Browsing by Author "Birke, Kai Peter"

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Open Access
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.
Open Access
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.
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, Daniel
Considering 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).
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 Peter
In 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.
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 Peter
Modern 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.
Open Access
Cycle tests on the influence of different charging currents : a case study on different commercial, cylindrical lithium ion cells
(2023) Parschau, Anke; Degler, David; Fill, Alexander; Birke, Kai Peter; Allmendinger, Frank
On the way to a Precise Battery, the generation of measurement results and findings based on them play an important role. Although cycle life tests are time-consuming and expensive, they can provide support and important information. Especially in the current topic of accelerating the charging process, it is important to know how different charging currents affect different cell types. The CC CV charging method is still the most common, widely used method. Therefore, long-term cycle tests are carried out in this work in order to clarify the influence of different charging currents, as recommended by the cell manufacturers. Common high-energy and high-power cylindrical lithium ion cells are investigated and compared. In addition to the influence of the charging protocol on the aging, charging time and heating, the effects on the dispersion of the cells as well as the effects on the constant current and the constant voltage part of the charging process are considered. From the results it can be seen how different the investigated cells behave in response to increased charging currents. Even supposedly similar cells show significant differences in aging behavior.
Open Access
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.
Open Access
Design, properties, and manufacturing of cylindrical Li-ion battery cells : a generic overview
(2023) Baazouzi, Sabri; Feistel, Niklas; Wanner, Johannes; Landwehr, Inga; Fill, Alexander; Birke, Kai Peter
Battery cells are the main components of a battery system for electric vehicle batteries. Depending on the manufacturer, three different cell formats are used in the automotive sector (pouch, prismatic, and cylindrical). In the last 3 years, cylindrical cells have gained strong relevance and popularity among automotive manufacturers, mainly driven by innovative cell designs, such as the Tesla tabless design. This paper investigates 19 Li-ion cylindrical battery cells from four cell manufacturers in four formats (18650, 20700, 21700, and 4680). We aim to systematically capture the design features, such as tab design and quality parameters, such as manufacturing tolerances and generically describe cylindrical cells. We identified the basic designs and assigned example cells to them. In addition, we show a comprehensive definition of a tabless design considering the current and heat transport paths. Our findings show that the Tesla 4680 design is quasi-tabless. In addition, we found that 25% of the cathode and 30% of the anode are not notched, resulting in long electrical and thermal transport paths. Based on CT and post-mortem analyses, we show that jelly rolls can be approximated very well with the Archimedean spiral. Furthermore, we compare the gravimetric and volumetric energy density, the impedance, and the heating behavior at the surface and in the center of the jelly rolls. From the generic description, we present and discuss production processes focusing on format and design flexible manufacturing of jelly rolls.
Open Access
Feasible energy density pushes of Li-metal vs. Li-ion cells
(2021) Karabelli, Duygu; Birke, Kai Peter
Li-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.
Open Access
High flashpoint and eco-friendly electrolyte solvent for lithium-ion batteries
(2023) Ströbel, Marco; Kiefer, Larissa; Pross-Brakhage, Julia; Hemmerling, Jessica; Finster, Philipp; Ziebert, Carlos; Birke, Kai Peter
Since Sony launched the commercial lithium-ion cell in 1991, the composition of the liquid electrolytes has changed only slightly. The electrolyte consists of highly flammable solvents and thus poses a safety risk. Solid-state ion conductors, classified as non-combustible and safe, are being researched worldwide. However, they still have a long way to go before being available for commercial cells. As an alternative, this study presents glyceryl tributyrate (GTB) as a flame retardant and eco-friendly solvent for liquid electrolytes for lithium-ion cells. The remarkably high flashpoint (𝑇FP=174∘C) and the boiling point (𝑇BP=287∘C) of GTB are approximately 150 K higher than that of conventional linear carbonate components, such as ethyl methyl carbonate (EMC) or diethyl carbonate (DEC). The melting point (𝑇MP=-75∘C) is more than 100 K lower than that of ethylene carbonate (EC). A life cycle test of graphite/NCM with 1 M LiTFSI dissolved in GTB:EC (85:15 wt) achieved a Coulombic efficiency of above 99.6% and the remaining capacity resulted in 97% after 50 cycles (𝐶/4) of testing. The flashpoint of the created electrolyte is 𝑇FP=172∘C and, therefore, more than 130 K higher than that of state-of-the-art liquid electrolytes. Furthermore, no thermal runaway was observed during thermal abuse tests. Compared to the reference electrolyte LP40, the conductivity of the GTB-based is reduced, but the electrochemical stability is highly improved. GTB-based electrolytes are considered an interesting alternative for improving the thermal stability and safety of lithium-ion cells, especially in low power-density applications.
Open Access
A high frequency alternating current heater using the advantages of a damped oscillation circuit for low voltage Li-ion batteries
(2024) Oehl, Joachim; Gleiter, Andreas; Manka, Daniel; Fill, Alexander; Birke, Kai Peter
In many cases, batteries used in light e-mobility vehicles such as e-bikes and e-scooters do not have an active thermal management system. This poses a challenge when these batteries are stored in sub-zero temperatures and need to be charged. In such cases, it becomes necessary to move the batteries to a warmer location and allow them to acclimatize before charging. However, this is not always feasible, especially for batteries installed permanently in vehicles. In this work, we present an internal high-frequency AC heater for a 48 V battery, which is used for light electric vehicles of EU vehicle classes L1e and L3e-A1 for a power supply of up to 11 kW. We have taken advantage of the features of a damped oscillating circuit to improve the performance of the heater. Additionally, only a small inductor was added to the main current path through a cable with three windings. Furthermore, as the power electronics of the heater is part of the battery main switch, fewer additional parts inside the battery are required and therefore a cost and space reduction compared to other heaters is possible. For the chosen setup we reached a heating rate of up to 2.13 K min -1 and it was possible to raise the battery temperature from -10 °C to 10 °C using only 3.1% of its own usable capacity.
Open Access
How cell design affects the aging behavior : comparing electrode-individual aging processes of high-energy and high-power lithium-ion batteries using high precision coulometry
(2023) Jagfeld, Sebastian Michael Peter; Birke, Kai Peter; Fill, Alexander; Keil, Peter
The aging behavior of lithium-ion batteries is crucial for the development of electric vehicles and many other battery-powered devices. The cells can be generally classified into two types: high-energy (HE) and high-power (HP) cells. The cell type used depends on the field of application. As these cells differ in their electrical behavior, this work investigates whether both cell types also show different aging behavior. More precisely, the occurring capacity loss and internal side reactions are analyzed via the charge throughput. For comparison, aging tests are carried out with a high-precision battery tester, allowing the application of High Precision Coulometry (HPC). This enables early detection of aging effects and also allows us to break down the capacity loss into electrode-individual processes. A total of two sub-studies are performed: (1) a cyclic study focusing on lithium plating; and (2) an accelerated calendar aging study. It is found that HE cells exhibit stronger cyclic aging effects (lithium plating) and HP cells exhibit stronger calendar aging effects. The higher lithium plating can be explained by the higher diffusion resistance of the lithium ions within the electrodes of HE Cell. The higher calendar aging fits to the larger electrode surfaces of the HP cell. These results give deep insights into the proceeding aging in a novel way and are interesting for the selection of the appropriate cell type in the context of battery development. In a next step, the measured capacity losses could also be used for a simple parameterization of battery aging models.
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 Peter
Accurate 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.
Open Access
Impedance based temperature estimation of lithium ion cells using artificial neural networks
(2021) Ströbel, Marco; Pross-Brakhage, Julia; Kopp, Mike; Birke, Kai Peter
Open Access
Implementation of battery Digital Twin : approach, functionalities and benefits
(2021) Singh, Soumya; Weeber, Max; Birke, Kai Peter
The concept of Digital Twin (DT) is widely explored in literature for different application fields because it promises to reduce design time, enable design and operation optimization, improve after-sales services and reduce overall expenses. While the perceived benefits strongly encourage the use of DT, in the battery industry a consistent implementation approach and quantitative assessment of adapting a battery DT is missing. This paper is a part of an ongoing study that investigates the DT functionalities and quantifies the DT-attributes across the life cycles phases of a battery system. The critical question is whether battery DT is a practical and realistic solution to meeting the growing challenges of the battery industry, such as degradation evaluation, usage optimization, manufacturing inconsistencies or second-life application possibility. Within the scope of this paper, a consistent approach of DT implementation for battery cells is presented, and the main functions of the approach are tested on a Doyle-Fuller-Newman model. In essence, a battery DT can offer improved representation, performance estimation, and behavioral predictions based on real-world data along with the integration of battery life cycle attributes. Hence, this paper identifies the efforts for implementing a battery DT and provides the quantification attribute for future academic or industrial research.
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 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.
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 Peter
Lithium 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.
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, Daniel
For 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.
Open Access
Investigating the production atmosphere for sulfide-based electrolyte layers regarding occupational health and safety
(2023) Kreher, Tina; Jäger, Patrick; Heim, Fabian; Birke, Kai Peter
In all-solid-state battery (ASSB) research, the importance of sulfide electrolytes is steadily increasing. However, several challenges arise concerning the future mass production of this class of electrolytes. Among others, the high reactivity with atmospheric moisture forming toxic and corrosive hydrogen sulfide (H2S) is a major issue. On a production scale, excessive exposure to H2S leads to serious damage of production workers’ health, so additional occupational health and safety measures are required. This paper investigates the environmental conditions for the commercial fabrication of slurry-based sulfide solid electrolyte layers made of Li3PS4 (LPS) and Li10GeP2S12 (LGPS) for ASSBs. First, the identification of sequential production steps and processing stages in electrolyte layer production is carried out. An experimental setup is used to determine the H2S release of intermediates under different atmospheric conditions in the production chain, representative for the production steps. The H2S release rates obtained on a laboratory scale are then scaled up to mass production dimensions and compared to occupational health and safety limits for protection against H2S. It is shown that, under the assumptions made for the production of a slurry-based electrolyte layer with LPS or LGPS, a dry room with a dew point of = - 40 C and an air exchange rate of AER = 30 1h is sufficient to protect production workers from health hazards caused by H2S. However, the synthesis of electrolytes requires an inert gas atmosphere, as the H2S release rates are much higher compared to layer production.
Open Access
Investigation of a novel ecofriendly electrolyte-solvent for lithium-ion batteries with increased thermal stability
(2021) Ströbel, Marco; Kiefer, Larissa; Birke, Kai Peter