Universität Stuttgart
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Item Open Access Comprehensive study of failure mechanisms of field-aged automotive lead batteries(2023) Conradt, Rafael; Schröer, Philipp; Dazer, Martin; Wirth, Jonathan; Jöris, Florian; Schulte, Dominik; Birke, Kai PeterModern vehicles have increasing safety requirements and a need for reliable low-voltage power supply in their on-board power supply systems. Understanding the causes and probabilities of failures in a 12 V power supply is crucial. Field analyses of aged and failed 12 V lead batteries can provide valuable insights regarding this topic. In a previous study, non-invasive electrical testing was used to objectively determine the reasons for failure and the lifetime of individual batteries. By identifying all of the potential failure mechanisms, the Latin hypercube sampling method was found to effectively reduce the required sample size. To ensure sufficient confidence in validating diagnostic algorithms and calculating time-dependent failure rates, all identified aging phenomena must be considered. This study presents a probability distribution of the failure mechanisms that occur in the field, as well as provides insights into potential opportunities, but it also challenges diagnostic approaches for current and future vehicles.Item Open Access Analytic free-energy expression for the 2D-Ising model and perspectives for battery modeling(2023) Markthaler, Daniel; Birke, Kai PeterAlthough originally developed to describe the magnetic behavior of matter, the Ising model represents one of the most widely used physical models, with applications in almost all scientific areas. Even after 100 years, the model still poses challenges and is the subject of active research. In this work, we address the question of whether it is possible to describe the free energy A of a finite-size 2D-Ising model of arbitrary size, based on a couple of analytically solvable 1D-Ising chains. The presented novel approach is based on rigorous statistical-thermodynamic principles and involves modeling the free energy contribution of an added inter-chain bond DAbond(b, N) as function of inverse temperature b and lattice size N. The identified simple analytic expression for DAbond is fitted to exact results of a series of finite-size quadratic N N-systems and enables straightforward and instantaneous calculation of thermodynamic quantities of interest, such as free energy and heat capacity for systems of an arbitrary size. This approach is not only interesting from a fundamental perspective with respect to the possible transfer to a 3D-Ising model, but also from an application-driven viewpoint in the context of (Li-ion) batteries where it could be applied to describe intercalation mechanisms.Item Open Access Modeling and experimental investigation of the interaction between pressure-dependent aging and pressure development due to the aging of lithium-ion cells(2023) Avdyli, Arber; Fill, Alexander; Birke, Kai PeterIn order to meet the increasing demands of the battery in terms of range, safety and performance, it is necessary to ensure optimal operation conditions of a lithium-ion cell. In this thesis, the influence of mechanical boundary conditions on the cell is investigated theoretically and experimentally. First, fundamental equations are derived that lead to coupled models that can be parameterized based on specific cell measurements and predict the pressure evolution due to capacity aging and vice versa. The model is used to derive optimal operating points of the cell, which can be considered in the module design.Item Open Access A performance and cost overview of selected solid-state electrolytes : race between polymer electrolytes and inorganic sulfide electrolytes(2021) Karabelli, Duygu; Birke, Kai Peter; Weeber, MaxElectrolytes are key components in electrochemical storage systems, which provide an ion-transport mechanism between the cathode and anode of a cell. As battery technologies are in continuous development, there has been growing demand for more efficient, reliable and environmentally friendly materials. Solid-state lithium ion batteries (SSLIBs) are considered as next-generation energy storage systems and solid electrolytes (SEs) are the key components for these systems. Compared to liquid electrolytes, SEs are thermally stable (safer), less toxic and provide a more compact (lighter) battery design. However, the main issue is the ionic conductivity, especially at low temperatures. So far, there are two popular types of SEs: (1) inorganic solid electrolytes (InSEs) and (2) polymer electrolytes (PEs). Among InSEs, sulfide-based SEs are providing very high ionic conductivities (up to 10−2 S/cm) and they can easily compete with liquid electrolytes (LEs). On the other hand, they are much more expensive than LEs. PEs can be produced at less cost than InSEs but their conductivities are still not sufficient for higher performances. This paper reviews the most efficient SEs and compares them in terms of their performances and costs. The challenges associated with the current state-of-the-art electrolytes and their cost-reduction potentials are described.Item Open Access Impedance based temperature estimation of lithium ion cells using artificial neural networks(2021) Ströbel, Marco; Pross-Brakhage, Julia; Kopp, Mike; Birke, Kai PeterItem Open Access Non-uniform circumferential expansion of cylindrical Li-ion cells - the potato effect(2021) Hemmerling, Jessica; Guhathakurta, Jajnabalkya; Dettinger, Falk; Fill, Alexander; Birke, Kai PeterThis paper presents the non-uniform change in cell thickness of cylindrical Lithium (Li)-ion cells due to the change of State of Charge (SoC). Using optical measurement methods, with the aid of a laser light band micrometer, the expansion and contraction are determined over a complete charge and discharge cycle. The cell is rotated around its own axis by an angle of α=10° in each step, so that the different positions can be compared with each other over the circumference. The experimental data show that, contrary to the assumption based on the physical properties of electrode growth due to lithium intercalation in the graphite, the cell does not expand uniformly. Depending on the position and orientation of the cell coil, there are different zones of expansion and contraction. In order to confirm the non-uniform expansion around the circumference of the cell in 3D, X-ray computed tomography (CT) scans of the cells are performed at low and at high SoC. Comparison of the high resolution 3D reconstructed volumes clearly visualizes a sinusoidal pattern for non-uniform expansion. From the 3D volume, it can be confirmed that the thickness variation does not vary significantly over the height of the battery cell due to the observed mechanisms. However, a slight decrease in the volume change towards the poles of the battery cells due to the higher stiffness can be monitored.Item Open Access Cycling of double-layered graphite anodes in pouch-cells(2022) Müller, Daniel; Fill, Alexander; Birke, Kai PeterIncremental improvement to the current state-of-the-art lithium-ion technology, for example regarding the physical or electrochemical design, can bridge the gap until the next generation of cells are ready to take Li-ions place. Previously designed two-layered porosity-graded graphite anodes, together with LixNi0.6Mn0.2Co0.2O2 cathodes, were analysed in small pouch-cells with a capacity of around 1 Ah. For comparison, custom-made reference cells with the average properties of two-layered anodes were tested. Ten cells of each type were examined in total. Each cell pair, consisting of one double-layer and one single-layer (reference) cell, underwent the same test procedure. Besides regular charge and discharge cycles, electrochemical impedance spectroscopy, incremental capacity analysis, differential voltage analysis and current-pulse measurement are used to identify the differences in ageing behaviour between the two cell types. The results show similar behaviour and properties at beginning-of-life, but an astonishing improvement in capacity retention for the double-layer cells regardless of the cycling conditions. Additionally, the lifetime of the single-layer cells was strongly influenced by the cycling conditions, and the double-layer cells showed less difference in ageing behaviour.Item Open Access Introducing a concept for designing an aqueous electrolyte with pH buffer properties for Zn-MnO2 batteries with Mn2+/MnO2 deposition/dissolution(2023) Fitz, Oliver; Wagner, Florian; Pross-Brakhage, Julia; Bauer, Manuel; Gentischer, Harald; Birke, Kai Peter; Biro, DanielFor large-scale energy-storage systems, the aqueous rechargeable zinc–manganese dioxide battery (ARZMB) attracts increasing attention due to its excellent advantages such as high energy density, high safety, low material cost, and environmental friendliness. Still, the reaction mechanism and its influence on the electrolyte's pH are under debate. Herein, a pH buffer concept for ARZMB electrolytes is introduced. Selection criteria for pH buffer substances are defined. Different buffered electrolytes based on a zinc salt (ZnSO4, Zn(CH3COO)2, Zn(CHOO)2), and pH buffer substances (acetic acid, propionic acid, formic acid, citric acid, 4-hydrobenzoic acid, potassium bisulfate, potassium dihydrogen citrate, and potassium hydrogen phthalate) are selected and compared to an unbuffered 2 m ZnSO4 reference electrolyte using titration, galvanostatic cycling with pH tracking, and cyclic voltammetry. By adding buffer substances, the pH changes can be reduced and controlled within the defined operating window, supporting the Mn2+/MnO2 deposition/dissolution mechanism. Furthermore, the potential plateau during discharge can be increased from ≈1.3 V (ZnSO4) to ≈1.7 V (ZnSO4 + AA) versus Zn/Zn2+ and the energy retention from ≈30% after 268 cycles (ZnSO4) to ≈86% after 494 cycles (ZnSO4 + AA). Herein, this work can serve as a basis for the targeted design of long-term stable ARZMB electrolytes.Item Open Access Optimization of disassembly strategies for electric vehicle batteries(2021) Baazouzi, Sabri; Rist, Felix Paul; Weeber, Max; Birke, Kai PeterVarious studies show that electrification, integrated into a circular economy, is crucial to reach sustainable mobility solutions. In this context, the circular use of electric vehicle batteries (EVBs) is particularly relevant because of the resource intensity during manufacturing. After reaching the end-of-life phase, EVBs can be subjected to various circular economy strategies, all of which require the previous disassembly. Today, disassembly is carried out manually and represents a bottleneck process. At the same time, extremely high return volumes have been forecast for the next few years, and manual disassembly is associated with safety risks. That is why automated disassembly is identified as being a key enabler of highly efficient circularity. However, several challenges need to be addressed to ensure secure, economic, and ecological disassembly processes. One of these is ensuring that optimal disassembly strategies are determined, considering the uncertainties during disassembly. This paper introduces our design for an adaptive disassembly planner with an integrated disassembly strategy optimizer. Furthermore, we present our optimization method for obtaining optimal disassembly strategies as a combination of three decisions: (1) the optimal disassembly sequence, (2) the optimal disassembly depth, and (3) the optimal circular economy strategy at the component level. Finally, we apply the proposed method to derive optimal disassembly strategies for one selected battery system for two condition scenarios. The results show that the optimization of disassembly strategies must also be used as a tool in the design phase of battery systems to boost the disassembly automation and thus contribute to achieving profitable circular economy solutions for EVBs.Item Open Access Influence of temperature and electrolyte composition on the performance of lithium metal anodes(2021) Boroujeni, Sanaz Momeni; Fill, Alexander; Ridder, Alexander; Birke, Kai PeterLithium metal anodes have again attracted widespread attention due to the continuously growing demand of cells with higher energy density. However, the lithium deposition mechanism and the affecting process of influencing factors, such as temperature, cycling current density, and electrolyte composition are not fully understood and require further investigation. In this article, the behavior of lithium metal anode at different temperatures (25, 40, and 60 ∘C), lithium salts, electrolyte concentrations (1 and 2 M), and the applied cell current (equivalent to 0.5 C, 1 C, and 2 C). is investigated. Two different salts were evaluated: lithium bis(fluorosulfonyl)imide (LiFSI) and lithium bis(trifluoromethanesul-fonyl)imide (LiTFSI). The cells at a medium temperature (40 ∘C) show the highest Coulombic efficiency (CE). However, shorter cycle life is observed compared to the experiments at room temperature (25 ∘C). Regardless of electrolyte type and C-rate, the higher temperature of 60 ∘C provides the worst Coulombic efficiency and cycle life among those at the examined temperatures. A higher C-rate has a positive effect on the stability over the cycle life of the lithium cells. The best performance in terms of long cycle life and relatively good Coulombic efficiency is achieved by fast charging the cell with high concentration LiFSI in 1,2-dimethoxyethane (DME) electrolyte at a temperature of 25 ∘C. The cell has an average Coulombic efficiency of 0.987 over 223 cycles. In addition to galvanostatic experiments, Electrochemical Impedance Spectroscopy (EIS) measurements were performed to study the evolution of the interface under different conditions during cycling.