05 Fakultät Informatik, Elektrotechnik und Informationstechnik
Permanent URI for this collectionhttps://elib.uni-stuttgart.de/handle/11682/6
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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 All-inorganic CsPbI2Br perovskite solar cells with thermal stability at 250 °C and moisture-resilience via polymeric protection layers(2025) Roy, Rajarshi; Byranvand, Mahdi Malekshahi; Zohdi, Mohamed Reza; Magorian Friedlmeier, Theresa; Das, Chittaranjan; Hempel, Wolfram; Zuo, Weiwei; Kedia, Mayank; Rendon, Jose Jeronimo; Boehringer, Stephan; Hailegnanw, Bekele; Vorochta, Michael; Mehl, Sascha; Rai, Monika; Kulkarni, Ashish; Mathur, Sanjay; Saliba, MichaelAll-inorganic perovskites, such as CsPbI2Br, have emerged as promising compositions due to their enhanced thermal stability. However, they face significant challenges due to their susceptibility to humidity. In this work, CsPbI2Br perovskite is treated with poly(3-hexylthiophen-2,5-diyl) (P3HT) during the crystallization resulting in significant stability improvements against thermal, moisture and steady-state operation stressors. The perovskite solar cell retains ∼90% of the initial efficiency under relative humidity (RH) at ∼60% for 30 min, which is among the most stable all-inorganic perovskite devices to date under such harsh conditions. Furthermore, the P3HT treatment ensures high thermal stress tolerance at 250 °C for over 5 h. In addition to the stability enhancements, the champion P3HT-treated device shows a higher power conversion efficiency (PCE) of 13.5% compared to 12.7% (reference) with the stabilized power output (SPO) for 300 s. In addition, the P3HT-protected perovskite layer in ambient conditions shows ∼75% of the initial efficiency compared to the unprotected devices with ∼28% of their initial efficiency after 7 days of shelf life.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 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.Item Open Access Coordination chemistry as a universal strategy for a controlled perovskite crystallization(2023) Zuo, Weiwei; Byranvand, Mahdi Malekshahi; Kodalle, Tim; Zohdi, Mohammadreza; Lim, Jaekeun; Carlsen, Brian; Magorian Friedlmeier, Theresa; Kot, Małgorzata; Das, Chittaranjan; Flege, Jan Ingo; Zong, Wansheng; Abate, Antonio; Sutter‐Fella, Carolin M.; Li, Meng; Saliba, MichaelThe most efficient and stable perovskite solar cells (PSCs) are made from a complex mixture of precursors. Typically, to then form a thin film, an extreme oversaturation of the perovskite precursor is initiated to trigger nucleation sites, e.g., by vacuum, an airstream, or a so-called antisolvent. Unfortunately, most oversaturation triggers do not expel the lingering (and highly coordinating) dimethyl sulfoxide (DMSO), which is used as a precursor solvent, from the thin films; this detrimentally affects long-term stability. In this work, (the green) dimethyl sulfide (DMS) is introduced as a novel nucleation trigger for perovskite films combining, uniquely, high coordination and high vapor pressure. This gives DMS a universal scope: DMS replaces other solvents by coordinating more strongly and removes itself once the film formation is finished. To demonstrate this novel coordination chemistry approach, MAPbI3 PSCs are processed, typically dissolved in hard-to-remove (and green) DMSO achieving 21.6% efficiency, among the highest reported efficiencies for this system. To confirm the universality of the strategy, DMS is tested for FAPbI3 as another composition, which shows higher efficiency of 23.5% compared to 20.9% for a device fabricated with chlorobenzene. This work provides a universal strategy to control perovskite crystallization using coordination chemistry, heralding the revival of perovskite compositions with pure DMSO.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 Unified model for laser doping of silicon from precursors(2021) Hassan, Mohamed; Dahlinger, Morris; Köhler, Jürgen R.; Zapf-Gottwick, Renate; Werner, Jürgen H.Laser doping of silicon with the help of precursors is well established in photovoltaics. Upon illumination with the constant or pulsed laser beam, the silicon melts and doping atoms from the doping precursor diffuse into the melted silicon. With the proper laser parameters, after resolidification, the silicon is doped without any lattice defects. Depending on laser energy and on the kind of precursor, the precursor either melts or evaporates during the laser process. For high enough laser energies, even parts of the silicon’s surface evaporate. Here, we present a unified model and simulation program, which considers all these cases. We exemplify our model with experiments and simulations of laser doping from a boron oxide precursor layer. In contrast to previous models, we are able to predict not only the width and depth of the patterns on the deformed silicon surface but also the doping profiles over a wide range of laser energies. In addition, we also show that the diffusion of the boron atoms in the molten Si is boosted by a thermally induced convection in the silicon melt: the Gaussian intensity distribution of the laser beam increases the temperature-gradient-induced surface tension gradient, causing the molten Si to circulate by Marangoni convection. Laser pulse energy densities above H > 2.8 J/cm2 lead not only to evaporation of the precursor, but also to a partial evaporation of the molten silicon. Without considering the evaporation of Si, it is not possible to correctly predict the doping profiles for high laser energies. About 50% of the evaporated materials recondense and resolidify on the wafer surface. The recondensed material from each laser pulse forms a dopant source for the subsequent laser pulses.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.