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Author |
Berthelot, A.; Bogaerts, A. |
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Title |
Modeling of CO2Splitting in a Microwave Plasma: How to Improve the Conversion and Energy Efficiency |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
The journal of physical chemistry: C : nanomaterials and interfaces |
Abbreviated Journal |
J Phys Chem C |
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Volume |
121 |
Issue |
121 |
Pages |
8236-8251 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
Microwave plasmas are one of the most promising techniques for CO2 conversion into value-added chemicals and fuels since they are very energy efficient. Nevertheless, experiments show that this high energy efficiency is only reached at low pressures and significantly drops toward atmospheric pressure, which is a clear limitation for industrial applications. In this paper, we use a zerodimensional reaction kinetics model to simulate a CO2 microwave plasma in a pressure range from 50 mbar to 1 bar, in order to evaluate the reasons for this decrease in energy efficiency at atmospheric pressure. The code includes a detailed description of the vibrational kinetics of CO2, CO, and O2 as well as the energy exchanges between them because the vibrational kinetics is known to be crucial for energy efficient CO2 splitting. First, we use a self-consistent gas temperature calculation in order to assess the key performance indicators for CO2 splitting, i.e., the CO2 conversion and corresponding energy efficiency. Our results indicate that lower pressures and higher power densities lead to more vibrational excitation, which is beneficial for the conversion. We also demonstrate the key role of the gas temperature. The model predicts the highest conversion and energy efficiencies at pressures around 300 mbar, which is in agreement with experiments from the literature. We also show the beneficial aspect of fast gas cooling in the afterglow at high pressure. In a second step, we study in more detail the effects of pressure, gas temperature, and power density on the vibrational distribution function and on the dissociation and recombination mechanisms of CO2, which define the CO2 splitting efficiency. This study allows us to identify the limiting factors of CO2 conversion and to propose potential solutions to improve the process. |
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Wos |
000400039300002 |
Publication Date |
2017-04-20 |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.536 |
Times cited |
47 |
Open Access |
OpenAccess |
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Notes |
Federaal Wetenschapsbeleid; |
Approved |
Most recent IF: 4.536 |
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Call Number |
PLASMANT @ plasmant @ c:irua:142809 |
Serial |
4567 |
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Author |
Trenchev, G.; Kolev, S.; Wang, W.; Ramakers, M.; Bogaerts, A. |
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Title |
CO2Conversion in a Gliding Arc Plasmatron: Multidimensional Modeling for Improved Efficiency |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
The journal of physical chemistry: C : nanomaterials and interfaces |
Abbreviated Journal |
J Phys Chem C |
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Volume |
121 |
Issue |
44 |
Pages |
24470-24479 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
The gliding arc plasmatron (GAP) is a highly efficient atmospheric plasma source, which is very promising for CO2 conversion applications. To understand its operation principles and to improve its application, we present here comprehensive modeling results, obtained by means of computational fluid dynamics simulations and plasma modeling. Because of the complexity of the CO2 plasma, a full 3D plasma model would be computationally impractical. Therefore, we combine a 3D turbulent gas flow model with a 2D plasma and gas heating model in order to calculate the plasma parameters and CO2 conversion characteristics. In addition, a complete 3D gas flow and plasma model with simplified argon chemistry is used to evaluate the gliding arc evolution in space and time. The calculated values are compared with experimental data from literature as much as possible in order to validate the model. The insights obtained in this study are very helpful for improving the application of CO2 conversion, as they allow us to identify the limiting factors in the performance, based on which solutions can be provided on how to further improve the capabilities of CO2 conversion in the GAP. |
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Wos |
000415140400014 |
Publication Date |
2017-11-09 |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.536 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
H2020 Marie Sklodowska-Curie Actions, 657304 ; Fonds Wetenschappelijk Onderzoek, 11U5316N G038316N ; |
Approved |
Most recent IF: 4.536 |
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Call Number |
PLASMANT @ plasmant @c:irua:147193 |
Serial |
4765 |
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Permanent link to this record |
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Author |
Heijkers, S.; Bogaerts, A. |
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Title |
CO2Conversion in a Gliding Arc Plasmatron: Elucidating the Chemistry through Kinetic Modeling |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
The journal of physical chemistry: C : nanomaterials and interfaces |
Abbreviated Journal |
J Phys Chem C |
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Volume |
121 |
Issue |
41 |
Pages |
22644-22655 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
By means of chemical kinetics modeling, it is possible to elucidate the main dissociation mechanisms of CO2 in a gliding arc plasmatron (GAP). We obtain good agreement between the calculated and experimental conversions and energy efficiencies, indicating that the model can indeed be used to study the underlying mechanisms. The calculations predict that vibration-induced dissociation is the main dissociation mechanism of CO2, but it occurs mainly from the lowest vibrational levels because of fast thermalization of the vibrational distribution. Based on these findings, we propose ideas for improving the performance of the GAP, but testing of these ideas in the simulations reveals that they do not always lead to significant enhancement, because of other side effects, thus illustrating the complexity of the process. Nevertheless, the model allows more insight into the underlying mechanisms to be obtained and limitations to be identified. |
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Wos |
000413617900007 |
Publication Date |
2017-10-19 |
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Series Editor |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.536 |
Times cited |
6 |
Open Access |
OpenAccess |
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Notes |
Federaal Wetenschapsbeleid, IAP/7 ; Fonds Wetenschappelijk Onderzoek, G.0383.16N ; |
Approved |
Most recent IF: 4.536 |
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Call Number |
PLASMANT @ plasmant @c:irua:147436 |
Serial |
4801 |
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Permanent link to this record |
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Author |
Wang, W.; Snoeckx, R.; Zhang, X.; Cha, M.S.; Bogaerts, A. |
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Title |
Modeling Plasma-based CO2and CH4Conversion in Mixtures with N2, O2, and H2O: The Bigger Plasma Chemistry Picture |
Type |
A1 Journal article |
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Year |
2018 |
Publication |
The journal of physical chemistry: C : nanomaterials and interfaces |
Abbreviated Journal |
J Phys Chem C |
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Volume |
122 |
Issue |
16 |
Pages |
8704-8723 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
Because of the unique properties of plasma technology, its use in gas conversion applications is gaining significant interest around the globe. Plasma-based CO2 and CH4 conversion has become a major research area. Many investigations have already been performed regarding the single-component gases, that is, CO2 splitting and CH4 reforming, as well as for two-component mixtures, that is, dry reforming of methane
(CO2/CH4), partial oxidation of methane (CH4/O2), artificial photosynthesis (CO2/H2O), CO2 hydrogenation (CO2/H2), and even first steps toward the influence of N2 impurities have been taken, that is, CO2/N2 and CH4/N2. In this Feature Article we briefly discuss the advances made in literature for these different steps from a plasma chemistry modeling point of view. Subsequently, we present a comprehensive plasma chemistry set, combining the knowledge gathered in this field so far and supported with extensive experimental data. This set can be used for chemical kinetics plasma modeling for all possible combinations of CO2, CH4, N2, O2, and H2O to investigate the bigger picture of the underlying plasmachemical pathways for these mixtures in a dielectric barrier discharge plasma. This is extremely valuable
for the optimization of existing plasma-based CO2 conversion and CH4 reforming processes as well as for investigating the influence of N2, O2, and H2O on these processes and even to support plasma-based multireforming processes. |
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Wos |
000431151200002 |
Publication Date |
2018-04-26 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.536 |
Times cited |
28 |
Open Access |
OpenAccess |
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Notes |
Federaal Wetenschapsbeleid, IAP/7 ; King Abdullah University of Science and Technology; H2020 Marie Sklodowska-Curie Actions, 657304 ; Fonds Wetenschappelijk Onderzoek, G.0217.14N G.0383.16N G.0254.14N ; |
Approved |
Most recent IF: 4.536 |
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Call Number |
PLASMANT @ plasmant @c:irua:150969 |
Serial |
4922 |
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Permanent link to this record |
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Author |
Huygh, S.; Bogaerts, A.; Bal, K.M.; Neyts, E.C. |
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Title |
High Coke Resistance of a TiO2Anatase (001) Catalyst Surface during Dry Reforming of Methane |
Type |
A1 Journal Article |
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Year |
2018 |
Publication |
Journal Of Physical Chemistry C |
Abbreviated Journal |
J Phys Chem C |
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Volume |
122 |
Issue |
17 |
Pages |
9389-9396 |
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Keywords |
A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
The resistance of a TiO2 anatase (001) surface to coke formation was studied in the context of dry reforming of methane using density functional theory (DFT) calculations. As carbon atoms act as precursors for coke formation, the resistance to coke formation can be measured by the carbon coverage of the surface. This is related to the stability of different CHx (x = 0−3) species and their rate of hydrogenation and dehydrogenation on the TiO2 surface. Therefore, we studied the reaction mechanisms and their corresponding rates as a function of the temperature for the dehydrogenation of the species on the surface. We found that the stabilities of C and CH are significantly lower than those of CH3 and CH2. The hydrogenation rates of the different species are significantly higher than the dehydrogenation rates in a temperature range of 300−1000 K. Furthermore, we found that dehydrogenation of CH3, CH2, and CH will only occur at appreciable rates starting from 600, 900, and 900 K, respectively. On the basis of these results, it is clear that the anatase (001) surface has a high coke resistance, and it is thus not likely that the surface will become poisoned by coke during dry reforming of methane. As the rate limiting step in dry reforming is the dissociative adsorption of CH4, we studied an alternative approach to thermal catalysis. We found that the temperature threshold for dry reforming is at least 700 K. This threshold temperature may be lowered by the use of plasma-catalysis, where the appreciable rates of adsorption of plasma-generated CHx radicals result in bypassing the rate limiting step of the reaction. |
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Wos |
000431723700014 |
Publication Date |
2018-05-03 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.536 |
Times cited |
1 |
Open Access |
OpenAccess |
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Notes |
Federaal Wetenschapsbeleid, IAP/7 ; Fonds Wetenschappelijk Onderzoek, G.0217.14N ; Onderzoeksfonds, Universiteit Antwerpen, 32249 ; |
Approved |
Most recent IF: 4.536 |
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Call Number |
PLASMANT @ plasmant @c:irua:151529c:irua:152816 |
Serial |
5000 |
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Permanent link to this record |
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Author |
Vermeiren, V.; Bogaerts, A. |
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Title |
Supersonic Microwave Plasma: Potential and Limitations for Energy-Efficient CO2Conversion |
Type |
A1 Journal Article |
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Year |
2018 |
Publication |
Journal Of Physical Chemistry C |
Abbreviated Journal |
J Phys Chem C |
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Volume |
122 |
Issue |
45 |
Pages |
25869-25881 |
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Keywords |
A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
Supersonic flows provide a high thermodynamic
nonequilibrium, which is crucial for energy-efficient conversion of
CO 2 in microwave plasmas and are therefore of great interest.
However, the effect of the flow on the chemical reactions is poorly
understood. In this work, we present a combined flow and plasma
chemical kinetics model of a microwave CO 2 plasma in a Laval
nozzle setup. The effects of the flow field on the different dissociation
and recombination mechanisms, the vibrational distribution, and the
vibrational transfer mechanism are discussed. In addition, the effect
of experimental parameters, like position of power deposition, outlet
pressure, and specific energy input, on the CO 2 conversion and
energy efficiency is examined. The short residence time of the gas in
the plasma region, the shockwave, and the maximum critical heat,
and thus power, that can be added to the flow to avoid thermal
choking are the main obstacles to reaching high energy efficiencies. |
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Wos |
000451101400016 |
Publication Date |
2018-11-15 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.536 |
Times cited |
5 |
Open Access |
Not_Open_Access |
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Notes |
Fonds Wetenschappelijk Onderzoek, G.0383.16N ; |
Approved |
Most recent IF: 4.536 |
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Call Number |
PLASMANT @ plasmant @c:irua:155412 |
Serial |
5070 |
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Permanent link to this record |
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Author |
Heijkers, S.; Martini, L.M.; Dilecce, G.; Tosi, P.; Bogaerts, A. |
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Title |
Nanosecond Pulsed Discharge for CO2Conversion: Kinetic Modeling To Elucidate the Chemistry and Improve the Performance |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
The journal of physical chemistry: C : nanomaterials and interfaces |
Abbreviated Journal |
J Phys Chem C |
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Volume |
123 |
Issue |
19 |
Pages |
12104-12116 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
We study the mechanisms of CO2 conversion in a nanosecond repetitively pulsed (NRP) discharge, by means of a chemical kinetics model. The calculated conversions and energy efficiencies are in reasonable agreement with experimental results over a wide range of specific energy input values, and the same applies to the evolution of gas temperature and CO2 conversion as a function of time in the afterglow, indicating that our model provides a realistic picture of the underlying mechanisms in the NRP discharge and can be used to identify its limitations and thus to suggest further improvements. Our model predicts that vibrational excitation is very important in the NRP discharge, explaining why this type of plasma yields energy-efficient CO2 conversion. A significant part of the CO2 dissociation occurs by electronic excitation from the lower vibrational levels toward repulsive electronic states, thus resulting in dissociation. However, vibration−translation (VT) relaxation (depopulating the higher vibrational levels) and CO + O recombination (CO + O + M → CO2 + M), as well as mixing of the converted gas with fresh gas entering the plasma in between the pulses, are limiting factors for the conversion and energy efficiency. Our model predicts that extra cooling, slowing down the rate of VT relaxation and of the above recombination reaction, thus enhancing the contribution of the highest vibrational levels to the overall CO2 dissociation, can further improve the performance of the NRP discharge for energy-efficient CO2 conversion. |
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Wos |
000468368800009 |
Publication Date |
2019-05-16 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.536 |
Times cited |
4 |
Open Access |
Not_Open_Access: Available from 26.04.2020
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Notes |
Fonds Wetenschappelijk Onderzoek, G.0383.16N ; The authors acknowledge financial support from the Fund for Scientific Research, Flanders (FWO; Grant no. G.0383.16N). |
Approved |
Most recent IF: 4.536 |
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Call Number |
PLASMANT @ plasmant @UA @ admin @ c:irua:159976 |
Serial |
5174 |
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Permanent link to this record |
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Author |
Jafarzadeh, A.; Bal, K.M.; Bogaerts, A.; Neyts, E.C. |
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Title |
CO2 activation on TiO2-supported Cu5 and Ni5 nanoclusters : effect of plasma-induced surface charging |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
The journal of physical chemistry: C : nanomaterials and interfaces |
Abbreviated Journal |
J Phys Chem C |
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Volume |
123 |
Issue |
11 |
Pages |
6516-6525 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
Surface charging is an often overlooked factor in many plasma-surface interactions and in particular in plasma catalysis. In this study, we investigate the effect of excess electrons induced by a plasma on the adsorption properties of CO2 on titania-supported Cu-5 and Ni-5 clusters using spin-polarized and dispersion-corrected density functional theory calculations. The effect of excess electrons on the adsorption of Ni and Cu pentamers as well as on CO2 adsorption on a pristine anatase TiO2(101) slab is studied. Our results indicate that adding plasma-induced excess electrons to the system leads to further stabilization of the bent CO2 structure. Also, dissociation of CO2 on charged clusters is energetically more favorable than on neutral clusters. We hypothesize that surface charge is a plausible cause for the synergistic effects sometimes observed in plasma catalysis. |
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Wos |
000462260700024 |
Publication Date |
2019-02-21 |
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Edition |
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ISSN |
1932-7447; 1932-7455 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.536 |
Times cited |
4 |
Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 4.536 |
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Call Number |
UA @ admin @ c:irua:159422 |
Serial |
5281 |
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Permanent link to this record |
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Author |
Vermeiren, V.; Bogaerts, A. |
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Title |
Improving the Energy Efficiency of CO2Conversion in Nonequilibrium Plasmas through Pulsing |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
The journal of physical chemistry: C : nanomaterials and interfaces |
Abbreviated Journal |
J Phys Chem C |
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Volume |
123 |
Issue |
29 |
Pages |
17650-17665 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
Nonequilibrium plasmas offer a pathway for energy-efficient CO2 conversion through vibrationally induced dissociation. However, the efficiency of this pathway is limited by a rise in gas temperature, which increases vibrational−translational (VT) relaxation and quenches the vibrational levels. Therefore, we investigate here the effect of plasma pulsing on the VT nonequilibrium and on the CO2 conversion by means of a zerodimensional chemical kinetics model, with self-consistent gas temperature calculation. Specifically, we show that higher energy efficiencies can be reached by correctly tuning the plasma pulse and interpulse times. The ideal plasma pulse time corresponds to the time needed to reach the highest vibrational temperature. In addition, the highest energy efficiencies are obtained with long interpulse times, that is, ≥0.1 s, in which the gas temperature can entirely drop to room temperature. Furthermore, additional cooling of the reactor walls can give higher energy efficiencies at shorter interpulse times of 1 ms. Finally, our model shows that plasma pulsing can significantly improve the energy efficiency at low reduced electric fields (50 and 100 Td, typical for microwave and gliding arc plasmas) and intermediate ionization degrees (5 × 10−7 and 10−6). |
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Place of Publication |
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Wos |
000477785000003 |
Publication Date |
2019-07-25 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.536 |
Times cited |
1 |
Open Access |
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Notes |
Fonds Wetenschappelijk Onderzoek, G.0383.16N ; This research was supported by the FWO project (grant G.0383.16N). The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UAntwerpen), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI), and the UAntwerpen. We also like to thank N. Britun (ChIPS) for the interesting discussions. |
Approved |
Most recent IF: 4.536 |
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Call Number |
PLASMANT @ plasmant @c:irua:161621 |
Serial |
5289 |
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Permanent link to this record |
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Author |
Van Alphen, S.; Vermeiren, V.; Butterworth, T.; van den Bekerom, D.C.M.; van Rooij, G.J.; Bogaerts, A. |
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Title |
Power Pulsing To Maximize Vibrational Excitation Efficiency in N2Microwave Plasma: A Combined Experimental and Computational Study |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Journal Of Physical Chemistry C |
Abbreviated Journal |
J Phys Chem C |
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Volume |
124 |
Issue |
3 |
Pages |
1765-1779 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
Plasma is gaining increasing interest for N2 fixation, being a flexible, electricity-driven alternative for the current conventional fossil fuel-based N2 fixation processes. As the vibrational-induced dissociation of N2 is found to be an energy-efficient pathway to acquire atomic N for the fixation processes, plasmas that are in vibrational nonequilibrium seem promising for this application. However, an important challenge in using nonequilibrium plasmas lies in preventing vibrational−translational (VT) relaxation processes, in which vibrational energy crucial for N2 dissociation is lost to gas heating. We present here both experimental and modeling results for the vibrational and gas temperature in a microsecond-pulsed microwave (MW) N2 plasma, showing how power pulsing can suppress this unfavorable VT relaxation and achieve a maximal vibrational nonequilibrium. By means of our kinetic model, we demonstrate that pulsed plasmas take advantage of the long time scale on which VT processes occur, yielding a very pronounced nonequilibrium over the whole N2 vibrational ladder. Additionally, the effect of pulse parameters like the pulse frequency and pulse width are investigated, demonstrating that the advantage of pulsing to inhibit VT relaxation diminishes for high pulse frequencies (around 7000 kHz) and long power pulses (above 400 μs). Nevertheless, all regimes studied here demonstrate a clear vibrational nonequilibrium while only requiring a limited power-on time, and thus, we may conclude that a pulsed plasma seems very interesting for energyefficient vibrational excitation. |
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Wos |
000509438600001 |
Publication Date |
2020-01-23 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.7 |
Times cited |
|
Open Access |
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Notes |
Fonds Wetenschappelijk Onderzoek, 30505023 GoF9618n ; This research was supported by the Excellence of Science FWO-FNRS project (FWO Grant ID GoF9618n, EOS ID 30505023). The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UAntwerpen), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the UAntwerpen. |
Approved |
Most recent IF: 3.7; 2020 IF: 4.536 |
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Call Number |
PLASMANT @ plasmant @c:irua:165586 |
Serial |
5443 |
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Permanent link to this record |
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Author |
Cordeiro, R.M.; Yusupov, M.; Razzokov, J.; Bogaerts, A. |
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Title |
Parametrization and Molecular Dynamics Simulations of Nitrogen Oxyanions and Oxyacids for Applications in Atmospheric and Biomolecular Sciences |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Journal Of Physical Chemistry B |
Abbreviated Journal |
J Phys Chem B |
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Volume |
124 |
Issue |
6 |
Pages |
1082-1089 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
Nitrogen oxyanions and oxyacids are important agents in atmospheric chemistry and medical biology. Although their chemical behavior in solution is relatively well understood, they may behave very differently at the water/air interface of atmospheric aerosols or at the membrane/water interface of cells. Here, we developed a fully classical model for molecular dynamics simulations of NO3−, NO2−, HNO3, and HNO2 in the framework of the GROMOS 53A6 and 54A7 force field versions. The model successfully accounted for the poorly structured solvation shell and ion pairing tendency of NO3−. Accurate pure-liquid properties and hydration free energies were obtained for the oxyacids. Simulations at the water/air interface showed a local enrichment of HNO3 and depletion of NO3−. The effect was discussed in light of earlier spectroscopic data and ab initio calculations, suggesting that HNO3 behaves as a weaker acid at the surface of water. Our model will hopefully allow for efficient and accurate simulations of nitrogen oxyanions and oxyacids in solution and at microheterogeneous interface environments. |
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Wos |
000512222500015 |
Publication Date |
2020-02-13 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1520-6106 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.3 |
Times cited |
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Open Access |
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Notes |
We thank Universidade Federal do ABC for providing the computational resources needed for completion of this work. This study was financed in part by the Coordenaçaõ de Aperfeiçoamento de Pessoal de Nı ́vel Superior – Brasil (CAPES) – Finance Code 001. |
Approved |
Most recent IF: 3.3; 2020 IF: 3.177 |
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Call Number |
PLASMANT @ plasmant @c:irua:166488 |
Serial |
6340 |
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Permanent link to this record |
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Author |
Heijkers, S.; Aghaei, M.; Bogaerts, A. |
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Title |
Plasma-Based CH4Conversion into Higher Hydrocarbons and H2: Modeling to Reveal the Reaction Mechanisms of Different Plasma Sources |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Journal Of Physical Chemistry C |
Abbreviated Journal |
J Phys Chem C |
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Volume |
124 |
Issue |
13 |
Pages |
7016-7030 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
Plasma is gaining interest for CH4 conversion into higher hydrocarbons and H2. However, the performance in terms of conversion and selectivity toward different hydrocarbons is different for different plasma types, and the underlying mechanisms are not yet fully understood. Therefore, we study here these mechanisms in different plasma sources, by means of a chemical kinetics model. The model is first validated by comparing the calculated conversions and hydrocarbon/H2 selectivities with experimental results in these different plasma types and over a wide range of specific energy input (SEI) values. Our model predicts that vibrational−translational nonequilibrium is negligible in all CH4 plasmas investigated, and instead, thermal conversion is important. Higher gas temperatures also lead to a more selective production of unsaturated hydrocarbons (mainly C2H2) due to neutral dissociation of CH4 and subsequent dehydrogenation processes, while three-body recombination reactions into saturated hydrocarbons (mainly C2H6, but also higher hydrocarbons) are dominant in low temperature plasmas. |
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Place of Publication |
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Language |
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Wos |
000526328500007 |
Publication Date |
2020-04-02 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.7 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
Universiteit Antwerpen; Vlaamse regering; Fonds Wetenschappelijk Onderzoek, G.0383.16N ; H2020 European Research Council, 810182 ; We acknowledge financial support from the Fund for Scientific Research, Flanders (FWO; Grant No. G.0383.16N), the Methusalem Grant, and the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (Grant Agreement No. 810182 − SCOPE ERC Synergy project). This work was carried out in part using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen, a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the University of Antwerp. |
Approved |
Most recent IF: 3.7; 2020 IF: 4.536 |
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Call Number |
PLASMANT @ plasmant @c:irua:168096 |
Serial |
6358 |
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Permanent link to this record |
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Author |
Jafarzadeh, A.; Bal, K.M.; Bogaerts, A.; Neyts, E.C. |
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Title |
Activation of CO2on Copper Surfaces: The Synergy between Electric Field, Surface Morphology, and Excess Electrons |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Journal Of Physical Chemistry C |
Abbreviated Journal |
J Phys Chem C |
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Volume |
124 |
Issue |
12 |
Pages |
6747-6755 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
In this work, we use density functional theory calculations to study the combined effect of external electric fields, surface morphology, and surface charge on CO2 activation over Cu(111), Cu(211), Cu(110), and Cu(001) surfaces. We observe that the binding energy of the CO2 molecule on Cu surfaces increases significantly upon increasing the applied electric field strength. In addition, rougher surfaces respond more effectively to the presence of the external electric field toward facilitating the formation of a carbonate-like CO2 structure and the transformation of the most stable adsorption mode from physisorption to chemisorption. The presence of surface charges further strengthens the electric field effect and consequently causes an improved bending of the CO2 molecule and C−O bond length elongation. On the other hand, a net charge in the absence of an externally applied electric field shows only a marginal effect on CO2 binding. The chemisorbed CO2 is more stable and further activated when the effects of an external electric field, rough surface, and surface charge are combined. These results can help to elucidate the underlying factors that control CO2 activation in heterogeneous and plasma catalysis, as well as in electrochemical processes. |
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Wos |
000526396900030 |
Publication Date |
2020-03-26 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.7 |
Times cited |
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Open Access |
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Notes |
Bijzonder Onderzoeksfonds, 32249 ; The financial support from the TOP research project of the Research Fund of the University of Antwerp (grant ID: 32249) is highly acknowledged by the authors. The computational resources used in this study were provided by the VSC (Flemish Supercomputer Center), funded by the FWO and the Flemish Governmentdepartment EWI. |
Approved |
Most recent IF: 3.7; 2020 IF: 4.536 |
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Call Number |
PLASMANT @ plasmant @c:irua:168606 |
Serial |
6361 |
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Permanent link to this record |
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Author |
Vermeiren, V.; Bogaerts, A. |
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Title |
Plasma-Based CO2Conversion: To Quench or Not to Quench? |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Journal Of Physical Chemistry C |
Abbreviated Journal |
J Phys Chem C |
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Volume |
124 |
Issue |
34 |
Pages |
18401-18415 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
Plasma technology is gaining increasing interest for CO2 conversion. The gas temperature in (and after) the plasma reactor largely affects the performance. Therefore, we examine the effect of cooling/quenching, during and after the plasma, on the CO2 conversion and energy efficiency, for typical “warm” plasmas, by means of chemical kinetics modeling. For plasmas at low specific energy input (SEI ∼ 0.5 eV/molecule), it is best to quench at the plasma end, while for high-SEI plasmas (SEI ∼ 4 eV/molecule), quenching at maximum conversion is better. For low-SEI plasmas, quenching can even increase the conversion beyond the dissociation in the plasma, known as superideal quenching. To better understand the effects of quenching at different plasma conditions, we study the dissociation and recombination rates, as well as the vibrational distribution functions (VDFs) of CO2, CO, and O2. When a high vibrational−translational (VT) nonequilibrium exists at the moment of quenching, the dissociation and recombination reaction rates both increase. Depending on the conversion degree at the moment of quenching, this can lead to a net increase or decrease of CO2 conversion. In general, however, and certainly for equilibrium plasmas at high temperature, quenching after the plasma helps prevent recombination reactions and clearly enhances the final CO2 conversion. We also investigate the effect of different quenching cooling rates on the CO2 conversion and energy efficiency. Finally, we compare plasma-based conversion to purely thermal conversion. For warm plasmas with typical temperatures of 3000−4000 K, the conversion is roughly thermal. |
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Wos |
000566481000003 |
Publication Date |
2020-08-27 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.7 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
Fonds Wetenschappelijk Onderzoek, G.0383.16N ; H2020 European Research Council, 810182 ; This research was supported by the FWO project (grant no. G.0383.16N) and the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (grant agreement no. 810182SCOPE ERC Synergy project). The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UAntwerpen), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI), and the UAntwerpen. |
Approved |
Most recent IF: 3.7; 2020 IF: 4.536 |
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Call Number |
PLASMANT @ plasmant @c:irua:172052 |
Serial |
6407 |
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Permanent link to this record |
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Author |
van ‘t Veer, K.; Engelmann, Y.; Reniers, F.; Bogaerts, A. |
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Title |
Plasma-Catalytic Ammonia Synthesis in a DBD Plasma: Role of Microdischarges and Their Afterglows |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Journal Of Physical Chemistry C |
Abbreviated Journal |
J Phys Chem C |
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Volume |
124 |
Issue |
42 |
Pages |
22871-22883 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Movement Antwerp (MOVANT) |
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Abstract |
Plasma-catalytic ammonia synthesis is receiving ever increasing attention, especially in packed bed dielectric barrier discharge (DBD) reactors. The latter typically operate in the filamentary regime when used for gas conversion applications. While DBDs are in principle well understood and already applied in the industry, the incorporation of packing materials and catalytic surfaces considerably adds to the complexity of the plasma physics and chemistry governing the ammonia formation. We employ a plasma kinetics model to gain insights into the ammonia formation mechanisms, paying special attention to the role of filamentary microdischarges and their afterglows. During the microdischarges, the synthesized ammonia is actually decomposed, but the radicals created upon electron impact dissociation of N2 and H2 and the subsequent catalytic reactions cause a net ammonia gain in the afterglows of the microdischarges. Under our plasma conditions, electron impact dissociation of N2 in the gas phase followed by the adsorption of N atoms is identified as a rate-limiting step, instead of dissociative adsorption of N2 on the catalyst surface. Both elementary Eley−Rideal and Langmuir−Hinshelwood reaction steps can be found important in plasma-catalytic NH3 synthesis. |
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Wos |
000585970300002 |
Publication Date |
2020-10-22 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.7 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
Fonds Wetenschappelijk Onderzoek, 30505023 GoF9618n ; Fonds De La Recherche Scientifique – FNRS, 30505023 GoF9618n ; H2020 European Research Council, 810182 ;This research was supported by the Excellence of Science FWOFNRS project (FWO grant ID GoF9618n, EOS ID 30505023) and by the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement no 810182-SCOPE ERC Synergy project). The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UAntwerpen), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the UAntwerpen. The authors would also like to thank Järi Van den Hoek and Dr. Yury Gorbanev for providing the experimentally measured electrical characteristics and Dr. Fatme Jardali for creating the TOC graphics. |
Approved |
Most recent IF: 3.7; 2020 IF: 4.536 |
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Call Number |
PLASMANT @ plasmant @c:irua:173587 |
Serial |
6428 |
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Permanent link to this record |
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Author |
Michiels, R.; Engelmann, Y.; Bogaerts, A. |
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Title |
Plasma Catalysis for CO2Hydrogenation: Unlocking New Pathways toward CH3OH |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Journal Of Physical Chemistry C |
Abbreviated Journal |
J Phys Chem C |
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Volume |
124 |
Issue |
47 |
Pages |
25859-25872 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Movement Antwerp (MOVANT) |
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Abstract |
We developed a microkinetic model to reveal the effects of plasma-generated radicals, intermediates, and vibrationally excited species on the catalytic hydrogenation of CO2 to CH3OH on a Cu(111) surface. As a benchmark, we first present the mechanisms of thermal catalytic CH3OH formation. Our model predicts that the reverse water-gas shift reaction followed by CO hydrogenation, together with the formate path, mainly contribute to CH3OH formation in thermal catalysis. Adding plasma-generated radicals and intermediates results in a higher CH3OH turnover frequency (TOF) by six to seven orders of magnitude, showing the potential of plasma-catalytic CO2 hydrogenation into CH3OH, in accordance with the literature. In addition, CO2 vibrational excitation further increases the CH3OH TOF, but the effect is limited due to relatively low vibrational temperatures under typical plasma catalysis conditions. The predicted increase in CH3OH formation by plasma catalysis is mainly attributed to the increased importance of the formate path. In addition, the conversion of plasma-generated CO to HCO* and subsequent HCOO* or H2CO* formation contribute to CH3OH formation. Both pathways bypass the HCOO* formation from CO2, which is the main bottleneck in the process. Hence, our model points toward the important role of CO, but also O, OH, and H radicals, as they influence the reactions that consume CO2 and CO. In addition, our model reveals that the H pressure should not be smaller than ca. half of the O pressure in the plasma as this would cause O* poisoning, which would result in very small product TOFs. Thus, plasma conditions should be targeted with a high CO and H content as this is favorable for CH3OH formation, while the O content should be minimized. |
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Wos |
000595545800023 |
Publication Date |
2020-11-25 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.7 |
Times cited |
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Open Access |
Not_Open_Access: Available from 15.07.2021 |
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Notes |
Universiteit Antwerpen; Fonds Wetenschappelijk Onderzoek, 1114921N ; H2020 European Research Council, 810182 ; We acknowledge the financial support from the Fund for Scientific Research (FWO-Vlaanderen; grant ID 1114921N) and from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement no. 810182 − SCOPE ERC Synergy project) as well as from the DOC-PRO3 and the TOPBOF projects of the University of Antwerp. |
Approved |
Most recent IF: 3.7; 2020 IF: 4.536 |
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Call Number |
PLASMANT @ plasmant @c:irua:173864 |
Serial |
6443 |
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Permanent link to this record |
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Author |
Loenders, B.; Engelmann, Y.; Bogaerts, A. |
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Title |
Plasma-Catalytic Partial Oxidation of Methane on Pt(111): A Microkinetic Study on the Role of Different Plasma Species |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Journal Of Physical Chemistry C |
Abbreviated Journal |
J Phys Chem C |
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Volume |
125 |
Issue |
5 |
Pages |
2966-2983 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Movement Antwerp (MOVANT) |
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Abstract |
We use microkinetic modeling to examine the potential of plasma-catalytic partial oxidation (POX) of CH4 as a promising new approach to produce oxygenates. We study how different plasma species affect POX of CH4 on the Pt(111) surface, and we discuss the associated kinetic and mechanistic changes. We discuss the effect of vibrationally excited CH4 and O2, as well as plasma-generated radicals and stable intermediates. Our results show that vibrational excitation enhances the turnover frequency (TOF) of catalytic CH4 dissociation and has good potential for improving the selectivities toward CH3OH, HCOOH, and C2 hydrocarbons. Nevertheless, when also considering plasma-generated radicals, we find that these species mainly govern the surface chemistry. Additionally, we find that plasma-generated radicals and stable intermediates enhance the TOFs of COx and oxygenates, increase the selectivity toward oxygenates, and make the formation of HCOOH more significant on Pt(111). We also briefly illustrate the potential impact of Eley−Rideal reactions that involve plasma-generated radicals. Finally, we reveal how various radicals affect the catalyst surface chemistry and we link this to the formation of different products. This allows us to make suggestions on how the plasma composition should be altered to improve the formation of desired products. |
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Wos |
000619760700017 |
Publication Date |
2021-02-11 |
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Series Editor |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.536 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
Universiteit Antwerpen; Fonds Wetenschappelijk Onderzoek, S001619N ; H2020 European Research Council, 810182 ; We thank Tom Butterworth for the interesting discussions regarding the calculation of the vibrational populations of methane and for taking the time to share his thoughts and experiences on the matter. This research is supported by the FWO-SBO project PLASMACATDesign (grant number S001619N). We also acknowledge financial support from the TOP-BOF project of the University of Antwerp and from the European Research Council (ERC) under the European Union’s Horizon 2020 Research and Innovation Program (grant agreement no. 810182SCOPE ERC Synergy project). The calculations were carried out using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen, a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (Department EWI), and the University of Antwerp. |
Approved |
Most recent IF: 4.536 |
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Call Number |
PLASMANT @ plasmant @c:irua:175873 |
Serial |
6672 |
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Permanent link to this record |
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Author |
Ranjbar, S.; Shahmansouri, M.; Attri, P.; Bogaerts, A. |
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Title |
Effect of plasma-induced oxidative stress on the glycolysis pathway of Escherichia coli |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Computers In Biology And Medicine |
Abbreviated Journal |
Comput Biol Med |
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Volume |
127 |
Issue |
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Pages |
104064 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
Antibiotic resistance is one of the world’s most urgent public health problems. Due to its antibacterial properties, cold atmospheric plasma (CAP) may serve as an alternative method to antibiotics. It is claimed that oxidative stress caused by CAP is the main reason of bacteria inactivation. In this work, we computationally investigated the effect of plasma-induced oxidation on various glycolysis metabolites, by monitoring the production of the biomass. We observed that in addition to the significant reduction in biomass production, the rate of some reactions has increased. These reactions produce anti-oxidant products, showing the bacterial defense mechanism to escape the oxidative damage. Nevertheless, the simulations show that the plasma-induced oxidation effect is much stronger than the defense mechanism, causing killing of the bacteria. |
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Place of Publication |
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Wos |
000603362700001 |
Publication Date |
2020-11-02 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0010-4825 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7.7 |
Times cited |
|
Open Access |
|
|
|
Notes |
Ministry of Science and Technology of Iran; Hercules Foundation; Flemish Government; EWI; S. R. acknowledges funding from the Ministry of Science and Technology of Iran. The computational work was carried out using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UA), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the universitteit Antwerpen. We also would like to thank Dr. Charlotta Bengtson for her suggestions in writing this paper. |
Approved |
Most recent IF: 7.7; 2020 IF: 1.836 |
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Call Number |
PLASMANT @ plasmant @c:irua:173860 |
Serial |
6437 |
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Permanent link to this record |
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Author |
Cai, Y.; Michiels, R.; De Luca, F.; Neyts, E.; Tu, X.; Bogaerts, A.; Gerrits, N. |
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Title |
Improving Molecule–Metal Surface Reaction Networks Using the Meta-Generalized Gradient Approximation: CO2Hydrogenation |
Type |
A1 Journal Article |
|
Year |
2024 |
Publication |
The Journal of Physical Chemistry C |
Abbreviated Journal |
J. Phys. Chem. C |
|
|
Volume |
128 |
Issue |
21 |
Pages |
8611-8620 |
|
|
Keywords |
A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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|
Abstract |
Density functional theory is widely used to gain insights into molecule−metal surface reaction networks, which is important for a better understanding of catalysis. However, it is well-known that generalized gradient approximation (GGA)
density functionals (DFs), most often used for the study of reaction networks, struggle to correctly describe both gas-phase molecules and metal surfaces. Also, GGA DFs typically underestimate reaction barriers due to an underestimation of the selfinteraction energy. Screened hybrid GGA DFs have been shown to reduce this problem but are currently intractable for wide usage. In this work, we use a more affordable meta-GGA (mGGA) DF in combination with a nonlocal correlation DF for the first time to study and gain new insights into a catalytically important surface
reaction network, namely, CO2 hydrogenation on Cu. We show that the mGGA DF used, namely, rMS-RPBEl-rVV10, outperforms typical GGA DFs by providing similar or better predictions for metals and molecules, as well as molecule−metal surface adsorption
and activation energies. Hence, it is a better choice for constructing molecule−metal surface reaction networks. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Language |
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Wos |
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Publication Date |
2024-05-30 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
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Edition |
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ISSN |
1932-7447 |
ISBN |
|
Additional Links |
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Impact Factor |
3.7 |
Times cited |
|
Open Access |
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|
Notes |
H2020 Marie Sklodowska-Curie Actions, 813393 ; Fonds Wetenschappelijk Onderzoek, 1114921N ; H2020 European Research Council, 810182 ; Nederlandse Organisatie voor Wetenschappelijk Onderzoek, 019.202EN.012 ; |
Approved |
Most recent IF: 3.7; 2024 IF: 4.536 |
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|
Call Number |
PLASMANT @ plasmant @ |
Serial |
9248 |
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Permanent link to this record |
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Author |
Michiels, R.; Gerrits, N.; Neyts, E.; Bogaerts, A. |
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Title |
Plasma Catalysis Modeling: How Ideal Is Atomic Hydrogen for Eley–Rideal? |
Type |
A1 Journal Article |
|
Year |
2024 |
Publication |
The Journal of Physical Chemistry C |
Abbreviated Journal |
J. Phys. Chem. C |
|
|
Volume |
128 |
Issue |
27 |
Pages |
11196-11209 |
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Keywords |
A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
Plasma catalysis is an emerging technology, but a lot of questions about the underlying surface mechanisms remain unanswered. One of these questions is how important Eley−Rideal (ER) reactions are, next to Langmuir−Hinshelwood reactions. Most plasma catalysis kinetic models predict ER reactions to be important and sometimes even vital for the surface chemistry. In this work, we take a critical look at how ER reactions involving H radicals are incorporated in kinetic models describing CO2 hydrogenation and NH3 synthesis. To this end, we construct potential energy surface (PES) intersections, similar to elbow plots constructed for dissociative chemisorption. The results of the PES intersections are in agreement with ab initio molecular dynamics (AIMD) findings in literature while being computationally much cheaper. We find that, for the reactions studied here, adsorption is more probable than a reaction via the hot atom (HA) mechanism, which in turn is more probable than a reaction via the ER mechanism. We also conclude that kinetic models of plasma-catalytic systems tend to overestimate the importance if ER reactions. Furthermore, as opposed to what is often assumed in kinetic models, the choice of catalyst will influence the ER reaction probability. Overall, the description of ER reactions is too much “ideal” in models. Based on our indings, we make a number of recommendations on how to incorporate ER reactions in kinetic models to avoid overestimation of their importance. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
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Publication Date |
2024-07-11 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
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Impact Factor |
3.7 |
Times cited |
|
Open Access |
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|
Notes |
Fonds Wetenschappelijk Onderzoek, 1114921N ; Horizon 2020 Framework Programme, 810182 ; |
Approved |
Most recent IF: 3.7; 2024 IF: 4.536 |
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Call Number |
PLASMANT @ plasmant @ |
Serial |
9251 |
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Permanent link to this record |
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Author |
Vanraes, P.; Bogaerts, A. |
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Title |
The essential role of the plasma sheath in plasma–liquid interaction and its applications—A perspective |
Type |
A1 Journal Article |
|
Year |
2021 |
Publication |
Journal Of Applied Physics |
Abbreviated Journal |
J Appl Phys |
|
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Volume |
129 |
Issue |
22 |
Pages |
220901 |
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Keywords |
A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
Based on the current knowledge, a plasma–liquid interface looks and behaves very differently from its counterpart at a solid surface. Local processes characteristic to most liquids include a stronger evaporation, surface deformations, droplet ejection, possibly distinct mechanisms behind secondary electron emission, the formation of an electric double layer, and an ion drift-mediated liquid resistivity. All of them can strongly influence the interfacial charge distribution. Accordingly, the plasma sheath at a liquid surface is most likely unique in its own way, both with respect to its structure and behavior. However, insights into these properties are still rather scarce or uncertain, and more studies are required to further disclose them. In this Perspective, we argue why more research on the plasma sheath is not only recommended but also crucial to an accurate understanding of the plasma–liquid interaction. First, we analyze how the sheath regulates various elementary processes at the plasma–liquid interface, in terms of the electrical coupling, the bidirectional mass transport, and the chemistry between plasma and liquid phase. Next, these three regulatory functions of the sheath are illustrated for concrete applications. Regarding the electrical coupling, a great deal of attention is paid to the penetration of fields into biological systems due to their relevance for plasma medicine, plasma agriculture, and food processing. Furthermore, we illuminate the role of the sheath in nuclear fusion, nanomaterial synthesis, and chemical applications. As such, we hope to motivate the plasma community for more fundamental research on plasma sheaths at liquid surfaces. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000681700000013 |
Publication Date |
2021-06-14 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0021-8979 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
2.068 |
Times cited |
|
Open Access |
OpenAccess |
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Notes |
P.V. thanks Dr. Angela Privat Maldonado (University of Antwerp) for the fruitful discussions on Sec. III and Professor Mark J. Kushner (University of Michigan) for the interesting discussion on Ref. 198. |
Approved |
Most recent IF: 2.068 |
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Call Number |
PLASMANT @ plasmant @c:irua:178814 |
Serial |
6794 |
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Permanent link to this record |
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Author |
Bruggeman, P.J.; Bogaerts, A.; Pouvesle, J.M.; Robert, E.; Szili, E.J. |
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Title |
Plasma–liquid interactions |
Type |
A1 Journal Article |
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Year |
2021 |
Publication |
Journal Of Applied Physics |
Abbreviated Journal |
J Appl Phys |
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Volume |
130 |
Issue |
20 |
Pages |
200401 |
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Keywords |
A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
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Publication Date |
2021-11-28 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0021-8979 |
ISBN |
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Additional Links |
UA library record |
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Impact Factor |
2.068 |
Times cited |
|
Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 2.068 |
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Call Number |
PLASMANT @ plasmant @c:irua:184245 |
Serial |
6830 |
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Permanent link to this record |
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Author |
Bals, S.; Batenburg, K.J.; Liang, D.; Lebedev, O.; Van Tendeloo, G.; Aerts, A.; Martens, J.A.; Kirschhock, C.E. |
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Title |
Quantitative three-dimensional modeling of zeotile through discrete electron tomography |
Type |
A1 Journal article |
|
Year |
2009 |
Publication |
Journal of the American Chemical Society |
Abbreviated Journal |
J Am Chem Soc |
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Volume |
131 |
Issue |
13 |
Pages |
4769-4773 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Vision lab |
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Abstract |
Discrete electron tomography is a new approach for three-dimensional reconstruction of nanoscale objects. The technique exploits prior knowledge of the object to be reconstructed, which results in an improvement of the quality of the reconstructions. Through the combination of conventional transmission electron microscopy and discrete electron tomography with a model-based approach, quantitative structure determination becomes possible. In the present work, this approach is used to unravel the building scheme of Zeotile-4, a silica material with two levels of structural order. The layer sequence of slab-shaped building units could be identified. Successive layers were found to be related by a rotation of 120°, resulting in a hexagonal space group. The Zeotile-4 material is a demonstration of the concept of successive structuring of silica at two levels. At the first level, the colloid chemical properties of Silicalite-1 precursors are exploited to create building units with a slablike geometry. At the second level, the slablike units are tiled using a triblock copolymer to serve as a mesoscale structuring agent. |
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Place of Publication |
Washington, D.C. |
Editor |
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Language |
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Wos |
000264806300050 |
Publication Date |
2009-03-16 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0002-7863;1520-5126; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.858 |
Times cited |
58 |
Open Access |
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Notes |
Fwo; Iap; Esteem 026019 |
Approved |
Most recent IF: 13.858; 2009 IF: 8.580 |
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Call Number |
UA @ lucian @ c:irua:76393 |
Serial |
2767 |
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Permanent link to this record |
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Author |
Neyts, E.C.; Bogaerts, A. |
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Title |
Combining molecular dynamics with Monte Carlo simulations : implementations and applications |
Type |
A1 Journal article |
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Year |
2013 |
Publication |
Theoretical chemistry accounts : theory, computation, and modeling |
Abbreviated Journal |
Theor Chem Acc |
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Volume |
132 |
Issue |
2 |
Pages |
1320-12 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
In this contribution, we present an overview of the various techniques for combining atomistic molecular dynamics with Monte Carlo simulations, mainly in the context of condensed matter systems, as well as a brief summary of the main accelerated dynamics techniques. Special attention is given to the force bias Monte Carlo technique and its combination with molecular dynamics, in view of promising recent developments, including a definable timescale. Various examples of the application of combined molecular dynamics / Monte Carlo simulations are given, in order to demonstrate the enhanced simulation efficiency with respect to either pure molecular dynamics or Monte Carlo. |
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Wos |
000318294700010 |
Publication Date |
2012-12-19 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1432-881X;1432-2234; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
1.89 |
Times cited |
27 |
Open Access |
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Notes |
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Approved |
Most recent IF: 1.89; 2013 IF: 2.143 |
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Call Number |
UA @ lucian @ c:irua:104725 |
Serial |
404 |
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Permanent link to this record |
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Author |
Neyts, E.C.; van Duin, A.C.T.; Bogaerts, A. |
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Title |
Changing chirality during single-walled carbon nanotube growth : a reactive molecular dynamics/Monte Carlo study |
Type |
A1 Journal article |
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Year |
2011 |
Publication |
Journal of the American Chemical Society |
Abbreviated Journal |
J Am Chem Soc |
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Volume |
133 |
Issue |
43 |
Pages |
17225-17231 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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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 |
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Publisher |
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Place of Publication |
Washington, D.C. |
Editor |
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Language |
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Wos |
000297380900026 |
Publication Date |
2011-10-06 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0002-7863;1520-5126; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.858 |
Times cited |
116 |
Open Access |
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Notes |
|
Approved |
Most recent IF: 13.858; 2011 IF: 9.907 |
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Call Number |
UA @ lucian @ c:irua:92043 |
Serial |
309 |
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Permanent link to this record |
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Author |
Petrović, D.; Martens, T.; van Dijk, J.; Brok, W.J.M.; Bogaerts, A. |
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Title |
Modeling of a dielectric barrier discharge used as a flowing chemical reactor |
Type |
A1 Journal article |
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Year |
2008 |
Publication |
Journal of physics : conference series |
Abbreviated Journal |
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Volume |
133 |
Issue |
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Pages |
012023,1-012023,8 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
Our aim is to develop and optimize a model for a dielectric barrier discharge used as a chemical reactor for gas treatment. In order to determine the optimum operating conditions, we have studied the influence of the gas flow rate, reactor geometry and applied voltage parameters on the discharge characteristics. For this purpose, a two-dimensional time-dependent fluid model has been applied to an atmospheric pressure DBD in helium with nitrogen impurities, in a cylindrical geometry. The numerical model is based on the continuity and flux equations for each type of particles treated, the electron energy equation and the Poisson equation. The gas flow is incorporated in the flux equations as a source term. The set of coupled partial differential equations is solved by the so-called modified strongly implicit method. The background gas flow is numerically treated separately, assuming in the model that there is no influence of the plasma on the flow. Indeed, the gas convection velocity is calculated using the commercial code Fluent and it is used as input into the 2D fluid model. The plasma characteristics have been studied in terms of gas flow rate, applied voltage amplitude and frequency, and geometrical effects. The electric currents as a function of time for a given applied potential have been obtained, as well as the number densities and fluxes of plasma species. |
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Publisher |
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Place of Publication |
Bristol |
Editor |
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Language |
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Wos |
000265684100023 |
Publication Date |
2008-11-07 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1742-6596; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
|
Times cited |
6 |
Open Access |
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Notes |
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Approved |
Most recent IF: NA |
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Call Number |
UA @ lucian @ c:irua:71282 |
Serial |
2115 |
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Permanent link to this record |
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Author |
Neyts, E.C.; van Duin, A.C.T.; Bogaerts, A. |
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Title |
Insights in the plasma-assisted growth of carbon nanotubes through atomic scale simulations : effect of electric field |
Type |
A1 Journal article |
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Year |
2012 |
Publication |
Journal of the American Chemical Society |
Abbreviated Journal |
J Am Chem Soc |
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Volume |
134 |
Issue |
2 |
Pages |
1256-1260 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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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 |
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Thesis |
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Publisher |
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Place of Publication |
Washington, D.C. |
Editor |
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Language |
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Wos |
000301084300086 |
Publication Date |
2011-11-30 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0002-7863;1520-5126; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.858 |
Times cited |
56 |
Open Access |
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Notes |
|
Approved |
Most recent IF: 13.858; 2012 IF: 10.677 |
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Call Number |
UA @ lucian @ c:irua:97163 |
Serial |
1673 |
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Permanent link to this record |
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Author |
Oliveira, M.C.; Yusupov, M.; Cordeiro, R.M.; Bogaerts, A. |
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Title |
Unraveling the permeation of reactive species across nitrated membranes by computer simulations |
Type |
A1 Journal Article;Reactive oxygen and nitrogen species |
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Year |
2021 |
Publication |
Computers In Biology And Medicine |
Abbreviated Journal |
Comput Biol Med |
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Volume |
136 |
Issue |
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Pages |
104768 |
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Keywords |
A1 Journal Article;Reactive oxygen and nitrogen species; Nitro-oxidative stress; Molecular dynamics simulations; Nitrated membranes; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
Reactive oxygen and nitrogen species (RONS) are involved in many biochemical processes, including nitrooxidative stress that causes cancer cell death, observed in cancer therapies such as photodynamic therapy and cold atmospheric plasma. However, their mechanisms of action and selectivity still remain elusive due to the complexity of biological cells. For example, it is not well known how RONS generated by cancer therapies permeate the cell membrane to cause nitro-oxidative damage. There are many studies dedicated to the permeation of RONS across native and oxidized membranes, but not across nitrated membranes, another lipid product also generated during nitro-oxidative stress. Herein, we performed molecular dynamics (MD) simulations to calculate the free energy barrier of RONS permeation across nitrated membranes. Our results show that hydrophilic RONS, such as hydroperoxyl radical (HO2) and peroxynitrous acid (ONOOH), have relatively low barriers compared to hydrogen peroxide (H2O2) and hydroxyl radical (HO), and are more prone to permeate the membrane than for the native or peroxidized membranes, and similar to aldehyde-oxidized membranes. Hydrophobic RONS like molecular oxygen (O2), nitrogen dioxide (NO2) and nitric oxide (NO) even have insignificant barriers for permeation. Compared to native and peroxidized membranes, nitrated membranes are more permeable, suggesting that we must not only consider oxidized membranes during nitro-oxidative stress, but also nitrated membranes, and their role in cancer therapies. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000696938800003 |
Publication Date |
2021-08-17 |
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Series Editor |
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Series Title |
|
Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0010-4825 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
1.836 |
Times cited |
|
Open Access |
OpenAccess |
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Notes |
We thank University of Antwerp and Coordination of Superior Level Staff Improvement (CAPES, Brazil) for the scholarship granted and for providing the computational resources needed for completion of this work. M. Yusupov acknowledges the Flanders Research Foundation (grant 1200219N) for financial support. |
Approved |
Most recent IF: 1.836 |
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Call Number |
PLASMANT @ plasmant @c:irua:181082 |
Serial |
6807 |
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Permanent link to this record |
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Author |
Attri, P.; Razzokov, J.; Yusupov, M.; Koga, K.; Shiratani, M.; Bogaerts, A. |
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Title |
Influence of osmolytes and ionic liquids on the Bacteriorhodopsin structure in the absence and presence of oxidative stress: A combined experimental and computational study |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
International Journal Of Biological Macromolecules |
Abbreviated Journal |
Int J Biol Macromol |
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Volume |
148 |
Issue |
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Pages |
657-665 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
Understanding the folding and stability of membrane proteins is of great importance in protein science. Recently, osmolytes and ionic liquids (ILs) are increasingly being used as drug delivery systems in the biopharmaceutical industry. However, the stability of membrane proteins in the presence of osmolytes and ILs is not yet fully understood. Besides, the effect of oxidative stress on membrane proteins with osmolytes or ILs has not been investigated. Therefore, we studied the influence of osmolytes and ILs as co-solvents on the stability of a model membrane protein (i.e., Bacteriorhodopsin in purple membrane of Halobacterium salinarum), using UV–Vis spectroscopy and molecular dynamics (MD) simulations. The MD simulations allowed us to determine the flexibility and solvent accessible surface area (SASA) of Bacteriorhodopsin protein in the presence and/or absence of cosolvents, as well as to carry out principal component analysis (PCA) to identify the most important movements in this protein. In addition, by means of UV–Vis spectroscopy we studied the effect of oxidative stress generated by cold atmospheric plasma on the stability of Bacteriorhodopsin in the presence and/or absence of co-solvents. This study is important for a better understanding of the stability of proteins in the presence of oxidative stress. |
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Place of Publication |
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Wos |
000522094600066 |
Publication Date |
2020-01-20 |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0141-8130 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
8.2 |
Times cited |
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Open Access |
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Notes |
Horizon2020, 743546 ; JSPS, 19H05462 16H03895 ; Nagoya University; We gratefully acknowledge the European Marie Skłodowska-Curie Individual Fellowship “Anticancer-PAM” within Horizon2020 (grant number 743546). This work was also supported by JSPS-KAKENHI 19H05462 and 16H03895, the joint usage/research program of Center for Low-temperature Plasma Science, Nagoya University and also supported by JSPS and RCL under the Japan-Lithuania Research Cooperative Program. The computational work was carried out using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UA), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the UA. |
Approved |
Most recent IF: 8.2; 2020 IF: 3.671 |
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Call Number |
PLASMANT @ plasmant @c:irua:165585 |
Serial |
5444 |
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Permanent link to this record |
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Author |
Peng, L.; Philippaerts, A.; Ke, X.; van Noyen, J.; de Cleppel, F.; Van Tendeloo, G.; Jacobs, P.A.; Sels, B.F. |
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Title |
Preparation of sulfonated ordered mesoporous carbon and its use for the esterification of fatty acids |
Type |
A1 Journal article |
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Year |
2010 |
Publication |
Catalysis today |
Abbreviated Journal |
Catal Today |
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Volume |
150 |
Issue |
1/2 |
Pages |
140-146 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Mesoporous carbon, which can be replicated from mesoporous silica and whose surface is hydrophobic, can be an ideal catalyst for the esterification of fatty acids. Here we report an easy and low cost way to prepare sulfonic acid group-functionalized mesoporous carbon. A sample of calcined mesoporous silica SBA-15 was added to an aqueous sucrose solution followed by drying and calcination at different temperatures. In contrast to existing procedures, the obtained hybrid Si/C material was then first sulfonated in H2SO4, before the final removal of the silica template in order to stabilize the porous structure towards the liquid phase sulfonation treatment. Thus the silicacarbon composites, instead of the mesoporous carbon, were successfully sulfonated to introduce SO3H groups, while keeping the ordered mesoporous structure intact. The influence of carbonization temperature was investigated, suggesting an optimum temperature of 873 K. The SO3H group-functionalized mesoporous carbon, denoted as CMK-3-873-SO3H, was characterized by means of XRD, N2 physisorption, SEM, FT-IR, elemental analysis and TEM. It followed that a uniform mesoporous carbon was obtained with an average pore size of 3.89 nm, a specific surface of 807 m2/g and a SO3H group loading of 0.39 meq/g of dry material. Compared with other solid acid catalysts, the resulting material shows enhanced activity in the acid-catalyzed esterification of oleic acid with methanol, and can be used repeatedly. The increased catalytic performance is attributed to the hydrophobic surface and larger pore size of the new catalyst. It can effectively accommodate long chain fatty acids and reject formed water, making the active sites easily accessible. |
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Publisher |
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Place of Publication |
Amsterdam |
Editor |
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Wos |
000275566700024 |
Publication Date |
2009-09-04 |
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Abbreviated Series Title |
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Series Issue |
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Edition |
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ISSN |
0920-5861; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.636 |
Times cited |
132 |
Open Access |
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Notes |
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Approved |
Most recent IF: 4.636; 2010 IF: 2.993 |
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Call Number |
UA @ lucian @ c:irua:81739 |
Serial |
2706 |
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Permanent link to this record |