05 Fakultät Informatik, Elektrotechnik und Informationstechnik

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

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    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, Michael
    The 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.
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    Revealing the local pH value changes of acidic aqueous zinc ion batteries with a manganese dioxide electrode during cycling
    (2020) Bischoff, Christian Friedrich; Fitz, Oliver Sebastian; Burns, Jordan; Bauer, Manuel; Gentischer, Harald; Birke, Kai Peter; Henning, Hans-Martin; Biro, Daniel
    The research on aqueous zinc ion batteries (AZIB) is getting more attention as the energy transition continues to develop and the need for inexpensive and safe stationary storage batteries is growing. As the detailed reaction mechanisms are not conclusively revealed, we want to take an alternative approach to investigate the importance of pH value changes during cycling. By adding a pH-indicator to the electrolyte (2 M ZnSO4 + 0.1 M MnSO4), the local pH-value change during operation is visualized in operando. The overall pH value was found to increase during cycling whereas a major temporary pH drop in close proximity of the manganese dioxide electrode surface occurs. Additionally, this pH value change was quantified locally by in operando measurements with a pH micro electrode. Different electrolyte compositions with additives (sodium dodecyl sulfate (SDS), sulfuric acid (H2SO4)) and operation voltages were tested. The pH-potential-diagrams of manganese and zinc reveal pH value and potential limits, leading to active material dissolution at lower pH values and oxygen gas evolution at higher potentials >1.7 V. The procedure of combining a pH indicator, pH microelectrode measurements and pH-potential diagrams can be seen as an appropriate method to determine the recommendable working window of aqueous batteries.
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    Plasmonic gratings from highly doped Ge1-ySny films on Si
    (2021) Berkmann, Fritz; Ayasse, Markus; Schlipf, Jon; Mörz, Florian; Weißhaupt, David; Oehme, Michael; Prucnal, Slawomir; Kawaguchi, Yuma; Schwarz, Daniel; Fischer, Inga Anita; Schulze, Jörg
    Plasmonic modes in metal structures are of great interest for optical applications. While metals such as Au and Ag are highly suitable for such applications at visible wavelengths, their high Drude losses limit their usefulness at mid-infrared wavelengths. Highly n-doped Ge1-ySny alloys are interesting possible alternative materials for plasmonic applications in this wavelength range. Here, we investigate the use of highly n-doped Ge1-ySny films grown directly on Si by molecular beam epitaxy with varying Sn-content from 0% up to 7.6% for plasmonic grating structures. We compare plasma wavelengths and relaxation times obtained from electrical and optical characterization. While theoretical considerations indicate that the decreasing effective mass with increasing Sn content in Ge1-ySny films could improve performance for plasmonic applications, our optical characterization results show that the utilization of Ge1-ySny films grown directly on Si is only beneficial if material quality can be improved.
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    Towards sustainable sulfide‐based all‐solid‐state‐batteries : an experimental investigation of the challenges and opportunities using solid electrolyte free silicon anodes
    (2024) Neumann, Tobias; Alexander Dold, Lukas; Thomas Cerny, Alain; Tröster, Eric; Günthel, Michael; Fischer, Anna; Peter Birke, Kai; Krossing, Ingo; Biro, Daniel
    Silicon is one of the most promising anode active materials for future high–energy lithium‐ion‐batteries (LIB). Due to limitations related to volume changes during de-/lithiation, implementation of this material in commonly used liquid electrolyte‐based LIB needs to be accompanied by material enhancement strategies such as particle structure engineering. In this work, we showcase the possibility to utilize pure silicon as anode active material in a sulfide electrolyte‐based all‐solid‐state battery (ASSB) using a thin separator layer and LiNi0.6Mn0.2Co0.2O2 cathode. We investigate the integration of both solid electrolyte blended anodes and solid electrolyte free anodes and explore the usage of non‐toxic and economically viable solvents suitable for standard atmospheric conditions for the latter. To give an insight into the microstructural changes as well as the lithiation path inside the anode soft X‐ray emission and X‐ray photoelectron spectroscopy were performed after the initial lithiation. Using standard electrochemical analysis methods like galvanostatic cycling and impedance spectroscopy, we demonstrate that both anode types exhibit commendable performance as structural distinctions between two‐dimensional and three‐dimensional interfaces became evident only at high charge rates (8 C).