Prediction of metal recovery potential of end-of-life NEV batteries in China based on GRA-BiLSTM.

As Chinese new energy vehicle (NEV) sales continue to grow, end-of-life batteries have great potential for recycling in the future. In this study, a combined model based on Gray Relation Analysis and Bi-directional Long Short-Term Memory (GRA-BiLSTM) is proposed for predicting NEV sales, and the NEV battery life is modeled using the Weibull distribution. Then, the amount of end-of-life batteries, secondary utilization and metal recycling are calculated. The impact of end-of-life battery recycling on the supply and demand of key metals is studied. The results show that in 2040, the secondary utilization of end-of-life batteries in the Standard Growth Rate-Lithium Iron Phosphate Battery Dominated-High Secondary Utilization rate scenario (SGR-LFPH) is 391.76 GWh. The recycling volumes of lithium, nickel and cobalt are 45,900 tons, 92,900 tons and 22,100 tons, respectively. In the Standard Growth Rate-lithium nickel cobalt manganese oxide Battery Dominated-Low Secondary Utilization rate scenario (SGR-NCML), the recycling of lithium, nickel and cobalt is even greater, at 62,600 tons, 372,200 tons and 71,700 tons, respectively. End-of-life batteries recycling can reduce the demand for metals. However, as NEV sales continue to grow, the gap between metal supply and demand remains significant. The findings urge the Chinese government develop appropriate battery management strategies to increase the recycling rate of end-of-life batteries; and to encourage enterprises to research new types of batteries to resolve the conflict between supply and demand for metals.

Removal and recovery of phosphorus and fluorine in process water from water based direct physical lithium-ion battery recycling.

In the present work, the recovery of phosphorus and fluorine from process water generated in a water based direct physical recycling process of Li-ion batteries has been studied. The recycling process considered in this work produces significant amounts of process water, which is generated during the opening of the batteries by means of electro-hydraulic fragmentation and the subsequent sorting of the components in aqueous solution. This process produces between 21.6 L and 30.3 L of process water per kg of batteries with a total phosphorus and a total fluorine concentration of 60-85 mg/L and 120-470 mg/L, respectively. Currently, the process water has to be disposed of as hazardous waste. The goal is to discharge the wastewater into the sewer system. For this the total phosphorus and total fluorine concentration must be reduced. The process water is mainly contaminated by the released electrolyte consisting of organic carbonates and conducting salts. 31-P and 19-F NMR shows conclusively that no hydrolysis takes place in this process water. The phosphorus is present exclusively in the form of the complex anion PF6- and fluorine as F-, namely as FSI- from the conducting salt LiFSI and PF6- from the conducting salt LiPF6. In order to meet the regulatory requirements for discharge into the sewage system, 70.4% of the phosphorus and 89.3% of the fluorine must be removed. The conducting salts are hydrolyzed by adding acid and thereby phosphate and fluoride are precipitated. After critical and valuable materials are recovered the process water can be discharged into the sewer system.

Phase-separated solvothermal high yields recovery of lithium and cobalt cathode precursors from end-of-life LiCoO2 lithium-ion batteries.

Lithium-ion batteries (LIBs) recycling is one of the most urgent challenges affecting this technological sector. Indeed, their continuously growing production and demand is already leading to the creation of large volumes of end-of-life LIBs (EoL-LIBs). At the same time, the growing demand for LIBs is not sustainable from the point of view of supply of the critical raw materials needed to produce the essential components of LIBs. The development of efficient and sustainable recycling strategies provides a solution to these two urgent issues. Here we propose a new ternary deep eutectic solvent (DES) composition based on choline chloride, citric acid, and ethylene glycol in molar ratio 1:1:1 for the reductive degradation of LiCoO2 cathode. The optimized leaching process (5g of DES for 100 mg of black mass for 30 min at 140 °C) leads to the full degradation of the cathode with extraction yields above 97% for both Li and Co. Simple electrochemical tests confirm irreversible DES degradation, making its recovery and reuse impractical. We demonstrate that a subsequent thermal treatment, using DES as a sacrificial agent, allows to separate and recover Co3O4 and LiCl with adequate purity to be exploited for LiCoO2 resynthesis. As a proof of concept, a new batch of LiCoO2 is synthesized and used for new cells' assembly. The performance of the resynthesized material is comparable with that of the commercial benchmark material, demonstrating the possibility of a full closed-loop recycling route.

Magnetic Supraparticles as Identifiers in Single-Layer Lithium-Ion Battery Pouch Cells.

The development of effective recycling technologies is essential for the recovery and reuse of the raw materials required for lithium-ion batteries (LIBs). Future recycling processes depend on accessible information, necessitating the implementation of a digital battery passport. The European battery regulation mandates the use of a machine-readable identifier physically attached to the batteries for accessing digital information. Since externally applied optical labels are vulnerable to mechanical damage, technologies for identification without these restrictions could be beneficial. This study demonstrates that magnetic supraparticles (SPs) can be used for contactless identification of lithium nickel manganese cobalt oxide (NMC) battery pouch cells via magnetic particle spectroscopy (MPS) and that multiple pouch cells can be discriminated based on their specific magnetic code. A comparison of three independent model scenarios revealed that the detection of SPs and the impact on cell performance are dependent on the integration location. The results validate the concept of magnetic identification in metallic environments with MPS as an alternative to optical labeling methods. This study provides a foundation for the development of a new selective labeling and identification technology for batteries, with the potential to facilitate recycling and contribute to a more sustainable future.

Comparison of blood lead levels between battery recycling workers and controls in Northern Nigeria.

About 80% of the global lead production is consumed by the battery industry. As old batteries are increasingly being recycled without adequate recourse to safety and protection in many developing countries, there is well-documented evidence of lead poisoning among the workers. This study compared blood lead levels (BLL) of battery recycling workers (BRW) with controls in Northern Nigeria. This cross-sectional study assessed the BLL of BRW (self-employed informal workers, n = 98) and controls (healthcare workers, n = 98). Respondents were selected using systematic random sampling from the lists of BRW and healthcare workers. All respondents in the two groups were males, matched for age (27.81 ± 7.2, 27.67 ± 7.0 years; p = 0.890). The mean BLL was significantly higher (p < 0.001) among the BRW compared to the controls (40.17 ± 4.2 and 3.61 ± 0.4 µg/dL, respectively), with 78.1% of the BRW having elevated BLL (≥20.0 µg/dL) and none (0.0%) of the controls having elevated BLL. Logistic regression shows none of the variables was an independent predictor of BLL in this study, implying battery reclamation as the main source of lead. Federal and state government policies should ban informal battery recycling and emphasize on plants through national collection system to consolidate used batteries only to smelters that meet minimum regulatory requirements.

Consumer preference and willingness-to-pay for formal recycling of electric vehicle batteries: A discrete choice experiment in China.

The burgeoning electric vehicle (EV) market poses a substantial challenge to battery recycling systems, yet understanding EV battery recycling behavior from the demand side remains limited. Previous studies have analyzed perceptual or attitudinal factors, neglecting the observable attributes of EV battery recycling. To this end, we proposed a discrete choice model to investigate the differences between formal and informal recycling behaviors, identifying consumer preferences and willingness to pay. By analyzing 1190 sample data collected from Chongqing, China, we find that: (1) The formal recycling market exhibits greater sensitivity to prices compared to the informal recycling market. (2) The formal recycling market favors recycling by EV battery producers, whereas the informal recycling market shows the least preference for recycling by automobile producers. (3) Door-to-door recycling services are the most effective in facilitating the transition from informal to formal recycling markets for EV batteries. (4) Capacity subsidy policies outperform one-time fixed subsidy policies in incentivizing formal recycling. (5) The formal recycling market for EV batteries necessitates "traceability to the recycling outlet", as opposed to being untraceable. (6) The high-awareness group exhibits greater sensitivity to government policies compared to those with lower environmental concerns and less knowledge of EV battery recycling.

Multiple benefits of new-energy vehicle power battery recycling strategies based on the theory of planned behavior and stimulus organism response.

With the yearly increasing market penetration of new-energy vehicles in China, the retirement of power batteries has gradually become a scale, and most of the waste batteries have entered informal recycling channels, which has induced a series of environmental problems. Considering this issue, we introduced the system dynamics (SD), stimulus organism response (SOR), and the theory of planned behavior (TPB) in behavioral economics to establish the environmental economic benefit evaluation model of power battery recycling strategies, and we performed a dynamic simulation analysis on the effect of government subsidy policy, policy advocacy, and other recycling strategies. The results show that: (1) the recovery subsidy policy can improve the formal recycling quantity and economic benefits of recovery, but the effect on the degree of environmental pollution is limited. (2) The combination of environmental awareness promotion strategy and subsidy policy can overcome the shortcomings of subsidy policy and has significant environmental and economic performance. (3) Compared with the benchmark scenario, the formal recycling quantity, the CO2 emission reduction, and the economic benefits of recovery in scenario 4 (high subsidy-high policy propaganda strategy) increased by approximately 112 %, 208 %, and 223 %, respectively, and the degree of environmental pollution decreased by approximately 65 %.

All-in-All: Dead Lithium-Ion Battery to Active Lithium-Ion Capacitor.

Here, we have developed lithium-ion capacitors (LICs) with all the components, except the electrolyte solution, effectively recycled from the spent Lithium-ion batteries (LIBs). Hybrid capacitors, such as LICs, are potential breakthroughs in electrochemical energy storage devices, where most research is focused. These devices can simultaneously guarantee high energy and power by hybridizing battery-type and capacitive-type electrodes with two different reaction mechanisms. We have successfully upcycled the graphite, current collector, separator, etc., from the spent LIBs to fabricate a high-performance LIC. Our LIC consists of recovered graphite (RG) coated over recovered copper foil as an anode, recycled polypropylene as the separator, and reduced graphene oxide (rGO) synthesized from RG as the cathode. The RG half-cell exhibited an excellent specific capacity of 302 mAh g-1 even after 75 charge-discharge cycles with a coulombic efficiency of >99 %. The Li/rGO displayed remarkable cycling performance for over 1000 cycles with high stability and reversibility. Subsequently, the pre-lithiated RG (p-RG) electrode is paired with the rGO electrode under the balanced loading conditions to construct LIC, rGO/p-RG, delivering a maximum energy density of 185 Wh kg-1 with ultra-long durability of more than 10,000 cycles. The possibility of LIC under different climatic conditions is also explored, and its remarkable performance under various temperature conditions is worth mentioning.

Emerging Processes for Sustainable Li-Ion Battery Cathode Recycling.

The colossal growth in the use of Li-ion batteries (LiBs) has raised serious concerns over the supply chain of strategic minerals, e.g., Co, Ni, and Li, that make up the cathode active materials (CAM). Recycling spent LiBs is an important step toward sustainability that can establish a circular economy by effectively tackling large amounts of e-waste while ensuring an unhindered supply of critical minerals. Among the various methods of LiB recycling available, pyro- and hydrometallurgy have been utilized in the industry owing to their ease of operation and high efficiency, although they are associated with significant environmental concerns. Direct recycling, a more recent concept that aims to relithiate spent LiBs without disrupting the lattice structure of the CAMs, has been realized only in the laboratory scale so far and further optimization is required before it can be extended to the bulk scale. Additionally, significant progress has been made in the areas of hydrometallurgy in terms of using ecofriendly green lixiviants and alternate sources of energy, e.g., microwave and electrochemical, that makes the recycling processes more efficient and sustainable. In this review, the latest developments in LiB recycling are discussed that have focused on environmental and economic viability, as well as process intensification. These include deep eutectic solvent based recycling, electrochemical and microwave-assisted recycling, and various types of direct recycling.

Toward Sustainable Polymer Materials for Rechargeable Batteries: Utilizing Natural Feedstocks and Recycling/Upcycling of Polymer Waste.

The ever-increasing demand for rechargeable battery systems in the era of electric vehicles has spurred extensive research into developing polymeric components for batteries, such as separators, polymer electrolytes, and binders. However, current battery systems rely on expensive and nonrenewable resources, which potentially have a negative environmental impact. Therefore, polymer materials derived from natural resources have gained significant attention, primarily due to their cost-effective and environmentally sustainable features. Moreover, natural feedstocks often possess highly polar functional groups and high molecular weights, offering desirable electro-chemo-mechanical features when applied as battery materials. More recently, various recycling and upcycling strategies for polymeric battery components have also been proposed given the substantial waste generation from end-of-life batteries. Recycling polymeric materials includes an overall process of recovering the components from spent batteries followed by regeneration into new materials. Polymer upcycling into battery materials involves transforming daily-used plastic waste into high-value-added battery components. This review aims to give a state-of-the-art overview of contemporary methods to develop sustainable polymeric materials and recycling/upcycling strategies for various battery applications.

Leaching of NMC industrial black mass in the presence of LFP.

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.

What determines the batteries recycling behavior of e-bike citizens in Guangzhou?: Integrating place identity and environmental concern into the extended norm activation model.

Battery recycling is viewed in China as an important means of achieving primary sustainability goals and greater economic and environmental development. With the notice of high battery recycling intentions through relevant investigations, this study examine the influencing factors of these recycling behaviors of e-bikes citizens by incorporating the place identity and environmental concern into the Extended Normative Activation Model (NAM), which fill the research gap on how place identity and environmental concern affect the batteries recycling behavior. This study proposes that the consequence awareness, personal norms, and attitudes have mediating effect on place identity to the recycling behavior, and the environmental concern has moderating effect on consequence awareness, personal norms, and attitudes to the recycling behavior, respectively. Based on 1068 valid surveys, hypotheses were examined using partial least square structural equation modeling (PLS-SEM). The results show that personal norms and awareness of consequences positively impact e-bike users' intentions to recycle waste batteries, and environmental concerns have no moderating effect on attitude, recycling intention, personal norms, and recycling intention. Theoretical and practical implications are discussed at last.

Sustainable reprocessing of lithium iron phosphate batteries: A recovery approach using liquid-phase method at reduced temperature.

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 N2H4·H2O 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 LiFePO4 matches commercial LiFePO4 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 LiFePO4 and similar materials.

Recyclable Organic Radical Electrodes for Metal-Free Batteries.

Organic batteries are one of the possible routes for transitioning to sustainable energy storage solutions. However, the recycling of organic batteries, which is a key step toward circularity, is not easily achieved. This work shows the direct recycling of poly(2,2,6,6-tetramethylpiperidinyloxy-4-yl) (PTMA) and poly(2,2,6,6-tetramethylpiperidinyloxy-4-yl acrylamide) (PTAm) based composite electrodes. After charge-discharge cycling, the electrodes are deconstructed using a solubilizing-solvent and then reconstructed using a casting-solvent. The electrochemical properties of the original and recycled electrodes are compared using cyclic voltammetry (CV) and galvanostatic charge-discharge (GCD) cycling, from which it is discovered using time-of-flight secondary ion mass spectrometry (ToF-SIMS) that recycling can be challenged by the formation of a cathode electrolyte interphase (CEI). In turn, an additive is proposed to modify the CEI layer and improve the properties after recycling. Last, an anionic rocking chair battery consisting of PTAm electrodes as both positive and negative electrodes is demonstrated, in which the electrodes are recycled to form a new battery. This work demonstrates the recycling of composite electrodes for organic batteries and provides insights into the challenges and possible solutions for recycling the next-generation electrochemical energy storage devices.

Approaching Sustainable Lithium-Ion Batteries through Voltage-Responsive Smart Prelithiation Separator with Surface-Engineered Sacrificial Lithium Agents.

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.

Circular And Sustainable: Evaluating Lithium-Ion Battery Recycling using a Combined Statistical Entropy and Life Cycle Assessment Methodology.

While there has been a growing interest on the concept of Circular Economy (CE), its correlation with sustainability remains controversial. In this work, the combination of Statistical Entropy Analysis (SEA) and Life Cycle Assessment (LCA) is proposed as a new methodology to evaluate recycling processes from the perspective of materials circularity and environmental impacts using a Li-ion battery recycling process as a case study. This work addresses the need of quantitative circularity indicators, as SEA evaluates the concentration of materials at a systems level, while LCA measures the environmental impact of recycling processes in comparison with virgin raw materials production. It was found that process optimization points can be found by simultaneously accounting for materials recovery and the LCA categories of global warming potential, ozone depletion and mineral resource scarcity. Furthermore, a strong correlation was found for the first time between the recovery of critical elements and the environmental impact of raw materials production. The proposed methodology thus offers a robust analysis of a product lifecycle that aids in its design and optimization from the CE perspective.

A study on recovery strategies of graphite from mixed lithium-ion battery chemistries using froth flotation.

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-TiO2 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 TiO2 resulted in a low grade product (<96 %) attributed to the significant entrainment of ultrafine TiO2 particles. These results suggest that flotation of graphite should be preferably carried out before hydrometallurgical treatment of black mass.

Fast Li Replenishment Channels-Assisted Recycling of Degraded Layered Cathodes with Enhanced Cycling Performance and Thermal Stability.

The direct recycling of cathode materials in lithium-ion batteries is important for environmental protection and resource conservation. The key regeneration processes are composition replenishment and atom rearrangement, both of which depend on the migration and diffusion of atoms. However, for the direct recycling of degraded LiNi0.5Co0.2Mn0.3O2 (D-NCM523) cathode, the irreversible phase transitions that accumulate during the long-term cycles block the Li diffusion channels with a high diffusion energy barrier, making it difficult to fully repair the layered structure and resulting in rapid capacity decay. To address the challenge, fast Li replenishment channels are rebuilt to regulate the surface phase and effectively assist the regeneration process with a reduced energy barrier. This method reduces the amount of Li supplement by >75% and shortens the sintering time (only 2 h) to fully regenerate D-NCM523, compared to general direct recycling methods. The regenerated NCM523 (LCMB-NCM523) exhibits a satisfactory repaired specific capacity of 160 mAh g-1 and excellent cycling stability, retaining 78% of its capacity after 300 cycles. In addition, LCMB-NCM523 is recycled with improved thermal decomposition peak temperature and enables 200 cycles even at 60 °C, greatly improving safety. This work proposes a promising way for the large-scale direct regeneration of layered cathodes.

Selective Extraction of Critical Metals from Spent Li-Ion Battery Cathode: Cation-Anion Coordination and Anti-Solvent Crystallization.

Owing to continuing global use of lithium-ion batteries (LIBs), in particular in electric vehicles (EVs), there is a need for sustainable recycling of spent LIBs. Deep eutectic solvents (DESs) are reported as "green solvents" for low-cost and sustainable recycling. However, the lack of understanding of the coordination mechanisms between DESs and transition metals (Ni, Mn and Co) and Li makes selective separation of transition metals with similar physicochemical properties practically difficult. Here, it is found that the transition metals and Li have a different stable coordination structure with the different anions in DES during leaching. Further, based on the different solubility of these coordination structures in anti-solvent (acetone), a leaching and separation process system is designed, which enables high selective recovery of transition metals and Li from spent cathode LiNi1/3Co1/3Mn1/3O2 (NCM111), with recovery of acetone. Recovery of spent LiCoO2 (LCO) cathode is also evidenced and a significant selective recovery for Co and Li is established, together with recovery and reuse of acetone and DES. It is concluded that the tuning of cation-anion coordination structure and anti-solvent crystallization are practical for selective recovery of critical metal resources in the spent LIBs recycling.

Resource recovery and regeneration strategies for spent lithium-ion batteries: Toward sustainable high-value cathode materials.

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 LiCoO2 and LiMn2O4. 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.