The European Union (EU) Battery Regulation aims to establish a circular battery production and sets minimum battery material recycled targets for new batteries from post‐production and post‐consumer waste batteries. However, it is uncertain whether these targets can be met due to dynamic market developments and if their compliance results in environmental benefits. Therefore, this study examines the circular battery production in the EU and its impact on material flows and the environment from a market perspective. We combined a system dynamic market model with process models for battery production and recycling, using prospective life cycle assessment. According to our analysis, the projected amount of post‐consumer waste alone may not meet the specified levels of recycled materials due to long battery lifetimes. Thereby, the targets for cobalt are particularly ambitious, with a gap of between 9.8 and 14.6 percentage points for most scenarios. In the case of reduced battery lifetimes, the achievable recycled content across all materials increases by more than 75% in 2032 and by more than 85% in 2037. The avoidance of post‐production waste leads to 9% lower greenhouse gas (GHG) emissions compared to recycling with 100% recycling efficiency. Thus, attributable amounts of post‐production waste and unfavorable prolonged use of batteries create misguided incentives to meet legal targets. Additionally, the delay between production and recycling limits the potential for circular production as this depends significantly on market conditions. Our study highlights, that besides recycling, the industry should especially advance production processes including upstream material extraction and refinement to reduce environmental impacts. [ABSTRACT FROM AUTHOR]

Lithium‐containing components in batteries, electronics, and renewable energy pose material and waste challenges. Ongoing research focuses on eco‐friendly recycling, emphasizing electrostatic separation as a method to recover, for instance, lithium, especially in battery recycling. This study investigates forced dry triboelectric charging and electrostatic separation of powdered materials, with a focus on the charging behavior of lithium aluminate and talcum. The electrostatic separation efficiency for a blend of powders is also evaluated. Collected samples are analyzed via inductively coupled plasma‐mass spectrometry testing to assess component enrichment. Results show successful lithium enrichment from a talcum‐lithium aluminate mixture, highlighting significant separation success. [ABSTRACT FROM AUTHOR]

Recycling spent lithium-ion batteries is integral to today's low-carbon environmental protection efforts. The concept of direct regeneration, acknowledged for its environmental sustainability, economic viability, and consistent performance of recycled materials, is gaining prominence. This study presents an efficient and nondestructive approach by utilizing an ultrafast microwave technology to directly regenerate spent lithium cobaltate (LCO) cathode materials. In contrast to conventional furnace-based processes, this method significantly reduces the regeneration timeframe. By subjecting the spent LCO mixed with lithium sources to three microwave heating cycles (at approximately 1,350 K), LCO regeneration is achieved, yielding a specific capacity of 140.8 mAh g−1 (0.2 C) with a robust cycle stability. With further environmental and economic benefits, the ultrafast microwave technology holds scientific promise for directly regenerating cathode materials, while establishing competitiveness for industrial applications. [ABSTRACT FROM AUTHOR]

Abstract This study focuses on the effect of an emerging source of waste, lithium iron phosphate (LFP) cathode materials, on the hydrometallurgical recycling of the currently dominant industrial battery waste that is rich in transition metals (Ni, Co, Mn, and Li). The effects of the dosage of LFP, initial acidity, and timing of LFP reductant addition were investigated in sulfuric acid (H2SO4) leaching (t = 3 h, T = 60 °C, ω = 300 rpm). The results showed that addition of LFP increased both transition metal extraction and acid consumption. Further, the redox potential was lowered due to the increased presence of Fe2+. An initial acidity of 2.0 mol/L H2SO4 with acid consumption of 1.3 kg H2SO4/kg black mass provided optimal conditions for achieving a high leaching yield (Co = 100%, Ni = 87.6%, Mn = 91.1%, Li = 100%) and creating process solutions (Co 8.8 g/L, Ni 13.8 g/L, Li 6.7 g/L, Mn 7.6 g/L, P 12.1 g/L) favorable for subsequent hydrometallurgical processing. Additionally, the overall efficiency of H2O2 decreased due to its decomposition by high concentrations of Fe2+ and Mn2+ when H2O2 was added after t = 2 h, leading to only a minor increase in final battery metals extraction levels.

Lithium iron phosphate battery recycling is enhanced by an eco-friendly N 2 H 4 ·H 2 O method, restoring Li+ ions and reducing defects. Regenerated LiFePO 4 matches commercial quality, a cost-effective and eco-friendly solution. [Display omitted] • Low-temperature liquid-phase direct regeneration of LiFePO 4 with high efficiency. • Li+ ions anti-site defects being repaired Using N 2 H 4 ·H 2 O. • Regenerated LiFePO 4 showing good electrochemical performance. Lithium iron phosphate batteries, known for their durability, safety, and cost-efficiency, have become essential in new energy applications. However, their widespread use has highlighted the urgency of battery recycling. Inadequate management could lead to resource waste and environmental harm. Traditional recycling methods, like hydrometallurgy and pyrometallurgy, are complex and energy-intensive, resulting in high costs. To address these challenges, this study introduces a novel low-temperature liquid-phase method for regenerating lithium iron phosphate positive electrode materials. By using N 2 H 4 ·H 2 O as a reducing agent, missing Li+ ions are replenished, and anti-site defects are reduced through annealing. This process restores nearly all missing Li+ ions at 80 °C/6h. After high-temperature sintering at 700 °C/2h, the regenerated LiFePO 4 matches commercial LiFePO 4 in terms of anti-site defects and exhibits excellent performance with a 97 % capacity retention rate after 100 cycles at 1C. Compared to high-temperature techniques, this low-temperature liquid-phase method is simpler, safer, and more energy-efficient, offering a blueprint for reclaiming discarded LiFePO 4 and similar materials. [ABSTRACT FROM AUTHOR]

This study provides a comprehensive analysis of global patent trends in battery recycling, focusing on secondary batteries and related technologies across Korea, China, and the United States. The methodology involved collecting data from various patent databases, followed by quantitative analysis to identify technology trends and guide future development. The research employed statistical tools to analyze patent activities, including the frequency and scope of patent filings, and comparative analysis to highlight differences between countries. This study reveals distinct emphases on technologies such as lithium-ion and waste battery recycling, highlighting notable differences in patent activities among key companies and countries. China's large number of patents in battery manufacturing processes contrasts with the USA's focus on electrochemical cell construction and storage systems, while Korea shows significant activity in waste battery technology. The novelty of this paper lies in its detailed comparative analysis of patent trends across these three major economies, providing insights into the technological focuses and priorities of each country. The study also identifies key challenges, such as the need for consistent innovation and broader geographic coverage in Korea, enhancing patent influence and international presence in China, and ensuring high patent quality and fostering innovation in lagging sectors in the United States. Addressing these challenges through enhanced collaboration, increased R&D investments, and supportive policies is crucial for strengthening the global position and driving further innovation in the battery recycling sector. [ABSTRACT FROM AUTHOR]

The market for lithium-ion batteries (LiBs) is growing rapidly, the demand for lithium (Li) in the form of lithium carbonate (Li2CO3), which is the most common lithium mineralization form, is therefore also increasing significantly. Li is conventionally extracted as Li2CO3 using sodium carbonate (Na2CO3) to precipitate Li ions in an aqueous Li solution. However, Na2CO3 can also be replaced by CO2, which highlights the potential of using CO2 as a sustainable and economically viable alternative. This review focuses on technologies that utilize CO2 for Li2CO2 precipitation. First, the use of CO2 gas and Na2CO3 as carbonate sources are compared, and the need to consider important operating conditions with CO2 bubbling are then presented. Attempts made to increase the specific surface area of the reaction surface to enhance the utilization of CO2 gas and to produce micro-sized Li2CO3 powders are then reported, and the limitations associated with CO2 gas utilization are discussed. Although CO2 precipitation has limitations in terms of efficiency, scalability, and the fine-tuning of reaction conditions, this review shows that if CO2 precipitation technology is further developed, its use could be key to extracting and recycling next-generation Li. [ABSTRACT FROM AUTHOR]

• Insights were gained regarding graphite recovery from spent lithium-ion batteries. • New information about LTO behavior in froth flotation was discovered. • Graphite recoveries, grades and kinetic data was measured. • The research discusses optimal recycling strategies for NMC-LTO-graphite mixtures. The growing electric vehicle industry has increased the demand for raw materials used in lithium-ion batteries (LIBs), raising concerns about material availability. Froth flotation has gained attention as a LIB recycling method, allowing the recovery of low value materials while preserving the chemical integrity of electrode materials. Furthermore, as new battery chemistries such as lithium titanate (LTO) are introduced into the market, strategies to treat mixed battery streams are needed. In this work, laboratory-scale flotation separation experiments were conducted on two model black mass samples: i) a mixture containing a single cathode (i.e., NMC811) and two anode species (i.e., LTO and graphite), simulating a mixed feedstock prior to hydrometallurgical treatment; and ii) a graphite-TiO 2 mixture to reflect the expected products after leaching. The results indicate that graphite can be recovered with > 98 % grade from NMC811-LTO-graphite mixtures. Additionally, it was found that flotation kinetics are dependent on the electrode particle species present in the suspension. In contrast, the flotation of graphite from TiO 2 resulted in a low grade product (<96 %) attributed to the significant entrainment of ultrafine TiO 2 particles. These results suggest that flotation of graphite should be preferably carried out before hydrometallurgical treatment of black mass. [ABSTRACT FROM AUTHOR]

This study focuses on the effect of an emerging source of waste, lithium iron phosphate (LFP) cathode materials, on the hydrometallurgical recycling of the currently dominant industrial battery waste that is rich in transition metals (Ni, Co, Mn, and Li). The effects of the dosage of LFP, initial acidity, and timing of LFP reductant addition were investigated in sulfuric acid (H2SO4) leaching (t = 3 h, T = 60 °C, ω = 300 rpm). The results showed that addition of LFP increased both transition metal extraction and acid consumption. Further, the redox potential was lowered due to the increased presence of Fe2+. An initial acidity of 2.0 mol/L H2SO4 with acid consumption of 1.3 kg H2SO4/kg black mass provided optimal conditions for achieving a high leaching yield (Co = 100%, Ni = 87.6%, Mn = 91.1%, Li = 100%) and creating process solutions (Co 8.8 g/L, Ni 13.8 g/L, Li 6.7 g/L, Mn 7.6 g/L, P 12.1 g/L) favorable for subsequent hydrometallurgical processing. Additionally, the overall efficiency of H2O2 decreased due to its decomposition by high concentrations of Fe2+ and Mn2+ when H2O2 was added after t = 2 h, leading to only a minor increase in final battery metals extraction levels. [ABSTRACT FROM AUTHOR]

Among the technologies used for spent lithium-ion battery recycling, the common approaches include mechanical treatment, pyrometallurgical processing and hydrometallurgical processing. These technologies do not stand alone in a complete recycling process but are combined. The constant changes in battery materials and battery design make it a challenge for the existing recycling processes, and the need to design efficient and robust recycling processes for current and future battery materials has become a critical issue today. Therefore, this paper simplifies the current treatment technologies into three recycling routes, namely, the hot pyrometallurgical route, warm mechanical route and cold mechanical route. By using the same feedstock, the three routes are compared based on the recovery rate of the six elements (Al, Cu, C, Li, Co and Ni). The three different recycling routes represent specific application scenarios, each with their own advantages and disadvantages. In the hot pyrometallurgical route, the recovery of Co is over 98%, and the recovery of Ni is over 99%. In the warm mechanical route, the recovery of Li can reach 63%, and the recovery of graphite is 75%. In the cold mechanical route, the recovery of Cu can reach 75%, and the recovery of Al is 87%. As the chemical compositions of battery materials and various doping elements continue to change today, these three recycling routes could be combined in some way to improve the overall recycling efficiency of batteries. [ABSTRACT FROM AUTHOR]

The increasing importance of recycling makes the recovery of valuable elements from slags interesting. The concept of engineered artificial minerals aims at the formation of phase(s) with a high content of the to‐be‐recovered element(s) from slags of pyrometallurgical recycling processes. For this, understanding the phase constitution of the slag systems, such as the spinel‐forming subsystem Mg–Mn–Al–O from Li‐ion battery recycling, is of great importance. Herein, the phase constitution is investigated using a thin film materials library (ML) that covers the composition space (Mg14−69Mn11−38Al14−74)Ox. High‐throughput energy‐dispersive X‐ray spectroscopy and X‐ray diffraction confirm the formation of the spinel solid solution phase for a wide composition space. The Mn oxidation state is shown to be a mixture of Mn2+ and Mn3+ by analyzing Mn 2p3/2 spectra from X‐ray photoelectron spectroscopy. For one measurement area of the ML containing equal atomic amounts of Mg, Mn, and Al, transmission electron microscopy shows columnar spinel grains with Mg, Mn, and Al evenly distributed. Based on these results, it is suggested that the high likelihood of spinel formation in slags can be influenced by controlling the Mn oxidation state to allow the formation of desirable engineered artificial minerals for Li recovery. [ABSTRACT FROM AUTHOR]

[Display omitted] • A universal and scalable method is developed for recycling spent lithium batteries. • The mechanism on selective sulfidation of NCM is elucidated by DFT and experiments. • The regenerated· NCM· materials exhibit excellent electrochemical performance. • In situ XRD reveals the evolution process of transition metal sulfides into NCM. Traditional cathode recycling methods have become outdated amid growing concerns for high-value output and environmental friendliness in spent Li-ion battery (LIB) recycling. Our study presents a closed-loop approach that involves selective sulfurization roasting, water leaching, and regeneration, efficiently transforming spent ternary Li batteries (i.e., NCM) into high-performance cathode materials. By combining experimental investigations with density functional theory (DFT) calculations, we elucidate the mechanisms within the NCM-C-S roasting system, providing a theoretical foundation for selective sulfidation. Utilizing in situ X-ray diffraction techniques and a series of consecutive experiments, the study meticulously tracks the evolution of regenerating cathode materials that use transition metal sulfides as their primary raw materials. The Li-rich regenerated NCM exhibits exceptional electrochemical performance, including long-term cycling, high-rate capabilities, reversibility, and stability. The closed-loop approach highlights the sustainability and environmental friendliness of this recycling process, with potential applications in other cathode materials, such as LiCoO 2 and LiMn 2 O 4. Compared with traditional methods, this short process approach avoids the complexity of leaching, solvent extraction, and reverse extraction, significantly increasing metal utilization and Li recovery rates while reducing pollution and resource waste. [ABSTRACT FROM AUTHOR]

The emerging field of direct recycling for spent Li-ion batteries offers significant advantages, such as reduced energy expenses and minimized secondary pollution, when compared to traditional pyrometallurgical and hydrometallurgical methods. This is due to its direct utilization of the spent cathodes as raw materials. However, efficient harvesting of spent cathode particles remains a challenge. To address this issue, this technical brief is the first to incorporate resonant acoustic vibration technology (RAV) as an efficient method for stripping cathode powders from spent Li-ion batteries. Our findings indicate that RAV-based techniques can achieve a stripping efficiency of up to 92%. A comparative analysis with conventional stripping methods, such as magnetic stirring, sonication, and curling-uncurling, reveals that RAV coupled with heat treatment provides unparalleled scalability and efficiency, eliminating the need for post-processing. Furthermore, the resulting cathode powders retain their original polycrystalline particle structures, with no impurities, such as carbon black or small aluminum fragments detected. These findings highlight the promise of RAV technology for large-scale recovery of electrode powders and its potential role in direct recycling of spent Li-ion batteries. [ABSTRACT FROM AUTHOR]

It is noteworthy today that the creation and popularization of new energy has piqued the world's interest. As a result, new energy electric cars are liked and acknowledged by most customers as a representation of the development and use of new energy. The advancement of electric vehicles (EVs) has important implications for the sustainable use of energy resources. As the number of new energy EVs grows, so does the need for charging stations for these vehicles. Maximum simplification of charging station distribution may successfully satisfy the charging demands of EVs. As a result, determining the appropriate arrangement of EV charging stations has become an essential study issue. This paper proposed a novel algorithm for EV charging station optimization based on a neural network. The main idea is to optimize the cost of charging cost and the user's budget. Then, considering the target planning region of the charging station, the historical data is deployed to predict the time distribution of EVs based on the backpropagation neural network algorithm. Finally, the performance of swarm optimization is improved through the dynamic probability mutation method. Simulation results show that the proposed algorithm has better performance than existing algorithms in terms of global economic cost and low-power and high-power charging station's spatial location. [ABSTRACT FROM AUTHOR]

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The recycling of spent batteries has become increasingly important owing to their wide applications, abundant raw material supply, and sustainable development. Compared with the degraded cathode, spent anode graphite often has a relatively intact structure with few defects after long cycling. Yet, most spent graphite is simply burned or discarded due to its limited value and inferior performance on using conventional recycling methods that are complex, have low efficiency, and fail in performance restoration. Herein, we propose a fast, efficient, and "intelligent" strategy to regenerate and upcycle spent graphite based on defect‐driven targeted remediation. Using Sn as a nanoscale healant, we used rapid heating (~50 ms) to enable dynamic Sn droplets to automatically nucleate around the surface defects on the graphite upon cooling owing to strong binding to the defects (~5.84 eV/atom), thus simultaneously achieving Sn dispersion and graphite remediation. As a result, the regenerated graphite showed enhanced capacity and cycle stability (458.9 mAh g−1 at 0.2 A g−1 after 100 cycles), superior to those of commercial graphite. Benefiting from the self‐adaption of Sn dispersion, spent graphite with different degrees of defects can be regenerated to similar structures and performance. EverBatt analysis indicates that targeted regeneration and upcycling have significantly lower energy consumption (~99% reduction) and near‐zero CO2 emission, and yield much higher profit than hydrometallurgy, which opens a new avenue for direct upcycling of spend graphite in an efficient, green, and profitable manner for sustainable battery manufacture. [ABSTRACT FROM AUTHOR]

Fig. 1 The framework of this review work. [Display omitted] • This review summarises the evolution and degradation mechanisms of LiFePO 4 cathode materials. • The main recycling techniques of LiFePO 4 cathode materials from laboratory scale to industrial production were discussed. • The challenges and opportunities of different recycling techniques were highlighted and perspectives of LiFePO 4 cathode recycling were proposed. Lithium iron phosphate (LiFePO 4) has emerged as one of the most popular cathodes due to its excellent properties of low cost, high safety and stability. However, owing to the limited lifespan caused by degradation, the widespread use of LiFePO 4 batteries would generate a large number of spent batteries, the improper disposal of which causes environmental pollution and waste of resources. Therefore, the recycling of these batteries is important for environmental protection, resource conservation and economic efficiency. This review summarises LiFePO 4 cathode materials from their development and degradation mechanisms, illustrating the reasons and necessity of their recycling. In addition, battery recycling technologies are systematically discussed from laboratory scale to industrial production in terms of efficiency, economic benefits and environmental impact. Finally, we identify the challenges of LiFePO 4 cathode recycling and offer some perspectives on these challenges. These endeavors demonstrate that the degradation of large-scale batteries drives the formation of recycling demand. Therefore, it is necessary to accurately assess the degradation mechanism which is a precondition of cathode recycling. Besides, the cathode recycling mechanism should be paid much attention, simplifying the recycling process. Moreover, it is essential to illustrate the impact of impurities and defects generated during the cycling. As such, this review provides valuable insights in innovating and boosting LiFePO 4 cathode recycling technologies on an industrial scale. [ABSTRACT FROM AUTHOR]

Considering the increasing demand for Li-ion batteries, there is a need for sophisticated recycling strategies with both high recovery rates and low costs. Applying optical sensors for automating component detection is a very promising approach because of the non-contact, real-time process monitoring and the potential for complete digitization of mechanical sorting processes. In this work, mm-scale particles from shredded end-of-life Li-ion batteries are investigated by five different reflectance sensors, and a range from the visible to long-wave infrared is covered to determine the ideal detection window for major component identification as relevant input signals to sorting technologies. Based on the characterization, a spectral library including Al, Cu, separator foil, inlay foil, and plastic splinters was created, and the visible to near-infrared range (400–1000 nm) was identified as the most suitable spectral range to reliably discriminate between Al, Cu, and other battery components in the recycling material stream of interest. The evaluation of the different sensor types outlines that only imaging sensors meet the requirements of recycling stream monitoring and can deliver sufficient signal quality for subsequent mechanical sorting controls. Requirements for the setup parameters were discussed leading to the setup recommendation of a fast snapshot camera with a sufficiently high spectral resolution and signal-to-noise ratio. [ABSTRACT FROM AUTHOR]

The recycling of heavy metals contained in alkaline batteries allows minimizing the environmental impact and gives an alternative use to this waste, which can be used in the pyrometallurgical industry. In the present research work, we evaluated the possibility of reducing the manganese oxide black mass from discarded alkaline batteries to produce metallic manganese, using charcoal as a reducing agent. The procedure begins with the characterization of the raw materials, the stoichiometric calculations and the preparation of a practical method to produce self-reducing pellets, composed of manganiferous material, charcoal and bentonite as agglomerant. Computer simulations were performed, to establish the appropriate thermodynamic conditions for reduction. The tests were carried out in a tubular-type furnace, and the results obtained were evaluated using optical microscopy, scanning electron microscopy coupled with microchemical analyses and X-ray diffraction techniques. It was verified that the agglomerates showed a self-reducing behavior, so an increase of the %Mn in the samples due to increasing the temperature of the reduction treatment was found, as well as the presence of a metallic manganese phase that was identified by X-ray diffraction analysis. Flow sheet for the production of self-reducing pellets containing eucalyptus charcoal for the recycling of manganese contained in spent alkaline batteries [ABSTRACT FROM AUTHOR]

The increasing significance of batteries in the 21st century and the challenges posed by the anticipated surge in end-of-life batteries, particularly within the European context, are examined in this study. Forecasts predict a notable escalation in battery waste, necessitating a focus on the recycling of black mass (BM)—a complex and hazardous byproduct of the battery recycling process. Employing systematic analysis, this research investigates the hazardous nature of BM derived from various battery types. The study underscores the urgent need for definitive legislative classification of BM's hazardous properties (HPs), in accordance with European regulations. This comprehensive examination of BM's HPs contributes significantly to the understanding of BM recycling complexities, proving essential for industry stakeholders and guiding future developments in this field. Additionally, the study explores innovative technologies and strategies that could improve recycling efficiency and reduce associated risks. A pivotal finding of this investigation is the inherently hazardous nature of BM, leading to the recommendation that BM should be classified at a minimum under the "HP3—Flammable" category. This discovery underscores the critical need for stringent management protocols and robust regulatory frameworks to address the burgeoning challenge of battery waste in Europe. [ABSTRACT FROM AUTHOR]

Recent studies in hydrometallurgy are focused on developing eco-friendly and selective leach agents such as organic acids. These agents can extract metal ions, which are usually separated through precipitation methods. When traditional methods are used, the separation is complex and time-consuming, and each metal cation is required to be isolated separately. Moreover, extracted metal salts are subsequently recombined in the regeneration of cathode materials. To simplify this, a novel simultaneous precipitation approach has been developed, allowing the separation of metal salts that can directly contribute to regenerating novel cathode materials, bypassing the need for separate isolation. This study aimed to recover cobalt, nickel, and manganese from the organic leach solution of spent lithium-ion batteries (LIBs) through co-precipitation of metal oxalates. The investigation includes the selection of organic acids and the best parameters for the leaching process, as well as testing different molar ratios of the metals M2+ (M = Co, Ni, Mn) to oxalic acid (1:3, 1:4.5, 1:6, and 1:7.5) to examine the effects of the precipitating agent on the recovery percentages of the metals. The findings indicate that 2 M citric acid and 4 vol% H2O2 is the optimal parameter in the leaching process. Meanwhile, in the co-precipitation process, an increase in the molar ratio leads to a corresponding rise in the resulting metal recoveries. At the ratio of 1:7.5, cobalt, nickel, and manganese were recovered to the extent of 99.26%, 98.93%, and 94.01%, respectively. Nevertheless, at the increased molar ratio, the co-extraction of lithium and aluminum was observed, resulting in reduced selectivity and decreased precipitate purity. [ABSTRACT FROM AUTHOR]

Lithium-ion batteries (LIBs) are a widely used energy storage technology as they possess high energy density and are characterized by the reversible intercalation/deintercalation of Li ions between electrodes. The rapid development of LIBs has led to increased production efficiency and lower costs for manufacturers, resulting in a growing demand for batteries and their application across various industries, particularly in different types of vehicles. In order to meet the demand for LIBs while minimizing climate-impacting emissions, the reuse, recycling, and repurposing of LIBs is a critical step toward achieving a sustainable battery economy. This paper provides a comprehensive review of lithium-ion battery recycling, covering topics such as current recycling technologies, technological advancements, policy gaps, design strategies, funding for pilot projects, and a comprehensive strategy for battery recycling. Additionally, this paper emphasizes the challenges associated with developing LIB recycling and the opportunities arising from these challenges, such as the potential for innovation and the creation of a more sustainable and circular economy. The environmental implications of LIB recycling are also evaluated with methodologies able to provide a sustainability analysis of the selected technology. This paper aims to enhance the comprehension of these trade-offs and encourage discussion on determining the "best" recycling route when targets are in conflict. [ABSTRACT FROM AUTHOR]

Abstract The recycling of spent batteries has become increasingly important owing to their wide applications, abundant raw material supply, and sustainable development. Compared with the degraded cathode, spent anode graphite often has a relatively intact structure with few defects after long cycling. Yet, most spent graphite is simply burned or discarded due to its limited value and inferior performance on using conventional recycling methods that are complex, have low efficiency, and fail in performance restoration. Herein, we propose a fast, efficient, and “intelligent” strategy to regenerate and upcycle spent graphite based on defect‐driven targeted remediation. Using Sn as a nanoscale healant, we used rapid heating (~50 ms) to enable dynamic Sn droplets to automatically nucleate around the surface defects on the graphite upon cooling owing to strong binding to the defects (~5.84 eV/atom), thus simultaneously achieving Sn dispersion and graphite remediation. As a result, the regenerated graphite showed enhanced capacity and cycle stability (458.9 mAh g−1 at 0.2 A g−1 after 100 cycles), superior to those of commercial graphite. Benefiting from the self‐adaption of Sn dispersion, spent graphite with different degrees of defects can be regenerated to similar structures and performance. EverBatt analysis indicates that targeted regeneration and upcycling have significantly lower energy consumption (~99% reduction) and near‐zero CO2 emission, and yield much higher profit than hydrometallurgy, which opens a new avenue for direct upcycling of spend graphite in an efficient, green, and profitable manner for sustainable battery manufacture.

The expected large growth in electric mobility presents challenges, such as requiring a very large amount of critical raw materials like nickel, cobalt, and lithium. Due to this expected growth significant amounts of production scrap from cell and battery manufacturing will be generated. Over the next decade, increasingly larger amounts of Li-ion batteries from electric vehicles will also reach their end-of-life. Hence, in order to close the loop, the development and industrialization of sustainable battery recycling flowsheets are key so that both production scrap and end-of-life batteries can be recycled back to their 'battery grade' building blocks. Battery recycling flowsheets are typically categorized into two categories: (1) 'Pyro-Hydro', a combination of battery smelting in a pyrometallurgical process, followed by the further refining of the alloy via hydrometallurgy; and (2) '(Thermo)mechanical-Hydro', a combination of (thermo)mechanical pretreatment and further hydrometallurgical refining of the resulting black mass. In this paper, a carbon footprint analysis is presented comparing these two battery recycling approaches: 'Pyro-Hydro' and 'Thermomechanical-Hydro', taking into account the impact of the latest evolutions in process technology and efficiency. To facilitate this comparison, a prospective LCA was carried out for the respective flowsheets. The quantitative analysis shows that 'Pyro-Hydro' leads to the lowest overall carbon footprint but also that both 'Pyro-Hydro' and 'Thermomechanical-Hydro' flowsheets have their challenges and opportunities for decarbonization. The inclusion of the fate of side streams such as graphite and electrolyte in the analysis is shown to be critically important in order to gain an objective and complete view. [ABSTRACT FROM AUTHOR]

As the market share of electric vehicles continues to rise, the number of battery systems that are retired after their service life in the vehicle will also increase. This large growth in battery returns will also have a noticeable impact on processes such as battery disassembly. The purpose of this paper is, therefore, to examine the challenges of the battery disassembly process in relation to the required increase in the degree of automation. For this purpose, a survey of various experts along the battery value chain was conducted, and product-side hurdles, such as the wide range of variants, and process-side challenges, such as the opening of the housing cover or the removal of cables and connectors, were identified. Together with an assessment of the potential degree of automation in the context of downstream processes (reuse, repair, remanufacturing, and recycling), this results in a variety of streams for future research in the field of automated battery disassembly. The core aspect in this context is data availability consisting of product and component data as well as process-relevant parameters. [ABSTRACT FROM AUTHOR]

Life cycle strategies for traction batteries, such as remanufacturing, reuse, and recycling of retired automotive lithium-ion batteries (LIBs), have received growing attention, as large volumes of LIBs will retire in the near future and the demand for LIBs continues to grow. At the same time, the relevance of the sustainability of a battery system over its entire life cycle is increasing as factors such as the EU Battery Regulation provide greater market and product transparency. As a result, research and industry require forecasts in order to assess the future market situation and to make well-founded decisions. Therefore, this paper provides forecasts of the return volumes of battery systems from BEVs and PHEVs up to 2035. Additionally, a representative European battery pack for PHEVs and BEVs was evaluated for each year since 2013, based on the ten vehicles with the largest market share in each year until 2021. In addition, the battery return streams are divided into three different 3R strategies based on expert interviews in order to evaluate the upcoming workload in these areas. The term "3R" refers to the sum of the currently existing pathways around reuse, remanufacturing, and recycling. In 2030, about 38.8 GWh will return and enter the recycling process annually. For battery reuse, about 13 GWh will return every year from 2030 onwards, ready to be used in stationary storage for energy transition. Compared to this, battery remanufacturing is expected to be supplied with a slightly lower volume of approximately 11 GWh per year. [ABSTRACT FROM AUTHOR]

Life cycle assessment (LCA) quantifies the whole‐life environmental impacts of products and is essential for helping policymakers and manufacturers transition toward sustainable practices. However, typical LCA estimates future recycling benefits as if it happens today. For long‐lived products such as lithium‐ion batteries, this may be misleading since there is a considerable time gap between production and recycling. To explore this temporal mismatch problem, we apply future electricity scenarios from an integrated assessment model—IMAGE—using "premise" in Brightway2 to conduct a prospective LCA (pLCA) on the global warming potential of six battery chemistries and four recycling routes. We find that by 2050, electricity decarbonization under an RCP2.6 scenario mitigates production impacts by 57%, so to reach zero‐carbon batteries it is important to decarbonize upstream heat, fuels, and direct emissions. For the best battery recycling case, data for 2020 gives a net recycling benefit of −22 kg CO2e kWh−1 which reduces the net impact of production and recycling from 71 to 49 kg CO2e kWh−1. However, for recycling in 2040 with decarbonized electricity, net recycling benefits would be nearly 75% lower (−6 kg CO2e kWh−1), giving a net impact of 65 kg CO2e kWh−1. This is because materials recycled in the future substitute lower‐impact processes due to expected electricity decarbonization. Hence, more focus should be placed on mitigating production impacts today instead of relying on future recycling. These findings demonstrate the importance of pLCA in tackling problems such as temporal mismatch that are difficult to capture in typical LCA. [ABSTRACT FROM AUTHOR]

Ni-rich LiNixMnyCo1−x−yO2 (NMC) materials have been adopted in a range of applications, including electric vehicles. The recycled NMC material from a spent cell would be much more valuable if it could be upgraded to a Ni-rich, more energy-dense version of the material. This work demonstrates a simple, inexpensive, and facile method to upcycle LiNi1/3Mn1/3Co1/3O2 (NMC111, 160 mAh∙g−1), a cathode used in early generations of electric vehicle batteries, to LiNi0.8Mn0.1Co0.1O2 (NMC811, 190 mAh∙g−1), a more energy-dense cathode material. In this study, a preliminary investigation into a room-temperature eutectic synthesis of NMC811 is performed using NMC111, LiOH, and nickel nitrate as precursors. The synthesized material showed the desired crystal structure and stoichiometry, though the cycle life and Li diffusion coefficient need improvement when compared to commercially available NMC811. This study demonstrates an interesting proof of concept of the room-temperature eutectic synthesis process for LIB cathodes and could be improved by tuning the synthesis conditions. [ABSTRACT FROM AUTHOR]

This study provides a comprehensive analysis of global patent trends in battery recycling, focusing on secondary batteries and related technologies across Korea, China, and the United States. The methodology involved collecting data from various patent databases, followed by quantitative analysis to identify technology trends and guide future development. The research employed statistical tools to analyze patent activities, including the frequency and scope of patent filings, and comparative analysis to highlight differences between countries. This study reveals distinct emphases on technologies such as lithium-ion and waste battery recycling, highlighting notable differences in patent activities among key companies and countries. China’s large number of patents in battery manufacturing processes contrasts with the USA’s focus on electrochemical cell construction and storage systems, while Korea shows significant activity in waste battery technology. The novelty of this paper lies in its detailed comparative analysis of patent trends across these three major economies, providing insights into the technological focuses and priorities of each country. The study also identifies key challenges, such as the need for consistent innovation and broader geographic coverage in Korea, enhancing patent influence and international presence in China, and ensuring high patent quality and fostering innovation in lagging sectors in the United States. Addressing these challenges through enhanced collaboration, increased R&D investments, and supportive policies is crucial for strengthening the global position and driving further innovation in the battery recycling sector.

Tremendous efforts are being made toward electrification of the transport sector. Accordingly, next-generation recycling technologies to tackle the large volumes of spent batteries must be urgently innovated. Herein, ionic liquids and the promising ionometallurgy that can overcome some issues of traditional recycling methods are discussed. Ionic liquids-mediated recovery of metals from spent batteries represents a sustainable strategy, featured with new fundamental chemistries. The opportunities for regeneration and reuse of ionic liquids are promising toward a cost-levelized recycling process. The unique chemical environment of ionic liquids also allows the development of coupled electrochemical procedures and upcycling. Future development requires the assessment of continuous operation and holistic process efficiency, technoeconomic and environmental aspects.

As the demand for batteries continues to surge in various industries, effective recycling of used batteries has become crucial to mitigate environmental hazards and promote a sustainable future. This review article provides an overview of current technologies available for battery recycling, highlighting their strengths and limitations. Additionally, it explores the current challenges faced by the industry and discusses potential future advancements. Through an in-depth analysis of the state-of-the-art recycling methods, this review aims to shed light on the progress made in battery recycling and the path ahead for sustainable and efficient battery waste management. [ABSTRACT FROM AUTHOR]

In this paper, a novel procedure is proposed for comprehensively recovering zinc fluoride (ZnF2), manganese fluorides [MnFx(x = 2, 3)], manganese dioxide (MnO2), and carbon powder from the electrode powder of spent alkaline batteries. Firstly, hydrofluoric acid (HF) leaching is conducted on the electrode powder of spent alkaline batteries. Secondly, potassium permanganate (KMnO4) is introduced into the leachate to selectively precipitate manganese (Mn) ions to recover MnO2. Subsequently, the water content in the leachate is evaporated to recover ZnF2. Finally, the leaching residue is leached again by using HF, after which the water content in the leachate is evaporated to recover MnFx. The results indicated that under optimal conditions of a HF concentration of 4 M, a leaching time of 15 min, and a liquid–solid ratio of 5 mL/g, the optimal leaching selectivity for Zn and Mn was achieved and the leaching efficiencies of Zn and Mn were 97.83% and 39.94%, respectively. When KMnO4 with a dosage (KMnO4/Mn ion molar ratio) of 0.5:1 was added to the leachate, MnO2 with a grade of 91.68% and a Mn recovery of 39.07% was obtained. In addition, ZnF2 with a grade of 97.98% and a Zn recovery of 96.15% was also obtained after removing the water content from the leachate via evaporation. Under the optimal conditions of a HF concentration of 2 M, a leaching time of 15 min, and a liquid–solid ratio of 10 mL/g for the leaching residue, followed by removing the water content in the leachate via evaporation, MnFx with a grade of 94.20% and a Mn recovery of 59.46%, was obtained. The residue of the releaching process was carbon powder. The effectiveness of the proposed recovery procedure was confirmed. [ABSTRACT FROM AUTHOR]

The recovery of critical metals from spent lithium‐ion batteries (LIBs) is rapidly growing. Current methods are energy‐intensive and hazardous, while alternative solvent‐based strategies require more studies on their 'green' character, metal dissolution mechanism and industrial applicability. Herein, we bridged this gap by studying the effect of dilute HCl solutions in hydroxylated solvents to dissolve Co, Ni and Mn oxides. Ethylene glycol emerged consistently as the most effective solvent, dissolving up to four times more Co and Ni oxides than using aqueous acidic media, attributed to improved chloro‐complex formation and solvent effects. These effects had a significant contribution compared to acid type and concentration. The highest Co dissolution (0.27 M) was achieved in 0.5 M HCl in 25 % (v/v) glycerol in water, using less acid and a significant amount of water compared to other solvent systems, as well as mild temperatures (40 °C). This solvent was applied to dissolve battery cathode material, achieving 100 % dissolution of Co and Mn and 94 % dissolution of Ni, following what was concluded to be a mixed mechanism. These results offer a simple alternative to current leaching processes, reducing acid consumption, enhancing atomic efficiency, and paving the way for optimized industrial hydrometallurgical processes leaning to 'greener' strategies. [ABSTRACT FROM AUTHOR]

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Despite their safe and cost‐effective merits, the cycling durability of aqueous zinc–organic batteries is hindered by cathode dissolution and low coulombic efficiency of Zn metal anodes. Herein, a Zn metal‐free all‐organic zinc‐ion battery (ZIB) is proposed by using quinoxalino[2,3‐i]diquinoxalino[2′,3′:6,7]quinoxalino[2,3‐a:2,3‐c] phenazine (QDPA) cathode coupled with a 1,4,5,8‐Naphthalenetetracarboxylic diimide (NPI) anode, rendering excellent electrochemical reversibility with high utilization. Based on the molecular architecture strategy, a QDPA cathode with an enlarged aromatic ring system is designed and synthesized, which not only effectively inhibits structural collapse during cycling but also enhances the working voltage without lowering the active group ratio. Moreover, theoretical calculations and experimental results confirm the rapid H+ storage mechanism in the CN active sites of QDPA, affording ultra‐fast electrochemical kinetics. Thus, it delivers a negligible capacity decay of 0.002% up to 13 000 cycles at 20 A g−1. Moreover, the QDPA//NPI all‐organic aqueous ZIB with a high energy density of 43.1 Wh kg−1 is demonstrated to be easily disassembled and recycled by the incineration treatment after battery failure, ensuring outstanding environmental sustainability. [ABSTRACT FROM AUTHOR]

Lithium-ion battery (LIB) pack is the core component of electric vehicles (EVs). As the demand is continuously increasing, it puts a lot of strain on the battery raw material supply chains. Likewise, the large quantity of spent LIBs from different sources will add to the complexity of end-of-life (EoL) management. Battery recycling processing is a potential source of critical cathode precursor materials as an alternative to virgin raw material sourcing. Indeed, metal sulfates (nickel, cobalt, and manganese) and lithium carbonate could be recovered through EoL processing. This study aims to provide an economic and environmental life cycle sustainability assessment of recycled battery materials. This assessment is based on a bottom-up approach considering geographical boundaries and process data inputs. The two sources of critical cathode battery materials, virgin and recycled battery materials, are compared based on economic and environmental indicators. This study identified the province of Quebec in Canada as the geographical boundary where several battery processing plants have been recently announced. The best available recycling process (hydrometallurgy) was selected. For the virgin materials, this study considers the option of importing from other jurisdictions by using global average supply chain values. Furthermore, a comparison of alternative supply chain configurations was performed using a spatially differentiated approach. The main findings of this study are as follows: (i) the environmental credit of recycled cathode active materials (CAMs) is estimated as −6.46 kg CO2e/kg CAM, and (ii) the overall cost and environmental impacts of producing LIB cathode active material from recycled battery materials can be 48% and 54% lower than production from virgin materials, respectively, considering the upstream, midstream, and downstream stages of the CAM supply chain. The main drivers for the reduction in these financial costs and emissions are the local transportation and the hydrometallurgical process. The assessment results provide insights to support the development of appropriate policies and R&D solutions adapted to local considerations as well as offer additional possibilities to improve the design of sustainable supply chains for LIB recycling. [ABSTRACT FROM AUTHOR]