04 Fakultät Energie-, Verfahrens- und Biotechnik
Permanent URI for this collectionhttps://elib.uni-stuttgart.de/handle/11682/5
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Item Open Access Temperature reduction as operando performance recovery procedure for polymer electrolyte membrane fuel cells(2024) Zhang, Qian; Schulze, Mathias; Gazdzicki, Pawel; Friedrich, Kaspar AndreasTo efficiently mitigate the reversible performance degradation of polymer electrolyte membrane fuel cells, it is crucial to thoroughly understand recovery effects. In this work, the effect of operando performance recovery by temperature reduction is evaluated. The results reveal that operando reduction in cell temperature from 80 °C to 45 °C yields a performance recovery of 60-70% in the current density range below 1 A cm-2 in a shorter time (1.5 h versus 10.5 h), as opposed to a known and more complex non-operando recovery procedure. Notably, the absolute recovered voltage is directly proportional to the total amount of liquid water produced during the temperature reduction. Thus, the recovery effect is likely attributed to a reorganization/rearrangement of the ionomer due to water condensation. Reduction in the charge transfer and mass transfer resistance is observed after the temperature reduction by electrochemical impedance spectroscopy (EIS) measurement. During non-operando temperature reduction (i.e., open circuit voltage (OCV) hold during recovery instead of load cycling) an even higher recovery efficiency of >80% was achieved.Item Open Access Wetting behavior of aprotic Li-air battery electrolytes(2021) Kube, Alexander; Bienen, Fabian; Wagner, Norbert; Friedrich, Kaspar AndreasThe open architecture of cathodes in Li–air batteries implies the need for open porosity with adequate pore size distribution and surface energy optimization with regard to the electrolyte. The interaction of liquid and cathode material, especially the wetting properties, which depend on cathode material, roughness and porosity, and electrolyte properties, needs to be understood properly to avoid flooding and assure high active areas. In this work, contact angle goniometry, capillary rise method, and pressure saturation curves are used to investigate the wetting properties of dimethyl sulfoxide (DMSO), tetraethylene glycol dimethyl ether (Tetraglyme), a 1:1 mixture of ethylene carbonate and dimethyl carbonate (EC:DMC) and water on a gas diffusion layer (GDL) Sigracet 39BC, and a pure flat polytetrafluorethylene (PTFE) foil. Contact angle measurement shows that all three organic solvents wet the GDL hydrophobic agent PTFE. Capillary rise measurements show that all sample liquids slowly imbibe into the porous network. While for Tetraglyme an efficient penetration is limited by the high viscosity, water flow rate is slowed down by the hydrophobic pore network of the GDL. Pressure saturation curves for DMSO, Tetraglyme, and EC:DMC can be obtained for the first time and are compared with the water pressure saturation curve.Item Open Access Advanced impedance analysis for performance degradation during low-temperature CO2 electroreduction(2024) Chen, Qinhao; Kube, Alexander; Kopljar, Dennis; Friedrich, Kaspar AndreasElectrochemical impedance spectroscopy (EIS) is a powerful tool commonly used to study electrochemical systems. Nevertheless, its application in CO2 electroreduction has been so far limited due to its complex reaction mechanism and environment. Although initial findings have demonstrated the viability of applying EIS analysis in CO2 electrolyzers, the assignment of individual processes in the impedance spectra remains ambiguous. Therefore, a more detailed investigation, especially focused on its application in evaluating degradation mechanisms, is essential. In this study, a stable gas diffusion electrode (GDE) system was developed for a comprehensive EIS and distribution of relaxation time (DRT) evaluation to assess key degradation mechanisms under accelerated stress conditions such as high current density and low operating temperature. Validated by post-mortem analysis and complementary methods, we demonstrate the viability of this approach for operando monitoring of CO2 electroreduction by assigning individual mechanistic processes in the GDE and linking them to performance degradation over time.Item Open Access Elucidating the performance limitations of alkaline electrolyte membrane electrolysis : dominance of anion concentration in membrane electrode assembly(2020) Razmjooei, Fatemeh; Farooqui, Azharuddin; Reissner, Regine; Gago, Aldo Saul; Ansar, Syed Asif; Friedrich, Kaspar AndreasAnion exchange membrane water electrolyzers (AEMWEs) offer a cost‐effective technology for producing green hydrogen. Here, an AEMWE with atmospheric plasma spray non‐precious metal electrodes was tested in 0.1 to 1.0 M KOH solution, correlating performance with KOH concentration systematically. The highest cell performance was achieved at 1.0 M KOH (ca. 0.4 A cm-2 at 1.80 V), which was close to a traditional alkaline electrolysis cell with ≈6.0 M KOH. The cell exhibited 0.13 V improvement in the performance in 0.30 M KOH compared with 0.10 M KOH at 0.5 A cm−2. However, this improvement becomes more limited when further increasing the KOH concentration. Electrochemical impedance and numerical simulation results show that the ohmic resistance from the membrane was the most notable limiting factor to operate in low KOH concentration and the most sensitive to the changes in KOH concentration at 0.5 A cm-2. It is suggested that the effect of activation loss is more dominant at lower current densities; however, the ohmic loss is the most limiting factor at higher current densities, which is a current range of interest for industrial applications.Item Open Access A segmented cell measuring technique for current distribution measurements in batteries, exemplified by the operando investigation of a Zn-air battery(2021) Kube, Alexander; Meyer, Jens; Kopljar, Dennis; Wagner, Norbert; Friedrich, Kaspar AndreasA transimpedance amplifier circuit as well as an instrumental amplifier circuit were used to measure current densities of a zinc-air battery with an integrated segmented current collector foil. Error calculation showed that the transimpedance amplifier is superior to the used instrumental amplifier, but both methods provide valuable and consistent results. They both showed comparable results with operando insight into the current distribution of the battery. The knowledge about those distributions is essential to avoid fast degradation of battery materials and irreversible capacity loss due to heterogeneous dissolution of the anode during discharge. In this work we showed that oxygen starvation as well as gas flow rate leads to large current gradients. It was also demonstrated that heterogeneous current distributions on cathode side induces also a heterogenous dissolution behavior on the anode, resulting in irreversible capacity loss.Item Open Access Scalable fabrication of multi-layered Cu-based electrodes via solvent-free method for the selective electrochemical conversion of CO2 to C2+ products(2024) Chen, Qinhao; Kube, Alexander; Rana, Bhawna; Biswas, Indro; Morawietz, Tobias; Kopljar, Dennis; Friedrich, Kaspar AndreasIn the research field of CO2 electroreduction, gas diffusion electrodes (GDEs) are predominantly manufactured through solvent-based processes. Meanwhile, the solvent-free method has gained heightened attention due to its potential to reduce operational and production expenses, while considering ecological aspects such as solvent evaporation, circulation, and waste treatment. Drawing from its successful applications in other fields, we have specifically developed a solvent-free manufacturing method to produce multi-layered Cu-based GDEs for CO2 electroreduction. The procedure is compatible with industrial production lines, specifically through a roll-to-roll process. By evaluating the interplay between production parameters and electrochemical performance of GDEs via various characterization methods, key factors, i.e., hydrophobicity, gas permeability, thickness, and pore size, were adjusted and applied to achieve a highly selective GDE towards C2+ products (alcohols and ethylene) at industrial relevant currents up to 300 mA cm-2 (ethylene ∼40%, ethanol ∼10%, n-propanol ∼15%).Item Open Access Investigation of the degradation phenomena of a proton exchange membrane electrolyzer stack by successive replacement of aged components in single cells(2025) Kimmel, Benjamin; Morawietz, Tobias; Biswas, Indro; Sata, Noriko; Gazdzicki, Pawel; Gago, Aldo Saul; Friedrich, Kaspar AndreasDue to their compactness and high flexibility to operate under dynamic conditions, proton exchange membrane water electrolyzers (PEMWEs) are ideal systems for the production of green hydrogen from renewable energy sources. For the widespread implementation of PEMWEs, an understanding of their degradation mechanism is crucial. In this work, we analyze a commercial PEMWE stack via a novel approach of breaking down from the stack to the single-cell level. Therefore, the disassembled stack components are cut to fit into single cells. Then, the aged components are successively replaced with pristine or regenerated components (cleaned and polished), and electrochemical characterizations are conducted to investigate the contributions of the individual components on performance losses. In addition, several underlying degradation phenomena are identified using different physical ex-situ analysis methods. The catalyst-coated membrane (CCM) contributes the most to performance degradation because of contamination and ionomer rearrangement. Additionally, traces of calcium, likely due to insufficient water purification used during operation or for cleaning the cell components, were found. Significant oxidation was observed on the anodic components, while the electronic conductivity on the cathode side remained unchanged. The combination of electrochemical characterization with stepwise regeneration processes and physical ex-situ analysis allows to draw conclusions about the impact of different components on degradation and to analyze the underlying aging mechanisms occurring in each component.