Battery technologies are essential for achieving net-zero carbon dioxide emissions, but their large-scale production and recycling cause notable environmental burdens. Life cycle assessment (LCA) is therefore crucial for evaluating the environmental performance of battery technologies. While conventional LCAs mainly address mature systems, emerging battery technologies are often assessed at laboratory scale and thus require methodological upscaling to estimate industrial scale impacts. Our structured literature search identifies 28 peerreviewed studies published between 2014 and 2025. Since electrode materials are typically developed and optimized at laboratory scale, environmental assessments must address both process scaling and transfer to commercially relevant cell formats, including prismatic, pouch, and cylindrical cells. Product scaling can be supported by battery-specific tools such as BatPaC and CellEst 3.0, which enable representative bills of materials. Across the reviewed studies, five main approaches were identified for scaling material and energy flows from laboratory to industrial production. Battery cell manufacturing can also be upscaled using literature-based inventories or dedicated battery modeling tools. However, uncertainty remains insufficiently addressed, and process-related scaling parameters are rarely considered. Overall, the review underscores the need to integrate sustainability assessment and industrial scaling perspectives at early stages of battery development to support targeted improvements while implementation remains feasible.
Commercial off-the-shelf (COTS) Li ion cells offer an attractive and rechargeable power source for spacecraft applications. However, since these cells are typically designed for charging above 0°C, challenging sub-zero temperatures could inflict irreversible degradation and safety hazards during in-flight operation. To address these challenges, this work explores strategies affecting their low-temperature performance. Specifically, we investigate the Li plating behavior of the COTS LG Chem 18650 HG2 cell during galvanostatic cycling at −20°C and its dependence on prior high-temperature preconditioning protocols, involving either two-week galvanostatic cycling or storage at 30°C, as well as a reference case without preconditioning, i.e., direct cycling at −20°C. Experimental cycling tests reveal distinct differences in Li metal deposition between cells subjected to these conditions. To identify the origin of these discrepancies, we combine computed tomography of the electrode microstructure with three-dimensional, spatially resolved cell modeling and analyze the simulation results.
We derive a recursive transmission line model (TLM) for the cathode catalyst layer impedance in a working PEM fuel cell. The TLM results from the approximate solution of the macro-homogeneous model equations for impedance of the CCL with fast oxygen transport and a finite proton transport rate. The classic de Levie TLM requires two orders of magnitude more "stairs" to achieve the same impedance accuracy as the recursive TLM. The recursive TLM is suitable for any mixed-conducting electrode with high conductivity of one type of charged species and fast transport of feed molecules.
The rapid global expansion of lithium-ion battery manufacturing requires systematic methods to compare and evaluate established and innovative production technologies. This paper develops a multi-criteria decision analysis approach to assess process equipment along four dimensions: cost, throughput, quality and sustainability. Ten criteria are defined, derived from a literature review. Building on these criteria, PROMETHEE II is selected as a suitable multi-criteria decision analysis method and adapted to the battery manufacturing context. The adaptations include exclusion criteria for minimum performance requirements, modelling of parameter uncertainty via Monte Carlo simulation, tailored preference functions for different criteria, and a user-specific weighting scheme reflecting different stakeholder priorities. The evaluation method is illustrated in a case study comparing knife and laser slitting of electrodes. The case study shows that advantages, such as improved quality, must always be weighed against disadvantages, such as higher investment costs. A tipping-point analysis demonstrates how the method can translate abstract trade-offs into concrete technological or economic targets, e.g., required cost reductions. The proposed approach provides a transparent, flexible decision-support framework for selecting production technologies and for guiding R&D and investment priorities in battery cell manufacturing.
Electrochemical energy storage has become a cornerstone of modern technology, highlighting the need for precise tools to monitor and evaluate cell states in order to design batteries that combine safety with high performance. In lithium-ion batteries (LIBs), reference electrodes (REs) serve as diagnostic probes that enable the measurement of key electrochemical parameters during operation. They make it possible to monitor potential variations of each cell component over cycling and to study the electrode-specific reaction mechanisms that govern battery performance. Despite their value, developing a RE that remains stable, reversible, and minimally polarizable over extended operation continues to be a major challenge for both research and industrial use. This review summarizes the main considerations in RE design, ranging from material composition and structural configuration to activation procedures, and discusses their respective strengths, drawbacks, and prospects for future development in lithium-ion battery systems.
A two-step approach has been developed to enable the recovery of electrolyte from lithium ion battery (LIB) recycling material (black mass), providing a suitable route for extracting and separating electrolyte components. In the first step, the electrolyte is extracted from black mass using supercritical carbon dioxide (ScCO2) in combination with sustainable modifiers such as methanol (MeOH) and isopropanol (IPA). In a second step a supercritical fluid chromatography (SFC) method enables the separation of the electrolyte compounds in five fractions. The electrolyte fractions demonstrate high purity, ensuring their reuse as LIB electrolyte. While IPA exhibits weak solvating capabilities when used as modifier for the ScCO2 extraction of the conducting salt anion PF6-, it was shown that MeOH leads to a high extraction. Total extraction rates of 5.83 wt% and 4.68 wt% of extracted electrolyte compounds could be achieved, respectively corresponding to an extraction yield of 62 to 81% for the main compounds, ethylene carbonate and hexafluorophosphate. The developed SFC method for the separation of the extracted electrolyte compounds yields in total five fractions, the first consists of linear carbonates, the second consists of the bicarbonate aging products, followed by separately eluting ethylene carbonate, water and PF6- .
As polymer electrolyte fuel cells (PEFCs) become more widespread, there is growing demand to reduce the environmental impact of their production and to comply with regulations covering perfluoroalkyl and polyfluoroalkyl substances (PFAS). In particular, the conventional polytetrafluoroethylene (PTFE)-based slurry process used to form the microporous layer (MPL) of the gas diffusion layer (GDL) requires high-temperature heat treatment and decomposition of surfactants, leading to significant energy consumption and a high environmental burden. In this study, a dry coating process was applied to the fabrication of GDLs using thermosetting melamine resin as a fluorine-free binder to develop a PFAS-free energy-efficient MPL. By combining hydrophilic carbon black with melamine resin and optimizing the heat treatment conditions, curing was achieved at a lower temperature (approximately 250 degrees C) than that of conventional PTFE-based MPLs, while significantly improving peel strength. Single cells were fabricated with the developed MPL applied to the anode, and their performance was evaluated. The results demonstrated performance equivalent to or higher than that of PTFE-based MPLs, confirming the practicality of this approach. This process provides a practical pathway toward high-performance, PFAS-free PEFC components with reduced environmental impact.
Dimethyl-sulfoxide (DMSO) is emerging as an alternative solvent for cathode slurry production, offering lower toxicity compared to commonly used reagents like N-methyl-2-pyrrolidone (NMP). In battery recycling operations, thermal pretreatment is often required for efficient removal of polyvinylidene fluoride (PVDF) binder, which facilitates downstream processes such as flotation and mineral acid leaching. DMSO leaching of black mass offers a solvent-based approach to reverse the slurry production process by dissolving and removing the binder of the battery cathode (PVDF), instead of applying temperature intensive process. This method has the potential to simplify subsequent recycling steps, such as flotation, by eliminating the need for thermal treatments. This study demonstrates the effectiveness of DMSO as a non-thermal-pretreatment for NMC black mass by selectively dissolving PVDF binder and electrolyte residues without additionally impacting the transition metal content. DMSO leaching at a solid-to-liquid ratio of 100 g/L, 80 degrees C, and 30 min achieved 89.46% F- removal, within the investigated ranges of 40-80 degrees C and 30-120 min. Subsequent water leaching of soluble fluorine species increased the accumulated removal to a maximum of 95.27 %. The process enables efficient fluorine removal from end-oflife black mass, avoids toxic off-gas emissions, and supports a circular flowsheet through solvent and binder recovery.
Scalable and sustainable lithium-ion battery recycling routes could be crucial for the future economic and ecological landscape of Europe. Although graphite is a critical raw material for the EU, the recycling of graphite from spent cells is currently limited to a small scale and is less developed than the recovery of cathode elements. In this study, we present a process for regenerating anode active material from spent lithium-ion cells with electrochemical performance comparable to that of commercial battery-grade graphite. The study is based on a direct recycling concept that employs green solvents and thermal treatment. The focus is on the direct impact of the applied temperature on the quality of the recycled graphite. The temperature range used for thermal treatment affects the physical and chemical properties of the particles, primarily impacting the surface functionalities, which are crucial for electrochemical performance. We demonstrate the electrochemical performance of regenerated graphite active materials by validating the short closed loop from spent cells to new anodes with high-performance.
The instability of the Solid Electrolyte Interphase (SEI) in carbonate-based electrolytes hinders the development of high-energy-density sodium batteries. This study elucidates the stabilization mechanism provided by a C65-coated aluminum electrode, representing the nucleation host in an anode-less sodium battery architecture, within a half-cell configuration against a sodium-metal counter electrode, using a carbonate-based electrolyte (1 M NaPF6 in EC:DMC with 5% FEC). We demonstrate that the high-surface-area C65-coating homogenizes the local current density, thereby facilitating the selective reduction of FEC prior to bulk solvent decomposition, fostering the formation of a flexible, NaF-rich SEI. Conversely, the high local current density on the bare aluminum electrode drives nonselective electrolyte decomposition, resulting in a brittle, inorganic-rich SEI and severe accumulation of “dead sodium”. Consequently, the C65-coated electrode enhances the average Coulombic Efficiency to 85%, representing a significant relative improvement over the bare substrate. Furthermore, X-ray photoelectron spectroscopy reveals that the SEI composition on the bare aluminum eventually evolves to resemble the stable SEI composition on the coated electrode, yet electrochemical performance remains inferior. This underscores the long-term impact of the early-stage SEI composition on cell cyclability.
Thermal runaway (TR) and its propagation (TRP) pose critical risks in the application of large-format lithium-ion batteries in heavy-duty electric vehicles. In this work, we apply a computational approach using a lumped heat release model. This model is calibrated with experimental data from accelerating rate calorimetry (ARC) and TRP tests to investigate battery aging effects on TR and TRP. It is seen that the simulations can effectively reproduce key experimental observations, such as TR onset temperature, maximum temperature, and TRP time. Furthermore, the influence of battery aging on TR behavior is investigated, specifically solid–electrolyte interphase (SEI) growth and electrolyte degradation. The findings reveal that aging significantly accelerates TR onset while lowering the heat release of batteries. The interplay between accelerated SEI layer growth and electrolyte degradation significantly influences TRP dynamics. Compared to new batteries, the total TRP time initially decreases during early aging, reaching 78% of the original TRP time at around 80% state of health (SOH). During late aging, TRP time slightly increases to 85% of the original time at 50% SOH. This computational approach provides crucial insights into the dynamic safety of aged batteries with regard to different combinations of electrolyte degradation and SEI thickness growth rate.
Sustainable recycling of lithium iron phosphate (LFP) cathodes is essential to process battery waste, thus reducing resource depletion and lowering the carbon footprint of battery production. This study introduces a contactless delamination process using high-frequency induction heating to partially decompose the water-based carboxymethyl cellulose and styrene-butadiene rubber binders in LFP electrode production scrap within a temperature range that avoids damage to the LFP. Eddy currents induced in the aluminum current collector enable localized heating at the LFP composite-foil interface, allowing clean separation without toxic solvents or high-temperature furnaces. Variation of the process parameters showed that moderate heating (similar to 240 degrees C) weakens binder adhesion effectively while preserving the integrity of the LFP. Electrodes were fabricated from the recovered LFP composite and evaluated in lithium metal half cells. The best-performing recovered sample (240 degrees C with added conductive carbon) achieved similar to 96 % of the discharge capacity of a recovered sample delaminated without the inductive heat treatment. These results confirm that inductive delamination, with careful temperature control, enables the recovery of high-quality LFP composite suitable for reuse. This method avoids the use of hazardous chemicals and is compatible with roll-to-roll processing, offering a scalable and environmentally-friendly route for direct cathode recycling.
A novel recycling route for spent lithium-ion batteries has been investigated. The end goal is to produce cathode active material (CAM) precursor directly from the recycled solution. The process begins with an oxalic acid leaching (0.6 M H2C2O4, 60 degrees C, 120 min, and S/L = 50 g/L), where Li is selectively recovered (along with Al) which reduces downstream contamination and enhances overall material efficiency. The resulting residue, a mixture of (Co,Ni,Mn)C2O4 & sdot; 2H2O, graphite, and Cu, is then leached with sulfuric acid to dissolve the metals and separate them from the graphite. This second leaching operation is investigated, and the optimum parameters are demonstrated (2 M H2SO4, 65 degrees C, 120 min, S/L = 20 g/L), yielding more than 95 % recovery of Ni, Co, and Mn and about 70 % of Cu. Lower acidity or S/L leads to the reprecipitation of a Ni oxalate phase. Solvent extraction is selected for Cu removal at a limit of 5 ppm; a 30 % v/v Acorga M5640 in ESCAID is applied for 30 min at 25 degrees C, with theta = 4 and 4 stages. The resulting recycled solution, containing Co, Ni, and Mn, and free from Al, Li, and Cu, represents a promising feedstock for producing NMC 111 (LiNi0.33Mn0.33Co0.33O2).
At present, industrial-scale recycling of lithium-ion batteries typically involves rather energy-intensive processes and toxic solvents to recover, in particular, the metallic elements from the positive electrode active material. These recovered metals subsequently serve as precursors for the synthesis of new electrode materials. One approach to reduce the energy and cost needed is the direct recycling of the electrode active materials. Herein, two recovery methods, namely thermal and solvent-based recovery, are investigated for single-crystalline Ni-rich LiNi1-x-yMnxCoyO2 (NMC) high-energy cathodes. The NMC obtained via the thermal recovery method exhibits poor performance due to the generation of HF and the degradation of the material. In contrast, the NMC obtained via the solvent-based method, utilizing dimethyl sulfoxide as a non-toxic solvent, demonstrates superior performance, with a reduction in capacity of only 1.5 % compared to pristine NMC. This comparative analysis highlights the critical role of the separation procedure and, particularly, the detrimental effect of any remaining fluorinated binder.
The rapid growth of Li-ion Batteries (LIBs), especially in the automotive sector, raises urgent concerns regarding End-of-Life (EoL) management and the secure supply of Critical Raw Materials (CRMs), including lithium, cobalt, and nickel. To mitigate risks of resource scarcity and environmental impact, sustainable collection and recycling practices are essential to support the transition toward a circular economy, enabling the recovery of both metallic and non-metallic components. A zero-waste approach to LIB recycling is therefore emerging as a key priority. Industrial innovation and academic research are deeply interconnected in this field. Industry depends on scientific discoveries to scale up efficient recycling technologies, while academia is driven by challenges arising from industrial practice and regulatory demands. This reciprocal relationship accelerates the development of advanced recycling strategies capable of addressing technical and economic barriers. This review provides an overview of LIB recycling in Europe, focusing on the evolving legislative framework designed to regulate the proper management of spent batteries and promote the recovery of CRMs. Current industrial practices are discussed with particular attention to their limitations, alongside emerging academic solutions that could redefine the efficiency, sustainability, and economic viability of LIB recycling.
Experiments reveal that the electrodes of a commercial NFM || hard carbon sodium-ion battery undergo excessive sodiation and desodiation at low charge and discharge rates. These effects are observed during cycling, despite operating strictly within the manufacturer’s recommended voltage limits of 1.5V to 4.1V. The resulting increase in charge capacity originates from an additional phase transition in the cathode active material, which manifests itself electrochemically as a voltage plateau that delays reaching the cut-off voltage during charging. The occurrence of the phase transition at high cell voltages is verified by operando X-ray diffraction measurements. During the subsequent discharge, the reverse transition takes place. Unusual deep discharge is enabled by the combination of low overpotentials and the characteristic potential profile of the cell. These phenomena are reproducibly observed across multiple test sequences. To separate the effects of the individual electrodes on this full cell behavior, harvested electrodes from a commercial cell are assembled into an experimental three-electrode setup and analyzed by differential voltage analysis. Since the high-voltage phase transition is reported to involve irreversible processes, adapting characterization and cycling protocols (especially voltage limits) may improve long-term performance and facilitate future analyses.
Developing efficient and low-Pt electrocatalysts is critical for the commercialization of direct ethanol fuel cells (DEFC). Herein, a novel bimetallic iron-nickel metal-organic framework, MIL-88B(Fe2/Ni)-NH2 ((Fe2/Ni)MOF), was synthesized using 2-aminoterephthalic acid as a linking ligand. Different loadings of reduced graphene oxide (rGO, 1-8wt%) were incorporated via solvothermal synthesis to enhance structural stability and conductivity, forming 1-8wt% rGO-(Fe2/Ni)MOF composites. These hybrids serve as supports for Pt catalysts, producing Pt/ [1-8wt% rGO-(Fe2/Ni)MOF] electrocatalysts. The synthesized materials were characterized using FT-IR, XRD, SEM, TEM, EDS mapping, XPS, cyclic voltammetry, chronoamperometry, electrochemical impedance spectroscopy, and direct ethanol fuel cell performance testing. Among the prepared catalysts, Pt/[5 wt% rGO-(Fe2/Ni) MOF] exhibited the highest electrocatalytic activity toward ethanol oxidation, achieving a current density of 50.37 mA cm-2 at 0.86 V. In DEFC testing at 60 degrees C with 3M ethanol, this catalyst delivered a power density three times higher than the Pt/CC as control catalyst, with an open-circuit voltage of 0.54 V compared to 0.35 V for Pt/ CC. These results demonstrate that the designed rGO-MOF hybrid is an efficient and durable Pt support, offering significant potential for DEFC applications and sustainable energy conversion.
Recycling of graphite from Li-batteries has attracted increased interest due to the substantial increase in global demand. In this work, leach residues of different battery recycling solutions were characterized as one potential secondary source for graphite. Sulfuric acid, hydrochloric acid, nitric acid, phosphoric acid, and sodium hydroxide were studied (2 M and 4 M concentrations, T = 60 degrees C, S/L = 100g/L, t = 3 h, V = 500 mL) to evaluate their impact on graphite purity and characteristics. Battery waste was industrial lithium nickel manganese cobalt oxide-rich (NMC) black mass. It was found that leaching with 4 M HCl achieved the highest removal of battery metals and resulted in the highest graphite purity (54 wt%) in the residue. Phosphoric acid was shown to cause in-situ precipitation of small MnPO4 & sdot;H2O and FePO4 particles, whereas coarser Mn-rich particles precipitated during sulfuric acid leaching. All the studied lixiviants were found to maintain the structure of graphite as there was no significant increase in the defects or changes to the degree of graphitization. These results demonstrate that a typical hydrometallurgical leaching process alone is insufficient for graphite purification but requires additional purification and processing steps to valorize graphite.
Protic ionic liquids (PILs) are an interesting class of electrolyte for energy storage devices thanks to their unique properties, which stem from their protonated cations. In this study, we investigate the use of PIL-based electrolyte in dual-ion batteries (DIBs) containing graphite as both positive and negative electrode. Specifically, we considered a mixture of 1-butylpyrrolidinium bis(trifluoromethanesulfonyl)imide (PYRH4TFSI) and lithium bis (trifluoromethanesulfonyl)imide (LiTFSI). Initially, insertion of TFSI- into graphite was investigated, which showed that PIL-based electrolyte allows highly reversible intercalation/de-intercalation processes. Furthermore, kinetics of interfacial charge transfer were analyzed. In the second part of the study, a dual-ion battery containing PIL-based electrolyte was tested. The proof-of-concept graphite-based DIB utilizing this electrolyte delivered a capacity of 54 mAh g(-1) at 25 degrees C while operating in a wide potential window (similar to 5.2 V). The results of these studies demonstrate, for the first time, that the use of PIL-based electrolyte in DIB is possible.
