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Mychinko, M. |
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Advanced Electron Tomography to Investigate the Growth and Stability of Complex Metal Nanoparticles = Geavanceerde Elektronentomografie om de Groei en Stabiliteit van Complexe Metallische Nanodeeltjes te Onderzoeken |
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Doctoral thesis |
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2024 |
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227 p. |
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Doctoral thesis; Electron microscopy for materials research (EMAT) |
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During the past decades, metallic nanoparticles (NPs) have attracted great attention in materials science due to their specific optical properties based on surface plasmon resonances. Because of these phenomena, plasmonic NPs (or nanoplasmonics) are very promising for application in biosensing, photocatalysts, medicine, data storage, solar energy conversion, etc. Currently, colloidal synthesis techniques enable scientists to routinely produce mono and bimetallic NPs of various shapes, sizes, composition, and elemental distribution, with superior properties for plasmonic applications. Two primary directions for further advancing nanoplasmonic-based technologies include synthesizing novel morphologies, such as highly asymmetric chiral NPs, and gaining deeper insights into the factors affecting the stability of produced nanoplasmonics. With the increasing complexity of nanoplasmonics morphologies and higher stability requirements, there is a pressing need for thorough investigations into their 3D structures and their evolution under different conditions, with high resolution. Electron tomography (ET) emerges as an ideal tool to retrieve shape and element-sensitive information about individual nanoparticles in 3D, achieving resolutions down to the atomic level. Moreover, ET techniques can be combined with in situ holders, enabling detailed studies of processes mimicking real applications of nanoplasmonic-based devices. The first part of this thesis will focus on detailed studies of chiral Au NPs, promising for spectroscopy techniques based on the differential absorption of left- and right-handed circularly polarized light. Specifically, I will discuss the primary strategies for wet-colloidal growth of the various types of intrinsically chiral Au NPs. Advanced ET methods will be demonstrated as powerful tools for characterizing the final helical morphologies of the produced Au NPs and for studying the chiral growth mechanisms by examining intermediate structures obtained during chiral growth. The second part will focus on the heat-induced stability of various Au@Ag core-shell NPs. Operating in real conditions, such as elevated temperatures, may cause particle reshaping and redistribution of metals between the core and shell, gradually altering nanoplasmonics properties. Hence, a thorough understanding of the influence of size, shape, and defects on these processes is crucial for further developments. Recently developed techniques, combining fast ET with in-situ heating holders, have allowed me to evaluate the influence of various parameters (size, shape, defect structure) on heat-induced elemental redistribution in Au@Ag core-shell nanoparticles qualitatively and quantitatively. Additionally, I will discuss the prospects of high-resolution ET for visualizing the diffusion of individual atoms within complex nanostructures. |
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UA @ admin @ c:irua:202976 |
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9001 |
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Schram, J. |
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Electrochemical sensing strategies for multiple illicit drugs |
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Doctoral thesis |
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2024 |
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290 p. |
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Doctoral thesis; Pharmacology. Therapy; Engineering sciences. Technology; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab) |
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Today, illicit drugs are omnipresent in society. Clandestine markets are growing faster than ever before, record amounts of cocaine are seized in seaports and airports, while the associated violence is spiralling out of control. In addition, drug monitoring centres worldwide are warning for the increasing complexity of the drug markets, as the traditionally popular drugs are joined by countless new synthetic variants, while medical drugs are also increasingly being abused. In order to provide services confronted with illicit drug samples (police, customs, forensic scientists, first responders, …) with important information on the identity of an unknown sample, suitable analytical tests are required. While these exist for laboratory environments, on-site applicable tests are important to accelerate the decision-making process. Electrochemical sensors have all the advantages required for such on-site tests: they are fast, portable, easy-to-use and reliable. Furthermore, they are not influenced by colours, which are frequently added to drug samples to deceive the existing tests. Previous work has mainly focussed on the detection of a single drug per analysis. However, many drugs could be encountered due to the diversity of the drug markets. Therefore, this project developed electrochemical strategies for the detection of multiple drugs simultaneously. First, the electrochemical behaviour of the individual drugs was studied in different measuring conditions (assessing the influence of pH, concentration and temperature). Then, all findings and strategies were combined to detect multiple targets simultaneously. An electrochemical sensor was developed for the four most popular drugs at music festivals: cocaine, MDMA, amphetamine and ketamine. This sensor generates a so-called ‘superfingerprint’ of the sample, which is then automatically interpreted by a developed algorithm in order to produce a straightforward output. Finally, a pill analysis sensor was developed in the context of drug checking services, where a consumer can anonymously have a sample chemically analysed to obtain information on the composition, dose and potentially harmful additives. The sensor achieved an outstanding accuracy in identifying the main component and provided the option to quantify, as well as an indication on the presence of other substances in the sample. The project’s findings demonstrate the potential for electrochemistry in illicit drug detection and provide a basis for the development of new sensors, targeting other drug combinations. |
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UA @ admin @ c:irua:203199 |
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9029 |
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Derks, K.; Youchaeva, M.; Van der Snickt, G.; Van der Stighelen, K.; Janssens, K. |
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Reconstructing Sweerts : practical insights into the historical dark halo technique based on paint reconstructions |
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P1 Proceeding |
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2024 |
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259-271
T2 - Alla maniera : technical art history |
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P1 Proceeding; Engineering sciences. Technology; Art; Antwerp Cultural Heritage Sciences (ARCHES); Antwerp X-ray Imaging and Spectroscopy (AXIS) |
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978-90-429-5216-4 |
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UA @ admin @ c:irua:203062 |
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9082 |
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Ahmadi Eshtehardi, H. |
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Combined computational-experimental study on plasma and plasma catalysis for N2 fixation |
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Doctoral thesis |
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2024 |
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160 p. |
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Doctoral thesis; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Humanity feels the urge of shifting to a sustainable society more than at any other time in its history. Electrification of chemical industry plays a key role in this transition. The possibility of producing fertilizers from air using renewable electricity, and simultaneously, no greenhouse gas emission, resulted in an increasing interest toward plasma technology as a solution for electrification of a part of the chemical industry in the past few years. Additionally, the activation of nitrogen molecules by vibrational and electronic excitation reactions in plasma can lead to an energy-efficient process. Last but not least, the modularity (fast on/off characteristic) of plasma technology makes it capable of using intermittent renewable electricity on site for the production of fertilizers using air. All these advantages offered by plasma technology make it a potential solution for the on-site production of fertilizers in small and decentralized plants using air and renewable electricity, which leads to a considerable reduction in fertilizer production and transportation costs. However, industrialization of plasma-based NF suffers from several challenges, including challenges of plasma catalysis for the selective production of desired species, the high energy cost of plasma-based NF compared to current industrial processes, and the design and development of scaled up and energy-efficient plasma reactors for industrial purposes. In the framework of this thesis we have tried to add to the state-of-the-art (SOTA) in plasma-based NOx production and deal with its limitations using a combination of experimental and modelling work. |
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2024-06-14 |
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UA @ admin @ c:irua:205246 |
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9139 |
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Cioni, M.; Delle Piane, M.; Polino, D.; Rapetti, D.; Crippa, M.; Arslan Irmak, E.; Pavan, G.M.; Van Aert, S.; Bals, S. |
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Data for Sampling Real‐Time Atomic Dynamics in Metal Nanoparticles by Combining Experiments, Simulations, and Machine Learning |
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2024 |
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Dataset; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Even at low temperatures, metal nanoparticles (NPs) possess atomic dynamics that are key for their properties but challenging to elucidate. Recent experimental advances allow obtaining atomic‐resolution snapshots of the NPs in realistic regimes, but data acquisition limitations hinder the experimental reconstruction of the atomic dynamics present within them. Molecular simulations have the advantage that these allow directly tracking the motion of atoms over time. However, these typically start from ideal/perfect NP structures and, suffering from sampling limits, provide results that are often dependent on the initial/putative structure and remain purely indicative. Here, by combining state‐of‐the‐art experimental and computational approaches, how it is possible to tackle the limitations of both approaches and resolve the atomistic dynamics present in metal NPs in realistic conditions is demonstrated. Annular dark‐field scanning transmission electron microscopy enables the acquisition of ten high‐resolution images of an Au NP at intervals of 0.6 s. These are used to reconstruct atomistic 3D models of the real NP used to run ten independent molecular dynamics simulations. Machine learning analyses of the simulation trajectories allows resolving the real‐time atomic dynamics present within the NP. This provides a robust combined experimental/computational approach to characterize the structural dynamics of metal NPs in realistic conditions. |
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UA @ admin @ c:irua:205843 |
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9143 |
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De Luca, F.; Abate, S.; Bogaerts, A.; Centi, G. |
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Electrified CO2 conversion : integrating experimental, computational, and process simulation methods for sustainable chemical synthesis |
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Doctoral thesis |
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2024 |
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xv, 152 p. |
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Doctoral thesis; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Nowadays, the burning of fossil fuels, particularly petroleum, natural gas, and coal, meets the rising need for power and fuels for automobiles and industries. This has given rise to ecological and climate challenges. This thesis explores these issues from three distinct perspectives: (i) experimental, (ii) computational, and (iii) process simulation, with a focus on studying CO2 as an alternative and economically viable raw material. Firstly, the experimental study is focused on the synthesis, characterization, and testing of novel catalysts for electroreduction of CO2 and oxalic acid, an intermediate product of CO2. Electrocatalysts based on Cu supported by citrus (orange and lemon) peel biomass are prepared. These catalysts exhibit activity in the electrochemical reduction of CO2, emphasizing the effectiveness of biomasses, particularly orange peels, as environmentally friendly precursors for sustainable and efficient electrocatalysts. In addition, graphitic carbon nitrides/TiO2 nanotubes (g-C3N4/TiNT) composites are prepared for the electrocatalytic reduction of oxalic acid to glycolic acid, revealing superior electrocatalytic properties compared to pristine TiNT. Characterization by X-ray diffraction, X-ray photoelectron spectroscopy, and scanning electronic microscopy were performed for all the prepared electrocatalysts. Delving into the reduction of CO2 on Cu catalysts, a computational study about the synthesis of methanol on Cu(111) surface is performed by using the Vienna Ab initio Simulation Package. A systematic study is carried out to define the activation energies of the elementary reactions by using mGGA DF. Consequently, it is shown that the rate-controlling step is CH3O* hydrogenation and the formate pathway on Cu(111) proceeds through the HCOOH* intermediate. Finally, the process simulation, performed by using the software Aspen Plus 11 from AspenTech Inc., is based on the comparison of a catalytic (oxidation of ethylene glycol) and an electrocatalytic process (CO2 electroreduction chain) to synthesize glycolic acid. An economic analysis of the operational and investment costs reveals that the catalytic process is more cost-effective due to the current instability of electrocatalysts and proton exchange membranes, resulting in increased maintenance costs and, consequently, higher prices for the product. |
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UA @ admin @ c:irua:205262 |
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9147 |
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Vlasov, E. |
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Exploiting secondary electrons in transmission electron microscopy for 3D characterization of nanoparticle morphologies |
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Doctoral thesis |
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2024 |
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x, 118 p. |
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Doctoral thesis; Electron microscopy for materials research (EMAT) |
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Electron tomography (ET) is an indispensable tool for determining the three-dimensional (3D) structure of nanomaterials in (scanning) transmission electron microscopy ((S)TEM). ET enables 3D characterization of a variety of nanomaterials across different fields, including life sciences, chemistry, solid-state physics, and materials science down to atomic resolution. However, the acquisition of a conventional tilt series for ET is a time-consuming process and thus cannot capture fast transformations of materials in realistic conditions. Moreover, only a limited number of nanoparticles (NPs) can be investigated, hampering a general understanding of the average properties of the material. Therefore, alternative characterization techniques that allow for high-resolution characterization of the surface structure without the need to acquire a full tilt series in ET are required which would enable a more time-efficient investigation with better statistical value. In the first part of this work, an alternative technique for the characterization of the morphology of NPs to improve the throughput and temporal resolution of ET is presented. The proposed technique exploits surface-sensitive secondary electron (SE) imaging in STEM employed using a modification of electron beam-induced current (EBIC) setup. The time- and dose efficiency of SEEBIC are tested in comparison with ET and superior spatial resolution is shown compared to conventional scanning electron microscopy. Finally, contrast artefacts arising in SEEBIC images are described, and their origin is discussed. The second part of my thesis focuses on real applications of the proposed technique and introduces a high-throughput methodology that combines images acquired by SEEBIC with quantitative image analysis to retrieve information about the helicity of gold nanorods. It shows that SEEBIC imaging overcomes the limitation of ET providing a general understanding of the connection between structure and chiroptical properties. |
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2024-06-17 |
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UA @ admin @ c:irua:204905 |
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9149 |
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Kummamuru, N.B. |
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Methane and hydrogen storage in clathrate hydrates |
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Doctoral thesis |
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2024 |
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XXV, 260 p. |
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Doctoral thesis; Engineering sciences. Technology; Antwerp engineering, PhotoElectroChemistry & Sensing (A-PECS) |
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In a world increasingly reliant on alternative energy sources, the quest for efficient and secure storage solutions is paramount. This doctoral thesis explores the exciting potential of a familiar material – water – to act as a vault for next-generation energy sources like hydrogen (H2) and methane (CH4). Nature offers a solution in the form of clathrate hydrates, fascinating cage-like structures formed from water molecules that can trap these gas molecules within their framework. This research investigates on improving the formation kinetics and gas storage capabilities of clathrate hydrates utilizing porous materials and the interstitial space between non-porous materials to augment the contact between gas and water thereby catalysing the growth of hydrates and unlocking their full potential as efficient and secure energy storage reservoirs. A key outcome of this research is the formulation of an empirical correlation, offering predictive insights into CH4 hydrate phase equilibrium conditions. Innovative approaches utilizing thermally conductive beads have yielded substantial enhancements in CH4 uptake. Furthermore, the identification of optimal water content within porous materials showcases a pathway to maximize CH4 storage capacity and hydrate growth kinetics. In the domain of hydrogen storage, attention is also directed towards unstirred systems, where the integration of functionalized porous materials has demonstrated a significant improvement in the rate of hydrate formation and the overall H2 storage capacity. A noteworthy achievement of this research lies in the successful storage of H2 within confined CH4 hydrates through a gas exchange process and the preliminary results show the potential for safer and more sustainable method for H2 storage at mild thermodynamic conditions, offering promising prospects for future energy systems. |
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UA @ admin @ c:irua:206258 |
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9160 |
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Lu, Q. |
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Precipitation behavior and heat resistance properties of Al-Cu-Mg-Ag-(Si) alloy |
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Doctoral thesis |
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2024 |
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VIII, 212 p. |
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Doctoral thesis; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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With the rapid increase in the speed of new-generation aerospace vehicles, conventional heat-resistant aluminum alloys cannot meet the long-term service of the equipment. Therefore, the development of new high-strength heat-resistant aluminum alloys is of great strategic for the sustainable and high-quality development of industries. Al-Cu-Mg-Ag alloy is an age-hardenable heat-resistant aluminum alloy and has high strength and heat resistance. The addition of alloying elements such as Si and Sc to Al-Cu-Mg-Ag alloy introduces a competitive relationship among the σ-Al5Cu6Mg2, θ′-Al2Cu, and Ω phases. Therefore, a systematic investigation of precipitation behavior and heat resistance of Al-Cu-Mg-Ag-(Si) is essential for guiding the design of high-strength heat-resistant aluminum alloys. Combined characterization testing methods such as scanning electron microscopy, transmission electron microscopy, atom probe tomography, microhardness testing, and tensile testing with simulation calculation methods such as calculation of phase diagram, first-principles calculations, and Ab initio molecular dynamics, the effects of heat treatment processes and element content on the precipitation behavior, mechanical properties, and heat resistance of Al-Cu-Mg-Ag-(Si) alloys were systematically investigated. Furthermore, a multiple interface segregation structure was constructed at the θ′/Al interface, and a new Al-Cu-Mg-Ag-Si-Sc alloy with synergistically improved strength and heat resistance was developed. The main conclusions are as follows: (1) Based on the Kampmann-Wagner-Numerical theory, the relationship between the coarsening rate of the Ω phase and the aging process was analyzed, revealing for the first time that the critical size of Ω phase ( ) under thermal exposure temperature was the key factor determining the coarsening rate of Ω phase during long time thermal exposure heat treatment. After artificial ageing, when the size of Ω phase was smaller than the critical size , the dissolution of smaller Ω phase leaded to a rapid decrease in the number density of Ω phases, thereby reducing the heat resistance of the alloy. When the size of Ω phase was greater than or equal to the critical size , the coarsening rate of Ω phase was consistent, but a larger initial size would result in a larger final size after long-term thermal exposure. Therefore, the closer the size of Ω phase in the alloy is to the critical size under heat exposure temperature, the better the heat resistance of the alloy. (2) A concept of constructing a multiple interface segregation structure at the precipitate/matrix interface was proposed, and based on this concept, a multiple interface segregation structure containing the C/L-AlMgSiCu interfacial phase, newly discovered χ-AgMg interfacial phase, and Sc segregation layer was successfully constructed at the θ′/Al interface. The existence of the multiple interface segregation structure ensured that the designed Al-Cu-Mg-Ag-Si-Sc alloy maintains a yield strength of 400 MPa after thermal exposure at 200 C for 100 h, with a strength retention rate of 97%, creating a new record for the synergistic improvement of strength and heat resistance in aluminum alloys. In addition, combining transmission electron microscopy ex-situ/in-situ characterization with first-principles calculations, it is shown that the χ-AgMg interface phase will be destroyed due to the diffusion of the outer Ag layer during thermal exposure, and gradually dissolve into the matrix, but it can still delay the coarsening behavior of θ′-Al2Cu phase. (3) The criteria for determining whether Ω phase can precipitate are updated in Al-Cu-Mg-Ag-Si alloys with low Mg/Si ratio based on phase diagram thermodynamic calculations and multi-scale structural characterization. When W(Mg)/W(Si) > 1.4 and X(Ag)/X(Mgexcess) > 1, Ω phase can precipitate in Al-Cu-Mg-Ag-Si alloys, where X(Mgexcess) represents the atomic percentage of residual Mg elements after the formation of the AlMgSiCu quaternary precipitate phase C/L phase in the supersaturated solid solution, and the W(Mg) is the mass fraction of Mg in the supersaturated solid solution before artificial ageing. (4) The effects of alloy element content on precipitation behavior and heat resistance of Al-Cu-Mg-Ag-Si alloys were systematically analyzed. Critical conditions for the precipitation of σ-Al5Cu6Mg2 and Ω phase in Al-Cu-Mg-Ag-Si alloys are revealed. Based on calculation of phase diagram results, the conditions for precipitating σ-Al5Cu6Mg2 phase in the alloy are: ① W(Mg)/W(Si) > 1.8; ② W(Cu) > 2.7W(Mg) – 5W(Si). When W(Mg)/W(Si) < 1.8, the alloy is mainly precipitated with C/L/Q′-AlMgSiCu. When W(Cu) < 2.7W(Mg) – 5W(Si), the alloy will generate GPB zone. In addition, W(Ag)/W(Si) > 4 is the critical condition which the Ω phase can the main precipitates in Al-Cu-Mg-Ag-Si alloys. Furthermore, the correlation between precipitate types and heat resistance was summarized, showing that Al-Cu-Mg-Ag-(Si) alloys with Ω phase as the main strengthening phase are more suitable for the preparation of structures with short service time but high temperature, while Al-Cu-Mg-Ag-(Si) alloys with low Mg content and multiple segregation structures are more suitable for structures requiring long-term service at medium to high temperatures. This study, for the first time, combines calculation of phase diagram with multi-scale microstructure characterization, systematically unraveling the effects of element content on precipitation behavior, strength, and heat resistance of Al-Cu-Mg-Ag-(Si) alloys. In addition, a concept of constructing a multiple interface segregation structure at the precipitate/matrix interface was proposed to synergistically improve alloy strength and heat resistance. This work provides theoretical guidance for optimizing the composition and processing of Al-Cu-Mg-Ag-(Si) alloy and regulating the microstructure. Furthermore, it also offers new ideas and theoretical guidance for the development of novel high-strength heat-resistant alloys in other systems. |
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UA @ admin @ c:irua:206180 |
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9167 |
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Manaigo, F. |
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Study of a gliding arc discharge for sustainable nitrogen fixation into NOx |
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Doctoral thesis |
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2024 |
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xxiv, 114 p. |
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Doctoral thesis; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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With the growth of the world population, the agricultural sector is required to meet an increasing demand for nutrients and currently relies on industrially produced fertilizers. Among them, nitrogen-based fertilizers are the most common choice and require N2 to be converted into more reactive molecules in a process called “nitrogen fixation”. This is mainly performed through the Haber-Bosch process, which, is not ideal since it requires large-scale facilities to be economical and is associated with a high energy cost and high CO2 emissions, resulting in an environmental impact that is pushing for the study of greener alternatives. Among these, plasma-based nitrogen fixation into NOx is promising, and gliding arc plasma, specifically, proved to be suitable for nitrogen fixation. This thesis aims to study plasma-based nitrogen fixation focusing on an atmospheric pressure gliding arc plasma on three different levels. On a fundamental level, an approach dealing with laser-based excitation of separate rotational lines was successfully developed. This method can be implemented on atmospheric discharges that produce rather high NOx densities and, thus, can impose essential restrictions for the use of “classical” laser-induced fluorescence methods. The approach is then implemented, providing a discussion on the two-dimensional distributions of both the gas temperature and the NO ground state density. A clear correlation between these quantities is found and the effects of both the gas temperature and the plasma power on NO and NO2 concentrations are discussed, revealing how the NO oxidation is already significant in the plasma afterglow region and how the gas flow rate is a crucial parameter affecting the temperature gradients. >From a technological level, the conventional approach of introducing external resistors to stabilize the arc is challenged by studying both its performance and its stability replacing the external resistor with an inductor. We conclude that similar stabilization results can be obtained while significantly lowering the overall energy cost, which decreased from up to a maximum of 7.9 MJ/mol N to 3 MJ/mol N. Finally, we study whether a small-scale fertilizer production facility based on a gliding arc plasma can be a local competitive alternative. This is done by proposing a comparative model to understand how capital, operative expenditures and transport costs affect the production costs. The model highlights how, with the current best available technology, plasma-based nitrogen fixation, while being an interesting alternative for NOx synthesis, still requires a more efficient use of H2 for direct NH3 production. |
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UA @ admin @ c:irua:205259 |
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9175 |
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Van Hoecke, L. |
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CFD-Assisted design of fluidized reactors for H2 release from LOHC |
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Doctoral thesis |
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2024 |
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XXXIII, 181 p. |
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Doctoral thesis; Engineering sciences. Technology |
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Hydrogen (H2) is expected to become a key molecule in the transition towards a society running on renewable energy. It can be used to store excess renewable energy at peak production moments and release this energy at a later stage when renewable energy production is less. However, storing H2 is challenging due to the low density of this gas. As a solution, Liquid Organic Hydrogen Carriers or LOHC molecules have been proposed in the passed to increase volumetric energy density of H2. LOHC are a class of molecules that have storage sites available, to which the H2 gas can be chemically bounded. The LOHC molecule under investigation was dibenzyltoluene (DBT), which is an oil like liquid, that is easy to transport and poses little fire or explosion risks. To release the H2 from the DBT carrier, via a so-called dehydrogenation reaction, efficient mass and heat transfer is required during the process, since a large volume increase is expected from H2 release and the reaction is endothermic, i.e., a self – cooling process that takes place at temperatures around 300 C. The heat has to be supplied specifically to the active sites of catalyst particles that are present inside the reactor and which enable the dehydrogenation to proceed. For heat transfer limited processes fluidized bed reactors are often used, which is a type of reactor where the particle phase is being agitated by the fluid flow. The research proposed in this work, was to explore via computational fluid dynamics (CFD) simulations the possibilities and challenges of using fluidized bed reactors for the dehydrogenation of LOHC. The model selection required for CFD simulations of a three-phase system was investigated in this work, with a main emphasis on the drag model selection. The CFD modelling study was focused on the use of swirling fluidized bed reactors, since it was hypothesised that the swirling effect could also aid in increased removal of the gas phase from the reaction medium to increase the efficiency of the process. Ultimately, it was shown that the main challenges in the design of fluidized bed reactors will be to create uniform particle distribution inside the reactor. A new design for a dehydrogenation reactor is proposed based on the insights gained in this thesis. |
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2024-06-14 |
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UA @ admin @ c:irua:205645 |
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9192 |
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Lembrechts, J.; Clavel, J.; Lenoir, J.; Haider, S.; McDougall, K.; Nunez, M.; Alexander, J.; Barros, A.; Milbau, A.; Seipel, T.; Verbruggen, E.; Nijs, I. |
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Dataset: Roadside disturbance promotes plant communities with arbuscular mycorrhizal associations in mountain regions worldwide |
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2024 |
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Dataset; Plant and Ecosystems (PLECO) – Ecology in a time of change |
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Aim: We aimed to assess the impact of road disturbances on the dominant mycorrhizal types in ecosystems at the global level and how this mechanism can potentially lead to lasting plant community changes. Location: Globally distributed mountain regions Time Period: 2007-2018 Taxa studied: Plants (linked to their associated mycorrhizal fungi) Methods: We used a database of coordinated plant community surveys following mountain roads from 894 plots in 11 mountain regions across the globe in combination with an existing database of mycorrhizal-plant associations in order to approximate the relative abundance of mycorrhizal types in natural and disturbed environments. Results: Our findings show that roadside disturbance promotes the cover of plants associated with arbuscular mycorrhizal (AM) fungi. This effect is especially strong in colder mountain environments and in mountain regions where plant communities are dominated by ectomycorrhizal (EcM) or ericoid-mycorrhizal (ErM) associations. Furthermore, non-native plant species, which we confirmed to be mostly AM plants, are more successful in environments dominated by AM associations. Main Conclusions: These biogeographical patterns suggest that changes in mycorrhizal types could be a crucial factor in the worldwide impact of anthropogenic disturbances on mountain ecosystems. Indeed, roadsides foster AM-dominated systems, where AM-fungi might aid AM-associated plant species while potentially reducing the biotic resistance against invasive non-native species, often also associated with AM networks. Restoration efforts in mountain ecosystems will have to contend with changes in the fundamental make-up of EcM- and ErM plant communities induced by roadside disturbance. |
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UA @ admin @ c:irua:206132 |
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9198 |
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De Keyzer, M.; Soens, T.; Verbruggen, C. |
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Mens en natuur : een geschiedenis |
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MA2 Book as author |
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2024 |
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313 p. |
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MA2 Book as author; History; Centre for Urban History |
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Onze relatie met de natuur om ons heen is, op zijn zachtst gezegd, ingewikkeld. Mensen gingen niet plots een bedreiging vormen voor het leven op aarde nadat ze er eeuwenlang mee in harmonie hadden geleefd. Verschillende ideeën over de omgang met de natuurlijke omgeving – sommige duurzaam, andere ronduit desastreus – hebben altijd naast elkaar bestaan. We waren er ons al verrassend vroeg van bewust dat ons handelen een nefaste impact kon hebben op de natuur. Maar die bezwaren werden geregeld aan de kant geschoven. Deze inleiding tot de milieugeschiedenis helpt de lezer te begrijpen hoe onze hedendaagse problematische omgang met de natuur en ons milieu tot stand is gekomen. Het is een introductie tot het recente onderzoek naar de relatie tussen mens en natuur doorheen de eeuwen, in de Lage Landen en ver daarbuiten. |
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978-94-014-0395-5 |
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UA @ admin @ c:irua:205213 |
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9212 |
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Clavel, J. |
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Plant-mycorrhizal interactions and their role in plant invasions in mountains |
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2024 |
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182 p. |
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Doctoral thesis; Plant and Ecosystems (PLECO) – Ecology in a time of change |
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Non-native species invasions are one of the most impactful drivers of biodiversity and ecosystem services loss worldwide. One aspect of plant species invasion, which is only recently starting to be recognized as a determinant of invasion success, is the symbiosis between plant and mycorrhizal fungi. Here, I focus on anthropogenic disturbance in mountain ecosystems and its impact on plant communities and mycorrhizal fungi to answer how these communities are impacted by disturbance and whether non-native plants can benefit to establish and spread. To this end I used a combination of different approaches: 1) repeated surveys of plants and arbuscular mycorrhizal fungi along disturbed roadsides in the mountains of Norway, 2) combining a global dataset of native and non-native plants along mountain roads with a database associating plants with their mycorrhizal types, and 3) an in-situ experiment measuring non-native plant success and changes in fungal community following different types of disturbances. Through these methods, I could assess the effects of anthropogenic disturbance on mycorrhizal symbiosis and non-native plant species at multiple scales and resolutions. We found that road disturbance has a globally consistent effect on mycorrhizal types in mountain systems, as plants associated with arbuscular mycorrhizal (AM) fungi were more abundant following disturbance. Conversely, vegetation associated with either ectomycorrhizal (EcM) or ericoid mycorrhizal (ErM) fungi was less abundant in disturbed sites. In the regional study, AM fungi were most abundant and diverse in the roots of plant communities affected by road disturbance. Non-native plants were also restricted to these disturbed sites. The experimental results showed that physical disturbance and nutrient addition have negative effects on EcM fungi and positive effects on fungal pathogens, and facilitate non-native plant success. Our results show that anthropogenic disturbance does have an effect on mycorrhizal fungi that in turn impacts the distribution of plant species in disturbed mountain systems. The resulting shift in mycorrhizal fungi benefiting AM fungi and AM plant species could have implications for non-native plant invasions. Indeed, we know that non-native plants predominantly form associations with AM fungi. Therefore, anthropogenic disturbance can facilitate non-native plant success through disruption of the native fungal communities, and especially so in high elevation and cold climate regions which are naturally less dominated by AM plants. I believe this highlights the importance of mycorrhizal symbiosis in understanding plant invasions and emphasizes the importance of monitoring sources of anthropogenic disturbance in mountains to prevent future establishment of non-native plants. |
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UA @ admin @ c:irua:204154 |
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9219 |
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Ramirez-Rojas, I. |
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Underground connections : the interplay between tropical rainforest trees and soil microbial communities |
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2024 |
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205 p. |
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Doctoral thesis; Plant and Ecosystems (PLECO) – Ecology in a time of change |
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Tropical rainforests host an exceptional biodiversity and play a fundamental role in the regulation of global climatic cycles. Soil fungi and bacteria are key players in the transformation and processing of nutrients in terrestrial ecosystems while having an essential role as tree mutualists or antagonists. Still, there are gaps in our understanding of the main variables driving soil microbes on these forests and it is unclear how future climate change scenarios may impact soil microbes and further affect the ecosystem. In this thesis, we first explored the drivers of the microbial community composition in two pristine forests in French Guiana by using amplicon DNA sequencing. The neighboring tree species were found to be a crucial factor influencing the fungal and bacterial community composition at our sites regardless of the season. Additionally, within the environmental factors explored, soil moisture, phosphorus (P) and nitrogen (N) availability were consistently the main soil properties controlling the composition of soil microbial communities. Secondly, as increased nutrient deposition due to anthropogenic activities are expected to affect tropical forests ecosystems N and P availability, a factorial N and P nutrient addition experiment in the same sites was used to assess the effects of changes in the soil nutrient stoichiometry on the soil microbial communities. These results showed that after 3 years of nutrient additions, the bacterial and fungal community composition was affected by both the N and P additions. Besides, the fungal community composition had a stronger response to the nutrient addition, especially when P was added. Moreover, when the nutrient addition effect was assessed in bacteria and fungi with different life strategies, we found different nutrient optima between them. Furthermore, to study the effect of the connection to an existing mycorrhizal mycelium on tree seedlings, I established a mycelium exclusion experiment. Interestingly, we could not detect an effect of the mycorrhizal mycelium exclusion on the seedling N uptake, performance, or fungal community composition in roots after one year. All together this work provides a deeper understanding of the factors influencing the soil microbial communities on these lowland tropical forests, demonstrating that the tree community composition exerts a higher influence on the soil microbial community composition than previously expected. Moreover, our results show that the fungal and bacterial community composition and its relationship with trees in the vicinity is highly dependent on the ecosystem nutrient availability. |
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UA @ admin @ c:irua:204907 |
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9237 |
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Montiel, F.N. |
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Voltage against illicit drug trafficking : capabilities of electrochemical fingerprinting to detect illicit drugs |
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2024 |
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256 p. |
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Doctoral thesis; Pharmacology. Therapy; Engineering sciences. Technology; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab) |
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UA @ admin @ c:irua:204707 |
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9243 |
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Van Alphen, S. |
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Modelling plasma reactors for sustainable CO2 conversion and N2 fixation |
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2023 |
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202 p. |
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Doctoral thesis; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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200 years ago, humanity started the industrial revolution by discovering fossil fuels, which lead to unprecedented technological advancements. However it has become alarmingly clear that the major environmental concerns associated with fossil fuels require a short-term transition from a carbon-based energy economy to a sustainable one based on green electricity. A key step concerning this transition exists in developing electricity-driven alternatives for chemical processes that rely on fossil fuels as a raw material. A technology that is gaining increasing interest to achieve this, is plasma technology. Using plasmas to induce chemical reactions by selectively heating electrons in a gas has already delivered promising results for gas conversion applications like CO2 conversion and N2 fixation, but plasma reactors still require optimization to be considered industrially competitive to existing fossil fuel-based processes and emerging other electricity-based technologies. In this thesis I develop computational models to describe plasma reactors and identify key mechanisms in three different plasma reactors for three different gas conversion applications, i.e. N2 fixation, combined CO2-CH4 conversion and CO2 splitting. I first developed models to describe a new rotating gliding arc (GA) reactor operating in two arc modes, which, as revealed by my model, are characterized by distinct plasma chemistry pathways. Subsequently, my colleague and I study the quenching effect of an effusion nozzle to this rotating GA reactor, reaching the best results to date for N2 fixation into NOx at atmospheric pressure, i.e., NOx concentrations up to 5.9%, at an energy cost down to 2.1 MJ/mol. Afterwards, I investigate the possible improvement of N2 admixtures in plasma-based CO2 and CH4 conversion, as significant amounts of N2 are often found in industrial CO2 waste streams, and gas separations are financially costly. Through combining my models with the experiment from a fellow PhD student, we reveal that moderate amounts of N2 (i.e. around 20%) increase both the electron density and the gas temperature to yield an overall energy cost reduction of 21%. Finally, I model quenching nozzles for plasma-based CO2 conversion in a microwave reactor, to explain the enhancements in CO2 conversion that were demonstrated in experiments. Through computational modelling I reveal that the nozzle introduces fast gas quenching resulting in the suppression of recombination reactions, which have more impact at low flow rates, where recombination is the most limiting factor in the conversion process. |
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UA @ admin @ c:irua:194811 |
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7270 |
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Kovács, A. |
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A structured methodology for natural deep eutectic solvent selection and formulation for enzymatic reactions |
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2023 |
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viii, 216 p. |
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Doctoral thesis; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Biochemical Wastewater Valorization & Engineering (BioWaVE); Intelligence in PRocesses, Advanced Catalysts and Solvents (iPRACS) |
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Natural deep eutectic solvents (NADES) show great promise as media for enzymatic reactions in areas where (bio)compatibility with natural or medicinal products is a must. While in theory they can be tailored to the intended reaction to ensure optimized yields, the knowledge to date is predominantly empirical, with some mechanistic reports providing a fragmented view at best. Therefore, it is not easy to explain experimental observations, let alone make predictions. The aim of this study was to develop a structured, holistic understanding of the effects of NADES media on enzymatic reactions, distinguishing between effects on solubility, solvation, viscosity, inhibition and denaturation. Experimental and computational chemistry methods were combined to separately study the interactions between enzyme, substrate, and NADES as reaction media. The initial enzyme activity and the final conversion of vinyl laurate transesterification by immobilized Candida antarctica lipase were studied experimentally. The direct effect of NADES on the same enzyme was modeled by molecular dynamics simulation. The effect of solubility was studied by both experimental and computational methods. To predict the solubility and viscosity of NADES, data-driven models were developed by combining group contribution and machine learning methods, based on the accumulated experimental knowledge on NADES found in the literature. Finally, the composed relationships and prediction models were applied to the practical example of deacetylation of mannosylerythritol lipids (MELs). The experimental findings show that the chosen NADES system has a significant effect on both the apparent initial activity and the final conversion. However, in the simulations, the enzyme retains its original structure; moreover, NADES has an additional stabilizing effect on the enzyme. In addition, changes in the molar ratio of the compounds in NADES do not show a significant effect on the stability of the enzyme. These results indicate that the main effect of NADES on the reaction is mainly related to the substrate-solvent interactions (solvation energy) and the viscosity of the system. On the other hand, the experimental results only confirmed the significance of solvation, viscosity did not show a clear correlation with the studied reaction parameters. The machine learning models built for solubility and viscosity gave quantitative predictions of these properties. The accumulated knowledge was used to optimize the yield in the deacetylation reaction of MELs. The combination of these methods provides fundamental knowledge about the effect of NADES on biocatalysis, but the results are also applicable to other uses of NADES. |
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UA @ admin @ c:irua:194886 |
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7276 |
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De Backer, J. |
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The versatile nature of cytoglobin, the Swiss army knife among globins, with a preference for oxidative stress |
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Doctoral thesis |
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2023 |
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XVIII, 232 p. |
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Doctoral thesis; Pharmacology. Therapy; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Proteinscience, proteomics and epigenetic signaling (PPES) |
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Since its discovery 20 years ago, many studies have been performed to gain insight into the functional role of cytoglobin (Cygb). However, Cygb has been proven to be a promiscuous protein. Yet, there is a consensus that Cygb is a cytoprotective protein involved in redox homeostasis. CYGB is a ubiquitously expressed hexacoordinated globin that is highly expressed in melanocytes and is often found to be downregulated during melanocyte-to-melanoma transition. In Chapter III, we investigated the molecular mechanism through which CYGB could be involved in redox regulation. Here, we showed that CYGB contains two redox-sensitive cysteine residues and that the formation of an intramolecular disulfide bridge resulted in the heme group becoming more accessible to external ligands. This supports the hypothesis that Cys38 and Cys83 serve as sensitive redox sensors. In Chapter IV we showed that CYGB mRNA and protein levels were elevated upon exposure to hypoxia. Interestingly, this upregulation was most likely HIF-2α-dependent. We propose that in melanoma, HIF-2α, rather than HIF-1α, positively regulates CYGB under hypoxic conditions in a cell type specific way. In Chapter V, the cytotoxic effect of indirect NTP treatment in two melanoma cell lines with divergent endogenous CYGB expression levels was investigated. We confirmed that NTP endows cytotoxicity that induces cell death through apoptosis and that this was mediated through the production of ROS. Moreover, we showed that CYGB protects melanoma cells from ROS-induced apoptosis by the scavenging of ROS. Interestingly, CYGB expression influenced the expression of NRF2 and HO-1. We identified the lncRNA MEG3 as a possible mechanism through which NRF2 expression and its downstream target HO-1 can be regulated by CYGB. In chapter VI, increased basal ROS levels and higher degree of lipid peroxidation upon RSL3 treatment contributed to the increased sensitivity of CYGB knockdown G361 cells to ferroptosis. Furthermore, transcriptome analysis demonstrates the enrichment of multiple cancer malignancy pathways upon CYGB knockdown, supporting a tumor-suppressive role for CYGB. Remarkably, CYGB expression regulation was identified as a critical determinant of the ferroptosis–pyroptosis therapy response. This suggests that CYGB is involved in the regulation of multiple modes of programmed cell death. FInally, we sought to delineate the RONS that are responsible for plasma-induced ICD. Our results highlight the importance of the short-lived species. Furthermore, we are first to demonstrate that NTP-created vaccine is safely prepared and offers complete protection. Moreover, we provide conclusive evidence that direct application of NTP induces ICD in melanoma. |
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UA @ admin @ c:irua:193568 |
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7277 |
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Khan, S.U. |
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Singlet oxygen-based photoelectrocatalysis : from photosensitizer structures to plasmonic enhancement |
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Doctoral thesis |
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2023 |
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182 p. |
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Doctoral thesis; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab) |
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Singlet molecular oxygen (1O2) has continuously attracted researchers' interest because of its involvement in various processes, such as in photodynamic reactions in biological and chemical systems. 1O2 is an effective electrophile and potent oxidizing agent and can be easily generated by photosensitization via the illumination of organic dyes with visible light. As described in Chapter 1, 1O2 has gained prominence in various applications such as wastewater treatment, photodynamic therapy of cancer, organic synthesis, and recently developed 1O2-based photoelectrochemical (PEC) sensing of phenolic compounds. Phenolic compounds are a potential source of contaminants that originates from industrial effluents and waste products of chemical and pharmaceutical industries. These phenolic compounds pose severe threats to humans and aquatic life after reaching the environment. Therefore, it is imperative to develop photoactive materials that efficiently generate 1O2 and oxidize phenolic compounds and antibiotics. The existing 1O2 generating photosensitizers (PSs) include porphyrins, phthalocyanines (Pcs), subphthalocyanines (SubPcs), and other dyes such as derivatives of xanthene (e.g., Rose Bengal (RB)), and fluorinated boron-dipyrromethene (BODIPYs), and phenothiazinium dyes (e. g. Methylene Blue (MB)) which display long-lived triplet excited state and can be used in 1O2-based applications. This thesis focuses on preparing efficient hybrid materials based on newly synthesized Pcs, different surface area titanium dioxide (TiO2) and plasmonic gold nanoparticles (AuNPs) for their use in the PEC detection of phenolic compounds. The first focus was on developing a fast amperometric method to test the photo-electrocatalytic activity of 1O2 producing PSs dissolved in MeOH based on the redox cycling of an electroactive phenolic compound, hydroquinone (HQ) (Chapter 2). This method of testing PSs does not require the accumulation of a reaction product since the amperometric signal develops near instantly when the light is on, which enables dynamic monitoring of a PSs activity at varying conditions in a single experiment. This method was crucial to measure high 1O2 quantum yield and low yield in the same experimental conditions. Moreover, the obtained results revealed a range of working parameters affecting the PEC activity of PSs. The next goal was to immobilize tert-butyl substituted aluminum Pc (t-BuPcAlCl) on the solid support, which showed a high 1O2 quantum yield. However, before immobilizing Pc on a solid support such as TiO2, it is essential to know the electronic energy level of Pcs for the possible electron transfers from Pcs to TiO2. Therefore, Chapter 3 explored the (spectro)electrochemical properties of t-BuPcAlCl Pc. Next, in Chapter 4, t-BuPcAlCl Pc and other tert-butyl substituted Pcs with Zn central metal, t-BuPcZn, and its metal-free derivative t-BuPcH2 were immobilized on different surface area TiO2. The PEC activity of immobilized Pcs on TiO2 toward different phenols and antibiotics was studied, and the action mechanism was revealed and compared with sterically hindered fluorinated Pc F64PcZn. In the final part of this thesis plasmonic AuNPs were introduced combined with trimethylsilane-protected acetylene functionalized ZnPc (TMSZnPc) to study the synergistic effect that boosts the overall activity toward the detection of phenols under visible light illumination (Chapter 5) . The TMSZnPc was coupled with AuNPs via a click chemistry approach. The 1O2 quantum yield of TMSZnPc improved significantly after conjugating with AuNPs, and, subsequently, the PEC activity for detecting HQ. The theoretical and experimental investigation demonstrated that the plasmonic enhancement of TMSZnPc is driven by the near-field mechanism. This shows the importance of plasmonic AuNPs with other photoactive species for their use in 1O2-based applications. The fundamental knowledge obtained in this doctoral study will ultimately deepen the understanding of developing 1O2-based PEC sensors for detecting phenolic compounds and pharmaceuticals in the wastewater stream, helping to choose efficient materials and, in the last instance, a more sustainable future especially access to clean water for everyone. |
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UA @ admin @ c:irua:193342 |
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7337 |
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Yang, T. |
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Characterization of Laves phase structural evolution and regulation of its precipitation behavior in Al-Zn-Mg based alloys |
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Doctoral thesis |
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2023 |
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ii, 106 p. |
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Doctoral thesis; Electron microscopy for materials research (EMAT) |
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Al-Zn-Mg-based high strength alloys are widely used in aerospace applications due to their low density and excellent mechanical properties. A systematic study of the structural evolution of the nano-precipitation phase and its growth mechanism is an important guide for the design of new high-strength alloys. In this work, the Laves structure precipitates in Al-Zn-Mg(-Cu/Y) alloy was systematically characterized. Based on the structure evolution, the structure of submicron Laves particles and quasicrystalline particles in the alloy at microscale, as well as the regulation of the precipitation behavior after adding Y at nanoscale were further investigated. The main innovative results are summarized as follows: (1) Investigation on coexistence of defect structures in Laves structural nanoprecipitates. Three types of Laves structures can coexist within the η-MgZn2 precipitates: C14, C15 and C36, and the Laves structure transition sequence of C14→C36→C15 in this system was determined. Meanwhile, it was found that there are diverse defect structures in the MgZn2 phase, including stacking faults, planar defects and five-fold domain structures, which have significant effects on relieving the internal stress/strain of the precipitates. (2) Investigation on multiple phase transition of Laves structural nanoprecipitates from C14 to C36 and from C14 to quasicrystal clusters. It is found that C14 precipitates can be completely transformed into the C36 precipitates. And it is also found that the C14 Laves phase structure can also transform into quasicrystalline clusters. These investigations on various phase transition mechanisms among Laves phases provide theoretical support for the microstructural characterization of materials containing multi-scale Laves phases. (3) Characterization of Laves and quasicrystal structural particles in submicron scale. Submicron-scale quasicrystal particles were obtained in conventional casting Al-Zn-Mg-Cu alloys for the first time. Industrial impurity elements Fe and Ni can induce the formation of quasicrystalline particles. When there is no Fe/Ni enriched in particles, the structure is characterized as C15-Laves phase. When Fe/Ni is as quasicrystalline core, a stable core-shell quasicrystalline structure with Al-Fe-Ni nucleus and Mg-Cu-Zn shell can be formed. (4) Investigation on the regulation of nanoscale Laves precipitates’ growth. To regulate the defect structure of the precipitates, rare earth element Y was added in Al-Zn-Mg alloys and its influence on the precipitation behavior was investigated. The addition of Y element can dynamically combine with different alloying elements during aging process, which can refine the size of precipitate and further improve the nucleation rate and precipitation rate of the precipitates. |
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UA @ admin @ c:irua:196404 |
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7631 |
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Voordeckers, D. |
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Design to breathe : understanding and altering wind patterns in street canyons to reduce human exposure to air pollution |
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Doctoral thesis |
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2023 |
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xxii, 303 p. |
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Doctoral thesis; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL); Research Group for Urban Development; Intelligence in PRocesses, Advanced Catalysts and Solvents (iPRACS) |
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Air pollution is proclaimed by the World Health Organiaation (WHO) as the biggest environmental threat to human health. Street canyons, or urban roads flanked by a continuous row of high buildings on both sides, are perceived as typical bottleneck areas for air quality due to their lack of natural ventilation. This doctoral thesis aims to integrate expert knowledge on in-canyon flow fields and pollution dispersion in street canyons from the specialized field of (bio)engineering into the field of urban planning and vice versa. In Chapter 1, a Geospatial Information System (GIS) method was developed to detect exposure zones and hotspot street canyons. A critical combination between aspect ratio (AR > 0.65) and traffic volume (TVmax > 300) was detected and subsequently used to detect hotspot street canyons in three major European cities (Antwerp, London and Paris). Chapter 2 focusses on acquiring in-depth knowledge on flow and concentration fields in street canyons by conducting an extensive literature review on over 200 studies and translates this knowledge into nineteen guidelines and eleven spatial tools, comprised in a toolbox for urban planning. Subsequently, computational fluid dynamics (CFD) was used into a research trough design process (Chapter 4) to illustrate how the design tools can be applied to a specific case study (Belgiëlei, Antwerp). Alternations to traffic lanes (traffic lane reduction and lateral displacement) combined with low boundary walls (LBWs), were found to reduce NO2 levels in the entire pedestrian area up to – 3.6 % and peak pollutions were reduced by -8 %. A maximum NO2 reduction was reached by combining a traffic lane displacement with hedges, adjustments to the tree planting pattern and an increased ground-level permeability, leading to reductions up to – 4.5 % in the pedestrian areas. In conclusion, urban design was found to be a valuable tool to enhance the effect of emission reduction strategies and draw in-canyon concentrations closer to the value of the background concentration. However, the background concentration seemed to dominate the efficiency of the urban design interventions and therefore, additional measures should be taken to reduce background pollution levels. This dissertation aims to contribute to the awareness of air pollution in street canyons, as well as support local governments in taking action by delivering spatial tools and guidelines applicable for urban planning and represents a framework for the dissemination of expert information on air quality in street canyons to the field of urban planning. |
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UA @ admin @ c:irua:196399 |
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7767 |
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Vizarim, N.P. |
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Dynamic behavior of Skyrmions under the influence of periodic pinning in chiral magnetic infinite thin films |
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Doctoral thesis |
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2023 |
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212 p. |
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Doctoral thesis; Condensed Matter Theory (CMT) |
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The miniaturization of transistors for application in new processors and logic devices poses a significant challenge in the field of materials. Spintronics, which relies on controlled movement of magnetic nanostructures, offers a promising solution. Among the candidates, magnetic skyrmions are considered one of the most promising. These chiral spin structures, characterized by topological protection and enhanced stability compared to vortices or magnetic bubbles, have been extensively studied. To advance in the control of skyrmion motion, essential for practical applications, we investigated their dynamic behavior in a two-dimensional chiral magnet at zero temperature. Our study focused on the influence of periodic arrays of pinning centers. The simulations considered skyrmions as point-like particles considering the following interactions: skyrmion-skyrmion interactions, interactions with pinning center arrays, a current of polarized spins, and the Magnus force. We conducted calculations for scenarios involving a single skyrmion as well as different skyrmion density values in the material. The aim was to explore possibilities for controlled skyrmion motion, investigate different dynamic regimes, and examine collective effects. The results demonstrate that by adjusting the size, strength, and density of the pinning centers, we can effectively control the motion of individual skyrmions and manage the flow of multiple skyrmions. Furthermore, we discovered that periodic arrays of pinning centers can facilitate topological selection when different species of skyrmions with distinct Magnus components are present. Employing alternating currents, we observed the significant role of the ratchet effect in the skyrmion dynamics. By fine-tuning the amplitudes of the alternating currents, we achieved direct and controlled motion of skyrmions in specific directions. These findings hold potential for advancing our understanding of skyrmion dynamics and can inspire future technological applications involving these quasi-particles. Overall, we anticipate that our results will be valuable to the scientific community, contributing to a deeper comprehension of skyrmion dynamics and paving the way for future technological applications. |
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UA @ admin @ c:irua:198101 |
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8852 |
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Hassani, H. |
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First-principles study of polarons in WO₃ |
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Doctoral thesis |
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2023 |
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181 p. |
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Doctoral thesis; Condensed Matter Theory (CMT) |
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Polarons are quasiparticles emerging in materials from the interaction of extra charge carriers with the surrounding atomic lattice. They appear in a wide va- riety of compounds and can have a profound impact on their properties, making the concept of a polaron a central and ubiquitous topic in material science. Al- though the concept is known for about 75 years, the origin of polarons is not yet fully elucidated. This thesis focuses on WO 3 as a well-known prototypical system for studying polarons, which inherent polaronic nature is linked to its remark- able electrical and chromic properties. The primary objective of this research is to provide a comprehensive atomistic description and understanding of polaron formation in WO 3 using first-principles density functional theory (DFT) calcula- tions. Additionally, the investigation explores the interactions between polarons and the possibility of bipolaron formation. Following a systematic strategy, we first extensively analyze the dielectric and lattice dynamical properties of WO 3 in both the room-temperature P 2 1 /n and ground-state P 2 1 /c phases. Our specific focus is on characterizing the zone-center phonons, which serve as the founda- tion for identifying the phonon modes involved in the polaron formation and charge localization process. Subsequently, we examine the impact of structural distortions on the electronic structure of WO 3 to elucidate the interplay between structural distortions and electronic properties, thereby laying the groundwork for understanding electron-phonon couplings. By incorporating these critical fac- tors, we address our primary research goals. The most common explanation for the polaron formation is associated with the electrostatic screening of the extra charge by the polarizable lattice. Here, we show that, even in ionic crystals, this is not necessarily the case. We demonstrate that polarons in this compound arise primarily from non-polar atomic distortions. We then unveil that this unexpected behavior originates from the undoing of distortive atomic motions, which lowers the bandgap. As such, we coin the name of anti-distortive polaron and validate its appearance through a simple quantum-dot model, in which charge localization is the result of balancing structural, electronic, and confinement energy costs. Then, we also study the polaron-polaron interaction and present the formation of the antiferromagnetic W 4+ bipolaronic state with relatively large formation energy. Our analysis of the W 4+ bipolaronic distortions on the global structure reveals the same behavior as in experiments where the highly distorted monoclinic phase transforms into a tetragonal phase as a function of doping. Additionally, leveraging our previous findings on asymmetric polaronic distortion and examin- ing different merging orientations, we stabilize the antiferromagnetic W 5+ -W 5+ bipolaronic state with an energy lower than the W 4+ state. This thesis clari- fies the formation of unusual medium-size 2D polarons and bipolarons in WO3,which might be relevant to the whole family of ABO 3 perovskites, to which WO 3 is closely related. The simplicity of the concept provides also obvious guidelines for tracking similar behavior in other families of compounds. |
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UA @ admin @ c:irua:198169 |
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8868 |
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Wittner, N. |
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Improving and characterising solid-state fungal pretreatment by Phanerochaete chrysosporium for sugar production from poplar wood |
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Doctoral thesis |
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2023 |
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206 p. |
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Doctoral thesis; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL); Biochemical Wastewater Valorization & Engineering (BioWaVE) |
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Pretreatment is a critical step in the conversion of lignocellulose into biofuels and biochemicals. During pretreatment, the recalcitrance of lignocellulose is reduced, e.g. by removing lignin, thereby making the carbohydrates more accessible for enzymatic saccharification. Fungal delignification by white-rot fungi is a biotechnological alternative to chemical/physicochemical methods, which is carried out in solid-state fermentation with mild reaction conditions and without the formation of microbial inhibitors. However, fungal pretreatment presents some challenges, such as long pretreatment time, non-selective and low delignification, low enzymatic digestibility and feedstock sterilisation requirement, making its commercial implementation challenging compared to conventional methods. This study investigates the possibility of improving and characterising the solid-state fungal pretreatment of poplar wood by Phanerochaete chrysosporium. The individual and combined effects of MnSO4 and CuSO4 supplements on the delignification of sterilised wood are investigated using response surface methodology to improve the degree and selectivity of fungal delignification. Spore-inoculated solid-state fermentations are carried out for 4 weeks in sterile vented bottles. The mechanism of the concerted action of the metal ions on lignin degradation is then elucidated by relating fungal growth and ligninolytic enzyme activities to lignocellulose degradation as a function of pretreatment time. The optimised metal-supplemented system is then applied to the pretreatment of non-sterilised wood using different inoculation techniques (spores and pre-colonised substrate), nutrients (metal ions with or without glucose and sodium nitrate) and cultivation environments (sterile aerated bottles and open trays). The fermentations are then characterised using infrared spectroscopy, in particular NIR and ATR-FTIR spectroscopy, with the aim of developing rapid lignin quantification methods as an alternative to conventional wet chemical methods. Finally, the feasibility of producing fermentable sugars from sterilised and non-sterilised poplar wood using fungal pretreatment is evaluated through a techno-economic analysis. Supplementing the pretreatment system with 2.01 µmol CuSO4 and 0.77 µmol MnSO4 g-1 wood resulted in 1.9-fold higher lignin degradation, 2.3-fold higher delignification selectivity value and 2.9-fold higher glucose yield. The improved delignification could be explained by the concerted action of Mn2+ and Cu2+ ions, with Mn2+ ions inducing and Cu2+ prolonging manganese peroxidase production responsible for delignification. Fungal pretreatment at non-sterile conditions was obtained using trays in a simple solid-state fermentation set-up without sterile aeration. A 1:3 ratio of pre-colonised and untreated wood was applied for inoculation and only Cu2+, Mn2+ and sodium nitrate as supplements. Remarkably, this technology resulted in a comparably high glucose yield (28.51 ± 0.28%) to the traditional method using sterilised wood, sterile aeration and spores as inoculum, while reducing the amount of wood to be sterilised by 71.2%. Infrared spectroscopy-based methods with high coefficients of determination (R_CV |
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UA @ admin @ c:irua:197185 |
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8883 |
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Van Putte, N. |
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Title |
Improving groundwater dynamics : a key factor for successful tidal marsh restoration |
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Doctoral thesis |
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2023 |
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166 p. |
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Doctoral thesis; Sustainable Energy, Air and Water Technology (DuEL); Ecosphere |
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Tidal marshes take up and release certain elements from and to the river water. Hence, they act as a filter, improving the estuarine water quality. This filtering function depends on the interaction between the marsh soil and water that infiltrates into the marsh platform at high tide and seeps out of the creek banks at low tide. In the past centuries, many tidal marshes disappeared due to large scale land reclamations, together with their associated ecosystem services. Nowadays, tidal marshes are increasingly restored on formerly embanked agricultural areas to regain these ecosystem services. Here, we studied the effect of historical agricultural land use on the contribution of restored tidal marshes to water quality improvement, and we investigated several solutions to stimulate the water quality improving function in newly restored tidal marshes. In restored tidal marshes, the soil is often compacted due to the historical agricultural land use, leading to a reduced organic matter content and micro- and macroporosity. In this compacted soil, groundwater flow is hindered, leading to a more waterlogged soil and reduced groundwater dynamics in the restored marsh as compared to a natural marsh. The depth of groundwater drainage and the groundwater flow velocity have important implications for the processes that contribute to water quality improvement, e.g. removal of nitrogen, phosphorus retention and silica cycling. Where groundwater drains deeper, i.e. in the vicinity of tidal creeks and in a more porous soil, these processes are promoted. We suggest that, in newly restored tidal marshes, the soil porosity can be increased by amending the soil (e.g. with organic matter), and the distance to the nearest tidal creek can be reduced by creek excavation. Numerical modelling showed that the largest gain in groundwater dynamics and seepage was attained when both measures were applied together. The effect of organic soil amendments on groundwater dynamics and nutrient cycling was further explored in a large scale in situ mesocosm experiment. Where the soil was amended, groundwater drained deeper and nitrogen removal increased. For new tidal marsh restoration projects, we advise to conduct an explorative soil study. When the soil is heavily compacted, design measures, such as creek initiation and organic soil amendments can be applied to jumpstart the contribution to water quality improvement of newly restored tidal marshes. |
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UA @ admin @ c:irua:196965 |
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8884 |
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Drăgan, A.-M. |
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Investigation of the electrochemical behaviour of illicit substances and their redox pathways in the development of nanomaterial-modified platforms for decentralized analysis |
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Doctoral thesis |
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2023 |
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169 p. |
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Doctoral thesis; Pharmacology. Therapy; Engineering sciences. Technology; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab) |
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UA @ admin @ c:irua:199086 |
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8892 |
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Shi, P.; Gielis, J.; Niklas, K.J.; Niinemets, Ü.; Schrader, J. |
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Leaf functional traits : ecological and evolutionary implications |
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ME3 Book as editor |
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2023 |
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185 p. |
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ME3 Book as editor; Sustainable Energy, Air and Water Technology (DuEL) |
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2023-04-14 |
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978-2-8325-2086-4; 1664-8714 |
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UA @ admin @ c:irua:198002 |
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8894 |
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De Meyer, S. |
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Macroscopic X-ray powder diffraction in reflection mode : a new technique for chemical imaging of artworks |
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Doctoral thesis |
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2023 |
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285 p. |
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Doctoral thesis; Engineering sciences. Technology; Art; Antwerp X-ray Imaging and Spectroscopy (AXIS) |
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Scientific research into cultural heritage has significantly grown in importance over the past decades. The growing popularity of macroscopic imaging techniques such as X-ray fluorescence or Fourier transform infrared now means that conservators and restorers have access to highly objective information on the chemical composition of a painting without the necessity for destructive sampling. As many works of art are heterogeneous on the macroscopic scale, it is clear that solely relying on microscopic samples does not provide sufficiently representative information on the condition of a painting and that macroscopic imaging techniques should be considered a crucial part of the analytical toolkit for conservation science. The goal of this research has been to investigate the added value of reflection-mode macroscopic X-ray powder diffraction (MA-XRPD) for scientific and art historical investigations of cultural heritage artefacts. A prototype scanner was developed after careful consideration of the individual components. This mobile instrument allows for the analysis of flat objects such as oil paintings with reflection MA-XRPD. In this manner images can be obtained that show the distribution of crystalline components present at the surface of the stratigraphy. These crystalline materials can originate from different sources and include original pigments and non-original pigments. MA-XRPD offers novel insights into original pigments such as ultramarine, copper sulfates and lead white. In Girl with a Pearl Earring by Vermeer the MA-XRPD instrument was used to prove that Vermeer used multiple subtypes of lead white to achieve subtle optical effects while in the painting The Night Watch by Rembrandt the lead white composition was studied in detail; multiple rare lead-based compounds were identified that could be linked to the usage of specific driers in the oil paint. By investigating the presence of degradation products, MA-XRPD can be used to assess the conservation state of an artwork. Secondary alteration products were identified in paintings by Nellius and Mignon, explaining why the paintings had visually deteriorated over time. MA-XRPD registered the presence of lead arsenates which were formed from the original yellow arsenic-based orpiment. By combining microscopic and macroscopic analysis, a chemical degradation pathway for the conversion of the unstable orpiment pigment was proposed. In this manner, MA-XRPD can also be used to provide highly valuable information for conservators and restorers by pinpointing areas that have undergone degradation and to guide sampling campaigns. |
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UA @ admin @ c:irua:198766 |
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8896 |
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Ysebaert, T. |
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Modelling and experimental validation of deposition on vegetation to facilitate urban particulate matter mitigation |
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Doctoral thesis |
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2023 |
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xxvi, 234 p. |
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Doctoral thesis; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL) |
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Exposure to air pollution, such as particulate matter (PM), causes adverse health effects, particularly to the respiratory tract and cardiovascular system. PM is the collective name for all kinds of particles ranging from small particles and liquid droplets, which contain organic compounds, acids and metals, to soil or dust particles. One distinguishes PM10, PM2.5 and PM0.1, which have aerodynamic particle sizes smaller than 10, 2.5 and 0.1 µm, respectively. It is mainly the latter that is the most harmful, as PM0.1 penetrates deep into the respiratory system and carries relatively more toxic substances than the other PM fractions. Over a 15-year period, PM concentrations in European member states have fallen by about 30%. Nevertheless, the World Health Organisation (WHO) air quality guidelines, which became stricter in 2021, are exceeded in most places around the world. Particularly in cities, excessive levels of PM are measured and it is here that PM mitigation should be investigated. For this, the implementation of urban green infrastructure, including trees, shrubs, green roofs and green walls, is being looked at. Plants hinder airflow and remove PM from the air by deposition on their leaves and branches. This process is known as dry deposition. Plants can capture PM very efficiently, due to their complex structure of leaves and branches. Green walls offer significant advantages over other types of urban green infrastructure because they can grow on the huge available wall area and, because they do not hinder air circulation, as we sometimes see with trees. Green walls are believed to have a much greater, untapped potential to reduce PM pollution. However, a literature review showed that we do not know the quantitative impact of green walls and lack the tools and/or general methodology to do so. The objective of this thesis is therefore to develop a method for assessing PM removal by green walls, based on predictive models and based on relevant parameters that are experimentally determined. Computational fluid dynamics (CFD) is a numerical method to simulate airflow in complex environments such as cities. These models can also simulate the vegetation-wind interaction in detail and are interesting tools to assess the effect of green walls on PM concentrations in real environments. It is important to first study the aerodynamic effect of green walls and parameterise it correctly in CFD models. Plants decrease the wind speed and create turbulence through a combination of viscous and form drag, which are determined by the permeability (K) and drag coefficient (Cd), respectively. Wind tunnel experiments were conducted with three commonly found climbers (Hedera helix, Parthenocissus tricuspidata and Parthenocissus quinquefolia) and the variation of leaf area density was investigated for two of them. It was observed that the air resistance depended on plant species, leaf area density and wind speed. The difference between the plant species was assigned to the functional leaf size (FLS), the ratio of the largest circle within the boundaries of the leaf to the total leaf area. FLS is likely associated with other morphological characteristics of plants that, when considered collectively, provide a more comprehensive representation of leaf complexity. The pressure and velocity measurements obtained were used to optimise the permeability and drag coefficient in a CFD model. At wind speeds below 0.6 m s-1, the resistance was mainly determined by viscous drag and a larger leaf size resulted in a higher viscous drag. At wind speeds above 1.5 m s-1, form drag was dominant and the parameterised Cd decreased with increasing wind speed due to the sheltering effect of successive plant elements. The leaf area density had a significant effect on K and Cd and, is therefore an important plant parameters in CFD models. The main conclusion here is that the common practice of using a constant Cd to model the influence of plants on the air flow leads to deviations from reality. Wind tunnels are highly suitable to study the impact of green walls on PM concentration under controlled environmental conditions. For this purpose, a new wind tunnel setup was built and great attention was paid to obtaining a uniform air flow. Thus, based on CFD models, appropriate flow controllers were chosen, consisting of honeycombs and screens with different mesh sizes. New PM generation devices and measuring equipment were installed and set up appropriately. Devices were available for generating and measuring ultrafine dust (<0.1 µm, i.e. PM0.1) and fine dust (<0.3 µm, i.e. PM0.3) consisting of soot particles, and, on the other hand, fine dust with particle sizes smaller than 2.5 (PM2.5) and 10 µm (PM10) consisting of 'Arizona fine test dust'. With the new wind tunnel setup, it was possible to measure the influence of Hedera helix (common ivy), grown in a planter against a climbing aid, on the PM concentration and this was expressed by a collection efficiency, i.e. the difference in concentration in front and behind the plants normalised for the incoming concentration. The collection efficiency of H. helix depended on the particle size of the PM and wind speed. The collection efficiency decreased when the particle size increased from 0.02 to 0.2 µm and increased again for particle sizes above 0.3 µm. The collection efficiency also increased with increasing wind speed, especially for particle sizes > 0.03 µm. On the other hand, relative humidity and the type of PM (soot or dust) did not significantly affect the collection efficiency. The main objective of this study was to obtain an optimised size-resolved deposition model. Dry deposition occurs through several mechanisms, in particular gravity, diffusion, impaction and interception, and the subsequent resuspension of deposited PM back to the environment. The modelling of these mechanisms was described by \citet{Zhang2001} and \citet{Petroff2010}. The data obtained from the wind tunnel experiments allowed validating these deposition models. It was for the first time that deposition of real PM on green walls was studied. The different PM deposition mechanisms were found to be strongly dependent on particle size and wind speed. The models of \citet{Zhang2001} and \citet{Petroff2010} each matched PM concentration measurements for only certain particle sizes. Therefore, a combination of the two models was investigated and the root mean square error was lower by on average 3.5% (PM < 0.03 µm) and 46% (PM > 0.03 µm) compared to the original models at wind speeds greater than 1.5 m s-1. For wind speeds less than 1.5 m s-1, the optimised model did not differ from the original models. The optimised model was able to meet the imposed criteria for air quality models, where a correct model exhibits low deviation from measurements ('normalised mean square error' < 1.5), low bias ('fractional bias' between -0.3 and 0.3) and high R2. In comparison, the R$2$ of the optimised model was 0.57, while that of Zhang et al. (2001) and Petroff et al. (2010) was 0.23 and 0.31, respectively. The optimised model was however characterised by a high scatter, with the fraction of modeled results located within a factor of two of the measurements being lower than 50. A model study with a green façade oriented parallel to the incoming airflow showed that deposition by interception and impaction reduced remarkably, but that the orientation had no effect on deposition by Brownian diffusion. A promising green wall form for PM mitigation is the living wall system (LWS). LWS consist of supporting structures with substrate to grow plants in and can be planted with a variety of plant species. This allows to select plant species with optimal characteristics to achieve PM deposition. These characteristics refer to the macro- and microstructure of the leaves, and research has been conducted mainly on these. On the other hand, the influence of the supporting structure and substrate on PM concentrations has rarely been studied. With the new wind tunnel setup, LWS from different manufacturers were tested for their ability to capture PM. The setups were subjected for three hours to an air flow with a low PM concentration (resuspension phase) and then for three hours to an air flow to which additional PM was added (deposition phase). Some setups were able to decrease the PM concentration during both phases, while others just caused the concentration to increase. Some systems were able to reduce particulate matter concentration during both phases, namely LWS consisting of planters (-2% and -4% for PM0.1 and PM2.5, respectively) and textile cloths (-23% and -5% for PM0.1 and PM2.5, respectively). While other systems actually resulted in an increase in concentration especially LWS existing textile fabrics consisting of geotextiles (+11% for both PM fractions) and with moss as substrate (+2% and +5% for PM0.1 and PM2.5, respectively). This highlights the importance of careful selection of suspension systems to reduce particulate matter concentrations. Further research is therefore needed on the materials used in these systems in relation to their particulate content, as well as on plant development in these systems. In addition to air measurements, measurements were taken of the amount of PM deposited on the leaves and suspension system of LWS. This allowed the difference in PM resuspension and deposition between plant species to be investigated. The amount of deposited particulate matter was determined based on 'saturation isothermal remanent magnetisation' (SIRM), a measure of magnetisable particulate matter. This was possible because the added 'Arizona fine test dust' contained iron oxide. However, no significant difference was observed between the SIRM values measured before the wind tunnel experiment, after resuspension and after deposition. This suggested that the iron oxide content in the Arizona fine test dust was too low to measure a significant difference in the SIRM values on leaves after three hours. The plant species did give rise to different SIRM values ranging between 5 and 260 µ A. In particular, SIRM values above 26 µ A were observed for the plant species that were grouped due to their significantly higher accumulation of PM. 'Specific leaf area' (SLA), specifically the ratio of the one-sided 'fresh' leaf area to its dry mass, was the significant leaf characteristic. SLA correlated with leaf complexity. In particular, plant species with elongated leaves were characterized by low SLA, high FLS and high complexity and showed significantly higher SIRM values. Finally, the optimised size-resolved deposition model was also tested in an urban model to get an idea of the impact of a green wall on PM concentrations in a so-called 'street canyon'. These are narrow streets with high buildings on both sides, making air pollution more persistent. To this end, an ideal scenario was tested in which a green wall was introduced along both sides of the street over a length of about 270 m. The model result showed a decrease in PM2.5 and PM10 of 46 ± 12% and 52 ± 14%. This result is of course for a very optimal scenario where the green wall covers the entire building façades. Since this is not feasible in reality, other ways of promoting contact between green walls and polluted air can be explored. The insights obtained illustrate that the use of climbing plants can be a cost-effective and environmentally friendly solution to reduce PM concentrations. Moreover, the findings showed that models can be used to investigate the impact of green walls on PM levels. These findings fit within the broader context of designing healthy and sustainable urban environments and developing innovative solutions based on solid scientific knowledge. |
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UA @ admin @ c:irua:199439 |
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8900 |
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