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Author | Ghasemitarei, M. | ||||
Title | Study of the interaction of plasma radicals with malignant tumor cells by means of Molecular Dynamics simulation | Type | Doctoral thesis | ||
Year | 2019 | Publication | Abbreviated Journal | ||
Volume | Issue | Pages | 117 p. | ||
Keywords | Doctoral thesis; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | abstract not available | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | |||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | ISBN | Additional Links | UA library record | ||
Impact Factor | Times cited | Open Access | |||
Notes | Approved | no | |||
Call Number | UA @ admin @ c:irua:164763 | Serial | 8606 | ||
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Author | Van Loenhout, J. | ||||
Title | Targeting pancreatic ductal adenocarcinoma and glioblastoma with oxidative stress-mediated treatment strategies : focus on tumor cell death and modulation of the tumor microenvironment | Type | Doctoral thesis | ||
Year | 2021 | Publication | Abbreviated Journal | ||
Volume | Issue | Pages | 167 p. | ||
Keywords | Doctoral thesis; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Center for Oncological Research (CORE) | ||||
Abstract | Pancreatic ductal adenocarcinoma (PDAC) and glioblastoma multiforme (GBM) are two of the most malignant solid tumor types with poor survival rates, which underscore the urgency of novel and efficacious treatment strategies. Within the last decade, immunotherapy has been established as a breakthrough in cancer therapy. This mainly has been driven by the clinical data and approval associated with several immune checkpoint inhibitors (e.g. anti-CTLA-4 and anti-PD-1/L1). Despite the clinical benefit in specific tumor types, these inhibitors have not yet fulfilled their promise in low immunogenic tumors such as PDAC and GBM. Oxidative stress in cancer cells due to elevated reactive oxygen species (ROS) and an inability to balance intracellular redox state has recently been highlighted as promising target for anticancer treatment strategies with possible immunogenic effects. In this PhD dissertation, I investigated novel oxidative stress-mediated treatment approaches to target PDAC and GBM and to enhance immunogenicity by inducing immunogenic cell death (ICD). In the first part of this thesis (chapter 2), I reviewed the mechanistic responses of cancer cells towards different oxidative stress-inducing treatment strategies and their immunomodulating effects. The resulting literature demonstrated that different exogenous and endogenous ROS-inducing therapies show direct and indirect immunomodulating effects, which can be either immunostimulatory or immunosuppressive. One of the indirect immunostimulatory effects of the ROS-mediating therapies is the capacity of inducing immunogenic cell death (ICD) in tumor cells, which can increase the immunogenicity and consequently can trigger an antitumoral immune response. In chapter 3, I investigated a novel exogenous ROS-inducing treatment method, namely cold atmospheric plasma, to determine the therapeutic and ICD-inducing effects in PDAC, in vitro. I revealed that plasma-treated PBS (pPBS) has the potential to induce ICD in pancreatic cancer cells (PCCs) and to reduce the immunosuppressive tumor microenvironment (TME) by attacking the tumor supportive pancreatic stellate cells (PSCs). Although the cell death induced in PSCs was non-immunogenic as seen by the lack of danger-associated molecular patterns (DAMPs) emission and DC activation, I showed that pPBS could disrupt the physical barrier and lower the immunosuppressive secretion profile (lower TGF-β) of PSCs. In contrast, DAMPs were released by PCCs after treatment with pPBS which resulted in activation and maturation of DCs and a more immunostimulatory secretion profile (higher TNF-α, IFN-γ). Hence, indirect plasma treatment via pPBS has the potential to enhance immunogenicity in PDAC by triggering ICD and by attacking the immunosuppressive PSCs. Tumor cells can evolve adaptation mechanisms to protect themselves against intrinsic oxidative stress by upregulation of pro-survival molecules and their antioxidant defense system to maintain the redox balance. As such, tumor cells can become resistant towards exogenous ROS-inducing therapies, like plasma. Dual targeting of the redox balance of tumor cells by increasing exogenous levels of ROS and inhibiting the antioxidant defense system can maximally exploit ROS-mediated cell death mechanisms as therapeutic anticancer strategy. In this regard, cold atmospheric plasma was combined with auranofin, a thioredoxin reductase inhibitor, in GBM (chapter 4). A synergistic effect was shown after this combination treatment in 2D and 3D, however, in 3D only high concentrations of auranofin synergized with plasma treatment. I confirmed a ROS-mediated response after combination treatment, which was able to induce distinct cell death mechanisms, specifically apoptosis and ferroptosis. Additionally, the auranofin and plasma combined treatment strategy induced cell death, which resulted in an increased release of DAMPs. Together with the observed DC maturation, these results indicates the potential increase in immunogenicity, though, the phagocytotic capacity of DCs was inhibited by auranofin. In chapter 5, I evaluated this promising oxidative stress combination therapy in GBM, in vivo. A decrease in tumor kinetics and an increased survival in GBM-bearing mice was observed when auranofin was sequentially combined with direct plasma treatment. No T cell infiltration was observed after auranofin monotherapy. However, further characterization of the TME after the combination therapy is necessary to provide more insight in the immunogenic effects in vivo. In conclusion, this PhD dissertation comprises novel and important therapeutic and immunogenic insights in cold atmospheric plasma and auranofin as promising oxidative stress-mediated treatment strategies for low immunogenic tumors, like PDAC and GBM. These preclinical results provide a solid basis for future research towards combinations with immunotherapeutic approaches. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | |||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | ISBN | Additional Links | UA library record | ||
Impact Factor | Times cited | Open Access | |||
Notes | Approved | Most recent IF: NA | |||
Call Number | UA @ admin @ c:irua:181309 | Serial | 8643 | ||
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Author | Xu, W. | ||||
Title | Plasma-catalytic DRM : study of LDH derived catalyst for DRM in a GAP plasma system | Type | Doctoral thesis | ||
Year | 2023 | Publication | Abbreviated Journal | ||
Volume | Issue | Pages | 350 p. | ||
Keywords | Doctoral thesis; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Plasma is considered one of the promising technologies to solve greenhouse gas problems, as it can activate CO2 and CH4 at relatively low temperatures. Among the various types of plasmas, the gliding arc plasmatron (GAP) is promising, as it has a high level of non-equilibrium and high electron density. Nevertheless, the conversion of CO2 and CH4 in the GAP reactor is limited. Therefore, combining the GAP reactor with catalysts and making use of the heat produced by the plasma to provide thermal energy to the catalyst, forming a post-plasma catalytic (PPC) system, is hypothesized to improve its performance. Therefore, in this PhD research, we investigate important aspects of the PPC concept towards the use of the heat produced by GAP plasma to heat the plasma bed, without additional energy input. Aiming at this, based on a literature study (chapter 1), Ni-loaded layered double hydroxide (LDH) derived catalyst with good thermal catalytic DRM performance were chosen as the catalyst material. Before applying the LDH as a support material, the rehydration property of calcined LDH in moist and liquid environment was studied as part of chapter 2. The data indicated that after high temperatures calcination (600-900 C), the obtained layered double oxides (LDOs) can rehydrate into LDH, although, the rehydrated LDH were different from the original LDH. In chapter 3, different operating conditions, such as gas flow rate, gas compositions (e.g. CH4/CO2 ratio and nitrogen dilution), and addition of H2O were studied to investigate optimal conditions for PPC DRM, identifying possible differences in temperature profiles and exhaust gas compositions that might influence the catalytic performance. Subsequently, the impact of different PPC configurations, making use of the heat and exhaust gas composition produced by the GAP plasma, is shown in Chapter 4. Experiments studying the impact of adjusting the catalyst bed distance to the post-plasma, the catalyst amount, the influence of external heating (below 250 C) and the addition of H2O are discussed. As only limited improvement in the performance was achieved, a new type of catalyst bed was designed and utilized, as described in chapter 5. This improved configuration can realize better heat and mass transfer by directly connecting to the GAP device. The performance was improved and became comparable to the traditional thermal catalytic DRM results obtained at 800 C, although obtained by a fully electrically driven plasma. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | |||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | ISBN | Additional Links | UA library record | ||
Impact Factor | Times cited | Open Access | |||
Notes | Approved | Most recent IF: NA | |||
Call Number | UA @ admin @ c:irua:201534 | Serial | 9074 | ||
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Author | Vervloessem, E. | ||||
Title | The role of pulsing and humidity in plasma-based nitrogen fixation : a combined experimental and modeling study | Type | Doctoral thesis | ||
Year | 2023 | Publication | Abbreviated Journal | ||
Volume | Issue | Pages | 358 p. | ||
Keywords | Doctoral thesis; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Nitrogen (N) is an indispensable building block for all living organisms as well as for pharmaceutical and chemical industry. In a nutshell, N is needed for plants to grow and beings to live and nitrogen fixation (NF) is the process that makes N available for plants as food by converting N2 into a reactive form, such as ammonia (NH3) or nitrogen oxides (NOx), upon reacting with O2 and H2. The aim of this thesis is to elucidate (wet) plasma-based nitrogen fixation with a focus on (1) the role of pulsing in achieving low energy consumption, (2) the role of H2O as a hydrogen source in nitrogen fixation and (3) elucidation of nitrogen fixation pathways in humid air and humid N2 plasma in a combined experimental and computational study. Furthermore, this thesis aims to take into account the knowledge-gaps and challenges identified in the discussion of the state of the art. Specifically, (1) we put our focus on branching out to another way of introducing water into the plasma system, i.e. H2O vapor, (2) we de-couple the problem for pathway elucidation by starting with characterization of the chosen plasma, next a simpler gas mixture and building up from there, (3) we include modelling, though not under wet conditions and (4) we focus on also analyzing species and performance outside liquid H2O. Firstly, based on the reaction analysis of a validated quasi-1D model, we can conclude that pulsing is indeed the key factor for energy-efficient NOx- formation, due to the strong temperature drop it causes. Secondly, the thesis shows that added H2O vapor, and not liquid H2O, is the main source of H for NH3 generation. Related to this, we discuss how the selectivity of plasma-based NF in humid air and humid N2 can be controlled by changing the humidity in the feed gas. Interestingly, NH3 production can be achieved in both N2 and air plasmas using H2O as a H source. Lastly, we identified a significant loss mechanism for NH3 and HNO2 that occurs in systems where these species are synthesized simultaneously, i.e. downstream from the plasma, HNO2 reacts with NH3 to form NH4NO2, which decomposes into N2 and H2O. This reduces the effective NF when not properly addressed, and should therefore be considered in future works aimed at optimizing plasma-based NF. In conclusion, this thesis adds further to the current state of the art of plasma-based NF both in the presence of H2O and in dry systems. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | |||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | ISBN | Additional Links | UA library record | ||
Impact Factor | Times cited | Open Access | |||
Notes | Approved | Most recent IF: NA | |||
Call Number | UA @ admin @ c:irua:197038 | Serial | 9088 | ||
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Author | Grünewald, L.; Chezganov, D.; De Meyer, R.; Orekhov, A.; Van Aert, S.; Bogaerts, A.; Bals, S.; Verbeeck, J. | ||||
Title | Supplementary Information for “In-situ Plasma Studies using a Direct Current Microplasma in a Scanning Electron Microscope” | Type | Dataset | ||
Year | 2023 | Publication | Abbreviated Journal | ||
Volume | Issue | Pages | |||
Keywords | Dataset; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Supplementary information for the article “In-situ Plasma Studies using a Direct Current Microplasma in a Scanning Electron Microscope” containing the videos of in-situ SEM imaging (mp4 files), raw data/images, and Jupyter notebooks (ipynb files) for data treatment and plots. Link to the preprint: https://doi.org/10.48550/arXiv.2308.15123 Explanation of the data files can be found in the Information.pdf file. The Videos folder contains the in-situ SEM image series mentioned in the paper. If there are any questions/bugs, feel free to contact me at lukas.grunewaldatuantwerpen.be | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | |||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | ISBN | Additional Links | UA library record | ||
Impact Factor | Times cited | Open Access | Not_Open_Access | ||
Notes | Approved | Most recent IF: NA | |||
Call Number | UA @ admin @ c:irua:203389 | Serial | 9100 | ||
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Author | Biondo, O. | ||||
Title | Towards a fundamental understanding of energy-efficient, plasma-based CO<sub>2</sub> conversion | Type | Doctoral thesis | ||
Year | 2023 | Publication | Abbreviated Journal | ||
Volume | Issue | Pages | 221 p. | ||
Keywords | Doctoral thesis; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Plasma-based CO2 conversion is worldwide gaining increasing interest. The aim of this work is to find potential pathways to improve the energy efficiency of plasma-based CO2 conversion beyond what is feasible for thermal chemistry. To do so, we use a combination of modeling and experiments to better understand the underlying mechanisms of CO2 conversion, ranging from non-thermal to thermal equilibrium conditions. Zero-dimensional (0D) chemical kinetics modelling, describing the detailed plasma chemistry, is developed to explore the vibrational kinetics of CO2, as the latter is known to play a crucial role in the energy efficient CO2 conversion. The 0D model is successfully validated against pulsed CO2 glow discharge experiments, enabling the reconstruction of the complex dynamics underlying gas heating in a pure CO2 discharge, paving the way towards the study of gas heating in more complex gas mixtures, such as CO2 plasmas with high dissociation degrees. Energy-efficient, plasma-based CO2 conversion can also be obtained upon the addition of a reactive carbon bed in the post-discharge region. The reaction between solid carbon and O2 to form CO allows to both reduce the separation costs and increase the selectivity towards CO, thus, increasing the energy efficiency of the overall conversion process. In this regard, a novel 0D model to infer the mechanism underlying the performance of the carbon bed over time is developed. The model outcome indicates that gas temperature and oxygen complexes formed at the surface of solid carbon play a fundamental and interdependent role. These findings open the way towards further optimization of the coupling between plasma and carbon bed. Experimentally, it has been demonstrated that “warm” plasmas (e.g. microwave or gliding arc plasmas) can yield very high energy efficiency for CO2 conversion, but typically only at reduced pressure. For industrial application, it will be important to realize such good energy efficiency at atmospheric pressure as well. However, recent experiments illustrate that the microwave plasma at atmospheric pressure is too close to thermal conditions to achieve a high energy efficiency. Hence, we use a comprehensive set of advanced diagnostics to characterize the plasma and the reactor performance, focusing on CO2 and CO2/CH4 microwave discharges. The results lead to a deeper understanding of the mechanism of power concentration with increasing pressure, typical of plasmas in most gases, which is of great importance for model validation and understanding of reactor performance. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | |||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | ISBN | Additional Links | UA library record | ||
Impact Factor | Times cited | Open Access | |||
Notes | Approved | Most recent IF: NA | |||
Call Number | UA @ admin @ c:irua:197213 | Serial | 9108 | ||
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Author | Ahmadi Eshtehardi, H. | ||||
Title | Combined computational-experimental study on plasma and plasma catalysis for N2 fixation | Type | Doctoral thesis | ||
Year | 2024 | Publication | Abbreviated Journal | ||
Volume | Issue | Pages | 160 p. | ||
Keywords | Doctoral thesis; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | 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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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2024-06-14 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | ISBN | Additional Links | UA library record | ||
Impact Factor | Times cited | Open Access | |||
Notes | Approved | Most recent IF: NA | |||
Call Number | UA @ admin @ c:irua:205246 | Serial | 9139 | ||
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Author | De Luca, F.; Abate, S.; Bogaerts, A.; Centi, G. | ||||
Title | Electrified CO2 conversion : integrating experimental, computational, and process simulation methods for sustainable chemical synthesis | Type | Doctoral thesis | ||
Year | 2024 | Publication | Abbreviated Journal | ||
Volume | Issue | Pages | xv, 152 p. | ||
Keywords | Doctoral thesis; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | 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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Language | Wos | Publication Date | |||
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Series Volume | Series Issue | Edition | |||
ISSN | ISBN | Additional Links | UA library record | ||
Impact Factor | Times cited | Open Access | |||
Notes | Approved | Most recent IF: NA | |||
Call Number | UA @ admin @ c:irua:205262 | Serial | 9147 | ||
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Author | Tsonev, I.; Ahmadi Eshtehardi, H.; Delplancke, M.-P.; Bogaerts, A. | ||||
Title | Importance of geometric effects in scaling up energy-efficient plasma-based nitrogen fixation | Type | A1 Journal article | ||
Year | 2024 | Publication | Sustainable energy & fuels | Abbreviated Journal | |
Volume | Issue | Pages | 1-19 | ||
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Despite the recent promising potential of plasma-based nitrogen fixation, the technology faces significant challenges in efficient upscaling. To tackle this challenge, we investigate two reactors, i.e., a small one, operating in a flow rate range of 5-20 ln min-1 and current range of 200-500 mA, and a larger one, operating at higher flow rate (100-300 ln min-1) and current (400-1000 mA). Both reactors operate in a pin-to-pin configuration and are powered by direct current (DC) from the same power supply unit, to allow easy comparison and evaluate the effect of upscaling. In the small reactor, we achieve the lowest energy cost (EC) of 2.8 MJ mol-1, for a NOx concentration of 1.72%, at a flow rate of 20 ln min-1, yielding a production rate (PR) of 33 g h-1. These values are obtained in air; in oxygen-enriched air, the results are typically better, at the cost of producing oxygen-enriched air. In the large reactor, the higher flow rates reduce the NOx concentration due to lower SEI, while maintaining a similar EC. This stresses the important effect of the geometrical configuration of the arc, which is typically concentrated in the center of the reactor, resulting in limited coverage of the reacting gas flow, and this is identified as the limiting factor for upscaling. However, our experiments reveal that by changing the reactor configuration, and thus the plasma geometry and power deposition mechanisms, the amount of gas treated by the plasma can be enhanced, leading to successful upscaling. To obtain more insights in our experiments, we performed thermodynamic equilibrium calculations. First of all, they show that our measured lowest EC closely aligns with the calculated minimum thermodynamic equilibrium at atmospheric pressure. In addition, they reveal that the limited NOx production in the large reactor results from the contracted nature of the plasma. To solve this limitation, we let the large reactor operate in so-called torch configuration. Indeed, the latter enhances the NOx concentrations compared to the pin-to-pin configuration, yielding a PR of 80 g h-1 at an EC of 2.9 MJ mol-1 and NOx concentration of 0.31%. This illustrates the importance of reactor design in upscaling. With the focus on feasibility evaluation of scaling-up plasma-based nitrogen fixation by combined experiments and thermodynamic modelling, we aim to tackle the challenge of design and development of an energy-efficient and scaled-up plasma reactor. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 001203657700001 | Publication Date | 2024-04-11 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | ISBN | Additional Links | UA library record; WoS full record | ||
Impact Factor | Times cited | Open Access | |||
Notes | Approved | Most recent IF: NA | |||
Call Number | UA @ admin @ c:irua:205435 | Serial | 9155 | ||
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Author | Long, Y.; Wang, X.; Zhang, H.; Wang, K.; Ong, W.-L.; Bogaerts, A.; Li, K.; Lu, C.; Li, X.; Yan, J.; Tu, X.; Zhang, H. | ||||
Title | Plasma chemical looping : unlocking high-efficiency CO₂ conversion to clean CO at mild temperatures | Type | A1 Journal article | ||
Year | 2024 | Publication | JACS Au | Abbreviated Journal | |
Volume | Issue | Pages | |||
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | We propose a plasma chemical looping CO2 splitting (PCLCS) approach that enables highly efficient CO2 conversion into O-2-free CO at mild temperatures. PCLCS achieves an impressive 84% CO2 conversion and a 1.3 mmol g(-1) CO yield, with no O-2 detected. Crucially, this strategy significantly lowers the temperature required for conventional chemical looping processes from 650 to 1000 degrees C to only 320 degrees C, demonstrating a robust synergy between plasma and the Ce0.7Zr0.3O2 oxygen carrier (OC). Systematic experiments and density functional theory (DFT) calculations unveil the pivotal role of plasma in activating and partially decomposing CO2, yielding a mixture of CO, O-2/O, and electronically/vibrationally excited CO2*. Notably, these excited CO2* species then efficiently decompose over the oxygen vacancies of the OCs, with a substantially reduced activation barrier (0.86 eV) compared to ground-state CO2 (1.63 eV), contributing to the synergy. This work offers a promising and energy-efficient pathway for producing O-2-free CO from inert CO2 through the tailored interplay of plasma and OCs. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 001225139200001 | Publication Date | 2024-05-08 | |
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Series Volume | Series Issue | Edition | |||
ISSN | ISBN | Additional Links | UA library record; WoS full record | ||
Impact Factor | Times cited | Open Access | |||
Notes | Approved | Most recent IF: NA | |||
Call Number | UA @ admin @ c:irua:205970 | Serial | 9166 | ||
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Author | Manaigo, F. | ||||
Title | Study of a gliding arc discharge for sustainable nitrogen fixation into NOx | Type | Doctoral thesis | ||
Year | 2024 | Publication | Abbreviated Journal | ||
Volume | Issue | Pages | xxiv, 114 p. | ||
Keywords | Doctoral thesis; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | 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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Language | Wos | Publication Date | |||
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Series Volume | Series Issue | Edition | |||
ISSN | ISBN | Additional Links | UA library record | ||
Impact Factor | Times cited | Open Access | |||
Notes | Approved | Most recent IF: NA | |||
Call Number | UA @ admin @ c:irua:205259 | Serial | 9175 | ||
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Author | O'Modhrain, C.; Trenchev, G.; Gorbanev, Y.; Bogaerts, A. | ||||
Title | Upscaling plasma-based CO₂ conversion : case study of a multi-reactor gliding arc plasmatron | Type | A1 Journal article | ||
Year | 2024 | Publication | ACS Engineering Au | Abbreviated Journal | |
Volume | Issue | Pages | |||
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Atmospheric pressure plasmas have shifted in recent years from being a burgeoning research field in the academic setting to an actively investigated technology in the chemical, oil, and environmental industries. This is largely driven by the climate change mitigation efforts, as well as the evident pathways of value creation by converting greenhouse gases (such as CO2) into useful chemical feedstock. Currently, most high technology readiness level (TRL) plasma-based technologies are based on volumetric and power-based scaling of thermal plasma systems, which results in large capital investment and regular maintenance costs. This work investigates bringing a quasi-thermal (so-called “warm”) plasma setup, namely, a gliding arc plasmatron, from a lab-scale to a pilot-scale capacity with an increase in throughput capacity by a factor of 10. The method of scaling is the parallelization of plasmatron reactors within a single housing, with the aim of maintaining a warm plasma regime while simultaneously improving build cost and efficiency (compared to separate reactors operating in parallel). Special attention is also given to the safety and control features implemented in the setup, a key component required for integration into industrial systems. The performance of the multi-reactor gliding arc plasmatron (MRGAP) reactor is investigated, focusing on the influence of flow rate and the number of active reactors. The location of active reactors was deemed to have a negligible effect on the monitored metrics of conversion, energy efficiency, and energy cost. The optimum operating conditions were found to be with the most active reactors (five) at the highest investigated flow rate (80 L/min). Analysis of results suggests that an optimum conversion (9%) and plug power-based energy efficiency (19%) can be maintained at a specific energy input (SEI) around 5.3 kJ/L (or 1 eV/molecule). The concept of parallelization of plasmatron reactors within a singular housing was demonstrated to be a viable method for scaling up from a lab-scale to a prototype-scale device, with performance analysis suggesting that increasing the power (through adding more reactor channels) and total flow rate, while maintaining an SEI around 5.3 or 4.2 kJ/L, i.e., 1.3 or 1 eV/molecule (based on plug power and plasma-deposited power, respectively), can result in increased conversion rate without sacrificing absolute conversion or energy efficiency. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 001166625200001 | Publication Date | 2024-02-14 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | ||
Impact Factor | Times cited | Open Access | |||
Notes | Approved | Most recent IF: NA | |||
Call Number | UA @ admin @ c:irua:204749 | Serial | 9182 | ||
Permanent link to this record | |||||
Author | Oleshko, V.; Schryvers, D.; Gijbels, R.; Jacob, W. | ||||
Title | Investigation of Ag, Ag2S and Ag(Br,I) small particles by HREM and AEM | Type | H3 Book chapter | ||
Year | 1998 | Publication | Abbreviated Journal | ||
Volume | Issue | Pages | 293-294 | ||
Keywords | H3 Book chapter; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | |||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | s.l. | Editor | ||
Language | Wos | Publication Date | 0000-00-00 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | ISBN | Additional Links | UA library record | ||
Impact Factor | Times cited | Open Access | |||
Notes | Approved | Most recent IF: NA | |||
Call Number | UA @ lucian @ c:irua:20553 | Serial | 1729 | ||
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Author | Wendelen, W.; Autrique, D.; Bogaerts, A. | ||||
Title | Space charge limited electron emission from a Cu surface under ultrashort pulsed laser irradiation | Type | A1 Journal article | ||
Year | 2010 | Publication | AIP conference proceedings | Abbreviated Journal | |
Volume | 1278 | Issue | Pages | 407-415 | |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | In this theoretical study, the electron emission from a copper surface under ultrashort pulsed laser irradiation is investigated using a one dimensional particle in cell model. Thermionic emission as well as multi-photon photoelectron emission were taken into account. The emitted electrons create a negative space charge above the target, consequently the generated electric field reduces the electron emission by several orders of magnitude. The simulations indicate that the space charge effect should be considered when investigating electron emission related phenomena in materials under ultrashort pulsed laser irradiation of metals.the word abstract, but do replace the rest of this text. ©2010 American Institute of Physics | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | New York | Editor | ||
Language | Wos | 000287183900042 | Publication Date | 2010-10-19 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | ISBN | Additional Links | UA library record; WoS full record | ||
Impact Factor | Times cited | Open Access | |||
Notes | Approved | Most recent IF: NA | |||
Call Number | UA @ lucian @ c:irua:88899 | Serial | 3058 | ||
Permanent link to this record | |||||
Author | Bogaerts, A. | ||||
Title | Glow discharge optical spectroscopy and mass spectrometry | Type | H1 Book chapter | ||
Year | 2016 | Publication | Abbreviated Journal | ||
Volume | Issue | Pages | 1-31 | ||
Keywords | H1 Book chapter; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Atomic Spectroscopy Optical (atomic absorption spectroscopy, AAS; atomic emission spectroscopy, AES; atomic fluorescence spectroscopy, AFS; and optogalvanic spectroscopy) and mass spectrometric (magnetic sector, quadrupole mass analyzer, QMA; quadrupole ion trap, QIT; Fourier transform ion cyclotron resonance, FTICR; and time-of-flight, TOF) instrumentation are well suited for coupling to the glow discharge (GD). The GD is a relatively simple device. A potential gradient (500–1500 V) is applied between an anode and a cathode. In most cases, the sample is also the cathode. A noble gas (mostly Ar) is introduced into the discharge region before power initiation. When a potential is applied, electrons are accelerated toward the anode. As these electrons accelerate, they collide with gas atoms. A fraction of these collisions are of sufficient energy to remove an electron from a support gas atom, forming an ion. These ions are, in turn, accelerated toward the cathode. These ions impinge on the surface of the cathode, sputtering sample atoms from the surface. Sputtered atoms that do not redeposit on the surface diffuse into the excitation/ionization regions of the plasma where they can undergo excitation and/or ionization via a number of collisional processes, and the photons or ions created in this way can be detected with optical emission spectroscopy or mass spectrometry. GD sources offer a number of distinct advantages that make them well suited for specific types of analyses. These sources afford direct analysis of solid samples, thus minimizing the sample preparation required for analysis. The nature of the plasma also provides mutually exclusive atomization and excitation processes that help to minimize the matrix effects that plague so many other elemental techniques. In recent years, there is also increasing interest for using GD sources for liquid and gas analyses. In this article, first, the principles of operation of the GD plasma are reviewed, with an emphasis on how those principles relate to optical spectroscopy and mass spectrometry. Basic applications of the GD techniques are considered next. These include bulk analysis, surface analysis, and the analysis of solution and gaseous samples. The requirements necessary to obtain optical information are addressed following the analytical applications. This article focuses on the instrumentation needed to make optical measurements using the GD as an atomization/excitation source. Finally, mass spectrometric instrumentation and interfaces are addressed as they pertain to the use of a GD plasma as an ion source. GD sources provide analytically useful gas-phase species from solid samples. These sources can be interfaced with a variety of spectroscopic and spectrometric instruments for both quantitative and qualitative analyses. | ||||
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Corporate Author | Thesis | ||||
Publisher | John Wiley & Sons | Place of Publication | Chichester | Editor | |
Language | Wos | Publication Date | 0000-00-00 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | ISBN | 978-0-470-02731-8 | Additional Links | UA library record | |
Impact Factor | Times cited | Open Access | |||
Notes | Approved | Most recent IF: NA | |||
Call Number | UA @ lucian @ c:irua:132064 | Serial | 4187 | ||
Permanent link to this record | |||||
Author | Bogaerts, A. | ||||
Title | Glow discharge optical spectroscopy and mass spectrometry | Type | A1 Journal article | ||
Year | 2016 | Publication | Abbreviated Journal | ||
Volume | Issue | Pages | |||
Keywords | A1 Journal article; PLASMANT | ||||
Abstract | Atomic Spectroscopy Optical (atomic absorption spectroscopy, AAS; atomic emission spectroscopy, AES; atomic fluorescence spectroscopy, AFS; and optogalvanic spectroscopy) and mass spectrometric (magnetic sector, quadrupole mass analyzer, QMA; quadrupole ion trap, QIT; Fourier transform ion cyclotron resonance, FTICR; and time-of-flight, TOF) instrumentation are well suited for coupling to the glow discharge (GD). The GD is a relatively simple device. A potential gradient (500–1500 V) is applied between an anode and a cathode. In most cases, the sample is also the cathode. A noble gas (mostly Ar) is introduced into the discharge region before power initiation. When a potential is applied, electrons are accelerated toward the anode. As these electrons accelerate, they collide with gas atoms. A fraction of these collisions are of sufficient energy to remove an electron from a support gas atom, forming an ion. These ions are, in turn, accelerated toward the cathode. These ions impinge on the surface of the cathode, sputtering sample atoms from the surface. Sputtered atoms that do not redeposit on the surface diffuse into the excitation/ionization regions of the plasma where they can undergo excitation and/or ionization via a number of collisional processes, and the photons or ions created in this way can be detected with optical emission spectroscopy or mass spectrometry. GD sources offer a number of distinct advantages that make them well suited for specific types of analyses. These sources afford direct analysis of solid samples, thus minimizing the sample preparation required for analysis. The nature of the plasma also provides mutually exclusive atomization and excitation processes that help to minimize the matrix effects that plague so many other elemental techniques. In recent years, there is also increasing interest for using GD sources for liquid and gas analyses. In this article, first, the principles of operation of the GD plasma are reviewed, with an emphasis on how those principles relate to optical spectroscopy and mass spectrometry. Basic applications of the GD techniques are considered next. These include bulk analysis, surface analysis, and the analysis of solution and gaseous samples. The requirements necessary to obtain optical information are addressed following the analytical applications. This article focuses on the instrumentation needed to make optical measurements using the GD as an atomization/excitation source. Finally, mass spectrometric instrumentation and interfaces are addressed as they pertain to the use of a GD plasma as an ion source. GD sources provide analytically useful gas-phase species from solid samples. These sources can be interfaced with a variety of spectroscopic and spectrometric instruments for both quantitative and qualitative analyses. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2006-09-11 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | ISBN | Additional Links | |||
Impact Factor | Times cited | Open Access | |||
Notes | Approved | Most recent IF: NA | |||
Call Number | PLASMANT @ plasmant @ | Serial | 4282 | ||
Permanent link to this record | |||||
Author | Bogaerts, A.; Snoeckx, R.; Trenchev, G.; Wang, W. | ||||
Title | Modeling for a Better Understanding of Plasma-Based CO2 Conversion | Type | H1 Book Chapter | ||
Year | 2018 | Publication | Plasma Chemistry and Gas Conversion | Abbreviated Journal | |
Volume | Issue | Pages | |||
Keywords | H1 Book Chapter; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | This chapter discusses modeling efforts for plasma-based CO2 conversion, which are needed to obtain better insight in the underlying mechanisms, in order to improve this application. We will discuss two types of (complementary) modeling efforts that are most relevant, that is, (i) modeling of the detailed plasma chemistry by zero-dimensional (0D) chemical kinetic models and (ii) modeling of reactor design, by 2D or 3D fluid dynamics models. By showing some characteristic calculation results of both models, for CO2 splitting and in combination with a H-source, and for packed bed DBD and gliding arc plasma, we can illustrate the type of information they can provide. | ||||
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Corporate Author | Thesis | ||||
Publisher | IntechOpen | Place of Publication | Rijeka | Editor | Britun, N.; Silva, T. |
Language | Wos | Publication Date | 2018-12-19 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | ISBN | Additional Links | UA library record | ||
Impact Factor | Times cited | Open Access | Not_Open_Access | ||
Notes | Approved | Most recent IF: NA | |||
Call Number | PLASMANT @ plasmant @ Bogaerts18c:irua:155915 | Serial | 5142 | ||
Permanent link to this record | |||||
Author | Geuens, I.; Gijbels, R.; Dekeyzer, R.; Verbeeck, A. | ||||
Title | Micro and surface analysis of individual silver halide microcrystals using a scanning ion microprobe | Type | P1 Proceeding | ||
Year | 1994 | Publication | Papers | Abbreviated Journal | |
Volume | Issue | Pages | 27-30 | ||
Keywords | P1 Proceeding; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | |||||
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Corporate Author | Thesis | ||||
Publisher | Soc imaging science technology | Place of Publication | Springfield | Editor | |
Language | Wos | A1994BC23W00013 | Publication Date | 0000-00-00 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0-89208-177-5 | ISBN | Additional Links | UA library record; WoS full record; | |
Impact Factor | Times cited | Open Access | |||
Notes | Approved | PHYSICS, CONDENSED MATTER 16/67 Q1 # | |||
Call Number | UA @ lucian @ c:irua:95946 | Serial | 2021 | ||
Permanent link to this record | |||||
Author | Charlier, E.; Gijbels, R.; Van Doorselaer, M.; De Keyzer, R. | ||||
Title | Functioning of thiocyanate ions during sulphur and sulphur-plus-gold Sensitization | Type | P1 Proceeding | ||
Year | 2000 | Publication | Abbreviated Journal | ||
Volume | Issue | Pages | 172-176 | ||
Keywords | P1 Proceeding; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Not much about the effect of thiocyanate addition on the sulphur ripening is known, although it is used for many applications in photographic practice. Via a combination of tracer analysis and diffuse reflectance spectroscopy the effect of thiocyanate addition on the sulphur and sulphur-plus-gold ripening could be unveiled. When thiocyanate is added prior to the sulphur addition, it appears to rearrange the silver halide surface in such way that the sulphur deposition rate is enhanced, but the supply of interstitials is limited. Addition of thiocyanate after the sulphur reaction results in the formation of thiocyanate complexes with silver, from which a silver ion is more easily deposited in a surface cell of the silver sulphide clusters thus enhancing the sensitization rate. For sulphur-plus-gold sensitized emulsions it was observed that part of the gold ions could be removed out of the Ag2-xAuxS clusters by addition of thiocyanate ions and subsequent washing. Hence, it was concluded that two different types of gold ions are present in the silver sulphide clusters; 1. gold ions which are substitutional for silver (bound between sulphur and bromide ions) 2. gold ions which bridge two or three sulphur atoms. Incorporation of gold ions into silver sulphide clusters suppresses their optical absorption in diffuse reflectance spectroscopy. Since the optical absorption at 505 nm can completely be restored by addition of thiocyanate, it is assumed that the entity absorbing at this wavelength is a monomer of silver sulphide. | ||||
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Publisher | Soc. imaging science technology | Place of Publication | Springfield | Editor | |
Language | Wos | 000183315900047 | Publication Date | 0000-00-00 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0-89208-229-1 | ISBN | Additional Links | UA library record; WoS full record; | |
Impact Factor | Times cited | Open Access | |||
Notes | Approved | Most recent IF: NA | |||
Call Number | UA @ lucian @ c:irua:95775 | Serial | 1307 | ||
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Author | Lenaerts, J.; Verlinden, G.; Gijbels, R.; Geuens, I.; Callant, P. | ||||
Title | The exchange of fluorinated dyes between different types of silver halide microcrystals studied by time of flight secondary ion mass spectrometry (TOF-SIMS) | Type | P1 Proceeding | ||
Year | 2000 | Publication | Abbreviated Journal | ||
Volume | Issue | Pages | 180-183 | ||
Keywords | P1 Proceeding; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | |||||
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Corporate Author | Thesis | ||||
Publisher | Soc Imaging Science Technology | Place of Publication | Springfield | Editor | |
Language | Wos | 000183315900049 | Publication Date | 0000-00-00 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | 2000 | Series Issue | Edition | ||
ISSN | 0-89208-229-1 | ISBN | Additional Links | UA library record; WoS full record; | |
Impact Factor | Times cited | Open Access | |||
Notes | Approved | Most recent IF: NA | |||
Call Number | UA @ lucian @ c:irua:95776 | Serial | 3580 | ||
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Author | Meng, S.; Wu, L.; Liu, M.; Cui, Z.; Chen, Q.; Li, S.; Yan, J.; Wang, L.; Wang, X.; Qian, J.; Guo, H.; Niu, J.; Bogaerts, A.; Yi, Y. | ||||
Title | Plasma‐driven<scp>CO2</scp>hydrogenation to<scp>CH3OH</scp>over<scp>Fe2O3</scp>/<scp>γ‐Al2O3</scp>catalyst | Type | A1 Journal Article | ||
Year | 2023 | Publication | AIChE Journal | Abbreviated Journal | AIChE Journal |
Volume | 69 | Issue | 10 | Pages | e18154 |
Keywords | A1 Journal Article; chemisorbed oxygen, CO2 hydrogenation, iron-based catalyst, methanol production, plasma catalysis; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | We report a plasma‐assisted CO<sub>2</sub>hydrogenation to CH<sub>3</sub>OH over Fe<sub>2</sub>O<sub>3</sub>/γ‐Al<sub>2</sub>O<sub>3</sub>catalysts, achieving 12% CO<sub>2</sub>conversion and 58% CH<sub>3</sub>OH selectivity at a temperature of nearly 80°C atm pressure. We investigated the effect of various supports and loadings of the Fe‐based catalysts, as well as optimized reaction conditions. We characterized catalysts by X‐ray powder diffraction (XRD), hydrogen temperature programmed reduction (H<sub>2</sub>‐TPR), CO<sub>2</sub>and CO temperature programmed desorption (CO<sub>2</sub>/CO‐TPD), high‐resolution transmission electron microscopy (HRTEM), scanning transmission electron microscopy (STEM), x‐ray photoelectron spectroscopy (XPS), Mössbauer, and Fourier transform infrared<bold>(</bold>FTIR). The XPS results show that the enhanced CO<sub>2</sub>conversion and CH<sub>3</sub>OH selectivity are attributed to the chemisorbed oxygen species on Fe<sub>2</sub>O<sub>3</sub>/γ‐Al<sub>2</sub>O<sub>3</sub>. Furthermore, the diffuse reflectance infrared Fourier transform spectroscopy (DRIFTs) and TPD results illustrate that the catalysts with stronger CO<sub>2</sub>adsorption capacity exhibit a higher reaction performance.<italic>In situ</italic>DRIFTS gain insight into the specific reaction pathways in the CO<sub>2</sub>/H<sub>2</sub>plasma. This study reveals the role of chemisorbed oxygen species as a key intermediate, and inspires to design highly efficient catalysts and expand the catalytic systems for CO<sub>2</sub>hydrogenation to CH<sub>3</sub>OH. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 001022420000001 | Publication Date | 2023-07-07 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0001-1541 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 3.7 | Times cited | Open Access | Not_Open_Access | |
Notes | Fundamental Research Funds for the Central Universities, DUT18JC42 ; National Natural Science Foundation of China, 21908016 21978032 ; | Approved | Most recent IF: 3.7; 2023 IF: 2.836 | ||
Call Number | PLASMANT @ plasmant @c:irua:197829 | Serial | 8959 | ||
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Author | Khalilov, U.; Bogaerts, A.; Neyts, E.C. | ||||
Title | Toward the Understanding of Selective Si Nano-Oxidation by Atomic Scale Simulations | Type | A1 Journal article | ||
Year | 2017 | Publication | Accounts of chemical research | Abbreviated Journal | Accounts Chem Res |
Volume | 50 | Issue | 50 | Pages | 796-804 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | The continuous miniaturization of nanodevices, such as transistors, solar cells, and optical fibers, requires the controlled synthesis of (ultra)thin gate oxides (<10 nm), including Si gate-oxide (SiO2) with high quality at the atomic scale. Traditional thermal growth of SiO2 on planar Si surfaces, however, does not allow one to obtain such ultrathin oxide due to either the high oxygen diffusivity at high temperature or the very low sticking ability of incident oxygen at low temperature. Two recent techniques, both operative at low (room) temperature, have been put forward to overcome these obstacles: (i) hyperthermal oxidation of planar Si surfaces and (ii) thermal or plasma-assisted oxidation of nonplanar Si surfaces, including Si nanowires (SiNWs). These nanooxidation processes are, however, often difficult to study experimentally, due to the key intermediate processes taking place on the nanosecond time scale. In this Account, these Si nano-oxidation techniques are discussed from a computational point of view and compared to both hyperthermal and thermal oxidation experiments, as well as to well-known models of thermal oxidation, including the Deal−Grove, Cabrera−Mott, and Kao models and several alternative mechanisms. In our studies, we use reactive molecular dynamics (MD) and hybrid MD/Monte Carlo simulation techniques, applying the Reax force field. The incident energy of oxygen species is chosen in the range of 1−5 eV in hyperthermal oxidation of planar Si surfaces in order to prevent energy-induced damage. It turns out that hyperthermal growth allows for two growth modes, where the ultrathin oxide thickness depends on either (1) only the kinetic energy of the incident oxygen species at a growth temperature below Ttrans = 600 K, or (2) both the incident energy and the growth temperature at a growth temperature above Ttrans. These modes are specific to such ultrathin oxides, and are not observed in traditional thermal oxidation, nor theoretically considered by already existing models. In the case of thermal or plasma-assisted oxidation of small Si nanowires, on the other hand, the thickness of the ultrathin oxide is a function of the growth temperature and the nanowire diameter. Below Ttrans, which varies with the nanowire diameter, partially oxidized SiNW are formed, whereas complete oxidation to a SiO2 nanowire occurs only above Ttrans. In both nano-oxidation processes at lower temperature (T < Ttrans), final sandwich c-Si|SiOx|a-SiO2 structures are obtained due to a competition between overcoming the energy barrier to penetrate into Si subsurface layers and the compressive stress (∼2−3 GPa) at the Si crystal/oxide interface. The overall atomic-simulation results strongly indicate that the thickness of the intermediate SiOx (x < 2) region is very limited (∼0.5 nm) and constant irrespective of oxidation parameters. Thus, control over the ultrathin SiO2 thickness with good quality is indeed possible by accurately tuning the oxidant energy, oxidation temperature and surface curvature. In general, we discuss and put in perspective these two oxidation mechanisms for obtaining controllable ultrathin gate-oxide films, offering a new route toward the fabrication of nanodevices via selective nano-oxidation. |
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000399859800016 | Publication Date | 2017-04-18 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0001-4842 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 20.268 | Times cited | 5 | Open Access | OpenAccess |
Notes | Fonds Wetenschappelijk Onderzoek, 12M1315N ; | Approved | Most recent IF: 20.268 | ||
Call Number | PLASMANT @ plasmant @ c:irua:142638 | Serial | 4561 | ||
Permanent link to this record | |||||
Author | Ostrikov, K.; Neyts, E.C.; Meyyappan, M. | ||||
Title | Plasma nanoscience : from nano-solids in plasmas to nano-plasmas in solids | Type | A1 Journal article | ||
Year | 2013 | Publication | Advances in physics | Abbreviated Journal | Adv Phys |
Volume | 62 | Issue | 2 | Pages | 113-224 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | The unique plasma-specific features and physical phenomena in the organization of nanoscale soild-state systems in a broad range of elemental composition, structure, and dimensionality are critically reviewed. These effects lead to the possibility to localize and control energy and matter at nanoscales and to produce self-organized nano-solids with highly unusual and superior properties. A unifying conceptual framework based on the control of production, transport, and self-organization of precursor species is introduced and a variety of plasma-specific non-equilibrium and kinetics-driven phenomena across the many temporal and spatial scales is explained. When the plasma is localized to micrometer and nanometer dimensions, new emergent phenomena arise. The examples range from semiconducting quantum dots and nanowires, chirality control of single-walled carbon nanotubes, ultra-fine manipulation of graphenes, nano-diamond, and organic matter to nano-plasma effects and nano-plasmas of different states of matter. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | London | Editor | ||
Language | Wos | 000320913600001 | Publication Date | 2013-06-18 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0001-8732;1460-6976; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 21.818 | Times cited | 380 | Open Access | |
Notes | Approved | Most recent IF: 21.818; 2013 IF: 18.062 | |||
Call Number | UA @ lucian @ c:irua:108723 | Serial | 2639 | ||
Permanent link to this record | |||||
Author | Neyts, E.C.; van Duin, A.C.T.; Bogaerts, A. | ||||
Title | Changing chirality during single-walled carbon nanotube growth : a reactive molecular dynamics/Monte Carlo study | Type | A1 Journal article | ||
Year | 2011 | Publication | Journal of the American Chemical Society | Abbreviated Journal | J Am Chem Soc |
Volume | 133 | Issue | 43 | Pages | 17225-17231 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | The growth mechanism and chirality formation of a single-walled carbon nanotube (SWNT) on a surface-bound nickel nanocluster are investigated by hybrid reactive molecular dynamics/force-biased Monte Carlo simulations. The validity of the interatomic potential used, the so-called ReaxFF potential, for simulating catalytic SWNT growth is demonstrated. The SWNT growth process was found to be in agreement with previous studies and observed to proceed through a number of distinct steps, viz., the dissolution of carbon in the metallic particle, the surface segregation of carbon with the formation of aggregated carbon clusters on the surface, the formation of graphitic islands that grow into SWNT caps, and finally continued growth of the SWNT. Moreover, it is clearly illustrated in the present study that during the growth process, the carbon network is continuously restructured by a metal-mediated process, thereby healing many topological defects. It is also found that a cap can nucleate and disappear again, which was not observed in previous simulations. Encapsulation of the nanoparticle is observed to be prevented by the carbon network migrating as a whole over the cluster surface. Finally, for the first time, the chirality of the growing SWNT cap is observed to change from (11,0) over (9,3) to (7,7). It is demonstrated that this change in chirality is due to the metal-mediated restructuring process. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Washington, D.C. | Editor | ||
Language | Wos | 000297380900026 | Publication Date | 2011-10-06 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0002-7863;1520-5126; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 13.858 | Times cited | 116 | Open Access | |
Notes | Approved | Most recent IF: 13.858; 2011 IF: 9.907 | |||
Call Number | UA @ lucian @ c:irua:92043 | Serial | 309 | ||
Permanent link to this record | |||||
Author | Neyts, E.C.; van Duin, A.C.T.; Bogaerts, A. | ||||
Title | Insights in the plasma-assisted growth of carbon nanotubes through atomic scale simulations : effect of electric field | Type | A1 Journal article | ||
Year | 2012 | Publication | Journal of the American Chemical Society | Abbreviated Journal | J Am Chem Soc |
Volume | 134 | Issue | 2 | Pages | 1256-1260 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Carbon nanotubes (CNTs) are nowadays routinely grown in a thermal CVD setup. State-of-the-art plasma-enhanced CVD (PECVD) growth, however, offers advantages over thermal CVD. A lower growth temperature and the growth of aligned freestanding single-walled CNTs (SWNTs) makes the technique very attractive. The atomic scale growth mechanisms of PECVD CNT growth, however, remain currently entirely unexplored. In this contribution, we employed molecular dynamics simulations to focus on the effect of applying an electric field on the SWNT growth process, as one of the effects coming into play in PECVD. Using sufficiently strong fields results in (a) alignment of the growing SWNTs, (b) a better ordering of the carbon network, and (c) a higher growth rate relative to thermal growth rate. We suggest that these effects are due to the small charge transfer occurring in the Ni/C system. These simulations constitute the first study of PECVD growth of SWNTs on the atomic level. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Washington, D.C. | Editor | ||
Language | Wos | 000301084300086 | Publication Date | 2011-11-30 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0002-7863;1520-5126; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 13.858 | Times cited | 56 | Open Access | |
Notes | Approved | Most recent IF: 13.858; 2012 IF: 10.677 | |||
Call Number | UA @ lucian @ c:irua:97163 | Serial | 1673 | ||
Permanent link to this record | |||||
Author | Adams, F.; Adriaens, A.; Bogaerts, A. | ||||
Title | Can plasma spectrochemistry assist in improving the accuracy of chemical analysis? | Type | A1 Journal article | ||
Year | 2002 | Publication | Analytica chimica acta | Abbreviated Journal | Anal Chim Acta |
Volume | 456 | Issue | Pages | 63-75 | |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | |||||
Address | |||||
Corporate Author | Thesis | ||||
Publisher | Place of Publication | Amsterdam | Editor | ||
Language | Wos | 000174676000007 | Publication Date | 2002-10-14 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0003-2670; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 4.95 | Times cited | 6 | Open Access | |
Notes | Approved | Most recent IF: 4.95; 2002 IF: 2.114 | |||
Call Number | UA @ lucian @ c:irua:38375 | Serial | 272 | ||
Permanent link to this record | |||||
Author | Cidu, R.; Fanfani, L.; Shaud, P.; Edmunds, W.M.; Van 't dack, L.; Gijbels, R. | ||||
Title | Determination of gold at the ultratrace level in natural waters | Type | A1 Journal article | ||
Year | 1994 | Publication | Analytica chimica acta | Abbreviated Journal | Anal Chim Acta |
Volume | 296 | Issue | Pages | 295-304 | |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | |||||
Address | |||||
Corporate Author | Thesis | ||||
Publisher | Place of Publication | Amsterdam | Editor | ||
Language | Wos | A1994PM14000010 | Publication Date | 2002-07-25 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0003-2670; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 4.513 | Times cited | 20 | Open Access | |
Notes | Approved | no | |||
Call Number | UA @ lucian @ c:irua:10252 | Serial | 668 | ||
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Author | Shazali, I.; Van 't dack, L.; Gijbels, R. | ||||
Title | Determination of precious metals in ores and rocks by thermal neutron activation/\gamma-spectrometry after preconcentration by nickel sulphide fire assay and coprecipitation with tellurium | Type | A1 Journal article | ||
Year | 1987 | Publication | Analytica chimica acta | Abbreviated Journal | Anal Chim Acta |
Volume | 196 | Issue | Pages | 49-58 | |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | The six platinum group elements (Ru, Rh, Pd, Os, Ir and Pt) can be determined in geological samples down to the μg kg−1 level, by using nickel sulphide fire assay and neutron activation of the residue ramaining after dissolution of the nickel sulphide button in concentrated hydrochloric acid. Losses for the platinum group elements during this dissolution step are usually insignificant, except when the elements are present at ultra-trace levels. The can be recovered from the filtrate by coprecipitation with tellerium. The latter approach also permits determination of silver, which is significantly lost in the hydrochloric acid treatment (recovery <98% instead of typically ≈ 10%). The coprecipitation with tellurium considerably improves the results for gold (recovery ≈ 95% instead of typically 75%). | ||||
Address | |||||
Corporate Author | Thesis | ||||
Publisher | Place of Publication | Amsterdam | Editor | ||
Language | Wos | A1987K058900006 | Publication Date | 2002-07-25 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0003-2670; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 4.513 | Times cited | 49 | Open Access | |
Notes | Approved | no | |||
Call Number | UA @ lucian @ c:irua:111403 | Serial | 670 | ||
Permanent link to this record | |||||
Author | Gijbels, R.; Dams, R. | ||||
Title | Determination of silicon in natural and pollution aerosols by 14-MeV neutron activation analysis | Type | A1 Journal article | ||
Year | 1973 | Publication | Analytica chimica acta | Abbreviated Journal | Anal Chim Acta |
Volume | 63 | Issue | 2 | Pages | 369-381 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | The determination of silicon via the 28Si(n,p)28 Al reaction by means of 14-MeV neutrons is applied to the analysis of pollution and natural aerosols. A Whatman 41 filter (40 cm2) on which airborne particulate material has been collected is compressed into a 3 × 12.7 mm pellet. Standards are prepared in the same way from clean filters spiked with a silicate solution. After a 50-s irradiation and a 75-s decay time, the sample is counted for 2 min with 5 × 5 NaI(Tl) well detector. The 1.779-MeV photopeak of 28Al is measured with a single channel sealer chain or with a multichannel analyser. The reproducibility, sensitivity and liability to interference from other elements were investigated for both counting systems. The homogeneity of the pellets and the filters was checked. The overall precision of one single-channel determination was estimated to be 3.5% after a 24-h high-volume sampling time. Samples collected in urban, industrial and remote areas with concentrations ranging from 0.05 to 15 μg Si m-3 air were analysed and the results are discussed. | ||||
Address | |||||
Corporate Author | Thesis | ||||
Publisher | Place of Publication | Amsterdam | Editor | ||
Language | Wos | A1973O944700013 | Publication Date | 2002-07-25 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0003-2670; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 4.513 | Times cited | 16 | Open Access | |
Notes | Approved | no | |||
Call Number | UA @ lucian @ c:irua:116365 | Serial | 672 | ||
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Author | van Grieken, R.; Gijbels, R.; Speecke, A.; Hoste, J. | ||||
Title | The determination of silicon in steel by 14-mev neutron activation analysis | Type | A1 Journal article | ||
Year | 1968 | Publication | Analytica chimica acta | Abbreviated Journal | Anal Chim Acta |
Volume | 43 | Issue | Pages | 199-209 | |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) | ||||
Abstract | A fast (25 min) non-destructive determination of silicon in steel by 14-MeV neutron activation is described. The 1.78-MeV 28Al activity, induced by the reaction 28Si(n,p)28Al, is counted on a NaI(Tl) detector. An oxygen flux monitor is used to normalise to the same neutron flux. Two methods are described to correct for the 56Mn activity (2.58 h), induced into the iron matrix via 56Fe(n,p)56Mn. Nuclear interferences of phosphorus and aluminium have been examined. Special attention has been paid to stainless steels. A sensitivity of 0.02 to 0.05% of silicon is obtained. The precision is 2 to 3% for steels containing above 1% silicon, and 7% for 0.1% of silicon. | ||||
Address | |||||
Corporate Author | Thesis | ||||
Publisher | Place of Publication | Amsterdam | Editor | ||
Language | Wos | A1968C007600004 | Publication Date | 2002-07-25 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0003-2670; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 4.513 | Times cited | 19 | Open Access | |
Notes | Approved | no | |||
Call Number | UA @ lucian @ c:irua:116357 | Serial | 673 | ||
Permanent link to this record |