05 Fakultät Informatik, Elektrotechnik und Informationstechnik

Permanent URI for this collectionhttps://elib.uni-stuttgart.de/handle/11682/6

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    A dual‐layered anode buffer layer structure for all solid‐state batteries
    (2024) Lu, Yushi; Chang, Hansen Michael; Birke, Kai Peter
    Over the past few decades, lithium‐ion batteries have garnered considerable attention, especially for their use in electric vehicles (EVs). In recent years, solid‐state batteries have become increasingly popular due to their excellent safety features and potential for high energy density. However, solid‐state batteries with lithium metal anodes present challenges in terms of electrochemical reactivity and cost. To address these challenges, alternative anode systems such as the “anode‐free” approach are being explored. In this study, we introduced a dual‐layered anode comprising a primary layer of physically vapor‐deposited zinc and a secondary layer of carbon black, focusing on investigating the influence of varying thicknesses of the lithiophilic zinc layer on cell cycling performance. Among the three different zinc thicknesses chosen for this purpose - categorized as thin (286 nm), medium (1.802 μm), and thick (6.519 μm) - the dual‐layered anode buffer layer was analyzed in a single‐layer full pouch cell. An in‐depth investigation into the lithium‐zinc alloying behavior was conducted through post‐mortem analysis. From the results, we found that the combination of the zinc layer with the carbon black layer improved cell cycling performance in terms of discharge capacity retention compared to a single layer of either zinc or carbon black. The cycling performance of this dual‐layered anode could be further enhanced by optimizing the zinc layer thickness, likely due to the irreversible alloying step of zinc and lithium. Among the various thicknesses evaluated, the thin zinc layer (286 nm) combined with the carbon black layer demonstrated the most promising cycling performance in all solid‐state batteries.
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    Analytic free-energy expression for the 2D-Ising model and perspectives for battery modeling
    (2023) Markthaler, Daniel; Birke, Kai Peter
    Although 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.
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    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 Peter
    This 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.
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    Influence of temperature and pressure on the wetting progress in 21700 lithium‐ion battery cells : experiment, model, and lattice Boltzmann simulation
    (2024) Wanner, Johannes; Burgard, Matthias; Othman, Nabih; Singh, Soumya; Birke, Kai Peter
    The electrolyte filling and subsequent wetting of the active material is a time‐critical process in the manufacturing of lithium‐ion batteries. Due to the metallic cell housing, the process phenomena are insufficiently accessible, preventing the replication of the wetting processes by mathematical or simulative methods and hindering efforts to accelerate the wetting process. Therefore, this publication employs a glass cell housing for electrolyte filling of a 21700 cylindrical cell to investigate the wetting at different temperatures and process pressures. In parallel, a mathematical replication of the wetting, as well as a lattice Boltzmann pore‐scale simulation, is used to evaluate the influence of these varying process boundary conditions. The results show a strong temperature dependence on electrolyte wetting and the positive effect of pressure changes in the wetting process. These findings are particularly relevant to the process design of large‐scale cylindrical cell manufacturing.
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    Cycling of double-layered graphite anodes in pouch-cells
    (2022) Müller, Daniel; Fill, Alexander; Birke, Kai Peter
    Incremental 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.
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    Multi-method model for the investigation of disassembly scenarios for electric vehicle batteries
    (2023) Baazouzi, Sabri; Grimm, Julian; Birke, Kai Peter
    Disassembly is a pivotal technology to enable the circularity of electric vehicle batteries through the application of circular economy strategies to extend the life cycle of battery components through solutions such as remanufacturng, repurposing, and efficient recycling, ultimately reintegrating gained materials into the production of new battery systems. This paper aims to develop a multi-method self-configuring simulation model to investigate disassembly scenarios, taking into account battery design as well as the configuration and layout of the disassembly station. We demonstrate the developed model in a case study using a Mercedes-Benz battery and the automated disassembly station of the DeMoBat project at Fraunhofer IPA. Furthermore, we introduce two disassembly scenarios: component-oriented and accessibility-oriented disassembly. These scenarios are compared using the simulation model to determine several indicators, including the frequency of tool change, the number and distribution of robot routes, tool utilization, and disassembly time.
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    Artificial feature extraction for estimating state-of-temperature in lithium-ion-cells using various long short-term memory architectures
    (2022) Kopp, Mike; Ströbel, Marco; Fill, Alexander; Pross-Brakhage, Julia; Birke, Kai Peter
    The temperature in each cell of a battery system should be monitored to correctly track aging behavior and ensure safety requirements. To eliminate the need for additional hardware components, a software based prediction model is needed to track the temperature behavior. This study looks at machine learning algorithms that learn physical behavior of non-linear systems based on sample data. Here, it is shown how to improve the prediction accuracy using a new method called “artificial feature extraction” compared to classical time series approaches. We show its effectiveness on tracking the temperature behavior of a Li-ion cell with limited training data at one defined ambient temperature. A custom measuring system was created capable of tracking the cell temperature, by installing a temperature sensor into the cell wrap instead of attaching it to the cell housing. Additionally, a custom early stopping algorithm was developed to eliminate the need for further hyperparameters. This study manifests that artificially training sub models that extract features with high accuracy aids models in predicting more complex physical behavior. On average, the prediction accuracy has been improved by ΔTcell=0.01 °C for the training data and by ΔTcell=0.007 °C for the validation data compared to the base model. In the field of electrical energy storage systems, this could reduce costs, increase safety and improve knowledge about the aging progress in an individual cell to sort out for second life applications.
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    Optimization of disassembly strategies for electric vehicle batteries
    (2021) Baazouzi, Sabri; Rist, Felix Paul; Weeber, Max; Birke, Kai Peter
    Various 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.
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    GREENcell : combination of a strain-hardened and passivated Al alloy foil anode with a F-free LiMn2O4 cathode
    (2025) Schad, Kathrin; Görnert, Nicolas; Mehlich, Christopher Markus; Zhan, Meichen; Birke, Kai Peter
    The rapid growth of lithium-ion battery (LiB) production calls for chemistries that combine high energy density with low environmental and economic impact. The GREENcell-concept addresses this challenge by pairing a fluorine (F)-free polyisobutylene (PIB) binder-based LiMn2O4 (LMO) cathode with an anode based on commercial aluminum (Al) alloy foil, whose theoretical capacity (993 mAh g-1) far exceeds that of graphite (372 mAh g-1). In this study cycling stability was improved through iterative optimization of the GREENcell-concept, targeting cathode formulation as well as Al foil composition, Al foil hardness, and Al surface passivation. Substituting polyvinylidene fluoride (PVDF)-based commercial LMO with a F-free PIB-based formulation reduced cathodic capacity fade by 17%, yet ∼20% of total losses in the full-cell set up remained cathode-related. To evaluate anode optimization strategies, full-cells incorporating the F-free LMO cathode were employed. Al alloy 8011 containing iron and silicon impurities outperformed high-purity Al 1050 reference foil, improving capacity retention by ∼10% through more uniform lithiation, while strain-hardened foils effectively suppressed plastic deformation compared with annealed counterparts. Surface passivation of the 8011 Al alloy foil provided further gains: a chrome(iii)-based passivation improved capacity retention by 11%, and an Al silicate layer enabled the most durable cell performance, maintaining a stable capacity profile for 100 cycles after the initial losses were overcome, likely by promoting a robust solid-electrolyte interface (SEI) able to accommodate anode volume changes. Collectively, these strategies increased capacity retention after 100 cycles from 4% for uncoated annealed high-purity Al 1050 foil to 67% for the strain-hardened, Al silicate-passivated 8011 Al alloy foil, demonstrating GREENcell's promise as a scalable, low-cost, and environmentally benign LiB architecture, as demonstrated in laboratory coin cells.
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    Towards high efficiency CO2 utilization by glow discharge plasma
    (2021) Renninger, Stephan; Rößner, Paul; Stein, Jan; Lambarth, Maike; Birke, Kai Peter
    Plasma technology reaches rapidly increasing efficiency in catalytic applications. One such application is the splitting reaction of CO2 to oxygen and carbon monoxide. This reaction could be a cornerstone of power-to-X processes that utilize electricity to produce value-added compounds such as chemicals and fuels. However, it poses problems in practice due to its highly endothermal nature and challenging selectivity. In this communication a glow discharge plasma reactor is presented that achieves high energy efficiency in the CO2 splitting reaction. To achieve this, a magnetic field is used to increase the discharge volume. Combined with laminar gas flow, this leads to even energy distribution in the working gas. Thus, the reactor achieves very high energy efficiency of up to 45% while also reaching high CO2 conversion efficiency. These results are briefly explained and then compared to other plasma technologies. Lastly, cutting edge energy efficiencies of competing technologies such as CO2 electrolysis are discussed in comparison.