04 Fakultät Energie-, Verfahrens- und Biotechnik
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Item Open Access Behavior of sulfur oxides in air and oxy-fuel combustion(2019) Spörl, Reinhold; Scheffknecht, Günter (Univ.-Prof. Dr. techn.)This thesis evaluates the behavior of sulfur oxides in pulverized fuel (PF) fired air and oxy-fuel systems. Sulfur oxides are responsible for certain operational problems and considerable gas cleaning requirements in air as well as oxy-fuel firing. A better understanding of the related issues will allow for a technical and economical optimization of the oxy-fuel combustion technology. A range of experimental investigations studying the stability and retention of sulfur oxides in ashes and deposits, acid gas (SO2, SO3, and HCl) control in air and oxy-fuel combustion by dry sorbent injection, and SO3 formation were conducted. The experimental work is in parts supported by theoretical considerations and thermodynamic equilibrium simulation. Studies for different coals and lignites showed that in practically relevant oxy-fuel configurations the exclusion of airborne N2 from combustion leads to an increase of the SO2 concentrations in oxy-fuel, compared to air firing, by a factor of about 3.4 to 4.2, referring to dry, and of about 2.9 to 3.5, when referring to wet flue gas conditions. The increased SO2 levels in oxy-fuel combustion are responsible for an increased stability of sulfates in oxy-fuel power boiler systems so that for example the decomposition temperature CaSO4 rises by about 50 to 80 °C, depending on flue gas atmospheres. The enhanced stability of sulfates in deposits at high temperatures when operating with increased SO2 levels was experimentally demonstrated. Compared to air firing, a considerable increase of the sulfur retention in the ash by 10 to 12 percentage points has been observed for oxy-fuel recycle combustion of Lusatian lignites. This leads to lower SO2 emissions and higher SO3 levels in process ashes and deposits. The results indicate that for fuels, such as the used lignites, the temperature level at which fouling by sulfatic deposits is problematic may be shifted to higher temperatures in oxy-fuel combustion and that the sintering of deposits by sulfation may be more pronounced. In contrast, in air and oxy-fuel combustion experiments with a hard coal with a low sulfur retention potential differences in the SO3 contents and degrees of sulfation of ashes and deposits were small. Besides higher SO3 contents and sulfation degrees, no other significant changes between the deposit samples from air and oxy-fuel combustion were identified. Experiments on dry sorbent injection in air and oxy-fuel mode showed that an increase of the average flue gas residence time in the furnace by flue gas recirculation and, to a lesser extent, the higher sulfate stability enhance the desulfurization efficiency in oxy-fuel recycle combustion considerably. SO2 capture efficiencies in oxy-fuel recycle combustion of 50 % to more than 80 % at moderate molar sulfur to calcium ratios between 1.7 and 2.9 were reached, when injecting CaCO3 and Ca(OH)2 together with the fuel or directly to the furnace. Under comparable injection conditions, the oxy-fuel performance was by as much as 29 percentage points higher than in air firing. Also an efficient SO3 and HCl control by DSI could be demonstrated. Experiments on formation of SO3 show that higher SO2 levels in oxy-fuel firing are the most important parameter responsible for the observed increase of the SO3 concentrations.Item Open Access Construction of robust Escherichia coli strains for large-scale production(2022) Ziegler, Martin; Takors, Ralf (Prof. Dr.-Ing.)The biotechnical production of many fine chemicals, proteins or pharmaceuticals depends on large-scale microbial cultivations. Due to limited mixing, heterogeneities in process relevant parameters such as nutrient concentrations arise in such fermentations. Escherichia coli (E. coli) is a model organism frequently used in the biotechnological industry. If E. coli is cultivated under heterogeneous conditions, biological reactions of the microorganism result in reduced process performance. Since large-scale fermentations are not economically feasible in academic settings, scale-down reactors that mimic aforementioned heterogeneities are used to investigate heterogenous fermentations. Previous studies in scale-down reactors unraveled that, depending on the process strategy, the unstable supply of a limiting primary carbon or nitrogen source such as glucose or ammonium is one of the underlying causes of process performance loss. Low concentrations of glucose or ammonium elicit the stringent response as a biological starvation reaction which comprises extensive transcriptional reactions. In the first project that contributes to this thesis, the regulatory and transcriptional reactions of the strains E. coli MG1655 and E. coli SR to repeated exposure to ammonium starvation zones were examined in a scale-down reactor. The scale-down reactor followed a two-compartment approach and consisted of a stirred tank reactor and a plug-flow reactor simulating passage through a starvation zone. E. coli SR is a strain with modulated stringent response. It was observed that short-term starvation stimuli do not trigger this regulatory program in E. coli SR and the transcriptional reaction was noticeably reduced. Long-term adaptation of the strain to repeated cycles of limitation and starvation also clearly differed from E. coli MG1655. Despite lack of the stringent response, E. coli SR showed no deficits in the assimilation of the limiting ammonium or in biomass yield on ammonium. In the second project of this thesis, a series of deletion strains with robust phenotype against glucose starvation zones were constructed. Candidate genes were identified and successively removed from the genome of E. coli MG1655 by Recombineering. The fundamental growth parameters of the strains were determined in shaking flask fermentations and no noticeable differences compared to E. coli MG1655 were found. Chemostat cultivations in a scale-down reactor with glucose as the limiting nutrient source revealed that the final strain of the deletion series, E. coli RM214, had a significantly lower maintenance coefficient under heterogeneous conditions than E. coli MG1655. Moreover, in an exemplary heterologous protein productionscenario E. coli RM214 rhaB- pJOE4056.2_tetA proved to be more robust to heterogeneities and showed a significantly higher product yield than E. coli MG1655 rhaB- pJOE4056.2_tetA. In the third project of this thesis, the production of pyruvate in E. coli MG1655 by inhibition of pyruvate dehydrogenase through CRISPR interference was investigated. A central goal was to achieve the stable production in nitrogen-limited conditions. For this, different target sequences in the operon pdhR-aceEF-lpd were tested and the strains cultivated in shaking flask fermentations. All tested target sequences were generally suitable to trigger the accumulation of pyruvate. Combined CRISPR interference against two target sequences did not lead to an increased pyruvate yield in most cases. In addition, the strains E. coli MG1655 pdCas9 psgRNA_aceE_234 and E. coli MG1655 pdCas9 psgRNA_aceE_234_pdhR_329 were characterized in two phase fermentations in lab-scale reactors. The initial phase was an unlimited exponential growth phase and was followed by an ammonium-limited production phase. E. coli MG1655 pdCas9 psgRNA_aceE_234 only produced pyruvate during the exponential phase, and reuptake of pyruvate occurred in the second phase. In contrast, E. coli MG1655 pdCas9 psgRNA_aceE_234_pdhR_329 stably produced pyruvate during the exponential and the ammonium-limited phase and is a potential chassis strain for the growth-decoupled production of pyruvate derived bioproducts. The overarching research issues of the projects were the characterization of strains in heterogeneous conditions and the development of new strategies to improve their performance. The collected data leads me to conclude that the construction of robust microbial strains for large-scale applications is both expedient and feasible. Tailored genetic modifications are the method of choice to achieve this goal. Furthermore, suitable genetic constructs offer promising possibilities for the stable growth-decoupled production of chemicals in nitrogen-limited conditions.Item Open Access Messung und Modellierung der effektiven Wärmeleitfähigkeit von Dämmstoffschüttungen für vakuumwärmegedämmte Warmwasserspeicher(2022) Lang, Stephan; Spindler, Klaus (apl. Prof. Dr.-Ing.)Das Ziel dieser Arbeit ist es, hinsichtlich Dämmwirkung und Kosten geeignete schüttfähige Wärmedämmstoffe für doppelwandige Warmwasserspeicher mit Vakuumwärmedämmung zu identifizieren und eine Vorhersage über die effektive Wärmeleitfähigkeit in Abhängigkeit von Luftdruck und Temperatur treffen zu können. Zu diesem Zweck werden expandierte Perlite unterschiedlicher mittlerer Korngrößen und Mischungen aus expandierten Perliten und pyrogener Kieselsäure untersucht. Schwerpunkt der Untersuchungen ist die Ermittlung der effektiven Wärmeleitfähigkeit bei unterschiedlichen Luftdrücken und Temperaturen. Die effektive Wärmeleitfähigkeit wird in einer eigens entwickelten Versuchsanlage, nach einem stationären Messprinzip, bei Luftdrücken zwischen 0,001 mbar und Atmosphärendruck von (960 ± 20) mbar sowie bei Probenmitteltemperaturen zwischen -5 °C und 90 °C bestimmt. Die maximale relative Messunsicherheit der Versuchsanlage beträgt < 8 % bei den geringsten und < 3 % bei den höchsten gemessenen effektiven Wärmeleitfähigkeiten. Reine feinkörnige expandierte Perlite mit Dichten der Schüttungen ≥ 182 kg/m³ erreichen bei Luftdrücken ≤ 0,1 mbar und allen gemessenen Probenmitteltemperaturen die geringsten effektiven Wärmeleitfähigkeiten. Bei einer Probenmitteltemperatur von 48 °C liegen diese bei ≤ 4,84 mW/(m·K). Mischungen aus einem vergleichsweise grobkörnigen expandierten Perlit mit einer sehr feinkörnigen und feinporigen pyrogenen Kieselsäure können hingegen, bei technisch einfacher zu handhabenden Luftdrücken von > 1 mbar, z. T. geringere effektive Wärmeleitfähigkeiten erreichen als reine expandierte Perlite. Mischungen dieser Komponenten werden in dieser Arbeit erstmals in Form einer losen Schüttung bzgl. ihrer effektiven Wärmeleitfähigkeit untersucht. Bei einer Probenmitteltemperatur von 48 °C werden in diesem Luftdruckbereich effektive Wärmeleitfähigkeiten dieser Mischungen von > 12,17 mW/(m·K) gemessen. Anhand der gemessenen effektiven Wärmeleitfähigkeiten sowie weiterer Stoffeigenschaften, werden vollständig prädiktive analytische Modelle der effektiven Wärmeleitfähigkeit entwickelt. Das Modell für Mischungen gilt für ein ausgewähltes Stoffpaar, während das Modell für expandierte Perlite für beliebige ungemahlene expandierte Perlite verwendbar ist. Es handelt sich nach Kenntnis des Autors um das erste vollständig prädiktive analytische Modell der effektiven Wärmeleitfähigkeit für expandierte Perlite, welches auch die Kopplung von Gas- und Festkörperwärmeleitung berücksichtigt und für welches lediglich drei einfach und kostengünstig zu messende Größen bestimmt werden müssen. Diese Größen sind der volumengewichtet gemittelte Korndurchmesser, die mittlere Korndichte sowie die Dichte der Schüttung des expandierten Perlits. Aus den Messwerten der effektiven Wärmeleitfähigkeit wird ein Zusammenhang von volumengewichtet gemitteltem Korndurchmesser zur Kopplung von Gas- und Festkörperwärmeleitung deutlich, der für das Modell für expandierte Perlite verwendet wird. Mit den Modellen ist es nun möglich, ohne entsprechende Messungen, die effektive Wärmeleitfähigkeit von Mischungen aus einem expandierten Perlit und einer pyrogenen Kieselsäure sowie für beliebige ungemahlene expandierte Perlite, mit zufriedenstellender bis hoher Genauigkeit vorherzusagen.Item Open Access Development of novel bispecific antibodies for cancer therapy targeting the receptor tyrosine kinases HER4 and EGFR(2024) Kühl, Lennart; Kontermann, Roland E. (Prof. Dr.)In this study, novel mono- and bispecific antibodies targeting the ErbB receptor family members EGFR and HER4 were investigated. Dual targeting of EGFR and HER4 by a bispecific, tetravalent antibody comprising a novel, antagonistic HER4-targeting antibody showed inhibition of proliferation and migration for a HB-EGF-stimulated ovarian cancer cell line. No inhibitory effects in a breast cancer cell line expressing EGFR and HER4 indicated that successful dual targeting does not solely rely on target expression. The complexity of HER4 with its isoforms and their different signaling properties makes HER4 a challenging cancer target that needs further in-depth research. To overcome resistances based on escape mutations located in the epitopes of clinically approved antibodies, novel antagonistic EGFR-targeting antibodies binding to a different epitope were developed. This epitope was mapped to domain III of EGFR and binding to clinically relevant EGFR ectodomain mutations resulted in inhibition of EGFR signaling in stable cell lines used as test systems. Favorable activities in comparison to clinically approved antibodies regarding inhibition of EGFR signaling and proliferation were observed for cancer cell lines expressing the EGFR wildtype. Bispecific T-cell engagers can lead to a T-cell mediated target cell killing independent of intracellular downstream signaling in the cancer cell. One challenge for the applicability of T-cell engagers in solid tumors is to keep the balance between T-cell mediated tumor cell killing and severe side-effects caused by a systemic activation of the immune system. Studies on eleven different eIg-based formats for EGFR-binding T-cell engagers showed that valency, geometry, and size influenced their activity profile. Furthermore, one bivalent and one trivalent, bispecific format were investigated for two novel EGFR-targeting moieties. As these molecules bind to clinically relevant escape mutations located in the ectodomain of EGFR, they are expected to show activity in patients with an acquired resistance to approved EGFR-targeting antibodies. These molecules led to a robust T-cell mediated cytotoxicity of cancer cells expressing EGFR. Additionally, benefits regarding an EGFR-level dependent cytotoxicity were observed for reduced binding to EGFR. An initial in vivo study using surrogate molecules in a syngeneic mouse model showed reduction of tumor growth and prolonged survival for treatment with a trivalent, bispecific T-cell engager comprising a novel EGFR-binding moiety. Taken together, beneficial effects of the novel molecules may contribute to improved therapies for patients with both pre-existing and acquired resistances to EGFR-targeting antibodies.Item Open Access Insights into the structural and functional properties of the eukaryotic porin Tom40(2012) Gessmann, Dennis; Nußberger, Stephan (Prof. Dr.)Tom40 forms the preprotein conducting channel in the outer membrane of mitochondria enabling transport of up to 1500 different preproteins through an optimized pore environment. Moreover, Tom40 exhibits a voltage-dependent gating mechanism in terms of an ‘electrical switch’ making this eukaryotic beta-barrel a promising target for nanopore based applications. In this work, new bioinformatics methods were developed and verified through practical approaches to shed light on the structural elements of Tom40 facilitating its particular function in mitochondria. Based on these results, Tom40 proteins were designed with modified and optimized structural properties. TmSIP, a physical interaction model developed for TM beta-barrel proteins, was used to identify weakly stable regions in the TM domain of Tom40 from mammals and fungi. Three unfavorable beta-strands were determined for human Tom40A. Via CD and Trp-fluorescence spectroscopy it was shown that substitution of key amino acid residues in theses strands resulted in an improved resistance of the protein to chemical and thermal perturbations. Further, the mutated form of hTom40A was strictly found in its monomeric state. Equal improvements were gained for the apparent stability of Tom40 from Aspergillus fumigatus. Tom40 was isolated and purified in its native state from Neurospora crassa mitochondria. Time-limited proteolysis of native NcTom40 coupled to mass spectrometry revealed comparable protease-accessibility to VDAC isoform 1 from mammals suggesting a similar fold. Thus, a homology model of NcTom40 was developed on the basis of the solved mouse VDAC-1 crystal structure. It was found that Tom40 forms a 19-stranded beta-barrel with an N-terminal alpha-helix inside the pore. Further, a conserved ‘polar slide’ in the pore interior is possibly involved in preprotein translocation and a second conserved domain, termed ‘helix anchor region’, in arresting the helix inside the Tom40 pore. Based on the homology model of NcTom40, the structure and function of the N-terminal domain of Tom40 was addressed. Examination of the model structure revealed two different domains for the N-terminus, the inner-barrel and outer-barrel N-terminus. In vivo investigations showed that both parts prevent a heat-induced dysfunction of Tom40 in N. crassa mitochondria independently. By applying CD spectroscopy the predicted N-terminal alpha-helix could be allocated to the inner-barrel N-terminus. Further, in combination with Trp-fluorescence spectroscopy it was found that the N-terminal alpha-helix unfolds independently from the Tom40 beta-barrel, but is not necessary for pore stability or integrity. However, a conserved amino acid residue, Ile47 of NcTom40, in the inner-barrel N-terminus is essential for the structural integrity of the N-terminal alpha-helix. In conclusion, these results may offer a basis for future works on TM beta-barrel proteins with the aim to alter the structural properties in the absence of a high atomic resolution structure or an established knowledge of the biochemical and biophysical properties.Item Open Access Wege zur Ermittlung von Energieeffizienzpotenzialen von Informations- und Kommunikationstechnologien(Stuttgart : Universität Stuttgart, Institut für Energiewirtschaft und Rationelle Energieanwendung, 2020) Miller, Michael; Hufendiek, Kai (Prof. Dr.-Ing.)Item Open Access Membrane electrode assembly for water electrolysis(2023) Nguyen, Thi Hai Van; Friedrich, K. Andreas (Prof. Dr. rer. nat.)Maintaining a sufficient energy supply while minimizing the impact on the environment and climate is one of the greatest social and scientific challenges of our times. There are various fields of research and technological developments in the context of global warming and limitless growing energy demand, and the focus of this PhD programme is on artificial photosynthesis, more specifically on the assembly of Membrane electrode assembly for water electrolyzer part. Mimicking photosynthesis in a scheme to trap solar energy in chemical bonds (fuels) is a scientific and technological challenge. Having a cost-effective and reliable process stays one of the main limitations in order to achieving the long-term goal of this approach. In this work, within the European eSCALED project, the elaboration of Membrane Electrode Assembly (MEA) for water electrolysis by introducing new materials and low-cost fabrication methods was investigated.Item Open Access Development of hydrodynamic density functional theory for mixtures and application to droplet coalescence(Stuttgart : Universität Stuttgart, Institut für Technische Thermodynamik und Thermische Verfahrenstechnik, 2021) Stierle, Rolf; Groß, Joachim (Prof. Dr.-Ing.)Predicting accurately coalescence phenomena is critical to the accurate description of the hydrodynamics of fluids and their mixtures. A promising framework for the development of models for such phenomena is dynamic density functional theory. Dynamic density functional theory enables the analysis of dynamical processes in inhomogeneous systems of pure fluids and fluid mixtures at the molecular level. In this work, a hydrodynamic density functional theory model for mixtures in conjunction with Helmholtz energy functionals based on the PC-SAFT equation of state is proposed, that obeys the first and second law of thermodynamics and simplifies to the isothermal Navier-Stokes equation for homogeneous systems. The hydrodynamic density functional theory model is derived from a variational principle and accounts for both viscous forces and diffusive molecular transport. A Maxwell-Stefan model is applied for molecular transport. This work identifies a suitable expression for the driving force for molecular diffusion of inhomogeneous systems that captures the effect of interfacial tension. The proposed hydrodynamic density functional theory is a non-local theory that requires the computation of weighted (spatial averaged) densities around each considered spatial coordinate by convolution, which is computationally expensive. This work uses Fourier-type transforms to determine the weighted densities. A pedagogical derivation is presented for the efficient computation of the convolution integrals occurring in the Helmholtz energy functionals in Cartesian, cylindrical, and spherical coordinates on equidistant grids using fast Fourier and similar transforms. The applied off-the-shelf algorithms allow to reduce dimensionality and complexity of many practical problems. Furthermore, an algorithm for a fast first-order Hankel transform is proposed, allowing fast and easy density functional theory calculations in rotationally symmetric systems. Application of the hydrodynamic density functional theory model using a well-balanced finite-volume scheme to one-dimensional droplet and bubble coalescence of pure fluids and binary mixtures is presented. The required transport coefficients, shear viscosity and Maxwell-Stefan diffusion coefficients, are obtained by applying entropy scaling to inhomogeneous fluids. The considered systems show a qualitative difference in the coalescence characteristics of droplets compared to bubbles. This constitutes a first step towards predicting the phase rupture leading to coalescence using dynamic density functional theory.Item Open Access A model-based framework for the assessment of energy-efficiency and CO2-mitigation measures in multi-cylinder paper drying(Stuttgart : Universität Stuttgart, Institut für Energiewirtschaft und Rationelle Energieanwendung, 2022) Godin, Hélène; Radgen, Peter (Prof. Dr.-Ing.)Thesis on the effect of energy-efficiency and CO2-mitigation measures in multi-cylinder paper drying.Item Open Access Brennstoffzellensysteme auf Basis regenerativer Energieträger(2010) Grüner, Heike; Scheffknecht, G. (Prof. Dr. techn.)Der Einsatz von regenerativen Energieträgern in Brennstoffzellensystemen ermöglicht eine beachtliche Reduzierung von Treibhausgasemissionen im Vergleich zur konventionellen Strom- und Wärmegewinnung. Im Rahmen dieser Arbeit wurde der am besten geeignete, nicht-leitungsgebundene regenerative Energieträger für ein stationäres PEM-Brennstoffzellen-BHKW identifiziert und ein ursprünglich auf Erdgas basierendes Gesamtsystem mit diesem Energieträger charakterisiert. Als leicht speicherbare Energieträger kommen dabei Methanol, Ethanol und Dimethylether (DME) sowie Pflanzenöl, Biodiesel und flüssige synthetische Kohlenwasserstoffe in Frage. Aus diesen wurden Methanol, Ethanol und DME vorselektiert und hinsichtlich der Brennstoffherstellung (Well-to-Tank-Wirkungsgrad) und -reformierung sowie der simulierten Gesamtsystemeffizienz und -komplexität bewertet. Bei vergleichbaren Werten in der Brennstoffherstellung sowie in der Systemeffizienz lässt sich dabei die Aussage treffen, dass grundsätzlich alle drei genannten Brennstoffe für ein stationäres PEM-Brennstoffzellen-BHKW geeignet sind. Die geringe Systemkomplexität sowie die einfache Dampfreformierung von DME führten zu dessen Auswahl als dem am besten geeigneten, nicht-leitungsgebundenen regenerativen Energieträger für ein stationäres Brennstoffzellensystem. Anschließend erfolgten die Charakterisierung des Gesamtsystems im DME-Betrieb sowie der Vergleich des Systems im Betrieb mit Erdgas. Erdgas diente dabei als Ersatz für biogenes Erdgassubstitut (SNG), welches stellvertretend für den Einsatz leitungsgebundener regenerativer Energieträger steht.