05 Fakultät Informatik, Elektrotechnik und Informationstechnik
Permanent URI for this collectionhttps://elib.uni-stuttgart.de/handle/11682/6
Browse
35 results
Search Results
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 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 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.Item Open Access Comparison of aqueous- and non-aqueous-based binder polymers and the mixing ratios for Zn//MnO2 batteries with mildly acidic aqueous electrolytes(2021) Fitz, Oliver; Ingenhoven, Stefan; Bischoff, Christian; Gentischer, Harald; Birke, Kai Peter; Saracsan, Dragos; Biro, DanielConsidering the literature for aqueous rechargeable Zn//MnO2 batteries with acidic electrolytes using the doctor blade coating of the active material (AM), carbon black (CB), and binder polymer (BP) for the positive electrode fabrication, different binder types with (non-)aqueous solvents were introduced so far. Furthermore, in most of the cases, relatively high passive material (CB+BP) shares ~30 wt% were applied. The first part of this work focuses on different selected BPs: polyacrylonitrile (PAN), carboxymethyl cellulose (CMC), styrene butadiene rubber (SBR), cellulose acetate (CA), and nitrile butadiene rubber (NBR). They were used together with (non-)aqueous solvents: DI-water, methyl ethyl ketone (MEK), and dimethyl sulfoxide (DMSO). By performing mechanical, electrochemical and optical characterizations, a better overall performance of the BPs using aqueous solvents was found in aqueous 2 M ZnSO4 + 0.1 M MnSO4 electrolyte (i.e., BP LA133: 150 mAh·g-1 and 189 mWh·g-1 @ 160 mA·g-1). The second part focuses on the mixing ratio of the electrode components, aiming at the decrease of the commonly used passive material share of ~30 wt% for an industrial-oriented electrode fabrication, while still maintaining the electrochemical performance. Here, the absolute CB share and the CB/BP ratio are found to be important parameters for an application-oriented electrode fabrication (i.e., high energy/power applications).Item Open Access The influence of micro-structured anode current collectors in combination with highly concentrated electrolyte on the Coulombic efficiency of in-situ deposited Li-metal electrodes with different counter electrodes(2020) Heim, Fabian; Kreher, Tina; Birke, Kai PeterThis paper compares and combines two common methods to improve the cycle performance of lithium metal (Li) electrodes. One technique is to establish a micro-structured current collector by chemical separation of a copper/zinc alloy. Furthermore, the use of a highly concentrated ether-based electrolyte is applied as a second approach for improving the cycling behavior. The influence of the two measures compared with a planar current collector and a 1 M concentrated carbonate-based electrolyte, as well as the combination of the methods, are investigated in test cells both with Li and lithium nickel cobalt manganese oxide (NCM) as counter electrodes. In all cases Li is in-situ plated onto the micro-structured current collectors respectively a planar copper foil without presence of any excess Li before first deposition. In experiments with Li counter electrodes, the effect of a structured current collector is not visible whereas the influence of the electrolyte can be observed. With NCM counter electrodes and carbonate-based electrolyte structured current collectors can improve Coulombic efficiency. The confirmation of this outcome in experiments with highly concentrated ether-based electrolyte is challenging due to high deviations. However, these results indicate, that improvements in Coulombic efficiency achieved by structuring the current collector’s surface and using ether-based electrolyte do not necessarily add up, if both methods are combined in one cell.Item Open Access Hybrid modeling of lithium-ion battery : physics-informed neural network for battery state estimation(2023) Singh, Soumya; Ebongue, Yvonne Eboumbou; Rezaei, Shahed; Birke, Kai PeterAccurate forecasting of the lifetime and degradation mechanisms of lithium-ion batteries is crucial for their optimization, management, and safety while preventing latent failures. However, the typical state estimations are challenging due to complex and dynamic cell parameters and wide variations in usage conditions. Physics-based models need a tradeoff between accuracy and complexity due to vast parameter requirements, while machine-learning models require large training datasets and may fail when generalized to unseen scenarios. To address this issue, this paper aims to integrate the physics-based battery model and the machine learning model to leverage their respective strengths. This is achieved by applying the deep learning framework called physics-informed neural networks (PINN) to electrochemical battery modeling. The state of charge and state of health of lithium-ion cells are predicted by integrating the partial differential equation of Fick’s law of diffusion from a single particle model into the neural network training process. The results indicate that PINN can estimate the state of charge with a root mean square error in the range of 0.014% to 0.2%, while the state of health has a range of 1.1% to 2.3%, even with limited training data. Compared to conventional approaches, PINN is less complex while still incorporating the laws of physics into the training process, resulting in adequate predictions, even for unseen situations.Item Open Access Feasible energy density pushes of Li-metal vs. Li-ion cells(2021) Karabelli, Duygu; Birke, Kai PeterLi-metal batteries are attracting a lot of attention nowadays. However, they are merely an attempt to enhance energy densities by employing a negative Li-metal electrode. Usually, when a Li-metal cell is charged, a certain amount of sacrificial lithium must be added, because irreversible losses per cycle add up much more unfavourably compared to conventional Li-ion cells. When liquid electrolytes instead of solid ones are used, additional electrolyte must also be added because both the lithium of the positive electrode and the liquid electrolyte are consumed during each cycle. Solid electrolytes may present a clever solution to the issue of saving sacrificial lithium and electrolyte, but their additional intrinsic weight and volume must be considered. This poses the important question of if and how much energy density can be gained in realistic scenarios if a switch from Li-ion to rechargeable Li-metal cells is anticipated. This paper calculates various scenarios assuming typical losses per cycle and reveals future e-mobility as a potential application of Li-metal cells. The paper discusses the trade-off if, considering only the push for energy density, liquid electrolytes can become a feasible option in large Li-metal batteries vs. the solid-state approach. This also includes the important aspect of cost.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 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 Comparison of different current collector materials for in situ lithium deposition with slurry-based solid electrolyte layers(2023) Kreher, Tina; Heim, Fabian; Pross-Brakhage, Julia; Hemmerling, Jessica; Birke, Kai PeterIn this paper, we investigate different current collector materials for in situ deposition of lithium using a slurry-based β-Li3PS4 electrolyte layer with a focus on transferability to industrial production. Therefore, half-cells with different current collector materials (carbon-coated aluminum, stainless steel, aluminum, nickel) are prepared and plating/stripping tests are performed. The results are compared in terms of Coulombic efficiency (CE) and overvoltages. The stainless steel current collector shows the best performance, with a mean efficiency of ηmean,SST=98%; the carbon-coated aluminum reaches ηmean,Al+C=97%. The results for pure aluminum and nickel indicate strong side reactions. In addition, an approach is tested in which a solvate ionic liquid (SIL) is added to the solid electrolyte layer. Compared to the cell setup without SIL, this cannot further increase the CE; however, a significant reduction in overvoltages is achieved.