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Institute: search.filters.UBSInstitut.Institut für Technische ChemieSubject: search.filters.subject.620

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    ItemOpen Access
    CHEMampere : technologies for sustainable chemical production with renewable electricity and CO2, N2, O2, and H2O
    (2022) Klemm, Elias; Lobo, Carlos M. S.; Löwe, Armin; Schallhart, Verena; Renninger, Stephan; Waltersmann, Lara; Costa, Rémi; Schulz, Andreas; Dietrich, Ralph‐Uwe; Möltner, Lukas; Meynen, Vera; Sauer, Alexander; Friedrich, K. Andreas
    The chemical industry must become carbon neutral by 2050, meaning that process‐, energy‐, and product‐related CO2 emissions from fossil sources are completely suppressed. This goal can only be reached by using renewable energy, secondary raw materials, or CO2 as a carbon source. The latter can be done indirectly through the bioeconomy or directly by utilizing CO2 from air or biogenic sources (integrated biorefinery). Until 2030, CO2 waste from fossil‐based processes can be utilized to curb fossil CO2 emissions and reach the turning point of global fossil CO2 emissions. A technology mix consisting of recycling technologies, white biotechnology, and carbon capture and utilization (CCU) technologies is needed to achieve the goal of carbon neutrality. In this context, CHEMampere contributes to the goal of carbon neutrality with electricity‐based CCU technologies producing green chemicals from CO2, N2, O2, and H2O in a decentralized manner. This is an alternative to the e‐Refinery concept, which needs huge capacities of water electrolysis for a centralized CO2 conversion with green hydrogen, whose demand is expected to rise dramatically due to the decarbonization of the energy sector, which would cause a conflict of use between chemistry and energy. Here, CHEMampere's core reactor technologies, that is, electrolyzers, plasma reactors, and ohmic resistance heating of catalysts, are described, and their technical maturity is evaluated for the CHEMampere platform chemicals NH3, NOx, O3, H2O2, H2, CO, and CxHyOz products such as formic acid or methanol. Downstream processing of these chemicals is also addressed by CHEMampere, but it is not discussed here.
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    ItemOpen Access
    Renewable district energy systems with formic acid based hydrogen storage
    (2022) Lust, Daniel; Eicker, Ursula (Prof. Dr.)
    In zukünftigen Energiesystemen mit einem hohen Anteil fluktuierender Energieerzeugung durch Windkraft und Photovoltaik, wird Wasserstoff aus einer Elektrolyse eine zunehmend wichtige Rolle einnehmen. Die lokale Speicherung und der Transport von Wasserstoff sind jedoch technologisch herausfordernd. Eine vielversprechende Möglichkeit zur Wasserstoffspeicherung ist das Laden und Entladen eines Trägermoleküls, was oftmals eine drucklose Speicherung und die Verwendung bestehender Transportinfrastruktur erlaubt. Ameisensäure enthält 4.4 Gew.-% Wasserstoff, ist unter Umgebungsbedingungen flüssig und damit ein potentiell geeignetes Wasserstoffträgermolekül. Die zugrunde liegende Forschungsfrage dieser Arbeit ist, ob und unter welchen Voraussetzungen ameisensäurebasierte Wasserstoffspeicher für eine Anwendung als saisonaler Energiespeicher im Gebäudesektor geeignet sind. Ein Ziel dieser Arbeit ist die Modellierung ameisensäurebasierter Wasserstoffspeichersysteme. Es werden drei Systeme beschrieben mit jeweils den folgenden Hauptkomponenten: eine reversible Wasserstoffbatterie, Flussreaktoren für die Hin- und Rückreaktion von Wasserstoff zu Ameisensäure und ein CO2-Elektrolyseur für die direkte elektrochemische Reduktion von gasförmigem CO2 mit Wasser zu Ameisensäure. Die entwickelten Modelle wurden mit experimentellen Daten oder Literaturwerten validiert. Weiterhin werden Verfahren zur Dimensionierung dieser Systeme, zur Betriebsführung und zur Integration in bestehende Energiesysteme gezeigt. In einer Fallstudie werden verschiedene Leistungsparameter der drei Systeme, wie Wirkungsgrad, Platzbedarf und Systemkomplexität, bewertet und einem Referenzsystem gegenübergestellt. Es hat sich gezeigt, dass eine übertragbare, regelbasierte Dimensionierung der Systeme aufgrund der hohen Systemkomplexität unzureichend ist. Optimierungsverfahren, z.B. mit genetischen Algorithmen, könnten zu besseren Ergebnissen führen, setzen jedoch das Vorhandensein von Systemmodellen voraus. Die Fallstudie für ein Gebäudecluster hat ergeben, dass der CO2-Elektrolyseur insgesamt das am besten geeignete System für eine Anwendung als Energiespeicher ist. Die Zugänglichkeit flüssiger Ameisensäure ermöglicht einen einfachen Energietransport und die Reaktion läuft unter moderaten Bedingungen ab. Der CO2-Elektrolyseur wurde daraufhin detaillierter betrachtet und wesentliche Parameter für die Fallstudie optimiert. Durch hohe Überspannungen der Elektrolysezellen weist der CO2-Elektrolyseur jedoch einen geringen Gesamtwirkungsgrad auf, wodurch in der betrachteten Fallstudie kein wirtschaftlicher Betrieb möglich ist. Auch die Erhöhung der Eingangsleistung durch die Hinzunahme von Kleinwindkraftanlagen hat nur einen geringen Einfluss auf die Gesamtperformance des Systems. Weiterer Forschungsbedarf zur hardwareseitigen Verbesserung des CO2-Elektrolyseurs und zur Steuerung und Betriebsführung mit fluktuierender elektrischer Last ist demnach notwendig um den Wirkungsgrad zu erhöhen und einen wirtschaftlichen Einsatz des Systems als saisonaler Energiespeicher zu ermöglichen.
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    Novel test protocols and characterization techniques for OER based reversal tolerant PEFC anodes for automotive applications
    (2023) Bentele, Dominik; Klemm, Elias (Prof. Dr.-Ing.)
    In a world facing climate change, the application of low temperature polymer electrolyte fuel cells (PEFCs) for automotive and stationary applications gained major attention recently. In particular, commercialization advances are being made for their usage in medium and heavy-duty vehicles. Durability is a key aspect for commercial success of PEFCs. To resist reversal events originating from gross fuel (i.e. H2) starvation in affected cells, the introduction of oxygen evolution reaction (OER) co-catalysts to the PEFC anode has been established as material-based mitigation strategy. This work focuses on the development of test protocols and characterization techniques on single cell level to investigate iridium-based reversal tolerant PEFCs regarding performance and degradation. The first part of this thesis aims at techniques which are providing insights into reversal tolerance of OER based PEFCs. An accelerated stress test (AST) was developed investigating short-term recurring reversal operation to meet the expectations of automotive field application. An OER recovery effect, indicated by unaffected OER activity, was observed for short-term reversal events while normal operation caused PEFC failure. In addition, a significant dependence between hydrogen oxidation reaction (HOR) catalyst and reversal tolerance was found. Using further characterization methods such as hydrogen pump polarization curves, PEFC failure for short-term reversal events could be ascribed to hydrogen oxidation mass transfer increase originating from severe carbon corrosion and structural collapse within the anode catalyst layer. The electrochemical results were validated analyzing scanning electron microscope images (SEM). The second part of the thesis focuses on PEFC degradation by transient anode conditions originating from start-up/shut-down (SUSD) events. SUSD ASTs were developed to provoke substantial anode degradation while minimizing cathode degradation due to the so-called reverse-current effect. Advanced characterization methods to investigate the significant degradation of the HOR and OER catalyst were developed, uncovering a structural change of the anode catalyst layer and a substantial decline in reversal tolerance when PEFCs were exposed to SUSD events. In addition, characterization methods are presented to investigate the crossover of IrO2 based OER catalyst to the cathode catalyst layer, promoted by transient anode conditions. Iridium crossover was found to significantly impact the determination of electrochemical surface area (ECSA) for platinum-based catalysts by state-of-the-art characterization methods. The introduction of a voltage clipping step during SUSD events was showing to have a minor impact on anode degradation and iridium crossover. Using energy dispersive X-ray spectroscopy (EDX) and SEM imaging, the electrochemical degradation characteristics were substantiated.
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    Comprehensive characterization and evaluation of the process chain and products from Euphausia superba exocuticles to chitosan
    (2023) Hahn, Thomas; Egger, Jeannine; Krake, Simon; Dyballa, Michael; Stegbauer, Linus; Seggern, Nils von; Bruheim, Inge; Zibek, Susanne
    Antarctic krill (Euphausia superba) is a source for compounds of high nutritive value. Within that process of extraction, exocuticles (shells) accumulate which are currently disposed. A valorization of the compounds of the exocuticle such as chitosan would be beneficial to avoid waste and to obtain a versatile polymer at the same time. In contrast to previous investigations focusing on chitosan production from whole krill, we applied and optimized process stages of the chitosan production from the exocuticles, performing a comprehensive analytical evaluation of the whole process, the side streams and the products for the first time. Degreasing was the first step resulting in a krill oil yield of 6.2% using ethanol. The fatty acid profile exhibited high contents of phospholipids (21.2%). Citric acid offered a demineralization efficiency of 93%. Deproteinization investigation revealed 2 M NaOH and 90°C for 2.5 h to be the best parameters, resulting in a deproteinization efficiency of 99.9% and a chitin content of 92.8%. The spectroscopic investigation indicated that the chitin has a crystallinity index of 76% and an acetylation degree of 88%. The deacetylation degrees of the resulting chitosans is determined to be 74%-88%, the molecular weight ranges from 102 to 126 kDa.