Search Results (457)

The literature clearly indicates that both academia and industry are strongly committed to developing comprehensive processes for spent Li-ion battery (LIB) recycling. In this regard, the current study presents an original contribution by providing a quantitative assessment of a large-scale recycling plant designed for the treatment of completely spent LIBs. In addition to a concept of the basic process, this assessment also considers a case study of a thermal integration and CO₂ capture subsystem. Process flow modeling software was used to evaluate the contribution of all process steps and equipment to overall energy consumption and to mass balance the data required for the technical assessment of the large-scale recycling plant. To underline the advantages and identify the optimal novel process concept, several key performance indicators were determined, such as recovery efficiency, specific energy/material consumption, and specific CO₂ emissions. In addition, the economic potential of the recycling plants was evaluated for the defined case studies based on capital and O&M costs. The results indicate that, even with CO₂ capture applied, the thermally integrated process with the combustion of hydrogen produced in the recycling plant remains the most promising large-scale configuration for spent LIB recycling. Full article

Lithium-ion batteries (LiBs) are utilized in numerous applications due to advancements in technology, and the recovery of end-of-life (EoL) LiBs is imperative for environmental and economic reasons. Pyrometallurgical and hydrometallurgical methods have been used in the recovery of metals such as Li, Co, and Ni in the EoL LiBs. Hydrometallurgical methods, which have been demonstrated to exhibit higher recovery efficiency and reduced energy consumption, have garnered increased attention in recent research. Inorganic acids, including HCl, HNO₃, and H₂SO₄, as well as organic acids such as acetic acid and citric acid, are employed in the hydrometallurgical recovery of these metals. It is imperative to acknowledge the environmental hazards posed by these acids. Consequently, solvometallurgical processes, which involve the use of organic solvents with minimal or no water, are gaining increasing attention as alternative or complementary techniques to conventional hydrometallurgical processes. In the context of solvent systems that have been examined for a range of solvometallurgical methods, deep eutectic solvents (DESs) have garnered particular interest due to their low toxicity, biodegradable nature, tunable properties, and efficient metal recovery potential. In this study, the leaching process of black mass containing graphite, LCO, NMC, and LMO was carried out in a short time using the ternary DES system. The ternary DES system consists of choline chloride (ChCl), glycolic acid (GLY), and ascorbic acid (AA). As a result of the leaching process of cathode powders in the black mass without any pre-enrichment process, Li, Co, Ni, and Mn elements passed into solution with an efficiency of over 95% at 60 °C and within 1 h. Moreover, the kinetics of the leaching process was investigated, and Density Functional Theory (DFT) calculations were used to explain the leaching mechanism. Full article

The growing demand for high-energy, safe, and sustainable lithium-ion batteries has increased interest in nickel-rich cathode materials and solid-state electrolytes. This study presents a scalable wet-processing method for fabricating composite cathodes for all-solid-state batteries. The cathodes studied herein are high-nickel LiNi_0.90Mn_0.05Co_0.05O₂, NMC955, the sulfide-based electrolyte Li₆PS₅Cl, and alternative binders—polyvinyl alcohol (PVA) and polyisobutylene (PIB)—dispersed in toluene, a non-polar solvent compatible with the electrolyte. After fabrication, the cathodes were characterized using SEM/EDX, sheet resistance, and Hall effect measurements. Electrochemical tests were additionally performed in all-solid-state battery half-cells comprising the synthesized cathodes, lithium metal anodes, and Li₆PS₅Cl as the separator and electrolyte. The results show that both PIB and PVA formulations yielded conductive cathodes with stable microstructures and uniform particle distribution. Electrochemical characterization exposed that the PVA-based cathode outperformed the PIB-based counterpart, achieving the theoretical capacity of 192 mAh·g⁻¹ even at 1C, whereas the PIB cathode reached a maximum capacity of 145 mAh.g⁻¹ at C/40. Post-mortem analysis confirmed the structural integrity of the cathodes. These findings demonstrate the viability of NMC955 as a high-capacity cathode material compatible with solid-state systems. Full article

The conventional spent lithium-ion batteries (LIBs) recycling method suffers from complex processes and excessive chemical consumption. Hence, this study proposes an electrochemical strategy for achieving reductant-free leaching of high-valence transition metals and efficient separation of valuable components from spent cathode sheets (CSs). An innovatively designed sandwich-structured electrochemical reactor achieved efficient reductive dissolution of cathode materials (CMs) while maintaining the structural integrity of aluminum (Al) foils in a dilute sulfuric acid system. Optimized current enabled leaching efficiencies exceeding 93% for lithium (Li), cobalt (Co), manganese (Mn), and nickel (Ni), with 88% metallic Al foil recovery via cathodic protection. Multi-scale characterization systematically elucidated metal valence evolution and interfacial reaction mechanisms, validating the technology’s tripartite innovation: simultaneous high metal extraction efficiency, high value-added Al foil recovery, and organic removal through single-step electrochemical treatment. The process synergized the dissolution of CM particles and hydrogen bubble-induced physical liberation to achieve clean separation of polyvinylidene difluoride (PVDF) and carbon black (CB) layers from Al foil substrates. This method eliminates crushing pretreatment, high-temperature reduction, and any other reductant consumption, establishing an environmentally friendly and efficient method of comprehensive recycling of battery materials. Full article

Pyrometallurgical recycling of lithium-ion batteries presents distinct advantages including streamlined processing, simplified pretreatment requirements, and high throughput capacity. However, its industrial implementation faces challenges associated with high energy demands and lithium loss into slag phases. This investigation develops an integrated reduction smelting–chloridizing volatilization process for the comprehensive recovery of strategic metals (Li, Mn, Cu, Co, Ni) from spent ternary lithium-ion batteries; calcium chloride was selected as the chlorinating agent for this purpose. Thermodynamic analysis was performed to understand the phase evolution during reduction smelting and to design an appropriate slag composition. Preliminary experiments compared carbon and aluminum powder as reducing agents to identify optimal operational parameters: a smelting temperature of 1450 °C, 2.5 times theoretical CaCl₂ dosage, and duration of 120 min. The process achieved effective element partitioning with lithium and manganese volatilizing as chloride species, while transition metals (Cu, Ni, Co) were concentrated into an alloy phase. Process validation in an induction furnace with N₂-O₂ top blowing demonstrated enhanced recovery efficiency through optimized oxygen supplementation (four times the theoretical oxygen requirement). The recovery rates of Li, Mn, Cu, Co, and Ni reached 94.1%, 93.5%, 97.6%, 94.4%, and 96.4%, respectively. This synergistic approach establishes an energy-efficient pathway for simultaneous multi-metal recovery, demonstrating industrial viability for large-scale lithium-ion battery recycling through minimized processing steps and maximized resource utilization. Full article

This work presents a comprehensive investigation into the interfacial charge storage mechanisms and lithium-ion transport behavior of Li-metal all-solid-state batteries (ASSBs) employing LiFePO₄ (LFP) cathodes fabricated via alternating current electrophoretic deposition (AC-EPD) and Li_1.3Al_0.3Ti_1.7(PO₄)₃ (LATP) as the solid-state electrolyte. We demonstrate that optimal sintering improves the LATP–LFP interfacial contact, leading to higher lithium diffusivity (~10⁻⁹ cm²∙s⁻¹) and diffusion-controlled kinetics (b ≈ 0.5), which directly translate to better rate capability. Structural and electrochemical analyses—including X-ray diffraction, scanning electron microscopy, cyclic voltammetry, and rate capability tests—demonstrate that the cell with LATP sintered at 900 °C delivers the highest Li-ion diffusivity (~10⁻⁹ cm²∙s⁻¹), near-ideal diffusion-controlled behavior (b-values ~0.5), and superior rate capability. In contrast, excessive sintering at 1000 °C led to reduced diffusivity (~10⁻¹⁰ cm²∙s⁻¹). The liquid electrolyte system showed higher b-values (~0.58), indicating the inclusion of surface capacitive behavior. The correlation between b-values, diffusivity, and morphology underscores the critical role of interface engineering and electrolyte processing in determining the performance of solid-state batteries. This study establishes AC-EPD as a viable and scalable method for fabricating additive-free LFP cathodes and offers new insights into the structure–property relationships governing the interfacial transport in ASSBs. Full article

In the wake of global energy transition and the “dual-carbon” goal, the rapid growth of electric vehicles has posed challenges for large-scale lithium-ion battery decommissioning. Retired batteries exhibit dual attributes of strategic resources (cobalt/lithium concentrations several times higher than natural ores) and environmental risks (heavy metal pollution, electrolyte toxicity). This paper systematically reviews pyrometallurgical and hydrometallurgical recovery technologies, identifying bottlenecks: high energy/lithium loss in pyrometallurgy, and corrosion/cost/solvent regeneration issues in hydrometallurgy. To address these, an integrated recycling process is proposed: low-temperature physical separation (liquid nitrogen embrittlement grinding + froth flotation) for cathode–anode separation, mild roasting to convert lithium into water-soluble compounds for efficient metal oxide separation, stepwise alkaline precipitation for high-purity lithium salts, and co-precipitation synthesis of spherical hydroxide precursors followed by segmented sintering to regenerate LiNi_1/3Co_1/3Mn_1/3O₂ cathodes with morphology/electrochemical performance comparable to virgin materials. This low-temperature, precision-controlled methodology effectively addresses the energy-intensive, pollutive, and inefficient limitations inherent in conventional recycling processes. By offering an engineered solution for sustainable large-scale recycling and high-value regeneration of spent ternary lithium ion batteries (LIBs), this approach proves pivotal in advancing circular economy development within the renewable energy sector. Full article

This study investigates the optimization of an ammonia-based leaching process for the recovery of lithium and cobalt from spent LiCoO₂ cathodes, coupled with an energy-efficient ammonia stripping approach. Kinetic analysis revealed that both lithium and cobalt extraction follow pseudo-first-order kinetics, with activation energies of 76.54 kJ/mol and 97.22 kJ/mol, respectively, indicating a chemically controlled process. Optimal leaching conditions were established at 6 M NH₃, 1.5 M (NH₄)₂CO₃, liquid-to-solid ratio of 10:1, and 70 °C for 5 h, achieving 82.5% lithium and 96.1% cobalt recovery. The ammonia stripping process was optimized for energy efficiency, with operations at 95–98 °C providing the best balance between rapid NH₃ removal and energy consumption. At 98 °C, energy demand was reduced to ~282 kJ/mol, a sevenfold improvement over lower temperature operations. A stepwise separation strategy was developed, involving selective lithium precipitation at pH 10.7–10.8, followed by controlled ammonia stripping to precipitate cobalt at pH 8.8–9.0. This integrated approach offers a promising alternative to conventional acid-based recycling methods, combining high metal recovery with improved energy efficiency and reagent recyclability. Full article

Next-generation recycling technologies must be urgently innovated to tackle huge volumes of spent batteries, photovoltaic panels or printed circuit boards (WPCBs). Current e-waste recycling industrial technology is dominated by traditional recycling technologies. Herein, ionic liquids (ILs), deep eutectic solvents (DESs) and promising oxidizing additives that can overcome some traditional recycling methods of metal ions from e-waste, used in our works from last year, are presented. The unique chemical environments of ILs and DESs, with the application of low-temperature extraction procedures, are important environmental aspects known as “Green Methods”. A closed-loop system for recycling zinc and manganese from the “black mass” (BM) of waste, Zn-MnO₂ batteries, is presented. The leaching process achieves a high efficiency and distribution ratio using the composition of two solvents (Cyanex 272 + diethyl phosphite (DPh)) for Zn(II) extraction. High extraction efficiency with 100% zinc and manganese recovery is also achieved using DESs (cholinum chloride/lactic acid, 1:2, DES 1, and cholinum chloride/malonic acid, 1:1, DES 2). New, greener recycling approaches to metal extraction from the BM of spent Li-ion batteries are presented with ILs ([N_8,8,8,1][Cl], (Aliquat 336), [P_6,6,6,14][Cl], [P_6,6,6,14][SCN] and [Benzet][TCM]) eight DESs, Cyanex 272 and D2EHPA. A high extraction efficiency of Li(I) (41–92 wt%) and Ni(II) (37–52 wt%) using (Cyanex 272 + DPh) is obtained. The recovery of Ni(II) and Cd(II) from the BM of spent Ni-Cd batteries is also demonstrated. The extraction efficiency of DES 1 and DES 2, contrary to ILs ([P_6,6,6,14][Cl] and [P_6,6,6,14][SCN]), is at the level of 30 wt% for Ni(II) and 100 wt% for Cd(II). In this mini-review, the option to use ILs, DESs and Cyanex 272 for the recovery of valuable metals from end-of-life WPCBs is presented. Next-generation recycling technologies, in contrast to the extraction of metals from acidic leachate preceded by thermal pre-treatment or from solid material only after thermal pre-treatment, have been developed with ILs and DESs using the ABS method, as well as Cyanex 272 (only after the thermal pre-treatment of WPCBs), with a process efficiency of 60–100 wt%. In this process, four new ILs are used: didecyldimethylammonium propionate, [N_10,10,1,1][C₂H₅COO], didecylmethylammonium hydrogen sulphate, [N_10,10,1,H][HSO₄], didecyldimethylammonium dihydrogen phosphate, [N_10,10,1,1][H₂PO₄], and tetrabutylphosphonium dihydrogen phosphate, [P_4,4,4,4][H₂PO₄]. The extraction of Cu(II), Ag(I) and other metals such as Al(III), Fe(II) and Zn(II) from solid WPCBs is demonstrated. Various additives are used during the extraction processes. The Analyst 800 atomic absorption spectrometer (FAAS) is used for the determination of metal content in the solid BM. The ICP-OES method is used for metal analysis. The obtained results describe the possible application of ILs and DESs as environmental media for upcycling spent electronic wastes. Full article

Objective: The rapid growth of electric vehicle (EV) adoption has led to an unprecedented increase in lithium-ion battery (LIB) demand and end-of-life waste, underscoring the urgent need for effective recycling strategies. This review evaluates current progress in EV battery recycling and explores future prospects. Design: Review based on PRISMA 2020. Data sources: Scientific publications indexed in major databases such as Scopus, Web of Science, and ScienceDirect were searched for relevant studies published between 2020 and 15 April 2025. Inclusion criteria: Studies were included if they were published in English between 2020 and 15 April 2025, and focused on the recycling of electric vehicle batteries. Eligible studies specifically addressed (i) recycling methods, technologies, and material recovery processes for EV batteries; (ii) the impact of recycled battery systems on power generation processes and grid stability; and (iii) assessments of materials used in battery manufacturing, including efficiency and recyclability. Review articles and meta-analyses were excluded to ensure the inclusion of only original research data. Data extraction: Data were independently screened and extracted by two researchers and analyzed for recovery rates, environmental impact, and system-level energy contributions. One researcher independently screened all articles and extracted relevant data. A second researcher validated the accuracy of extracted data. The data were then organized and analyzed based on reported quantitative and qualitative indicators related to recycling methods, material recovery rates, environmental impact, and system-level energy benefits. Results: A total of 23 studies were included. Significant progress has been made in hydrometallurgical and direct recycling processes, with recovery rates of critical metals (Li, Co, Ni) improving. Second-life battery applications also show promise for grid stabilization and renewable energy storage. Furthermore, recycled batteries show potential in stabilizing power grids through second-life applications in BESS. Conclusion: EV battery recycling is a vital strategy for addressing raw material scarcity, minimizing environmental harm, and supporting energy resilience. However, challenges persist in policy harmonization, technology scaling, and economic viability. Future progress will depend on integrated efforts across sectors and regions to build a circular battery economy. Full article

Na-layered Li-containing Mn-based cathodes (Na_xLi_yMn_1-yO₂, NLMOs) with additional Na⁺ storage ability resulting from the anionic redox reaction (ARR) hold great promise for sodium-ion batteries (NIBs). However, practical applications of NLMOs encounter challenges, such as migration of transition metal Mn, loss of lattice oxygen, and voltage decay during cycling. Here, we show that Cu plays an important role in enhancing the ARR via the reductive coupling mechanism (RCM). Results shows that a Cu²⁺/Fe³⁺ modified NLMO sample delivers a Na⁺ storage capacity as high as 174 mA h g⁻¹ at 0.2C, higher than that of a Zn²⁺/Fe³⁺ modified NLMO sample (130 mA h g⁻¹) and NLMO (154 mA h g⁻¹). Both in situ and ex situ characterization results indicate that the obvious improvement in the electrochemical performance of the Cu²⁺/Fe³⁺ modified NLMO is due to the additional overlaps between the Cu 3d and O 2p orbitals, which is beneficial for the RCM. As a result, the ARR is enhanced so as to increase the Na⁺ storage capacity. Full article

Polymer electrolytes (PEs) provide enhanced safety for high–energy–density lithium metal batteries (LMBs), yet their practical application is hampered by intrinsically low ionic conductivity and insufficient electrochemical stability, primarily stemming from suboptimal Li⁺ solvation environments and transport pathways coupled with slow polymer dynamics. Herein, we demonstrate a molecular design strategy to overcome these limitations by regulating the Li⁺ solvation structure through the synergistic interplay of conventional Lewis acid–base coordination and engineered hydrogen bond (H–bond) networks, achieved by incorporating specific H–bond donor functionalities (N,N′–methylenebis(acrylamide), MBA) into the polymer architecture. Computational modeling confirms that the introduced H–bonds effectively modulate the Li⁺ coordination environment, promote salt dissociation, and create favorable pathways for faster ion transport decoupled from polymer chain motion. Experimentally, the resultant polymer electrolyte (MFE, based on MBA) enables exceptionally stable Li metal cycling in symmetric cells (>4000 h at 0.1 mA cm⁻²), endows LFP|MFE|Li cells with long–term stability, achieving 81.0% capacity retention after 1400 cycles, and confers NCM622|MFE|Li cells with cycling endurance, maintaining 81.0% capacity retention after 800 cycles under a high voltage of 4.3 V at room temperature. This study underscores a potent molecular engineering strategy, leveraging synergistic hydrogen bonding and Lewis acid–base interactions to rationally tailor the Li⁺ solvation structure and unlock efficient ion transport in polymer electrolytes, paving a promising path towards high–performance solid–state lithium metal batteries. Full article

The increasing demand for lithium-ion batteries (LIBs) and their limited lifespan emphasize the urgent need for sustainable recycling strategies. This study investigates the application of tetrabutylphosphonium-based ionic liquids (ILs) as alternative leaching agents for recovering critical metals, Li(I), Co(II), Ni(II), and Mn(II), from spent NMC cathode materials. Initial screening experiments evaluated the leaching efficiencies of nine tetrabutylphosphonium-based ILs for Co(II), Ni(II), Mn(II), and Li(I), revealing distinct metal dissolution behaviors. Three ILs containing HSO₄⁻, EDTA²⁻, and DTPA³⁻ anions exhibited the highest leaching performance and were selected for further optimization. Key leaching parameters, including IL and acid concentrations, temperature, time, and solid-to-liquid ratio, were systematically adjusted, achieving leaching efficiencies exceeding 90%. Among the tested systems, [TBP][HSO₄] enabled near-complete metal dissolution (~100%) even at room temperature. Furthermore, an aqueous biphasic system (ABS) was investigated utilizing [TBP][HSO₄] in combination with ammonium sulfate, enabling the complete extraction of all metals into the salt-rich phase while leaving the IL phase metal-free and potentially suitable for reuse, indicating the feasibility of integrating leaching and extraction into a continuous, interconnected process. This approach represents a promising step forward in LIB recycling, highlighting the potential for sustainable and efficient integration of leaching and extraction within established hydrometallurgical frameworks. Full article

Gel electrolytes (GEs) play a pivotal role in the advancement of lithium metal batteries by offering high energy density and enhanced rate capability. Nevertheless, their real-world application is hampered by relatively low ionic conductivity and significant interfacial resistance at room temperatures. In this work, we developed a gel electrolyte membrane (GEM) by embedding Zeolitic Imidazolate Framework-8 (ZIF-8) metal–organic frameworks (MOFs) material into a poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) matrix through UV curing. The composite membrane, with 4 wt% ZIF-8, exhibited an ionic conductivity of 1.17 × 10⁻³ S/cm, an electrochemical stability window of 4.7 V, and a lithium-ion transference number of 0.7. The test results indicate that the electrochemical performance of LFP//GEM//Li battery has an initial specific capacity of 168 mAh g⁻¹ at 0.1 C rate. At 1 C, the discharge capacity was 88 mAh g⁻¹, and at 2 C, it was 68 mAh g⁻¹. Enhanced ionic transport, improved electrochemical stability, and optimized lithium-ion migration collectively contributed to superior rate performance and prolonged cycle life. This study offers novel insights and methodological advances for next-generation lithium metal batteries technologies. Full article

Li-rich Mn-based cathode materials are considered potential cathode materials for next-generation lithium-ion batteries due to their outstanding theoretical capacity and energy density. Nonetheless, challenges like oxygen loss, transition metal migration, and structural changes during cycling have limited their potential for commercialization. The work in this study employed a straightforward heat treatment to generate oxygen vacancies. This process led to the development of a spinel phase on the surface, which improved Li⁺ diffusion and boosted the electrochemical performance of Li-rich Mn-based oxides. The results demonstrate that the treated Li_1.2Mn_0.54Ni_0.13Co_0.13O₂ exhibits an initial specific capacity of 247 mAh·g⁻¹ at 0.2C, as well as a reversible capacity of 224 mAh·g⁻¹ after 100 cycles, with a capacity retention of 90.7%. The voltage decay is 1.221 mV per cycle under 1C long-term cycling conditions, indicating excellent cycling stability and minimal voltage drop. Therefore, this strategy of engineering through nanoscale oxygen vacancies provides a new idea for the development of high-stability layered oxide anodes and provides a reference for the development and application of new energy materials. Full article