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With the rapid increase of renewable energy in the electricity grids, the need for energy storage continues to grow. One of the technologies that are gaining interest for utility-scale energy storage is lithium-ion battery energy storage systems. However, their environmental impact is inevitably put into question against lead-acid battery storage systems. Therefore, this study aims to conduct a comparative life cycle assessment (LCA) to contrast the environmental impact of utilizing lithium-ion batteries and lead-acid batteries for stationary applications, specifically grid storage. The main tools in this study include Microsoft Excel for the life cycle inventory and OpenLCA for life cycle modelling and sensitivity analysis. In this research, a cradle-to-grave LCA for three lithium-ion battery chemistries (i.e. lithium iron phosphate, nickel cobalt manganese, and nickel cobalt aluminium) is conducted. The impact categories are aligned with the Environmental Footprint impact assessment methodology described by the European Commission. The standby grid operation scenario is considered for estimating the environmental impacts, where the batteries would deliver 4,800 kWh of electric energy throughout 20 years. Consequently, the functional unit will be in per kWh energy delivered. The lead-acid battery system has the following environmental impact values (in per kWh energy delivered): 2 kg CO2-eq. for climate change, 33 MJ for fossil resource use, 0.02 mol H+-eq. for acidification, 10-7 disease incidence for particulate emission, and 8x10-4 kg Sb-eq. for minerals resource use. Going back to the lithium-ion batteries systems, for the climate change and fossil resource use impact categories, the best performer is found to be the nickel cobalt aluminium (NCA) lithium-ion battery, with 46% and 45% less impact than lead-acid for the respective categories. On the other hand, the nickel manganese cobalt (NMC) was the best for the acidification and particulate emission impact categories with respective 65% and 51% better performance compared to lead-acid batteries. Finally, for the minerals and metals resource use category, the lithium iron phosphate battery (LFP) is estimated to be the best performer, which is 94% less than lead-acid. To conclude, the life cycle stage determined to have the largest contribution for most of the impact categories was the use stage, which then becomes the subject to a sensitivity analysis. The sensitivity analysis was done by varying the renewable contribution of the electricity grids in the use phase. Overall, the lithium-ion batteries systems have less environmental impact than lead-acid batteries systems, for the observed impact categories. The findings of this thesis can be used as a reference to decide whether to replace lead-acid batteries with lithium-ion batteries for grid energy storage from an environmental impact perspective. / Med den snabba ökningen av förnybar energi i elnäten, fortsätter behovet av energilagring att växa. En av de tekniker som växer intresse för energilagring på nyttan är litiumjon batteriets energilagringssystem. Emellertid, deras miljöpåverkan ifrågasätts oundvikligen mot blysyrabatteri lagringssystem. Därför syftar denna studie till att göra en komparativ livscykelanalys (LCA) för att komparera miljöpåverkan av att använda litiumjonbatterier och blybatterier för stationära applikationer, särskilt för nätlagring. I denna forskning genomfördes en vagga-till-grav-LCA (eller cradle-to-grave i engelska) för tre litiumjonbatterikemi (litium järn fosfat, nickel kobolt mangan, och nickel cobalt aluminium). Effektkategorier anpassades till miljökonsekvensbedömning metoden som beskrivs av Europeiska kommissionen. Det användningsfall scenariot för batterierna var standby läget, där batterierna leverera 4800 kWh elektrisk energi för 20 år. Följaktligen den funktionella unit är i ‘per kWh levererad energi’. Blysyrabatteriet hade följande ungefärliga miljöpåverkansvärden (i per kWh levererad energi): 2 kg CO2-eq. för climate change, 33 MJ för fossil resource use, 0.02 mol H+-eq. för acidification, 10-7 disease incidence för particulate emission, and 8x10-4 kg Sb-eq. för minerals resource use. Tillbaka till litiumjonbatterierna, för climate change och fossil resource use resursanvändnings kategorier, den bäst presterande var litiumjonbatteriet nickel kobolt aluminium (NCA). Det hade 46% och 45% mindre påverkan än blysyrabatteriet för respektive kategori. Å andra sidan, var nickel mangan kobolt (NMC) bäst för acidifcation och particulate emission kategorier. De är 65% och 51% bättre än blysyra för kategorierna. Slutligen, litium järn fosfat batteriet (LFP) är det bäst presterande för resource use of minerals and metals kategoriet, vilket det är 94% mindre än blysyra. Avslutningsvis, det livscykelstadier som var bestämt att ha det största bidraget för de flesta av påverkningskategorierna är användningsstadiet, som sedan blir föremål för en känslighetsanalys. I slutändan, litiumjonbatterierna ha mindre miljöpåverkan än blybatterier i detta projekt, för de observerade slagkategorierna. Resultaten av denna avhandling kan sedan användas som referens för att avgöra om bly-syrabatterier ska ersättas med litiumjonbatterier för energilagring ur ett miljöeffektperspektiv.

Transportsektorn är en av världens största producenter av växthusgas därav är dess avkarbonisering essentiell för att uppnå Parisavtalets mål för CO2-emissioner. Ett viktigt steg för att uppnå dessa mål utförs genom elektrifiering. Litium-jon-batterier (eng. litium-ion batteries, ’LIB’) har blivit väldigt populära energilagringssystem för batteridrivna elektriska fordon (eng. battery electric vehicles, ’BEV’) men tenderar att åldras, precis som alla andra batterier. Därav krävs forskning kring batteriföråldring på grund av nedbrytningsprocessernas inverkan på prissättningen, prestationerna och miljöpåverkan av BEV. Olika modeller används för att beskriva batteriernas åldrande. Datadrivna modeller som förutspår batteriers livstid ökar i popularitet vars noggrannhet och prestationer till stor del beror på indatats kvalitet. Formatet för tidsinhämtade data kräver enorma mängder lagringsutrymme, hög processkapacitet och längre processer; något ’reducerad’ eller ’aggregerad’ data delvis åtgärdar. Denna avhandling fokuserar på att utveckla en metodik för användning av dynamiska fordonsdata i ’aggregerad’ form. Tidsloggade data inhämtade från kallklimatstesting av Scanias BEV-prototyp användes varav interaktionseffekterna mellan diverse fordonsparametrar samt deras effekt på batteriåldring utifrån en batteriåldringsmodell analyserades. Olika tillvägagångssätt för strukturering av dynamiska fordonsdata i modellen undersöktes också. Tolv aggregeringsscenarion designades och testades. Dessutom valdes tre scenarion för uppskattningar och jämförelser av återstående användbar livslängd (eng. remaining-useful-life, ’RUL’) tillsammans med resultat från tidsinhämtade data. Slutligen drogs slutsatser om: parameterinteraktioner, struktur av dynamiska fordonsdata och RUL. Flera framtida utvecklingsområden har också föreslagits bland annat: tester av andra aggregeringstekniker, utöka modellen till tjänstefordon samt kategorisera användningsbeteenden av fordon för att förbättra RUL-uppskattningar. / The transport sector is one of the world’s largest greenhouse gas producing sector and it’s decarbonisation is imperative to achieve the CO2 emission targets set by the Paris Agreement. One important step towards achieving these targets is through electrification of the sector. Lithium-ion batteries (LIBs) have become very popular energy storage systems for battery electric vehicles (BEVs). However, LIBs like all other batteries, tend to age. Hence, the study of the battery ageing phenomena is very essential since the degradation in battery characteristics hugely determines the cost, performance and the environmental impact of BEVs. Different modelling approaches are used to represent battery ageing behaviour. Data-driven models for predicting the lifetime of batteries are becoming popular. However, the accuracy and performance of data-driven models largely depends upon the quality of data being used as the input. Time-sampled format of logging data results in huge data files requiring enormous amounts of storage space, high processing power requirements and longer processing times. Instead, using data in a ’reduced’ or ‘aggregated’ form can help in addressing these issues. This thesis work focuses on developing a methodology for using dynamic vehicle data in an ‘aggregated’ form. Time-sampled data from a Scania prototype BEV truck, recorded during cold climate test, was used. The interaction effects between various vehicle parameters and their effect on battery ageing in a battery ageing model were analyzed. Different approaches to structuring dynamic vehicle data for use in the model were also studied. Twelve aggregation scenarios were designed and tested. Furthermore, three scenarios were selected for making remaining-useful-life (RUL) estimations and compared alongside time-sampled data results. Finally, conclusions about parameter interactions, structuring of dynamic vehicle data and RUL estimations were drawn. Several next steps for future work have also been suggested such as testing other aggregation techniques, extending the model to vehicle fleets and categorizing vehicle usage behaviours to make better RUL estimations.

The Swedish Armed Forces are investigating high-risk applications where lithium-ion batteries (LIB) can replace traditional lead-acid batteries. Understanding the potential safety risks and evaluating a battery's instability is crucial for military applications. This report aimed to identify critical safety parameters (temperature, potential, and impedance) in commercial batteries with NMC and LFP electrode chemistries, and to investigate how surrounding cells are affected when a battery suffers from thermal runaway (TR) in a battery module developed by FOI. Accelerated rate calorimetry (ARC) experiments on NMC-based Samsung SDI INR21700-40T and INR21700-50E and LFP-based A123 Systems ANR26650m1-B batteries were conducted to identify critical onset conditions of TR. ARC experiments were conducted with continuous electrochemical impedance spectroscopy (EIS) measurements to correlate thermal behavior with electrochemical changes in the cell impedance and voltage. The NMC-based batteries showed a distinct endothermic reaction between 116 °C and 121 °C, an onset temperature of exothermic self-heating at around 120 °C, which progressed to an explosive decomposition at about 170 °C and resulted in an adiabatic temperature rise of 250 °C to 290 °C. A significant increase in the cell’s impedance at around 100 °C indicated that the current interrupt device (CID) was triggered due to gas formation and critical pressure build-up within the cell. The LFP-based battery demonstrated improved thermal stability during ARC measurements and did not suffer from TR when heated to 300 °C. Thermal runaway propagation experiments were conducted in a battery module developed by FOI. The identified onset temperatures and electrochemical markers were then used to evaluate the stability of the module cells. Cell temperature increases between 16 °C and 48 °C was observed in cells directly adjacent to the trigger cell. Cells further from the trigger cell experienced uniform temperature increases of between 8 °C and 30 °C. EIS measurements of the module cells revealed no significant changes in their impedance spectra. The insulating polymer wrap around each cell was found to be crucial in preventing TR propagation. TR propagated from cell-to-cell in the module when the insulating wraps were removed, and cells were in direct contact with the thermally conductive heat sink. / Försvarsmakten undersöker högriskapplikationer där litiumjonbatterier kan ersätta traditionella blysyrabatterier. Att förstå säkerhetsrisker och utvärdera ett batteris instabilitet är särskilt viktigt för militära tillämpningar. Denna rapport syftar till att identifiera kritiska säkerhetsparametrar (temperatur, spänning och impedans) för kommersiella batterier med NMC- och LFP-elektrodkemier samt undersöka hur omkringliggande celler påverkas när ett batteri termiskt rusar (TR) i en batterimodul utvecklad av FOI. ARC-experiment genomfördes på NMC-baserad Samsung SDI INR21700-40T och INR21700-50E och A123 Systems ANR26650m1-B batterier för att karakterisera förloppet av termisk rusning (TR). ARC-experiment utfördes med kontinuerliga elektrokemisk impedansspektroskopi (EIS) för att korrelera termiskt beteende med elektrokemiska förändringar i cellimpedansen och spänningen. Det NMC-baserade batterierna uppvisade en tydlig endotermisk reaktion mellan 116 °C och 121 °C, exotermiska reaktioner påbörjades vid 120 °C och ledde till explosiv termisk rusning vid cirka 170 °C, vilket gav upphov till en adiabatisk temperaturökning på 250 °C till 290 °C. En signifikant ökning av cellens impedans vid cirka 100 °C indikerade att den inre säkerhetsventilen utlöstes på grund av gasbildning och kritisk tryckuppbyggnad i cellen. Det LFP-baserade batteriet visade förbättrad termisk stabilitet under ARC-mätningar och drabbades inte av TR vid uppvärmning till 300 °C. Termiska rusningsförsök genomfördes på en batterimodul utvecklad av FOI. De identifierade starttemperaturerna och elektrokemiska markörerna användes för att utvärdera modulcellernas stabilitet. Celltemperaturökningar mellan 16 °C och 48 °C observerades i celler direkt intill triggcellen. Celler längre från triggcellen upplevde likformiga temperaturökningar mellan 8 °C och 30 °C. EIS-mätningar av modulcellerna avslöjade inga signifikanta förändringar i deras impedansspektra. Det isolerande polymeromslaget runt varje cell var avgörande för att förhindra propagering av termisk rusning i modulen. Termisk rusning propagerade från cell till cell i modulen när de isolerande omslagen togs bort och cellerna var i direkt kontakt med den värmeledande kylflänsen.

In the past decade, automobile manufacturers have gone through the initial adoption phase of electric mobility. The increasing momentum behind electric vehicles (EV) suggests that electrified storage systems will play an important role in electric mobility going forward. Lithium ion batteries have become one of the most common solutions for energy storage due to their light weight, high specific energy, low self-discharge rate, and non-memory effect. To fully benefit from a lithium-ion energy storage system and avoid its physical limitations, an accurate battery management system (BMS) is required. One of the key issues for successful BMS implementation is the battery model. A robust, accurate, and high fidelity battery model is required to mimic the battery dynamic behavior in a harsh environment. This dissertation introduces a robust and accurate model-based approach for lithium-ion battery management system. Many strategies for modeling the electrochemical processes in the battery have been proposed in the literature. The proposed models are often highly complex, requiring long computational time, large memory allocations, and real-time control. Thus, model-order reduction and minimization of the CPU run-time while maintaining the model accuracy are critical requirements for real-time implementation of lithium-ion electrochemical battery models. In this dissertation, different modeling techniques are developed. The proposed models reduce the model complexity while maintaining the accuracy. The thermal management of the lithium ion batteries is another important consideration for a successful BMS. Operating the battery pack outside the recommended operating conditions could result in unsafe operating conditions with undesirable consequences. In order to keep the battery within its safe operating range, the temperature of the cell core must be monitored and controlled. The dissertation implements a real-time electrochemical, thermal model for large prismatic cells used in electric vehicles' energy storage systems. The presented model accurately predicts the battery's core temperature and terminal voltage. / Thesis / Doctor of Philosophy (PhD)

The need for highly efficient energy storage devices has been steadily increasing due to growing energy demands. Research in electrochemical energy storage in the form of batteries has consequently become crucial. Currently, the most commercialized battery technology is the lithium ion battery (LIB). Concerns over the relatively limited global lithium supply, however, have led to the development of sodium ion batteries (SIBs). Solid-state nuclear magnetic resonance (ssNMR) spectroscopy is an ideal technique for analyzing battery materials as it can potentially distinguish between different ions within the material. The most typical cathode for commercial LIBs are the family of NMC layered oxides with the general form Li[NixMnyCo1-x-y]O2, which consist of Li layers between sheets of transition metals (TMs). The pj-MATPASS NMR technique, in conjunction with Monte Carlo simulations, was applied to investigate the ionic arrangement within TM layers of NMC622 (Li[Ni0.6Mn0.2Co0.2]O2), which revealed the presence of ion clustering in the pristine form of this material. This thesis also investigated the promising SIB cathode, Na3V2(PO4)2F3 (NVPF). NVPF has the capability to produce energy densities comparable to those of LIBs and is well understood from a structural standpoint, however ion dynamics within the material are still undetermined. A series of materials have, therefore, been synthesized with the general form, Na3V2-xGax(PO4)2F3 (where x = 0, 1, and 2), where diamagnetic Ga3+ was introduced into the structure to enable the establishment of a structural correlation with observed Na-ion dynamics. It, therefore, became possible to explore ionic site exchange using 23Na ssNMR. Density functional theory (DFT) calculations have also been performed alongside ssNMR to confirm chemical shift assignments and provide structural insight. Additionally, electron paramagnetic resonance (EPR) spectroscopy was also used to investigate the paramagnetic nature of NVPF and its variants. Insights into the ionic arrangement and very fast Na-ion dynamics within these materials were revealed. / Thesis / Master of Science (MSc) / The need for highly efficient energy storage devices, especially in the form of batteries, has been steadily increasing due to growing energy demands. Presently, the most commercialized types of batteries are lithium ion batteries (LIBs). Concerns over the relatively limited global lithium supply, however, have led to the development of sodium ion battery (SIB) alternatives. Various solid-state nuclear magnetic resonance (ssNMR) techniques have been employed in this thesis to investigate both LIB and SIB cathode materials. The LIB cathode Li[Ni0.6Mn0.2Co0.2]O2 was examined with a combination of ssNMR and Monte Carlo simulations, and it was found that ion clustering occurs in the pristine form of these materials. The promising family of SIB cathodes, Na3V2-xGax(PO4)2F3, was studied by a combination of ssNMR, ab initio calculations, and EPR, which allowed for a correlation to be established between the crystal structure and the fast ion dynamics within these materials.

Litiumjonbatterier (LIB) är viktiga komponenter i dagens teknologi och används för att driva en mängd olika elektroniska system, allt från datorer och mobiltelefoner till bilar och flygplan. Eftersom efterfrågan på effektiv energilagring fortsätter att växa finns ett fortsatt behov för forskning och utveckling inom området. Denna rapport undersöker hårt kol, ett lovande material för anoder i litiumjonbatterier och andra alkali-jon batterier. I likhet med grafit är hårt kol ett kolbaserat material som inte är en väldefinierad allotropp utan en komplex blandning med avseende på både hybridiseringstillstånd och långdistansordning.  Därför är den mycket dåligt definierat. Ändå är hårt kol ett önskvärt material eftersom det kan produceras från förnybara resurser samt på grund av dess kompatibilitet med natrium, vilket möjliggör natriumjonbatterier. I den här studien har elektroder av hårt kol syntetiserats och litierats i olika grader och sedan studerats med 7Li NMR-spektroskopi där både spektra och longitudinella relaxationshastigheter mättes. Vid lägre litieringsnivåer observerades tydliga smala 7Li toppar inom intervallet 4-16 ppm, vilket indikerar förekomsten av joniskt litium. Vid högre litieringsnivåer framträdde en bred topp vid 61 ppm. Utseendet av denna topp, tillsammans med en hög Knight-skift, indikerar närvaron av kvasi-metalliskt litium. Det är värt att notera att detta kvasi-metalliska litium finns i de oordnade och porösa områdena hos hård kol. 7Li longitudinella relaxationshastigheter, som rapporterar om jonisk dynamik, registrerades vid olika temperaturer och från det observerade temperaturberoendet beräknades den genomsnittliga aktiveringsenergin för de involverade joniska rörelserna. Intressant nog visade sig denna aktiveringsenergi vara lägre jämfört med den i PAN-baserade kolfibrer och grafit, som båda uppvisar en högre grad av ordning. Denna observation tyder på ett samband mellan lokal oordning och snabbare jondynamik. / Lithium-ion batteries (LIB) are vital components of modern technology, powering a wide range of devices from computers and cell phones to cars and aeroplanes. As the demand for efficient energy storage continues to grow, research and development in the field of lithium-ion batteries remain active. This report focuses on the investigation of hard carbon, a promising anode material for lithium-ion batteries and other alkali-ion batteries. Akin to graphite, hard carbon is a carbon-based material that is not a well-defined allotrope but a complex mixture with regard to both hybridization state and long-range order. Hence it is very poorly defined. Yet, hard carbon is a desirable material as it can be produced from renewable resources and because of its compatibility with sodium, allowing for sodium-ion batteries. In this study, hard carbon electrodes were synthesised and lithiated to various degrees and then studied with 7Li NMR spectroscopy where both spectra and longitudinal relaxation rates were measured.   At lower lithiation levels, distinct narrow 7Li peaks were observed within the 4-16 ppm range, indicating the presence of ionic lithium. At higher lithiation levels a broad peak at 61 ppm emerged. The appearance of this peak, along with a high Knight shift, signifies the presence of quasi-metallic lithium, presumably in the more disordered and more porous regions of hard carbon. The 7Li longitudinal relaxation rates, reporting on ionic dynamics, were recorded at different temperature and from the observed temperature dependence the average activation energy for the involved ionic motions was calculated. Interestingly, this activation energy was found to be lower compared to that for PAN-based carbon fibres and graphite, both of which exhibit a higher degree of order. This observation suggests a correlation between local disorder and faster ion dynamics.

Die experimentellen Daten können bei Dr. Sebastian Risse, Helmholtz-Zentrum Berlin, eingesehen werden. / Silizium-Elektroden werden aufgrund ihrer um eine Gröÿenordnung höheren Kapazität als mögliches Elektrodenmaterial in Lithium-Ionen-Batterien betrachtet. Diese Kapazität geht jedoch mit einer Volumenausdehnung von bis zu 310 % einher. Dies begünstigt einen schnellen Kapazitätsabfall und ein kontinuierliches Wachstum der SEI-Schicht. Ziel dieser Arbeit ist es daher, die Morphologie-Änderung der Siliziumelektrode während des Lithiierungs-Prozesses besser zu verstehen unter Nutzung von operando-Methoden Im ersten Teil wurde Neutronenreflektometrie (NR) genutzt, um die Morphologie-Änderung auf der Nanometerskala einer Siliziumelektrode zu untersuchen. Das Wachsen/Schrumpfen der lithiierten Zone im Silizium wurde beobachtet. Auf der Oberfläche der Elektrode wächst im delithiierten Zustand eine Grenzschicht, welche die Lithiierung verhindert. Nachdem diese Schicht aufgelöst ist, kann Lithium eingelagert werden. Im zweiten Teil wurde operando Röntgen- Phasenkontrast-Radiographie genutzt. Ein rechteckiges Riss-Gitter wurde dabei im delithiierten Zustand beobachtet, welches sich während der Lithiierung schließt. Dieses Gitter ist entlang der Kristallachsen des Siliziums orientiert. Im nächsten Zyklus entsteht das Gitter am selben Ort wieder, und breitet sich mit steigender Zyklenzahl über die Elektrode aus. Im dritten Teil wurde der Einfluss einer künstlichen Grenzschicht auf die Lithiierung untersucht. Erneut wurde NR genutzt. Die künstliche Schicht verringert das Wachstum der SEI-Schicht, unterdrückt es jedoch nicht komplett. Nach 2 Zyklen ist die Grenzschicht degradiert, und Seitenreaktionen können beobachtet werden. / Silicon electrodes receive great interest as potential electrode material in lithium-based batteries due to their one order of magnitude higher capacity. This is accompanied by a volume expansion of up to 310 %, leading to an accelerated capacity loss of the electrodes. The volume expansion creates mechanical stress, leading to fracturization of the electrode and the continuous growth of the solid-electrolyte-interphase (SEI) layer under the consumption of active material. The aim of this thesis is to investigate the morphological changes of silicon electrodes during lithiation/ delithiation. Especially operando-techniques are well-suited to investigate these morphological changes since they allow us to precisely link structural data and the electrochemical state. The first project uses operando neutron reflectometry (NR) and in-situ electrochemical impedance spectroscopy (EIS) to analyze the morphology change of the silicon surface on the nanometer-scale. The growth and shrinkage of the lithiated layers within the electrode as well as the lithium concentration was determined with this method. An SEI-layer forms on top of the silicon electrode in the delithiated state, which hinders the lithium uptake in the initial part of the subsequent lithiation. The second project analyzes the morphology-change of the electrode on the µm-scale. Here the fracturization of the silicon electrode is investigated by operando X-ray phase-contrast radiography. A rectangular fracturization pattern was observed during the second half of the delithiation, which vanished again during the lithiation. The third project investigates the influence of an artificial coating layer on the lithiation process. Again operando NR was chosen as analysis tool. The artificial coating decreased the formation of the SEI-layer within the first cycles, but did not suppress it completely. However, this layer degraded already in an early stage of cycling, resulting in the occurrence of side reactions afterward.

<p dir="ltr">Direct recycling of cathode materials from spent Li-ion batteries (LIBs) or electrode scraps necessitates efficiently recovering valuable active materials from the aluminum foil. The variability in electrode types and recovery processes across previous studies complicates the comparative assessment of the recovery performance of green solvents. Furthermore, constant requirements of high temperature during recovery and impurities retained on the active material surface inhibit the progress to full-scale commercialization. In this study, we evaluated the performance of three green solvents—triethyl phosphate (TEP), dihydrolevoglucosenone (Cyrene), and propylene carbonate (PC)—in recovering valuable active materials from industrial-grade cathode scraps. Using ultrasonication, we developed a standardized, energy-efficient recovery process that eliminated the need for conventional stirring and achieved complete cathode delamination from the aluminum foil. Additionally, solvent washing was implemented on recovered active materials for impurity removal to achieve competitive electrochemical performance. Furthermore, we successfully recovered the used green solvents after the process, ensuring their reuse and supporting a circular economy. The recovered materials retained their original morphology, chemical composition, and crystalline structure; however, the presence of surface impurities varied significantly depending on the choice of green solvent. These impurities considerably impacted the electrochemical performance of the recovered materials. TEP and PC yielded high-purity active materials and aluminum foils suitable for reuse or direct recycling, while Cyrene resulted in substantial residues of PVDF/solvent, requiring washing with stronger solutions such as reagent alcohol. Additionally, the recyclability of these green solvents was influenced by their solubility power for PVDF. This study provides valuable insights into the green solvent-based recycling process and the importance of post-recovery washing steps laying the groundwork for future sustainable practices in LIB recycling.</p>