Pub Date : 2025-12-01DOI: 10.1016/j.powera.2025.100194
Sandesh Darlami Magar , Christof Neumann , Nicolas Demarthe , Andrey Turchanin , Andrea Balducci
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 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 °C while operating in a wide potential window ( 5.2 V). The results of these studies demonstrate, for the first time, that the use of PIL-based electrolyte in DIB is possible.
质子离子液体（PILs）由于其独特的特性而成为一类有趣的储能电解质，这源于它们的质子化阳离子。在这项研究中，我们研究了基于pil的电解质在双离子电池（DIBs）中使用石墨作为正极和负极。具体来说，我们考虑了1-丁基吡咯烷二（三氟甲烷磺酰基）亚胺（PYRH4TFSI）和二（三氟甲烷磺酰基）亚胺锂（LiTFSI）的混合物。最初，研究了TFSI−插入石墨，结果表明，基于pil的电解质允许高度可逆的插入/脱插入过程。进一步分析了界面电荷转移动力学。在研究的第二部分，测试了一种含有pil基电解质的双离子电池。利用这种电解质的概念验证石墨基DIB在25°C下提供54 mAh g−1的容量，同时在宽电位窗口（~ 5.2 V）下工作。这些研究的结果首次表明，在DIB中使用基于pil的电解质是可能的。
{"title":"Protic ionic liquids as electrolytes for high voltage dual ion batteries","authors":"Sandesh Darlami Magar , Christof Neumann , Nicolas Demarthe , Andrey Turchanin , Andrea Balducci","doi":"10.1016/j.powera.2025.100194","DOIUrl":"10.1016/j.powera.2025.100194","url":null,"abstract":"<div><div>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 (PYR<sub>H4</sub>TFSI) and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI). Initially, insertion of <span><math><mrow><msup><mtext>TFSI</mtext><mo>−</mo></msup></mrow></math></span> 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<sup>−1</sup> at 25 °C while operating in a wide potential window (<span><math><mrow><mo>∼</mo></mrow></math></span> 5.2 V). The results of these studies demonstrate, for the first time, that the use of PIL-based electrolyte in DIB is possible.</div></div>","PeriodicalId":34318,"journal":{"name":"Journal of Power Sources Advances","volume":"36 ","pages":"Article 100194"},"PeriodicalIF":4.6,"publicationDate":"2025-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145690946","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The rapid expansion of electromobility and renewable energy storage has increased lithium-ion battery production, emphasizing the need for efficient end-of-life management and critical material recovery. Mechanical pretreatment of spent batteries yields a black mass containing valuable oxides and metallic impurities, primarily Al, Cu, and Fe. This study investigated the impact of Al3+, Cu2+ and Fe2+ impurities on the carbonate coprecipitation synthesis of LiNi0.8Mn0.1Co0.1O2 (NMC811) precursors to simplify cathode resynthesis from acid leachate. Electrochemical testing showed improved performance for NMC811 materials doped with 1–3 at% Al3+, 2 at% Fe2+, or co-doped with Al–Fe at total concentrations of 2–4 at%, compared to undoped NMC811. Rietveld refinement of XRD patterns revealed reduced Li+/Ni2+ cation mixing in these same concentrations, confirming structural stabilization. In contrast, Cu2+ doping beyond 1 at%, whether alone or in combination, did not yield additional benefits and instead led to increased disorder. These findings suggest that leachates containing up to these impurity levels could be used directly in resynthesis without further purification, as the resulting NMC811 retained equal or improved performance. This supports a more sustainable and resource-efficient recycling process by reducing water, reagent, and energy consumption.
{"title":"Black mass impurities effect on re-synthesized NMC811 by carbonate coprecipitation","authors":"Valérie Charbonneau , François Larouche , Kamyab Amouzegar , Ashok Vijh , Gervais Soucy , Jocelyn Veilleux","doi":"10.1016/j.powera.2025.100193","DOIUrl":"10.1016/j.powera.2025.100193","url":null,"abstract":"<div><div>The rapid expansion of electromobility and renewable energy storage has increased lithium-ion battery production, emphasizing the need for efficient end-of-life management and critical material recovery. Mechanical pretreatment of spent batteries yields a black mass containing valuable oxides and metallic impurities, primarily Al, Cu, and Fe. This study investigated the impact of Al<sup>3+</sup>, Cu<sup>2+</sup> and Fe<sup>2+</sup> impurities on the carbonate coprecipitation synthesis of LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> (NMC811) precursors to simplify cathode resynthesis from acid leachate. Electrochemical testing showed improved performance for NMC811 materials doped with 1–3 at% Al<sup>3+</sup>, 2 at% Fe<sup>2+</sup>, or co-doped with Al–Fe at total concentrations of 2–4 at%, compared to undoped NMC811. Rietveld refinement of XRD patterns revealed reduced Li<sup>+</sup>/Ni<sup>2+</sup> cation mixing in these same concentrations, confirming structural stabilization. In contrast, Cu<sup>2+</sup> doping beyond 1 at%, whether alone or in combination, did not yield additional benefits and instead led to increased disorder. These findings suggest that leachates containing up to these impurity levels could be used directly in resynthesis without further purification, as the resulting NMC811 retained equal or improved performance. This supports a more sustainable and resource-efficient recycling process by reducing water, reagent, and energy consumption.</div></div>","PeriodicalId":34318,"journal":{"name":"Journal of Power Sources Advances","volume":"36 ","pages":"Article 100193"},"PeriodicalIF":4.6,"publicationDate":"2025-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145576035","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-20DOI: 10.1016/j.powera.2025.100192
Almudena González González, Juan Manuel Pérez Rodríguez
Lithium-ion batteries (LiBs) are widely used today in many different applications. This provokes an increasing demand on critical raw materials (CRMs) which currently are difficult to obtain. This slows down the achievement of energy sovereignty. In this sense, recycling appears as a solution to avoid the over-exploitation of natural resources and to contribute to the energy self-sufficiency of the European Union. It is therefore necessary to develop efficient recycling processes as early as possible.
In this sense, bioleaching and bioelectrochemistry have been raised to be a cost-effective and sustainable technologies, which can be applied sequentially to remove and recover critical metals from spent LiBs. According to the results obtained under optimised laboratory conditions, bio-produced acids have been reported to leach 80–100 % of Ni, Mn, Co and Li and bioelectrochemistry can achieve recovery rates in excess of 95 %.
The main objective of this review is to present the recent advances in these technologies for batteries used in Electric Vehicles, which will allow the definition of the challenges that need to be addressed by research in order to achieve their implementation on an industrial scale.
{"title":"Bioleaching and bioelectrochemistry, eco-efficient technologies for the recycling of electric vehicle lithium-ion batteries. A review","authors":"Almudena González González, Juan Manuel Pérez Rodríguez","doi":"10.1016/j.powera.2025.100192","DOIUrl":"10.1016/j.powera.2025.100192","url":null,"abstract":"<div><div>Lithium-ion batteries (LiBs) are widely used today in many different applications. This provokes an increasing demand on critical raw materials (CRMs) which currently are difficult to obtain. This slows down the achievement of energy sovereignty. In this sense, recycling appears as a solution to avoid the over-exploitation of natural resources and to contribute to the energy self-sufficiency of the European Union. It is therefore necessary to develop efficient recycling processes as early as possible.</div><div>In this sense, bioleaching and bioelectrochemistry have been raised to be a cost-effective and sustainable technologies, which can be applied sequentially to remove and recover critical metals from spent LiBs. According to the results obtained under optimised laboratory conditions, bio-produced acids have been reported to leach 80–100 % of Ni, Mn, Co and Li and bioelectrochemistry can achieve recovery rates in excess of 95 %.</div><div>The main objective of this review is to present the recent advances in these technologies for batteries used in Electric Vehicles, which will allow the definition of the challenges that need to be addressed by research in order to achieve their implementation on an industrial scale.</div></div>","PeriodicalId":34318,"journal":{"name":"Journal of Power Sources Advances","volume":"36 ","pages":"Article 100192"},"PeriodicalIF":4.6,"publicationDate":"2025-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145575992","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-11DOI: 10.1016/j.powera.2025.100191
Ane Muguruza-Sánchez , Susan Sananes-Israel , Enrique Moliner , Edgar Contreras , Imanol Landa-Medrano , Verónica Palomares , Iratxe de Meatza
Current lithium-ion battery recycling processes are based on high-temperature calcination (pyrometallurgy) or leaching treatments (hydrometallurgy), requiring huge amounts of energy and producing considerable waste. Direct recycling protocols are based on the reconstruction and regeneration of materials, eliminating the need for further material processing. In this paper, graphite electrodes have been recycled via a direct recycling protocol based on mild leaching with H2SO4 and H2O2 and calcination to eliminate the impurities and regenerate the structure. A Design of Experiments (DOE) has been proposed to determine the leaching conditions that reduce the generated waste and environmental impact, for which a Life Cycle Assessment (LCA) has been carried out. This combination of experimental and analytical methods has been useful to determine the parameters that have the greatest impact on the environment and select the most sustainable leaching condition, which, in this case, has shown a reduction of 36 % in acidification and 14 % in water use. The established recycling route has been validated with graphite anodes from production scraps and cycled cells (End-of-Life condition, EoL, SOH%<80 %), and in both cases, the polymeric compounds used in the electrode slurry preparation have been eliminated and the graphitization degree has been restored. These results show that graphite can be recycled from LIBs to develop a direct recycling route that promotes a sustainable circular economy and diminishes material waste.
{"title":"Direct recycling of graphite from spent batteries and production scraps for the development of a circular and sustainable economy","authors":"Ane Muguruza-Sánchez , Susan Sananes-Israel , Enrique Moliner , Edgar Contreras , Imanol Landa-Medrano , Verónica Palomares , Iratxe de Meatza","doi":"10.1016/j.powera.2025.100191","DOIUrl":"10.1016/j.powera.2025.100191","url":null,"abstract":"<div><div>Current lithium-ion battery recycling processes are based on high-temperature calcination (pyrometallurgy) or leaching treatments (hydrometallurgy), requiring huge amounts of energy and producing considerable waste. Direct recycling protocols are based on the reconstruction and regeneration of materials, eliminating the need for further material processing. In this paper, graphite electrodes have been recycled via a direct recycling protocol based on mild leaching with H<sub>2</sub>SO<sub>4</sub> and H<sub>2</sub>O<sub>2</sub> and calcination to eliminate the impurities and regenerate the structure. A Design of Experiments (DOE) has been proposed to determine the leaching conditions that reduce the generated waste and environmental impact, for which a Life Cycle Assessment (LCA) has been carried out. This combination of experimental and analytical methods has been useful to determine the parameters that have the greatest impact on the environment and select the most sustainable leaching condition, which, in this case, has shown a reduction of 36 % in acidification and 14 % in water use. The established recycling route has been validated with graphite anodes from production scraps and cycled cells (End-of-Life condition, EoL, SOH%<80 %), and in both cases, the polymeric compounds used in the electrode slurry preparation have been eliminated and the graphitization degree has been restored. These results show that graphite can be recycled from LIBs to develop a direct recycling route that promotes a sustainable circular economy and diminishes material waste.</div></div>","PeriodicalId":34318,"journal":{"name":"Journal of Power Sources Advances","volume":"36 ","pages":"Article 100191"},"PeriodicalIF":4.6,"publicationDate":"2025-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145525346","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-10-10DOI: 10.1016/j.powera.2025.100190
Janik Ruppert , Philipp Voß , Lukas Ihlbrock , Jakob Palm , Simon Lux , Jens Leker
In the face of rising demand for efficient and reliable energy storage, this study evaluates the cost-effectiveness of lithium-ion and sodium-ion batteries across pouch, prismatic, and cylindrical cell formats. Introducing CellEst 3.0, an open-source, Excel-based model offering detailed insights into material and production costs for various battery chemistries and formats, including post-lithium technologies such as sodium-ion batteries (SIBs). Our analysis shows that NMC 811 lithium-ion cells offer the highest energy density but have higher material costs due to expensive cathode active material. In contrast, the affordable LFP cathode active material provides cost advantages over NMC. SIBs, particularly those based on NaNFM 111, are the most cost-effective at $54-$62 per kWh, primarily due to cheaper anode active material and aluminum current collector foils. Prismatic cells are identified as the cost leader, supporting the industry's shift towards this format despite other technological factors. Scenario analysis suggests that SIBs withstand volatile market conditions better due to lower material price dependency. While production cost savings correlate closely with cell energy, cylindrical cells are an exception due to their manufacturing processes. This study underlines the value of detailed cost modeling in battery development and demonstrates the economic potential of sodium-ion batteries in sustainable energy storage.
{"title":"Analyzing material and production costs for lithium-ion and sodium-ion batteries using process-based cost modeling - CellEst 3.0","authors":"Janik Ruppert , Philipp Voß , Lukas Ihlbrock , Jakob Palm , Simon Lux , Jens Leker","doi":"10.1016/j.powera.2025.100190","DOIUrl":"10.1016/j.powera.2025.100190","url":null,"abstract":"<div><div>In the face of rising demand for efficient and reliable energy storage, this study evaluates the cost-effectiveness of lithium-ion and sodium-ion batteries across pouch, prismatic, and cylindrical cell formats. Introducing CellEst 3.0, an open-source, Excel-based model offering detailed insights into material and production costs for various battery chemistries and formats, including post-lithium technologies such as sodium-ion batteries (SIBs). Our analysis shows that NMC 811 lithium-ion cells offer the highest energy density but have higher material costs due to expensive cathode active material. In contrast, the affordable LFP cathode active material provides cost advantages over NMC. SIBs, particularly those based on NaNFM 111, are the most cost-effective at $54-$62 per kWh, primarily due to cheaper anode active material and aluminum current collector foils. Prismatic cells are identified as the cost leader, supporting the industry's shift towards this format despite other technological factors. Scenario analysis suggests that SIBs withstand volatile market conditions better due to lower material price dependency. While production cost savings correlate closely with cell energy, cylindrical cells are an exception due to their manufacturing processes. This study underlines the value of detailed cost modeling in battery development and demonstrates the economic potential of sodium-ion batteries in sustainable energy storage.</div></div>","PeriodicalId":34318,"journal":{"name":"Journal of Power Sources Advances","volume":"36 ","pages":"Article 100190"},"PeriodicalIF":4.6,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145269211","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-09-29DOI: 10.1016/j.powera.2025.100188
Jonas Pfaff , Sebastian Schopferer , Henning Markötter , Alexander Rack , Giovanni Bruno , Anita Schmidt , Tim Tichter , Nils Böttcher
The dynamics of mechanically initiated thermal runaway (TR) events in cylindrical 18650 cells with NFM (Na(Ni1/3Fe1/3Mn1/3)O2), LFP (LiFePO4), and NMC532 (LiNi1/2Mn1/3Co1/5O2) cathode chemistries were investigated using high-speed synchrotron X-ray imaging. Structural similarity index measures (SSIM) were employed to identify and track rapid structural changes. In this manner, thermal decompositions and internal propagation dynamics, influencing the safety mechanisms of the cells, were studied. This lead to two major findings: (I) Among NFM, LFP, and NMC532 cells, the TR-characteristics differ significantly in temperature and internal propagation speed. Internal safety mechanisms appear, however, visually similar. Among all samples, LFP cells exhibit higher safety performance concerning the initiation of TR by nail penetration and the progression of TR. (II) The NFM cells used in this study displayed an almost explosive TR. This finding appears counterintuitive on a first glance, since sodium-ion batteries are usually considered safe. High-speed imaging revealed that the explosive TR is not necessarily caused by the thermochemical decomposition reactions, but rather by a failure of the venting mechanism. This results in a significant pressure buildup within the cell upon TR initiation and eventually a severely violent TR. These results underline that battery safety depends on many factors and not solely on optimized cell chemistries or materials.
{"title":"High-speed synchrotron radiography of nail penetration-induced thermal runaway: Understanding the explosive behavior of commercial sodium-ion batteries with NFM cathode","authors":"Jonas Pfaff , Sebastian Schopferer , Henning Markötter , Alexander Rack , Giovanni Bruno , Anita Schmidt , Tim Tichter , Nils Böttcher","doi":"10.1016/j.powera.2025.100188","DOIUrl":"10.1016/j.powera.2025.100188","url":null,"abstract":"<div><div>The dynamics of mechanically initiated thermal runaway (TR) events in cylindrical 18650 cells with NFM (Na(Ni<sub>1/3</sub>Fe<sub>1/3</sub>Mn<sub>1/3</sub>)O<sub>2</sub>), LFP (LiFePO<sub>4</sub>), and NMC532 (LiNi<sub>1/2</sub>Mn<sub>1/3</sub>Co<sub>1/5</sub>O<sub>2</sub>) cathode chemistries were investigated using high-speed synchrotron X-ray imaging. Structural similarity index measures (SSIM) were employed to identify and track rapid structural changes. In this manner, thermal decompositions and internal propagation dynamics, influencing the safety mechanisms of the cells, were studied. This lead to two major findings: (I) Among NFM, LFP, and NMC532 cells, the TR-characteristics differ significantly in temperature and internal propagation speed. Internal safety mechanisms appear, however, visually similar. Among all samples, LFP cells exhibit higher safety performance concerning the initiation of TR by nail penetration and the progression of TR. (II) The NFM cells used in this study displayed an almost explosive TR. This finding appears counterintuitive on a first glance, since sodium-ion batteries are usually considered safe. High-speed imaging revealed that the explosive TR is not necessarily caused by the thermochemical decomposition reactions, but rather by a failure of the venting mechanism. This results in a significant pressure buildup within the cell upon TR initiation and eventually a severely violent TR. These results underline that battery safety depends on many factors and not solely on optimized cell chemistries or materials.</div></div>","PeriodicalId":34318,"journal":{"name":"Journal of Power Sources Advances","volume":"36 ","pages":"Article 100188"},"PeriodicalIF":4.6,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145222154","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-09-20DOI: 10.1016/j.powera.2025.100187
Jesper Frost Thomsen , Simon Lux
Behind battery manufacturing lies a global supply chain that spans multiple continents. This study aims to examine the implications of the global battery supply chain from a transport perspective. A supply chain and market analysis serve as the foundation for simulating transportation within the supply chain, offering insights into the impact of transport on emissions and costs associated with battery cell manufacturing in Europe and China across various scenarios. The results indicate that (1) for Chinese and European cells, similar transport impacts are calculated if a final EV production facility in Europe is modelled; (2) transport-related emissions account for up to 5.2% of total supply chain emissions; (3) optimizing the supply chain to target the lowest transport-related emissions can result in savings of over 40% and 50% for transport-related emissions and costs respectively. The findings provide insight into the significance of transportation in designing and analyzing the battery supply chain.
{"title":"From mine to manufacturer: Assessing transport impacts in the battery supply chain","authors":"Jesper Frost Thomsen , Simon Lux","doi":"10.1016/j.powera.2025.100187","DOIUrl":"10.1016/j.powera.2025.100187","url":null,"abstract":"<div><div>Behind battery manufacturing lies a global supply chain that spans multiple continents. This study aims to examine the implications of the global battery supply chain from a transport perspective. A supply chain and market analysis serve as the foundation for simulating transportation within the supply chain, offering insights into the impact of transport on emissions and costs associated with battery cell manufacturing in Europe and China across various scenarios. The results indicate that (1) for Chinese and European cells, similar transport impacts are calculated if a final EV production facility in Europe is modelled; (2) transport-related emissions account for up to 5.2% of total supply chain emissions; (3) optimizing the supply chain to target the lowest transport-related emissions can result in savings of over 40% and 50% for transport-related emissions and costs respectively. The findings provide insight into the significance of transportation in designing and analyzing the battery supply chain.</div></div>","PeriodicalId":34318,"journal":{"name":"Journal of Power Sources Advances","volume":"36 ","pages":"Article 100187"},"PeriodicalIF":4.6,"publicationDate":"2025-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145108304","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-09-17DOI: 10.1016/j.powera.2025.100189
Leonard Kurz , Simon Glöser-Chahoud , Ralf Wörner , Frederik Reichert
Recycling is crucial for resilient value chains for lithium (Li)-ion batteries, as is ecological impact analysis, to ensure the sustainability of battery-recycling technologies. Early ecological assessments lead to greater potential for optimization and easier adaptations for the reduction of environmental impacts. In this study, we present an ex-ante life cycle assessment (LCA) of reactivation strategies for separated cathode active materials from end-of-life Li-ion batteries for direct battery recycling. Reactivation includes impurity removal, compensation for Li deficiency by relithiation, and subsequent recrystallization. In this LCA, we focus on the relithiation process as it is decisive for the variance in the reactivation procedure. Our results show that hydrothermal reactivation is associated with the lowest global warming potential across all cathode chemistries. In terms of the abiotic resource depletion (of elements) and human toxicity, solid-state reactivation has the least impacts, followed by hydrothermal relithiation. To better evaluate the ecological relevance of reactivation, we conducted a life cycle impact assessment for the entire direct recycling process chain using two different separation technologies to recover the end-of-life cathode active material. The first separation process is based on semi-automated disassembly, dismantling, and subsequent waterjet delamination of the active material from the collector foil. In the second process, the battery (modules) is mechanically shredded in an atmosphere of inert gas and subsequently fractionated. This enabled us to identify relithiation as a hotspot in the direct recycling process. On average, relithiation is responsible for 40–43 % of the global warming potential. The early ecological analysis proves to be extremely useful in this context, as the greenhouse potential in the overall process chain of strategy.
{"title":"Ex-ante environmental impact analysis of reactivation methods in the direct recycling of cathode active materials from spent lithium-ion batteries","authors":"Leonard Kurz , Simon Glöser-Chahoud , Ralf Wörner , Frederik Reichert","doi":"10.1016/j.powera.2025.100189","DOIUrl":"10.1016/j.powera.2025.100189","url":null,"abstract":"<div><div>Recycling is crucial for resilient value chains for lithium (Li)-ion batteries, as is ecological impact analysis, to ensure the sustainability of battery-recycling technologies. Early ecological assessments lead to greater potential for optimization and easier adaptations for the reduction of environmental impacts. In this study, we present an ex-ante life cycle assessment (LCA) of reactivation strategies for separated cathode active materials from end-of-life Li-ion batteries for direct battery recycling. Reactivation includes impurity removal, compensation for Li deficiency by relithiation, and subsequent recrystallization. In this LCA, we focus on the relithiation process as it is decisive for the variance in the reactivation procedure. Our results show that hydrothermal reactivation is associated with the lowest global warming potential across all cathode chemistries. In terms of the abiotic resource depletion (of elements) and human toxicity, solid-state reactivation has the least impacts, followed by hydrothermal relithiation. To better evaluate the ecological relevance of reactivation, we conducted a life cycle impact assessment for the entire direct recycling process chain using two different separation technologies to recover the end-of-life cathode active material. The first separation process is based on semi-automated disassembly, dismantling, and subsequent waterjet delamination of the active material from the collector foil. In the second process, the battery (modules) is mechanically shredded in an atmosphere of inert gas and subsequently fractionated. This enabled us to identify relithiation as a hotspot in the direct recycling process. On average, relithiation is responsible for 40–43 % of the global warming potential. The early ecological analysis proves to be extremely useful in this context, as the greenhouse potential in the overall process chain of strategy.</div></div>","PeriodicalId":34318,"journal":{"name":"Journal of Power Sources Advances","volume":"36 ","pages":"Article 100189"},"PeriodicalIF":4.6,"publicationDate":"2025-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145108305","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-08-30DOI: 10.1016/j.powera.2025.100186
Öykü Simsek , Alessandro Innocenti , Isaac Álvarez Moisés , Philip Zimmer , Ziyuan Lyu , Simon Muench , Jean-François Gohy , Dominic Bresser , Ulrich S. Schubert
We present a new gel polymer electrolyte (GPE) based on a dopamine-containing comonomer for lithium-organic battery cells. First, several liquid electrolyte solutions composed of an ionic liquid and a lithium salt were prepared and tested in Li-organic cells with poly(2,2,6,6-tetramethyl-1-piperidinyloxy-4-yl methacrylate) (PTMA) as the positive electrode active material to evaluate the compatibility. Among them, ionic liquid electrolyte (ILE) (1-ethyl-3-methylimidazolium bis(fluorosulfonyl)imide (EMIMFSI):lithium bis(fluorosulfonyl)imide (LiFSI), 0.8:0.2, mol:mol) was found to lead to the highest specific capacity (63.5 mAh g−1 at 1C). The polymer matrix composed of benzyl methacrylate (BnMA), poly(ethylene glycol) methyl ether methacrylate (mPEGMA), and dopamine methacrylamide (DMAAm) was synthesized by UV-polymerization. A literature-known polymer system without DMAAm was prepared for comparison. Samples from both polymer films were immersed in the ILE to obtain GPEs. It was found that the addition of DMAAm increased the electrolyte uptake significantly. GPEs comprising DMAAm reveal high ionic conductivity (2.3 mS cm−1 at 20 °C) and improved galvanostatic cycling performance in Li//PTMA cells compared to the GPEs without DMAAm.
我们提出了一种基于含多巴胺单体的新型有机锂电池凝胶聚合物电解质（GPE）。首先，制备了几种由离子液体和锂盐组成的液体电解质溶液，并在以聚（2,2,6,6-四甲基-1-胡椒酰氧基-4-甲基丙烯酸酯）（PTMA）为正极活性材料的锂有机电池中进行了测试，以评价其相容性。其中，离子液体电解质（ILE）（1-乙基-3-甲基咪唑双（氟磺酰基）亚胺（EMIMFSI）：锂双（氟磺酰基）亚胺（LiFSI）， 0.8:0.2, mol:mol）的比容量最高（1C时为63.5 mAh g−1）。采用紫外聚合法制备了由甲基丙烯酸苄酯（BnMA）、聚乙二醇甲基丙烯酸甲醚（mPEGMA）和多巴胺甲基丙烯酸酰胺（DMAAm）组成的聚合物基体。制备了一种文献已知的不含DMAAm的聚合物体系进行比较。将两种聚合物薄膜的样品浸泡在ILE中以获得GPEs。结果表明，DMAAm的加入显著增加了电解质的摄取。与不含DMAAm的gpe相比，含有DMAAm的gpe在Li//PTMA电池中具有较高的离子电导率（20°C时为2.3 mS cm−1）和更好的恒流循环性能。
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Pub Date : 2025-08-20DOI: 10.1016/j.powera.2025.100185
Matthieu Dessiex , Vincent Plouzennec , Sophia Haussener , Felix N. Büchi
CO2 reduction in an electrolysis cell with a forward bias bipolar membrane (BPM) ensures good selectivity and CO2 utilization, but still suffers from large overvoltages. Recent studies have shown that integrating metal-oxide catalysts at the BPM junction in reverse bias significantly enhances the performance of water electrolyzers. It remains unclear if this method has the same positive effect on CO2 electrolysis. We studied the performance of a specially designed zero-gap BPM CO2 electrolyzer operating in forward bias mode, incorporating metal-oxide nanoparticles at the BPM interface. For TiO2 catalyst, the optimal loading at the BPM junction was between 10 and 30 μg cm-2, resulting in a 75% higher current density for the same iR-free overpotential. Physical characterization using scanning electron microscopy of the catalyst layers revealed that the optimum performance of the CO2 electrolyzer correlates with a complete coverage. SiO2 and IrO2 metal-oxides were also tested at the BPM junction. SiO2 showed comparable performance to TiO2, whereas IrO2 improved the current density by approximately 100% at an iR-free overpotential of 0.7 V compared to the pristine BPM.
{"title":"Catalyst layer at the junction of a forward bias bipolar membrane for CO2 electrolysis","authors":"Matthieu Dessiex , Vincent Plouzennec , Sophia Haussener , Felix N. Büchi","doi":"10.1016/j.powera.2025.100185","DOIUrl":"10.1016/j.powera.2025.100185","url":null,"abstract":"<div><div>CO<sub>2</sub> reduction in an electrolysis cell with a forward bias bipolar membrane (BPM) ensures good selectivity and CO<sub>2</sub> utilization, but still suffers from large overvoltages. Recent studies have shown that integrating metal-oxide catalysts at the BPM junction in reverse bias significantly enhances the performance of water electrolyzers. It remains unclear if this method has the same positive effect on CO<sub>2</sub> electrolysis. We studied the performance of a specially designed zero-gap BPM CO<sub>2</sub> electrolyzer operating in forward bias mode, incorporating metal-oxide nanoparticles at the BPM interface. For TiO<sub>2</sub> catalyst, the optimal loading at the BPM junction was between 10 and 30 μg<!--> <!-->cm<sup>-2</sup>, resulting in a 75% higher current density for the same iR-free overpotential. Physical characterization using scanning electron microscopy of the catalyst layers revealed that the optimum performance of the CO<sub>2</sub> electrolyzer correlates with a complete coverage. SiO<sub>2</sub> and IrO<sub>2</sub> metal-oxides were also tested at the BPM junction. SiO<sub>2</sub> showed comparable performance to TiO<sub>2</sub>, whereas IrO<sub>2</sub> improved the current density by approximately 100% at an iR-free overpotential of 0.7 V compared to the pristine BPM.</div></div>","PeriodicalId":34318,"journal":{"name":"Journal of Power Sources Advances","volume":"35 ","pages":"Article 100185"},"PeriodicalIF":4.6,"publicationDate":"2025-08-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144878108","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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