Eunbin Park, Jiwon Jeong, Yung-Eun Sung, Seung-Ho Yu
Aqueous battery systems are increasingly recognized for their potential as environmentally friendly next-generation energy storage solutions. However, their commercialization faces challenges due to the need for electrolytes that can operate stably at high voltages and in low-temperatures. Traditional approaches to address these issues often involve materials that compromise the green nature. This review highlights the importance of developing environmentally friendly materials to improve the performance of aqueous electrolytes under high voltage in different types of aqueous electrolytes such as water-in-salt, molecular crowding electrolytes, eutectic electrolytes and cosolvents. In addition, we review advances in different types of aqueous electrolytes focused on using sustainable materials to achieve stable electrolytes at low-temperature by suppressing water crystallization and lowering the freezing point. By integrating these innovations, we envision a future where aqueous batteries offer both high performance and eco-friendliness, contributing significantly to the development of sustainable energy systems.
{"title":"Green Electrolytes for Aqueous Ion Batteries: Towards High-Energy and Low-Temperature Applications","authors":"Eunbin Park, Jiwon Jeong, Yung-Eun Sung, Seung-Ho Yu","doi":"10.1002/batt.202400579","DOIUrl":"https://doi.org/10.1002/batt.202400579","url":null,"abstract":"<p>Aqueous battery systems are increasingly recognized for their potential as environmentally friendly next-generation energy storage solutions. However, their commercialization faces challenges due to the need for electrolytes that can operate stably at high voltages and in low-temperatures. Traditional approaches to address these issues often involve materials that compromise the green nature. This review highlights the importance of developing environmentally friendly materials to improve the performance of aqueous electrolytes under high voltage in different types of aqueous electrolytes such as water-in-salt, molecular crowding electrolytes, eutectic electrolytes and cosolvents. In addition, we review advances in different types of aqueous electrolytes focused on using sustainable materials to achieve stable electrolytes at low-temperature by suppressing water crystallization and lowering the freezing point. By integrating these innovations, we envision a future where aqueous batteries offer both high performance and eco-friendliness, contributing significantly to the development of sustainable energy systems.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 2","pages":""},"PeriodicalIF":5.1,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143431498","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Dr.-Ing. Sabine Paarmann, Markus Schreiber, Ahmed Chahbaz, Felix Hildenbrand, Gereon Stahl, Marcel Rogge, Dr.-Ing. Philipp Dechent, Oliver Queisser, Sebastian Dominic Frankl, Pablo Morales Torricos, Yao Lu, Dr. Nikolay I. Nikolov, Prof. Maria Kateri, Prof. Dirk Uwe Sauer, Prof. Michael A. Danzer, Prof. Thomas Wetzel, Prof. Christian Endisch, Prof. Markus Lienkamp, Prof. Andreas Jossen, Dr. Meinert Lewerenz
For the battery industry, quick determination of the ageing behaviour of lithium-ion batteries is important both for the evaluation of existing designs as well as for R&D on future technologies. However, the target battery lifetime is 8–10 years, which implies low ageing rates that lead to an unacceptably long ageing test duration under real operation conditions. Therefore, ageing characterisation tests need to be accelerated to obtain ageing patterns in a period ranging from a few weeks to a few months. Known strategies, such as increasing the severity of stress factors, for example, temperature, current, and taking measurements with particularly high precision, need care in application to achieve meaningful results. We observe that this challenge does not receive enough attention in typical ageing studies. Therefore, this review introduces the definition and challenge of accelerated ageing along existing methods to accelerate the characterisation of battery ageing and lifetime modelling. We systematically discuss approaches along the existing literature. In this context, several test conditions and feasible acceleration strategies are highlighted, and the underlying modelling and statistical perspective is provided. This makes the review valuable for all who set up ageing tests, interpret ageing data, or rely on ageing data to predict battery lifetime.
{"title":"Short-Term Tests, Long-Term Predictions – Accelerating Ageing Characterisation of Lithium-Ion Batteries","authors":"Dr.-Ing. Sabine Paarmann, Markus Schreiber, Ahmed Chahbaz, Felix Hildenbrand, Gereon Stahl, Marcel Rogge, Dr.-Ing. Philipp Dechent, Oliver Queisser, Sebastian Dominic Frankl, Pablo Morales Torricos, Yao Lu, Dr. Nikolay I. Nikolov, Prof. Maria Kateri, Prof. Dirk Uwe Sauer, Prof. Michael A. Danzer, Prof. Thomas Wetzel, Prof. Christian Endisch, Prof. Markus Lienkamp, Prof. Andreas Jossen, Dr. Meinert Lewerenz","doi":"10.1002/batt.202300594","DOIUrl":"https://doi.org/10.1002/batt.202300594","url":null,"abstract":"<p>For the battery industry, quick determination of the ageing behaviour of lithium-ion batteries is important both for the evaluation of existing designs as well as for R&D on future technologies. However, the target battery lifetime is 8–10 years, which implies low ageing rates that lead to an unacceptably long ageing test duration under real operation conditions. Therefore, ageing characterisation tests need to be accelerated to obtain ageing patterns in a period ranging from a few weeks to a few months. Known strategies, such as increasing the severity of stress factors, for example, temperature, current, and taking measurements with particularly high precision, need care in application to achieve meaningful results. We observe that this challenge does not receive enough attention in typical ageing studies. Therefore, this review introduces the definition and challenge of accelerated ageing along existing methods to accelerate the characterisation of battery ageing and lifetime modelling. We systematically discuss approaches along the existing literature. In this context, several test conditions and feasible acceleration strategies are highlighted, and the underlying modelling and statistical perspective is provided. This makes the review valuable for all who set up ageing tests, interpret ageing data, or rely on ageing data to predict battery lifetime.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"7 11","pages":""},"PeriodicalIF":5.1,"publicationDate":"2024-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202300594","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642419","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Adrian Lindner, Svenja Both, Dr.-Ing. Wolfgang Menesklou, Dr. Simon Hein, Dr. Timo Danner, Prof. Dr. Arnulf Latz, Prof. Dr.-Ing. Ulrike Krewer
Nickel-rich stoichiometries such as NMC811 have gained increasing relevance for lithium-ion-batteries in recent years due to their high specific capacity and reduced use of critical resources. However, low intrinsic electronic conductivity of NMC active materials makes the use of carbon-based additives necessary. Volume fraction and distribution of the carbon-binder-domain (CBD) have a significant impact on the electrode performance. This work combines high-resolution tomography and microstructure-resolved simulations to characterize the three-dimensional transport networks of a commercial NMC811 cathode. FIB-SEM tomography reveals that low CBD volume fractions with suboptimal distribution cause a non-percolating conductive network in the microstructure and thus unfavourably low electronic conductivity. Increasing the CBD content through virtual electrode design enables percolation and enhances electronic conductivity fundamentally. Simulations on both the real and virtually designed structures demonstrate how percolating CBD networks lead to a significantly improved energy density.
{"title":"Analyzing and Improving Conductive Networks in Commercial High-Energy Ni-rich Cathodes","authors":"Adrian Lindner, Svenja Both, Dr.-Ing. Wolfgang Menesklou, Dr. Simon Hein, Dr. Timo Danner, Prof. Dr. Arnulf Latz, Prof. Dr.-Ing. Ulrike Krewer","doi":"10.1002/batt.202400503","DOIUrl":"https://doi.org/10.1002/batt.202400503","url":null,"abstract":"<p>Nickel-rich stoichiometries such as NMC811 have gained increasing relevance for lithium-ion-batteries in recent years due to their high specific capacity and reduced use of critical resources. However, low intrinsic electronic conductivity of NMC active materials makes the use of carbon-based additives necessary. Volume fraction and distribution of the carbon-binder-domain (CBD) have a significant impact on the electrode performance. This work combines high-resolution tomography and microstructure-resolved simulations to characterize the three-dimensional transport networks of a commercial NMC811 cathode. FIB-SEM tomography reveals that low CBD volume fractions with suboptimal distribution cause a non-percolating conductive network in the microstructure and thus unfavourably low electronic conductivity. Increasing the CBD content through virtual electrode design enables percolation and enhances electronic conductivity fundamentally. Simulations on both the real and virtually designed structures demonstrate how percolating CBD networks lead to a significantly improved energy density.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"7 12","pages":""},"PeriodicalIF":5.1,"publicationDate":"2024-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202400503","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142869093","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Muhammad Arif, Liujuan Yang, Qi Zhang, Haiyan Wang
Self-healing is a magical function that endows energy storage devices with extraordinary resilience and has become a promising strategy for advancing battery technology. This short review focus on the recent developments made in self-healing chemistry for electrolytes in term of extrinsic and intrinsic dynamical concepts. Firstly, the fundamental mechanism of electrolyte self-healing and repairing adaptation is introduced. The extrinsic self-healing mechanism adopts capsule-vascular networking while intrinsic self-healing lean physical and chemical routes. The Former healing adaptation, generally follows strong physical networking and covalent linkages, which are more prevalent and practical, compared to the latter case of self-healing. In addition to that, this review also evaluates the estimated healing capabilities and statistics using thermodynamic protocols. Finally, we propose some possible future research directions and development strategies to further apply the self-healing phenomenon for zinc ion batteries.
{"title":"Mechanistic Perspectives: Integration and Repairing Adaptation of Self-Healing Electrolytes for Zinc Ion Batteries","authors":"Muhammad Arif, Liujuan Yang, Qi Zhang, Haiyan Wang","doi":"10.1002/batt.202400487","DOIUrl":"https://doi.org/10.1002/batt.202400487","url":null,"abstract":"<p>Self-healing is a magical function that endows energy storage devices with extraordinary resilience and has become a promising strategy for advancing battery technology. This short review focus on the recent developments made in self-healing chemistry for electrolytes in term of extrinsic and intrinsic dynamical concepts. Firstly, the fundamental mechanism of electrolyte self-healing and repairing adaptation is introduced. The extrinsic self-healing mechanism adopts capsule-vascular networking while intrinsic self-healing lean physical and chemical routes. The Former healing adaptation, generally follows strong physical networking and covalent linkages, which are more prevalent and practical, compared to the latter case of self-healing. In addition to that, this review also evaluates the estimated healing capabilities and statistics using thermodynamic protocols. Finally, we propose some possible future research directions and development strategies to further apply the self-healing phenomenon for zinc ion batteries.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"7 12","pages":""},"PeriodicalIF":5.1,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142869028","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Abhilash Valisammagari, Joel Lachambre, Jerome Adrien, Ludovic Broche, Martin Petit, Vivien Esnault, Eric Maire
Increasing the silicon content in batteries is expected to enhance their capacity. However, its implementation comes with challenges, as silicon exhibits a large volumetric expansion. This expansion is a significant factor contributing to the decreased lifespan of these batteries. One of the critical degradation mechanisms from a mechanical perspective is the delamination of electrode structure. The cyclability of these negative electrodes is noted to be influenced by the interaction between the binder and particles during battery cycling. The heavy local strain experienced by particles in these electrodes often leads to binder failure, resulting in particle isolation, detachment, or delamination over multiple cycles. A good understanding of the local evolution of the strain is essential in advancing the mechanical modelling of the degradation mechanism and in realizing the complete potential of silicon-based electrodes. In this work, in situ global and local strain measurements were performed by combining synchrotron tomography with Digital Volume Correlation (DVC). The measurements showed that there is significant local strain in these electrodes which can lead to delamination. In addition to this, the spatial variability of the composite electrodes was characterized by estimating the characteristic length to strain, which can be used to replicate the strain field and model the delamination.
{"title":"Study of Microstructural Evolution and Strain Analysis in SiOx/C Negative Electrodes Using In-situ X-ray Tomography and Digital Volume Correlation","authors":"Abhilash Valisammagari, Joel Lachambre, Jerome Adrien, Ludovic Broche, Martin Petit, Vivien Esnault, Eric Maire","doi":"10.1002/batt.202400416","DOIUrl":"10.1002/batt.202400416","url":null,"abstract":"<p>Increasing the silicon content in batteries is expected to enhance their capacity. However, its implementation comes with challenges, as silicon exhibits a large volumetric expansion. This expansion is a significant factor contributing to the decreased lifespan of these batteries. One of the critical degradation mechanisms from a mechanical perspective is the delamination of electrode structure. The cyclability of these negative electrodes is noted to be influenced by the interaction between the binder and particles during battery cycling. The heavy local strain experienced by particles in these electrodes often leads to binder failure, resulting in particle isolation, detachment, or delamination over multiple cycles. A good understanding of the local evolution of the strain is essential in advancing the mechanical modelling of the degradation mechanism and in realizing the complete potential of silicon-based electrodes. In this work, in situ global and local strain measurements were performed by combining synchrotron tomography with Digital Volume Correlation (DVC). The measurements showed that there is significant local strain in these electrodes which can lead to delamination. In addition to this, the spatial variability of the composite electrodes was characterized by estimating the characteristic length to strain, which can be used to replicate the strain field and model the delamination.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 2","pages":""},"PeriodicalIF":5.1,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202400416","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249200","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yuna Hirai, Rio Ohnishi, Sou Taminato, Daisuke Mori, Hiroki Eimura, Kei Ikoma, Atsushi Sawamoto, Osamu Yamamoto, Yasuo Takeda, Nobuyuki Imanishi
The lithium metal anode is the best candidate for high energy density batteries because of its high specific capacity and low negative potential. Rechargeable lithium metal batteries (RLMB) have not yet been commercialized. The key factors that limit the practical use of RLMB are the formation and growth of lithium dendrites during the lithium deposition process and the reaction of the lithium anode with the organic solvent of the electrolyte, quantified by the Columbic efficiency (CE). To suppress the lithium dendrite formation and to improve CE, many approaches such as the formation of a protective layer on the lithium electrode and the use of additives to the electrolyte have been proposed. In this study, the effect of a thin cellulose film to improve CE of lithium deposition and stripping on the lithium electrode was examined. The cycle performance of a Li/Li symmetrical cell with a cellulose and polyethylene composite separator was examined for a carbonate electrolyte and an ether electrolyte. The improvements of CE were observed for both electrolytes with the cellulose film separator. The improvement could be explained by the good wettability of the cellulose film separator with the electrolyte.
{"title":"Microporous Polyethylene and Cellulose Composite Separators for Reversible Lithium Electrode in Lithium Rechargeable Batteries","authors":"Yuna Hirai, Rio Ohnishi, Sou Taminato, Daisuke Mori, Hiroki Eimura, Kei Ikoma, Atsushi Sawamoto, Osamu Yamamoto, Yasuo Takeda, Nobuyuki Imanishi","doi":"10.1002/batt.202400472","DOIUrl":"https://doi.org/10.1002/batt.202400472","url":null,"abstract":"<p>The lithium metal anode is the best candidate for high energy density batteries because of its high specific capacity and low negative potential. Rechargeable lithium metal batteries (RLMB) have not yet been commercialized. The key factors that limit the practical use of RLMB are the formation and growth of lithium dendrites during the lithium deposition process and the reaction of the lithium anode with the organic solvent of the electrolyte, quantified by the Columbic efficiency (CE). To suppress the lithium dendrite formation and to improve CE, many approaches such as the formation of a protective layer on the lithium electrode and the use of additives to the electrolyte have been proposed. In this study, the effect of a thin cellulose film to improve CE of lithium deposition and stripping on the lithium electrode was examined. The cycle performance of a Li/Li symmetrical cell with a cellulose and polyethylene composite separator was examined for a carbonate electrolyte and an ether electrolyte. The improvements of CE were observed for both electrolytes with the cellulose film separator. The improvement could be explained by the good wettability of the cellulose film separator with the electrolyte.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"7 12","pages":""},"PeriodicalIF":5.1,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202400472","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142862018","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sulfurized polyacrylonitrile (SPAN) is regarded as a promising organic sulphur cathode material for lithium-sulfur (Li−S) batteries. It undergoes a solid-solid conversion without forming polysulfide intermediate phases, overcoming the poor electrochemical performance caused by the shuttle effect of elemental S cathodes. However, realizing this unique conversion mechanism requires employing appropriate electrolytes. Furthermore, the direct application of metallic Li as the anode unavoidable introduces a series of issues triggered by Li dendrites in Li-SPAN batteries, such as low lifespan, short circuits, fire, etc. In this review, we endeavor to encapsulate recent advancements in electrolyte research, with a particular focus on the intrinsic relationship between the solvation structure of the electrolyte and the interfacial chemistry of the Li anode and SPAN electrode, aim to provide insights into the electrolytes design for high performance Li-SPAN full batteries.
{"title":"Challenges and Prospects of Electrolyte Design for Lithium-Sulfurized Polyacrylonitrile Batteries","authors":"Tao Ma, Zhanliang Tao","doi":"10.1002/batt.202400284","DOIUrl":"10.1002/batt.202400284","url":null,"abstract":"<p>Sulfurized polyacrylonitrile (SPAN) is regarded as a promising organic sulphur cathode material for lithium-sulfur (Li−S) batteries. It undergoes a solid-solid conversion without forming polysulfide intermediate phases, overcoming the poor electrochemical performance caused by the shuttle effect of elemental S cathodes. However, realizing this unique conversion mechanism requires employing appropriate electrolytes. Furthermore, the direct application of metallic Li as the anode unavoidable introduces a series of issues triggered by Li dendrites in Li-SPAN batteries, such as low lifespan, short circuits, fire, etc. In this review, we endeavor to encapsulate recent advancements in electrolyte research, with a particular focus on the intrinsic relationship between the solvation structure of the electrolyte and the interfacial chemistry of the Li anode and SPAN electrode, aim to provide insights into the electrolytes design for high performance Li-SPAN full batteries.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"7 12","pages":""},"PeriodicalIF":5.1,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249204","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Minh Tam Le, Liang-Yin Kuo, Yi-Zhan Wu, Martin Ihrig, Nguyet N. T. Pham
Carbon-based materials are the most important anode materials for Li-ion batteries (LIBs). To improve the electrochemical performance of LIBs for high energy density and fast charging, advanced carbon allotropes are in the research focus. In this work, we applied the density functional theory to investigate the atomic and electronic structures as well as high Li-ion specific capacity of graphdiyne (GDY). The atomic structures of monolayer graphdiyne (MGDY), bilayer AB(β1)-stacking graphdiyne (AB(β1)BGDY) and nitrogen-doped AB(β1)BGDY (N-AB(β1)BGDY) at different lithiation states were thoroughly investigated. The AB(β1)BGDY and N-AB(β1)BGDY exhibit promising characteristics in Li-ion adsorption and intercalation, enhancing its specific capacity from 744 mAhg−1 in the monolayer GDY to 807 mAhg−1 in the bilayer. Besides increasing the capacity through a bilayer-structure, it is possible to tailor its structural stability and band gap by doping. Especially shown for N-AB(β1)BGDY (~1 %), an increased structural stability and a decreased band gap of 0.24 eV is found. While this means that N doping in AB(β1)BGDY can lead to longer-lasting and more stable operatable high-capacity anodes in LIBs, it increases the open-circuit voltage (OCV).
{"title":"Enabling Fast-Charging and High Specific Capacity of Li-Ion Batteries with Nitrogen-Doped Bilayer Graphdiyne: A First-Principles Study","authors":"Minh Tam Le, Liang-Yin Kuo, Yi-Zhan Wu, Martin Ihrig, Nguyet N. T. Pham","doi":"10.1002/batt.202400352","DOIUrl":"10.1002/batt.202400352","url":null,"abstract":"<p>Carbon-based materials are the most important anode materials for Li-ion batteries (LIBs). To improve the electrochemical performance of LIBs for high energy density and fast charging, advanced carbon allotropes are in the research focus. In this work, we applied the density functional theory to investigate the atomic and electronic structures as well as high Li-ion specific capacity of graphdiyne (GDY). The atomic structures of monolayer graphdiyne (MGDY), bilayer AB(<i>β</i><sub>1</sub>)-stacking graphdiyne (AB(<i>β</i><sub>1</sub>)BGDY) and nitrogen-doped AB(<i>β</i><sub>1</sub>)BGDY (N-AB(<i>β</i><sub>1</sub>)BGDY) at different lithiation states were thoroughly investigated. The AB(<i>β</i><sub>1</sub>)BGDY and N-AB(<i>β</i><sub>1</sub>)BGDY exhibit promising characteristics in Li-ion adsorption and intercalation, enhancing its specific capacity from 744 mAhg<sup>−1</sup> in the monolayer GDY to 807 mAhg<sup>−1</sup> in the bilayer. Besides increasing the capacity through a bilayer-structure, it is possible to tailor its structural stability and band gap by doping. Especially shown for N-AB(<i>β</i><sub>1</sub>)BGDY (~1 %), an increased structural stability and a decreased band gap of 0.24 eV is found. While this means that N doping in AB(<i>β</i><sub>1</sub>)BGDY can lead to longer-lasting and more stable operatable high-capacity anodes in LIBs, it increases the open-circuit voltage (OCV).</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 1","pages":""},"PeriodicalIF":5.1,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249201","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Tobias Neumann, Lukas Alexander Dold, Alain Thomas Cerny, Eric Tröster, Michael Günthel, Anna Fischer, Kai Peter Birke, Ingo Krossing, Daniel Biro
Silicon is one of the most promising anode active materials for future high–energy lithium-ion-batteries (LIB). Due to limitations related to volume changes during de–/lithiation, implementation of this material in commonly used liquid electrolyte-based LIB needs to be accompanied by material enhancement strategies such as particle structure engineering. In this work, we showcase the possibility to utilize pure silicon as anode active material in a sulfide electrolyte-based all-solid-state battery (ASSB) using a thin separator layer and LiNi0.6Mn0.2Co0.2O2 cathode. We investigate the integration of both solid electrolyte blended anodes and solid electrolyte free anodes and explore the usage of non-toxic and economically viable solvents suitable for standard atmospheric conditions for the latter. To give an insight into the microstructural changes as well as the lithiation path inside the anode soft X-ray emission and X-ray photoelectron spectroscopy were performed after the initial lithiation. Using standard electrochemical analysis methods like galvanostatic cycling and impedance spectroscopy, we demonstrate that both anode types exhibit commendable performance as structural distinctions between two-dimensional and three-dimensional interfaces became evident only at high charge rates (8 C).
硅是未来高能锂离子电池(LIB)中最有前途的负极活性材料之一。由于在脱/锂化过程中体积变化的限制,在常用的基于液态电解质的锂离子电池中使用这种材料需要辅以粒子结构工程等材料增强策略。在这项工作中,我们展示了在基于硫化物电解质的全固态电池(ASSB)中使用纯硅作为阳极活性材料的可能性,并使用了薄隔膜层和 LiNi0.6Mn0.2Co0.2O2 阴极。我们研究了混合固态电解质阳极和无固态电解质阳极的整合,并探索了适合标准大气条件的无毒且经济可行的溶剂在无固态电解质阳极中的应用。为了深入了解阳极内部的微观结构变化和锂化路径,在初始锂化之后进行了软 X 射线发射和 X 射线光电子能谱分析。利用标准电化学分析方法(如电静循环和阻抗光谱),我们证明了这两种类型的阳极都表现出了值得称赞的性能,因为二维和三维界面之间的结构差异只有在高充电速率(8 C)下才会变得明显。
{"title":"Towards Sustainable Sulfide-Based All-Solid-State-Batteries: An Experimental Investigation of the Challenges and Opportunities Using Solid Electrolyte Free Silicon Anodes","authors":"Tobias Neumann, Lukas Alexander Dold, Alain Thomas Cerny, Eric Tröster, Michael Günthel, Anna Fischer, Kai Peter Birke, Ingo Krossing, Daniel Biro","doi":"10.1002/batt.202400412","DOIUrl":"10.1002/batt.202400412","url":null,"abstract":"<p>Silicon is one of the most promising anode active materials for future high–energy lithium-ion-batteries (LIB). Due to limitations related to volume changes during de–/lithiation, implementation of this material in commonly used liquid electrolyte-based LIB needs to be accompanied by material enhancement strategies such as particle structure engineering. In this work, we showcase the possibility to utilize pure silicon as anode active material in a sulfide electrolyte-based all-solid-state battery (ASSB) using a thin separator layer and LiNi<sub>0.6</sub>Mn<sub>0.2</sub>Co<sub>0.2</sub>O<sub>2</sub> cathode. We investigate the integration of both solid electrolyte blended anodes and solid electrolyte free anodes and explore the usage of non-toxic and economically viable solvents suitable for standard atmospheric conditions for the latter. To give an insight into the microstructural changes as well as the lithiation path inside the anode soft X-ray emission and X-ray photoelectron spectroscopy were performed after the initial lithiation. Using standard electrochemical analysis methods like galvanostatic cycling and impedance spectroscopy, we demonstrate that both anode types exhibit commendable performance as structural distinctions between two-dimensional and three-dimensional interfaces became evident only at high charge rates (8 C).</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 2","pages":""},"PeriodicalIF":5.1,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202400412","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249202","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Mohamed M. Elnagar, Hagar K. Hassan, Ludwig A. Kibler, Timo Jacob
The majority of research on magnesium (Mg) electrolytes has focused on enhancing reversible Mg deposition, often employing chloride-containing electrolytes. However, there is a notable gap in the literature regarding the influence of chloride ions in semi-solid Mg electrolytes. In this study, we systematically explore the impact of chloride ions on Mg deposition/dissolution on a copper (Cu) anode using a semi-solid electrolyte composed of Mg-based mixed metal-organic frameworks, MgCl2 and Mg[TFSI]2. We separate the Mg deposition/dissolution process from changes in the anode's surface morphology In this respect, the morphological and compositional transformations in the electrolyte and electrode following galvanostatic cycling are meticulously investigated. Initial potential cycling reveals the feasibility of Mg deposition/dissolution on Cu electrodes, albeit with reduced reversibility in subsequent cycles. Extending the upper potential limit to 4.0 V vs. Mg/Mg2+ enhances Mg dissolution, attributed to chloride ions facilitating Cu surface dissolution. Our findings provide insights into optimizing semi-solid electrolytes for advanced Magnesium battery technologies.
{"title":"Effect of Chloride Ions on the Electrochemical Performance of Magnesium Metal-Organic-Frameworks-Based Semi-Solid Electrolytes","authors":"Mohamed M. Elnagar, Hagar K. Hassan, Ludwig A. Kibler, Timo Jacob","doi":"10.1002/batt.202400420","DOIUrl":"10.1002/batt.202400420","url":null,"abstract":"<p>The majority of research on magnesium (Mg) electrolytes has focused on enhancing reversible Mg deposition, often employing chloride-containing electrolytes. However, there is a notable gap in the literature regarding the influence of chloride ions in semi-solid Mg electrolytes. In this study, we systematically explore the impact of chloride ions on Mg deposition/dissolution on a copper (Cu) anode using a semi-solid electrolyte composed of Mg-based mixed metal-organic frameworks, MgCl<sub>2</sub> and Mg[TFSI]<sub>2</sub>. We separate the Mg deposition/dissolution process from changes in the anode's surface morphology In this respect, the morphological and compositional transformations in the electrolyte and electrode following galvanostatic cycling are meticulously investigated. Initial potential cycling reveals the feasibility of Mg deposition/dissolution on Cu electrodes, albeit with reduced reversibility in subsequent cycles. Extending the upper potential limit to 4.0 V <i>vs</i>. Mg/Mg<sup>2+</sup> enhances Mg dissolution, attributed to chloride ions facilitating Cu surface dissolution. Our findings provide insights into optimizing semi-solid electrolytes for advanced Magnesium battery technologies.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 1","pages":""},"PeriodicalIF":5.1,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202400420","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249290","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}