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Green Electrolytes for Aqueous Ion Batteries: Towards High-Energy and Low-Temperature Applications
IF 5.1 4区 材料科学 Q2 ELECTROCHEMISTRY Pub Date : 2024-09-26 DOI: 10.1002/batt.202400579
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.

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引用次数: 0
Short-Term Tests, Long-Term Predictions – Accelerating Ageing Characterisation of Lithium-Ion Batteries 短期测试,长期预测 - 加速锂离子电池的老化表征
IF 5.1 4区 材料科学 Q2 ELECTROCHEMISTRY Pub Date : 2024-09-23 DOI: 10.1002/batt.202300594
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.

对于电池行业来说,快速确定锂离子电池的老化特性对于评估现有设计和研发未来技术都非常重要。然而,电池的目标使用寿命为 8-10 年,这意味着老化率较低,导致实际操作条件下的老化测试时间过长。因此,需要加快老化特性测试,以便在几周到几个月的时间内获得老化模式。已知的策略,如增加应力因素(如温度、电流)的严重程度,以及以特别高的精度进行测量,在应用时都需要小心谨慎,以获得有意义的结果。我们注意到,在典型的老化研究中,这一挑战并没有得到足够的重视。因此,本综述介绍了加速老化的定义和挑战,以及现有的加速电池老化表征和寿命建模方法。我们系统地讨论了现有文献中的方法。在此背景下,我们强调了几种测试条件和可行的加速策略,并提供了基本的建模和统计视角。因此,本综述对所有进行老化测试、解释老化数据或依靠老化数据预测电池寿命的人员都很有价值。
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引用次数: 0
Analyzing and Improving Conductive Networks in Commercial High-Energy Ni-rich Cathodes 商用高能富镍阴极导电网络的分析与改进
IF 5.1 4区 材料科学 Q2 ELECTROCHEMISTRY Pub Date : 2024-09-23 DOI: 10.1002/batt.202400503
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.

近年来,NMC811等富镍化学计量学由于其高比容量和减少关键资源的使用而与锂离子电池的相关性越来越大。然而,NMC活性材料的低本征电子导电性使得碳基添加剂的使用成为必要。碳结合物结构域(CBD)的体积分数和分布对电极性能有重要影响。这项工作结合了高分辨率断层扫描和微结构分辨率模拟来表征商用NMC811阴极的三维传输网络。FIB-SEM断层扫描显示,低CBD体积分数与次优分布导致微观结构中的非渗透导电网络,从而导致不利的低电子导电性。通过虚拟电极设计提高CBD含量,从根本上实现了渗透,提高了电子导电性。对真实和虚拟设计结构的模拟表明,渗透CBD网络如何显著提高能量密度。
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引用次数: 0
Mechanistic Perspectives: Integration and Repairing Adaptation of Self-Healing Electrolytes for Zinc Ion Batteries 机制视角:锌离子电池自愈电解质的整合与修复适应性
IF 5.1 4区 材料科学 Q2 ELECTROCHEMISTRY Pub Date : 2024-09-20 DOI: 10.1002/batt.202400487
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.

自我修复是一种神奇的功能,赋予储能设备非凡的弹性,已成为推进电池技术的一种有前途的策略。本文从外在动力学和内在动力学的角度综述了近年来电解质自愈化学的研究进展。首先,介绍了电解质自愈和修复适应的基本机理。外源性自愈机制采用胶囊-血管网络,内源性自愈则采用物理和化学途径。前一种愈合适应通常遵循强大的物理网络和共价联系,与后一种情况下的自我修复相比,这更为普遍和实用。除此之外,本综述还使用热力学协议评估了估计的愈合能力和统计数据。最后,我们提出了未来可能的研究方向和发展策略,以进一步应用锌离子电池的自愈现象。
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引用次数: 0
Study of Microstructural Evolution and Strain Analysis in SiOx/C Negative Electrodes Using In-situ X-ray Tomography and Digital Volume Correlation 利用原位 X 射线断层扫描和数字体积相关性研究 SiOx/C 负极中的微结构演变和应变分析
IF 5.1 4区 材料科学 Q2 ELECTROCHEMISTRY Pub Date : 2024-09-20 DOI: 10.1002/batt.202400416
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.

增加电池中的硅含量有望提高电池容量。然而,由于硅具有较大的体积膨胀性,因此在实施过程中也面临着挑战。这是导致这些电池寿命缩短的一个重要因素,而从机械角度来看,电极结构的分层是关键的退化机制之一。据悉,在电池循环过程中,粘合剂和颗粒之间的相互作用会影响这些阳极的循环性。这些电极中的微粒所经历的严重局部应变往往会导致粘结剂失效,从而导致微粒脱落或在多次循环过程中分层。充分了解应变的局部演变对于推进降解机制的机械建模和实现硅基电极的全部潜力至关重要。在这项工作中,我们结合同步辐射断层扫描和数字体积相关(DVC)技术,对整体和局部应变进行了原位测量。测量结果表明,这些电极存在显著的局部应变,可能导致分层。此外,还通过估算应变特征长度来确定复合电极的空间变化特征,该特征长度可用于复制应变场和建立分层模型。
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引用次数: 0
Microporous Polyethylene and Cellulose Composite Separators for Reversible Lithium Electrode in Lithium Rechargeable Batteries 用于锂充电电池中可逆锂电极的微孔聚乙烯和纤维素复合分离器
IF 5.1 4区 材料科学 Q2 ELECTROCHEMISTRY Pub Date : 2024-09-20 DOI: 10.1002/batt.202400472
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.

锂金属负极因其高比容量和低负电位而成为高能量密度电池的最佳选择。可充电锂金属电池(RLMB)尚未实现商业化。限制RLMB实际应用的关键因素是锂沉积过程中锂枝晶的形成和生长,以及锂阳极与电解质有机溶剂的反应,用哥伦比亚效率(CE)来量化。为了抑制锂枝晶的形成和提高CE,人们提出了许多方法,如在锂电极上形成保护层和在电解质中使用添加剂。在本研究中,考察了薄纤维素膜对锂电极上锂沉积和剥离CE的影响。研究了采用纤维素和聚乙烯复合隔膜制备的锂/锂对称电池在碳酸盐电解质和醚电解质下的循环性能。纤维素膜分离器对两种电解质的CE均有改善。纤维素膜分离器与电解质的良好润湿性可以解释这种改善。
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引用次数: 0
Challenges and Prospects of Electrolyte Design for Lithium-Sulfurized Polyacrylonitrile Batteries 锂硫化聚丙烯腈电池电解质设计的挑战与前景
IF 5.1 4区 材料科学 Q2 ELECTROCHEMISTRY Pub Date : 2024-09-19 DOI: 10.1002/batt.202400284
Tao Ma, Zhanliang Tao

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.

硫化聚丙烯腈(SPAN)被认为是一种用于锂硫(Li-S)电池的前景广阔的有机硫阴极材料。它可以进行固-固转换,而不会形成多硫化物中间相,从而克服了元素硫阴极的穿梭效应所造成的电化学性能低下的问题。然而,要实现这种独特的转换机制,需要采用适当的电解质。此外,直接使用金属锂作为阳极不可避免地会在锂-SPAN 电池中引入由锂枝晶引发的一系列问题,例如低寿命、短路、起火等。在这篇综述中,我们努力概括电解质研究的最新进展,尤其关注电解质的溶解结构与锂阳极和 SPAN 电极的界面化学之间的内在关系,旨在为高性能 Li-SPAN 全电池的电解质设计提供见解。
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引用次数: 0
Enabling Fast-Charging and High Specific Capacity of Li-Ion Batteries with Nitrogen-Doped Bilayer Graphdiyne: A First-Principles Study 利用掺氮双层石墨二炔实现锂离子电池的快速充电和高比容量:第一原理研究
IF 5.1 4区 材料科学 Q2 ELECTROCHEMISTRY Pub Date : 2024-09-19 DOI: 10.1002/batt.202400352
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).

碳基材料是锂离子电池(LIB)最重要的负极材料。为了提高锂离子电池的电化学性能,实现高能量密度和快速充电,先进的碳同素异形体成为研究的重点。在这项工作中,我们应用密度泛函理论研究了石墨二炔(GDY)的原子结构、电子结构以及高锂离子比容量。我们深入研究了单层石墨二炔(MGDY)、双层 AB(β1)堆积石墨二炔(AB(β1)BGDY)和掺氮 AB(β1)BGDY(N-AB(β1)BGDY)在不同光化状态下的原子结构。AB(β1)BGDY 和 N-AB(β1)BGDY 在锂离子吸附和插层方面表现出良好的特性,其比容量从单层 GDY 的 744 mAhg-1 提高到双层的 807 mAhg-1。除了通过双层结构提高容量外,还可以通过掺杂来定制其结构稳定性和带隙。特别是在 N-AB(β1)BGDY(约 1%)中,发现结构稳定性增加,带隙减小了 0.24 eV。这说明在 AB(β1)BGDY 中掺杂 N 可使锂离子电池中的高容量阳极更持久、更稳定,但同时也会增加 OCV。
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引用次数: 0
Towards Sustainable Sulfide-Based All-Solid-State-Batteries: An Experimental Investigation of the Challenges and Opportunities Using Solid Electrolyte Free Silicon Anodes 实现可持续的硫化物全固态电池:使用无固体电解质硅阳极的挑战与机遇实验研究
IF 5.1 4区 材料科学 Q2 ELECTROCHEMISTRY Pub Date : 2024-09-19 DOI: 10.1002/batt.202400412
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。
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引用次数: 0
Effect of Chloride Ions on the Electrochemical Performance of Magnesium Metal-Organic-Frameworks-Based Semi-Solid Electrolytes 氯离子对基于金属有机框架的镁半固态电解质电化学性能的影响
IF 5.1 4区 材料科学 Q2 ELECTROCHEMISTRY Pub Date : 2024-09-18 DOI: 10.1002/batt.202400420
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.

有关镁(Mg)电解质的大部分研究都集中在增强镁的可逆沉积上,通常采用含氯化物的电解质。然而,关于氯离子在半固态镁电解质中的影响,文献中还存在明显的空白。在本研究中,我们使用由镁基混合金属有机框架、MgCl2 和 Mg(TFSI)2 组成的半固态电解质,系统地探讨了氯离子对铜(Cu)阳极上镁沉积/溶解的影响。我们通过循环伏安法和电静态循环将镁的沉积/溶解过程与阳极表面形态的变化分离开来。为此,我们对电位循环后电解质和电极的形态和成分变化进行了细致的研究。初始电位循环揭示了镁在铜电极上沉积/溶解的可行性,尽管在随后的循环中可逆性有所降低。将相对于 Mg/Mg2+ 的电位上限扩展到 4.0 V,可增强镁的溶解,这归因于氯离子促进了铜表面的溶解。我们的研究结果为优化先进镁电池技术的半固体电解质提供了启示。
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引用次数: 0
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