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Records |
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Author |
Vets, C.; Neyts, E.C. |
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Title |
Stabilities of bimetallic nanoparticles for chirality-selective carbon nanotube growth and the effect of carbon interstitials |
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 |
28 |
Pages |
15430-15436 |
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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 |
Bimetallic nanoparticles play a crucial role in various applications. A better understanding of their properties would facilitate these applications and possibly even enable chirality-specific growth of carbon nanotubes (CNTs). We here examine the stabilities of NiFe, NiGa, and FeGa nanoparticles and the effect of carbon dissolved in NiFe nanoparticles through density functional theory (DFT) calculations and Born Oppenheimer molecular dynamics (BOMD) simulations. We establish that nanoparticles with more Fe in the core and more Ga on the surface are more stable and compare these results with well-known properties such as surface energy and atom size. Furthermore, we find that the nanoparticles become more stable with increasing carbon content, both at 0 K and at 700 K. These results provide a basis for further research into the chirality-specific growth of CNT's. |
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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 |
000406355700050 |
Publication Date |
2017-06-23 |
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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; 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 |
2 |
Open Access |
Not_Open_Access |
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Notes |
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Approved |
Most recent IF: 4.536 |
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Call Number |
UA @ lucian @ c:irua:145206 |
Serial |
4725 |
| Permanent link to this record |
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Author |
Cleiren, E.; Heijkers, S.; Ramakers, M.; Bogaerts, A. |
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Title |
Dry Reforming of Methane in a Gliding Arc Plasmatron: Towards a Better Understanding of the Plasma Chemistry |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
Chemsuschem |
Abbreviated Journal |
Chemsuschem |
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Volume |
10 |
Issue |
20 |
Pages |
4025-4036 |
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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 |
Dry reforming of methane (DRM) in a gliding arc plasmatron is studied for different CH4 fractions in the mixture. The CO2 and CH4 conversions reach their highest values of approximately 18 and 10%, respectively, at 25% CH4 in the gas mixture, corresponding to an overall energy cost of 10 kJ L@1 (or 2.5 eV per molecule) and an energy efficiency of 66%. CO and H2 are the major products, with the formation of smaller fractions of C2Hx (x=2, 4, or 6) compounds and H2O. A chemical kinetics model is used to investigate the underlying chemical processes. The calculated CO2 and CH4 conversion and the energy efficiency are in good agreement with the experimental data. The model calculations reveal that the reaction of CO2 (mainly at vibrationally excited levels) with H radicals is mainly responsible for
the CO2 conversion, especially at higher CH4 fractions in the mixture, which explains why the CO2 conversion increases with increasing CH4 fraction. The main process responsible for CH4 conversion is the reaction with OH radicals. The excellent energy efficiency can be explained by the non-equilibrium character of the plasma, in which the electrons mainly activate the gas molecules, and by the important role of the vibrational kinetics of CO2. The results demonstrate that a gliding arc plasmatron is very promising for DRM. |
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Corporate Author |
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Place of Publication |
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Wos |
000413565100012 |
Publication Date |
2017-10-02 |
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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 |
1864-5631 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7.226 |
Times cited |
23 |
Open Access |
OpenAccess |
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Notes |
Fonds Wetenschappelijk Onderzoek, G.0383.16N ; Federaal Wetenschapsbeleid; |
Approved |
Most recent IF: 7.226 |
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Call Number |
PLASMANT @ plasmant @c:irua:146665 |
Serial |
4759 |
| 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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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 |
000413617900007 |
Publication Date |
2017-10-19 |
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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 |
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 |
| 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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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 |
000431151200002 |
Publication Date |
2018-04-26 |
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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 |
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 |
| Permanent link to this record |
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Author |
Bal, K.M.; Neyts, E.C. |
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Title |
Overcoming Old Scaling Relations and Establishing New Correlations in Catalytic Surface Chemistry: Combined Effect of Charging and Doping |
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 |
10 |
Pages |
6141-6147 |
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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 |
Optimization of catalytic materials for a given application is greatly constrained by linear scaling relations. Recently, however, it has been demonstrated that it is possible to reversibly modulate the chemisorption of molecules on nanomaterials by charging (i.e., injection or removal of electrons) and hence reversibly and selectively modify catalytic activity beyond structure−activity correlations. The fundamental physical relation between the properties of the material, the charging process, and the chemisorption energy, however, remains unclear, and a systematic exploration and optimization of charge-switchable sorbent materials is not yet possible. Using hybrid DFT calculations of CO2 chemisorption on hexagonal boron nitride nanosheets with several types of defects and dopants, we here reveal the existence of fundamental correlations between the electron affinity of a material and charge-induced chemisorption, show how defect engineering can be used to modulate the strength and efficiency of the adsorption process, and demonstrate that excess electrons stabilize many topological defects. We then show how these insights could be exploited in the development of new electrocatalytic materials and the synthesis of doped nanomaterials. Moreover, we demonstrate that calculated chemical properties of charged materials are highly sensitive to the employed computational methodology because of the self-interaction error, which underlines the theoretical challenge posed by such systems. |
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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 |
000461537400035 |
Publication Date |
2019-03-14 |
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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 |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
| |
Impact Factor |
4.536 |
Times cited |
5 |
Open Access |
Not_Open_Access: Available from 21.02.2020
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Notes |
Fonds Wetenschappelijk Onderzoek, 11V8915N ; |
Approved |
Most recent IF: 4.536 |
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Call Number |
PLASMANT @ plasmant @UA @ admin @ c:irua:158117 |
Serial |
5160 |
| 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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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 |
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 |
| 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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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 |
000462260700024 |
Publication Date |
2019-02-21 |
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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; 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 |
| 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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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 |
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 |
| Permanent link to this record |
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Author |
Bal, K.M.; Bogaerts, A.; Neyts, E.C. |
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Title |
Ensemble-Based Molecular Simulation of Chemical Reactions under Vibrational Nonequilibrium |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Journal Of Physical Chemistry Letters |
Abbreviated Journal |
J Phys Chem Lett |
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Volume |
11 |
Issue |
2 |
Pages |
401-406 |
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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 present an approach to incorporate the effect of vibrational nonequilibrium in molecular dynamics (MD) simulations. A perturbed canonical ensemble, in which selected modes are excited to higher temperature while all others remain equilibrated at low temperature, is simulated by applying a specifically tailored bias potential. Our method can be readily applied to any (classical or quantum mechanical) MD setup at virtually no additional computational cost and allows the study of reactions of vibrationally excited molecules in nonequilibrium environments such as plasmas. In combination with enhanced sampling methods, the vibrational efficacy and mode selectivity of vibrationally stimulated reactions can then be quantified in terms of chemically relevant observables, such as reaction rates and apparent free energy barriers. We first validate our method for the prototypical hydrogen exchange reaction and then show how it can capture the effect of vibrational excitation on a symmetric SN2 reaction and radical addition on CO2. |
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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 |
000508473400008 |
Publication Date |
2020-01-16 |
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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 |
1948-7185 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
5.7 |
Times cited |
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Open Access |
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Notes |
Universiteit Antwerpen; Fonds Wetenschappelijk Onderzoek, 12ZI420N ; Departement Economie, Wetenschap en Innovatie van de Vlaamse Overheid; K.M.B. was funded as a junior postdoctoral fellow of the FWO (Research Foundation − Flanders), Grant 12ZI420N, and through a TOP-BOF research project of the University of Antwerp. The computational resources and services used in this work were provided by the VSC (Flemish Supercomputer Center), funded by the FWO and the Flemish Government− department EWI. |
Approved |
Most recent IF: 5.7; 2020 IF: 9.353 |
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Call Number |
PLASMANT @ plasmant @c:irua:165587 |
Serial |
5442 |
| 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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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 |
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 |
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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 |
| |
Call Number |
PLASMANT @ plasmant @c:irua:165586 |
Serial |
5443 |
| Permanent link to this record |
| |
|
| |
|
Author |
Slaets, J.; Aghaei, M.; Ceulemans, S.; Van Alphen, S.; Bogaerts, A. |
| |
Title |
CO2and CH4conversion in “real” gas mixtures in a gliding arc plasmatron: how do N2and O2affect the performance? |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Green Chemistry |
Abbreviated Journal |
Green Chem |
| |
Volume |
22 |
Issue |
4 |
Pages |
1366-1377 |
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
| |
Abstract |
In this paper we study dry reforming of methane (DRM) in a gliding arc plasmatron (GAP) in the presence of N<sub>2</sub>and O<sub>2</sub>. N<sub>2</sub>is added to create a stable plasma at equal fractions of CO<sub>2</sub>and CH<sub>4</sub>, and because emissions from industrial plants typically contain N<sub>2</sub>, while O<sub>2</sub>is added to enhance the process. We test different gas mixing ratios to evaluate the conversion and energy cost. We obtain conversions between 31 and 52% for CO<sub>2</sub>and between 55 and 99% for CH<sub>4</sub>, with total energy costs between 3.4 and 5.0 eV per molecule, depending on the gas mixture. This is very competitive when benchmarked with the literature. In addition, we present a chemical kinetics model to obtain deeper insight in the underlying plasma chemistry. This allows determination of the major reaction pathways to convert CO<sub>2</sub>and CH<sub>4</sub>, in the presence of O<sub>2</sub>and N<sub>2</sub>, into CO and H<sub>2</sub>. We show that N<sub>2</sub>assists in the CO<sub>2</sub>conversion, but part of the applied energy is also wasted in N<sub>2</sub>excitation. Adding O<sub>2</sub>enhances the CH<sub>4</sub>conversion, and lowers the energy cost, while the CO<sub>2</sub>conversion remains constant, and only slightly drops at the highest O<sub>2</sub>fractions studied, when CH<sub>4</sub>is fully oxidized into CO<sub>2</sub>. |
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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 |
000518034000032 |
Publication Date |
2020-01-30 |
| |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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| |
Series Volume |
|
Series Issue |
|
Edition |
|
| |
ISSN |
1463-9262 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
| |
Impact Factor |
9.8 |
Times cited |
|
Open Access |
OpenAccess |
| |
Notes |
H2020 European Research Council, 810182 ; Fonds Wetenschappelijk Onderzoek, GoF9618n 12M7118N ; We acknowledge financial support 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), the Excellence of Science FWO-FNRS project (FWO grant ID GoF9618n, EOS ID 30505023), and the FWO postdoctoral fellowship of M. A. (Grant number 12M7118N). 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: 9.8; 2020 IF: 9.125 |
| |
Call Number |
PLASMANT @ plasmant @c:irua:167136 |
Serial |
6339 |
| Permanent link to this record |
| |
|
| |
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Author |
Heijkers, S.; Aghaei, M.; Bogaerts, A. |
| |
Title |
Plasma-Based CH4Conversion into Higher Hydrocarbons and H2: Modeling to Reveal the Reaction Mechanisms of Different Plasma Sources |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Journal Of Physical Chemistry C |
Abbreviated Journal |
J Phys Chem C |
| |
Volume |
124 |
Issue |
13 |
Pages |
7016-7030 |
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
| |
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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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 |
000526328500007 |
Publication Date |
2020-04-02 |
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Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
| |
ISSN |
1932-7447 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
| |
Impact Factor |
3.7 |
Times cited |
|
Open Access |
OpenAccess |
| |
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 |
| |
Call Number |
PLASMANT @ plasmant @c:irua:168096 |
Serial |
6358 |
| Permanent link to this record |
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|
| |
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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 |
| |
Year |
2020 |
Publication |
Journal Of Physical Chemistry C |
Abbreviated Journal |
J Phys Chem C |
| |
Volume |
124 |
Issue |
12 |
Pages |
6747-6755 |
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
| |
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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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 |
000526396900030 |
Publication Date |
2020-03-26 |
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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 |
|
Edition |
|
| |
ISSN |
1932-7447 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
| |
Impact Factor |
3.7 |
Times cited |
|
Open Access |
|
| |
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 |
| |
Call Number |
PLASMANT @ plasmant @c:irua:168606 |
Serial |
6361 |
| Permanent link to this record |
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|
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Author |
Vervloessem, E.; Aghaei, M.; Jardali, F.; Hafezkhiabani, N.; Bogaerts, A. |
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Title |
Plasma-Based N2Fixation into NOx: Insights from Modeling toward Optimum Yields and Energy Costs in a Gliding Arc Plasmatron |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Acs Sustainable Chemistry & Engineering |
Abbreviated Journal |
Acs Sustain Chem Eng |
| |
Volume |
8 |
Issue |
26 |
Pages |
9711-9720 |
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
| |
Abstract |
Plasma technology provides a sustainable, fossil-free method for N2 fixation, i.e., the conversion of inert atmospheric N2 into valuable substances, such as NOx or ammonia. In this work, we present a novel gliding arc plasmatron at atmospheric pressure for NOx production at different N2/O2 gas feed ratios, offering a promising NOx yield of 1.5% with an energy cost of 3.6 MJ/mol NOx produced. To explain the underlying mechanisms, we present a chemical kinetics model, validated by experiments, which provides insight into the NOx formation pathways and into the ambivalent role of the vibrational kinetics. This allows us to pinpoint the factors limiting the yield and energy cost, which can help to further improve the process. |
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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 |
000548456600013 |
Publication Date |
2020-07-06 |
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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 |
|
Series Issue |
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Edition |
|
| |
ISSN |
2168-0485 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
| |
Impact Factor |
8.4 |
Times cited |
|
Open Access |
OpenAccess |
| |
Notes |
Herculesstichting; Universiteit Antwerpen; Vlaamse regering; H2020 European Research Council, 810182 ; N2 Applied; Excellence of Science FWO – FNRS project, 30505023 GoF9618n ; |
Approved |
Most recent IF: 8.4; 2020 IF: 5.951 |
| |
Call Number |
PLASMANT @ plasmant @c:irua:170138 |
Serial |
6392 |
| 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 |
| |
Year |
2020 |
Publication |
Journal Of Physical Chemistry C |
Abbreviated Journal |
J Phys Chem C |
| |
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) |
| |
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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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 |
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 |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
| |
Impact Factor |
3.7 |
Times cited |
|
Open Access |
OpenAccess |
| |
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 |
| Permanent link to this record |
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Author |
Mehta, A.N.; Mo, J.; Pourtois, G.; Dabral, A.; Groven, B.; Bender, H.; Favia, P.; Caymax, M.; Vandervorst, W. |
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Title |
Grain-boundary-induced strain and distortion in epitaxial bilayer MoS₂ lattice |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Journal Of Physical Chemistry C |
Abbreviated Journal |
J Phys Chem C |
| |
Volume |
124 |
Issue |
11 |
Pages |
6472-6478 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
| |
Abstract |
Grain boundaries between 60 degrees rotated and twinned crystals constitute the dominant type of extended line defects in two-dimensional transition metal dichalcogenides (2D MX2) when grown on a single crystalline template through van der Waals epitaxy. The two most common 60 degrees grain boundaries in MX2 layers, i.e., beta- and gamma-boundaries, introduce distinct distortion and strain into the 2D lattice. They impart a localized tensile or compressive strain on the subsequent layer, respectively, due to van der Waals coupling in bilayer MX2 as determined by combining atomic resolution electron microscopy, geometric phase analysis, and density functional theory. Based on these observations, an alternate route to strain engineering through controlling intrinsic van der Waals forces in homobilayer MX2 is proposed. In contrast to the commonly used external means, this approach enables the localized application of strain to tune the electronic properties of the 2D semiconducting channel in ultra-scaled nanoelectronic applications. |
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Place of Publication |
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Editor |
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Language |
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Wos |
000526396000067 |
Publication Date |
2020-02-21 |
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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; 1932-7455 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
| |
Impact Factor |
3.7 |
Times cited |
2 |
Open Access |
|
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Notes |
; ; |
Approved |
Most recent IF: 3.7; 2020 IF: 4.536 |
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Call Number |
UA @ admin @ c:irua:168625 |
Serial |
6528 |
| Permanent link to this record |
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Author |
Gorbanev, Y.; Vervloessem, E.; Nikiforov, A.; Bogaerts, A. |
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Title |
Nitrogen fixation with water vapor by nonequilibrium plasma : toward sustainable ammonia production |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Acs Sustainable Chemistry & Engineering |
Abbreviated Journal |
Acs Sustain Chem Eng |
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Volume |
8 |
Issue |
7 |
Pages |
2996-3004 |
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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 |
Ammonia is a crucial nutrient used for plant growth and as a building block in the pharmaceutical and chemical industry, produced via nitrogen fixation of the ubiquitous atmospheric N2. Current industrial ammonia production relies heavily on fossil resources, but a lot of work is put into developing nonfossil-based pathways. Among these is the use of nonequilibrium plasma. In this work, we investigated water vapor as a H source for nitrogen fixation into NH3 by nonequilibrium plasma. The highest selectivity toward NH3 was observed with low amounts of added H2O vapor, but the highest production rate was reached at high H2O vapor contents. We also studied the role of H2O vapor and of the plasma-exposed liquid H2O in nitrogen fixation by using isotopically labeled water to distinguish between these two sources of H2O. We show that added H2O vapor, and not liquid H2O, is the main source of H for NH3 generation. The studied catalyst- and H2-free method offers excellent selectivity toward NH3 (up to 96%), with energy consumption (ca. 95–118 MJ/mol) in the range of many plasma-catalytic H2-utilizing processes. |
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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 |
000516665500045 |
Publication Date |
2020-02-03 |
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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 |
2168-0485 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
| |
Impact Factor |
8.4 |
Times cited |
14 |
Open Access |
|
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Notes |
; This research was supported by the Excellence of Science FWO-FNRS project (FWO grant ID GoF9618n, EOS ID 30505023), the Catalisti Moonshot project P2C, and the Methusalem project of the University of Antwerp. ; |
Approved |
Most recent IF: 8.4; 2020 IF: 5.951 |
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Call Number |
UA @ admin @ c:irua:167134 |
Serial |
6568 |
| Permanent link to this record |
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Author |
Jardali, F.; Van Alphen, S.; Creel, J.; Ahmadi Eshtehardi, H.; Axelsson, M.; Ingels, R.; Snyders, R.; Bogaerts, A. |
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Title |
NOxproduction in a rotating gliding arc plasma: potential avenue for sustainable nitrogen fixation |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Green Chemistry |
Abbreviated Journal |
Green Chem |
| |
Volume |
23 |
Issue |
4 |
Pages |
1748-1757 |
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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 |
The fast growing world population demands food to survive, and nitrogen-based fertilizers are essential to ensure sufficient food production. Today, fertilizers are mainly produced from non-sustainable fossil fuels<italic>via</italic>the Haber–Bosch process, leading to serious environmental problems. We propose here a novel rotating gliding arc plasma, operating in air, for direct NO<sub>x</sub>production, which can yield high nitrogen content organic fertilizers without pollution associated with ammonia emission. We explored the efficiency of NO<sub>x</sub>production in a wide range of feed gas ratios, and for two arc modes: rotating and steady. When the arc is in steady mode, record-value NO<sub>x</sub>concentrations up to 5.5% are achieved which are 1.7 times higher than the maximum concentration obtained by the rotating arc mode, and with an energy consumption of 2.5 MJ mol<sup>−1</sup>(or<italic>ca.</italic>50 kW h kN<sup>−1</sup>);<italic>i.e.</italic>the lowest value so far achieved by atmospheric pressure plasma reactors. Computer modelling, using a combination of five different complementary approaches, provides a comprehensive picture of NO<sub>x</sub>formation in both arc modes; in particular, the higher NO<sub>x</sub>production in the steady arc mode is due to the combined thermal and vibrationally-promoted Zeldovich mechanisms. |
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Wos |
000629630600021 |
Publication Date |
2021-01-28 |
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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 |
1463-9262 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
| |
Impact Factor |
9.125 |
Times cited |
|
Open Access |
OpenAccess |
| |
Notes |
Fonds Wetenschappelijk Onderzoek, GoF9618n 30505023 ; H2020 European Research Council, 810182 ; This research was supported by a Bilateral Project with N2 Applied, the Excellence of Science FWO-FNRS 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. We also thank J.-L. Liu for the RGA design, L. Van ‘t dack and K. Leyssens for MS calibration and practical support, and K. Van ‘t Veer for the fruitful discussions on plasma kinetic modelling and for calculating the electron energy losses. |
Approved |
Most recent IF: 9.125 |
| |
Call Number |
PLASMANT @ plasmant @c:irua:176022 |
Serial |
6678 |
| Permanent link to this record |
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Author |
Vervloessem, E.; Gorbanev, Y.; Nikiforov, A.; De Geyter, N.; Bogaerts, A. |
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Title |
Sustainable NOxproduction from air in pulsed plasma: elucidating the chemistry behind the low energy consumption |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
Green Chemistry |
Abbreviated Journal |
Green Chem |
| |
Volume |
24 |
Issue |
2 |
Pages |
916-929 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
| |
Abstract |
N-Based fertilisers are paramount to support our still-growing world population. Current industrial N<sub>2</sub>fixation is heavily fossil fuel-dependent, therefore, a lot of work is put into the development of fossil-free pathways. Plasma technology offers a fossil-free and flexible method for N<sub>2</sub>fixation that is compatible with renewable energy sources. We present here a pulsed plasma jet for direct NO<sub><italic>x</italic></sub>production from air. The pulsed power allows for a record-low energy consumption (EC) of 0.42 MJ (mol N)<sup>−1</sup>. This is the lowest reported EC in plasma-based N<sub>2</sub>fixation at atmospheric pressure thus far. We compare our experimental data with plasma chemistry modelling, and obtain very good agreement. Hence, we can use our model to explain the underlying mechanisms responsible for this low EC. The pulsed power and the corresponding pulsed gas temperature are the reason for the very low EC: they provide a strong vibrational–translational non-equilibrium and promote the non-thermal Zeldovich mechanism. This insight is important for the development of the next generation of plasma sources for energy-efficient NO<sub><italic>x</italic></sub>production. |
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Place of Publication |
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Wos |
000739578400001 |
Publication Date |
2021-12-22 |
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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 |
|
| |
ISSN |
1463-9262 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
| |
Impact Factor |
9.8 |
Times cited |
|
Open Access |
Not_Open_Access |
| |
Notes |
H2020 European Research Council, grant agreement no. 810182 – SCOPE ERC Synergy project ; Herculesstichting; Fonds Wetenschappelijk Onderzoek, EOS ID 30505023 FWO grant ID GoF9618n ; Universiteit Antwerpen; This research was supported by the Excellence of Science FWO-FNRS project (NITROPLASM, FWO grant ID GoF9618n, EOS ID 30505023), the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement no. 810182 – SCOPE ERC Synergy project), and through long-term structural funding (Methusalem). 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 thank E. H. Choi and coworkers from the Plasma Bioscience Research Center (Korea) for providing the Soft Jet plasma source, as well as K. van’t Veer and C. Verheyen for the fruitful discussion on the electron loss fraction calculations. The graphical abstract was designed using resources from Flaticon.com. |
Approved |
Most recent IF: 9.8 |
| |
Call Number |
PLASMANT @ plasmant @c:irua:185450 |
Serial |
6906 |
| Permanent link to this record |
| |
|
| |
|
Author |
Hollevoet, L.; Vervloessem, E.; Gorbanev, Y.; Nikiforov, A.; De Geyter, N.; Bogaerts, A.; Martens, J.A. |
| |
Title |
Energy‐Efficient Small‐Scale Ammonia Synthesis Process with Plasma‐enabled Nitrogen Oxidation and Catalytic Reduction of Adsorbed NOx |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
Chemsuschem |
Abbreviated Journal |
Chemsuschem |
| |
Volume |
|
Issue |
|
Pages |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
| |
Abstract |
Industrial ammonia production without CO2 emission and with low energy consumption is one of the technological grand challenges of this age. Current Haber-Bosch ammonia mass production processes work with a thermally activated iron catalyst needing high pressure. The need for large volumes of hydrogen gas and the continuous operation mode render electrification of Haber-Bosch plants difficult to achieve. Electrochemical solutions at low pressure and temperature are faced with the problematic inertness of the nitrogen molecule on electrodes. Direct reduction of N2 to ammonia is only possible with very reactive chemicals such as lithium metal, the regeneration of which is energy intensive. Here, the attractiveness of an oxidative route for N2 activation was presented. N2 conversion to NOx in a plasma reactor followed by reduction with H2 on a heterogeneous catalyst at low pressure could be an energy-efficient option for small-scale distributed ammonia production with renewable electricity and without intrinsic CO2 footprint. |
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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 |
|
Wos |
000772893400001 |
Publication Date |
2022-03-25 |
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
| |
ISSN |
1864-5631 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
| |
Impact Factor |
8.4 |
Times cited |
|
Open Access |
OpenAccess |
| |
Notes |
Vlaamse regering, HBC.2019.0108 ; Vlaamse regering; KU Leuven, C3/20/067 ; We gratefully acknowledge financial support by the Flemish Government through the Moonshot cSBO project P2C (HBC.2019.0108). J.A.M. and A.B. acknowledge the Flemish Government for long-term structural funding (Methusalem). J.A.M. © 2022 Wiley-VCH GmbH |
Approved |
Most recent IF: 8.4 |
| |
Call Number |
PLASMANT @ plasmant @c:irua:187251 |
Serial |
7054 |
| Permanent link to this record |
| |
|
| |
|
Author |
Wang, Y.; Chen, Y.; Harding, J.; He, H.; Bogaerts, A.; Tu, X. |
| |
Title |
Catalyst-free single-step plasma reforming of CH4 and CO2 to higher value oxygenates under ambient conditions |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chem Eng J |
| |
Volume |
450 |
Issue |
|
Pages |
137860 |
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
| |
Abstract |
Direct conversion of CH4 and CO2 to liquid fuels and chemicals under mild conditions is appealing for biogas conversion and utilization but challenging due to the inert nature of both gases. Herein, we report a promising plasma process for the catalyst-free single-step conversion of CH4 and CO2 into higher value oxygenates (i.e., methanol, acetic acid, ethanol, and acetone) at ambient pressure and room temperature using a water-cooled dielectric barrier discharge (DBD) reactor, with methanol being the main liquid product. The distribution of liquid products could be tailored by tuning the discharge power, reaction temperature and residence time. Lower discharge powers (10–15 W) and reaction temperatures (5–20 ◦ C) were favourable for the production of liquid products, achieving the highest methanol selectivity of 43% at 5 ◦ C and 15 W. A higher discharge power and reaction temperature, on the other hand, produced more gaseous products, particularly H2 (up to 26% selectivity) and CO (up to 33% selectivity). In addition, varying these process parameters (discharge power, reaction temperature and residence time) resulted in a simultaneous change in key discharge properties, such as mean electron energy (Ee), electron density (ne) and specific energy input (SEI), all of which are essential determiners of plasma chemical reactions. According to the results of artificial neural network (ANN) models, the relative importance of these process parameters and key discharge indicators on reaction performance follows the order: discharge power > reaction temperature > residence time, and SEI > ne > Ee, respectively. This work provides new insights into the contributions and tuning mechanism of multiple parameters for optimizing the reaction performance (e.g., liquid production) in the plasma gas conversion process. |
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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 |
000830813300004 |
Publication Date |
0000-00-00 |
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Series Editor |
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Series Title |
|
Abbreviated Series Title |
|
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Series Volume |
|
Series Issue |
|
Edition |
|
| |
ISSN |
1385-8947 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
| |
Impact Factor |
15.1 |
Times cited |
|
Open Access |
OpenAccess |
| |
Notes |
This project received funding from the European Union’s Horizon 2020 research and innovation program under the Marie SklodowskaCurie grant agreement No. 813393. |
Approved |
Most recent IF: 15.1 |
| |
Call Number |
PLASMANT @ plasmant @c:irua:189502 |
Serial |
7100 |
| Permanent link to this record |
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|
| |
|
Author |
Pattyn, C.; Maira, N.; Buddhadasa, M.; Vervloessem, E.; Iseni, S.; Roy, N.C.; Remy, A.; Delplancke, M.-P.; De Geyter, N.; Reniers, F. |
| |
Title |
Disproportionation of nitrogen induced by DC plasma-driven electrolysis in a nitrogen atmosphere |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
Green Chemistry |
Abbreviated Journal |
Green Chem |
| |
Volume |
24 |
Issue |
18 |
Pages |
7100-7112 |
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
| |
Abstract |
Nitrogen disproportionation i.e. its simultaneous conversion to compounds of higher (NOx) and lower (NH3) oxidation states in a N-2 DC plasma-driven electrolysis process with a plasma cathode is investigated. This type of plasma-liquid interaction exhibits a growing interest for many applications, in particular nitrogen fixation where it represents a green alternative to the Haber-Bosch process. Optical emission spectroscopy, FTIR and electrochemical sensing systems are used to characterize the gas phase physico-chemistry while the liquid phase is analyzed via ionic chromatography and colorimetric assays. Experiments suggest that lowering the discharge current enhances nitrogen reduction and facilitates the transfer of nitrogen compounds to the liquid phase. Large amounts of water vapor appear to impact the gas discharge physico-chemistry and to favor the vibrational excitation of N-2, a key parameter for an energy-efficient nitrogen fixation. |
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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 |
|
Wos |
000847733600001 |
Publication Date |
2022-08-30 |
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Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
| |
ISSN |
1463-9262; 1463-9270 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
| |
Impact Factor |
9.8 |
Times cited |
|
Open Access |
OpenAccess |
| |
Notes |
|
Approved |
Most recent IF: 9.8 |
| |
Call Number |
UA @ admin @ c:irua:190655 |
Serial |
7145 |
| Permanent link to this record |
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Author |
Nematollahi, P.; Neyts, E.C. |
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Title |
Identification of a unique pyridinic FeN4Cx electrocatalyst for N₂ reduction : tailoring the coordination and carbon topologies |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
Journal Of Physical Chemistry C |
Abbreviated Journal |
J Phys Chem C |
| |
Volume |
126 |
Issue |
34 |
Pages |
14460-14469 |
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
| |
Abstract |
Although the heterogeneity of pyrolyzed Fe???N???C materials is known and has been reported previously, the atomic structure of the active sites and their detailed reaction mechanisms are still unknown. Here, we identified two pyridinic Fe???N4-like centers with different local C coordinates, i.e., FeN4C8 and FeN4C10, and studied their electrocatalytic activity for the nitrogen reduction reaction (NRR) based on density functional theory (DFT) calculations. We also discovered the influence of the adsorption of NH2 as a functional ligand on catalyst performance on the NRR. We confirmed that the NRR selectivity of the studied catalysts is essentially governed either by the local C coordination or by the dynamic structure associated with the FeII/FeIII. Our investigations indicate that the proposed traditional pyridinic FeN4C10 has higher catalytic activity and selectivity for the NRR than the robust FeN4C8 catalyst, while it may have outstanding activity for promoting other (electro)catalytic reactions. <comment>Superscript/Subscript Available</comment |
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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 |
|
Wos |
000859545200001 |
Publication Date |
2022-08-17 |
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Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
| |
ISSN |
1932-7447; 1932-7455 |
ISBN |
|
Additional Links |
UA library record; WoS full record |
| |
Impact Factor |
3.7 |
Times cited |
|
Open Access |
OpenAccess |
| |
Notes |
|
Approved |
Most recent IF: 3.7 |
| |
Call Number |
UA @ admin @ c:irua:191469 |
Serial |
7268 |
| Permanent link to this record |
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|
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Author |
Gerrits, N. |
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Title |
Accurate simulations of the reaction of H₂ on a curved Pt crystal through machine learning |
Type |
A1 Journal article |
| |
Year |
2021 |
Publication |
Journal Of Physical Chemistry Letters |
Abbreviated Journal |
J Phys Chem Lett |
| |
Volume |
12 |
Issue |
51 |
Pages |
12157-12164 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
| |
Abstract |
Theoretical studies on molecule-metal surface reactions have so far been limited to small surface unit cells due to computational costs. Here, for the first time molecular dynamics simulations on very large surface unit cells at the level of density functional theory are performed, allowing a direct comparison to experiments performed on a curved crystal. Specifically, the reaction of D-2 on a curved Pt crystal is investigated with a neural network potential (NNP). The developed NNP is also accurate for surface unit cells considerably larger than those that have been included in the training data, allowing dynamical simulations on very large surface unit cells that otherwise would have been intractable. Important and complex aspects of the reaction mechanism are discovered such as diffusion and a shadow effect of the step. Furthermore, conclusions from simulations on smaller surface unit cells cannot always be transfered to larger surface unit cells, limiting the applicability of theoretical studies of smaller surface unit cells to heterogeneous catalysts with small defect densities. |
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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 |
000734045900001 |
Publication Date |
2021-12-17 |
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Series Editor |
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Series Title |
|
Abbreviated Series Title |
|
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Series Volume |
|
Series Issue |
|
Edition |
|
| |
ISSN |
1948-7185 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
| |
Impact Factor |
9.353 |
Times cited |
|
Open Access |
OpenAccess |
| |
Notes |
|
Approved |
Most recent IF: 9.353 |
| |
Call Number |
UA @ admin @ c:irua:184717 |
Serial |
7413 |
| Permanent link to this record |
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Author |
Van de Sompel, P.; Khalilov, U.; Neyts, E.C. |
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Title |
Contrasting H-etching to OH-etching in plasma-assisted nucleation of carbon nanotubes |
Type |
A1 Journal article |
| |
Year |
2021 |
Publication |
Journal Of Physical Chemistry C |
Abbreviated Journal |
J Phys Chem C |
| |
Volume |
125 |
Issue |
14 |
Pages |
7849-7855 |
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
| |
Abstract |
To gain full control over the growth of carbon nanotubes (CNTs) using plasma-enhanced chemical vapor deposition (PECVD), a thorough understanding of the underlying plasma-catalyst mechanisms is required. Oxygen-containing species are often used as or added to the growth precursor gas, but these species also yield various radicals and ions, which may simultaneously etch the CNT during the growth. At present, the effect of these reactive species on the growth onset has not yet been thoroughly investigated. We here report on the etching mechanism of incipient CNT structures from OH and O radicals as derived from combined (reactive) molecular dynamics (MD) and force-bias Monte Carlo (tfMC) simulations. Our results indicate that the oxygen-containing radicals initiate a dissociation process. In particular, we show how the oxygen species weaken the interaction between the CNT and the nanocluster. As a result of this weakened interaction, the CNT closes off and dissociates from the cluster in the form of a fullerene. Beyond the specific systems studied in this work, these results are generically important in the context of PECVD-based growth of CNTs using oxygen-containing precursors. |
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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 |
000641307100032 |
Publication Date |
2021-04-06 |
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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 |
|
Series Issue |
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Edition |
|
| |
ISSN |
1932-7447; 1932-7455 |
ISBN |
|
Additional Links |
UA library record; WoS full record |
| |
Impact Factor |
4.536 |
Times cited |
|
Open Access |
OpenAccess |
| |
Notes |
|
Approved |
Most recent IF: 4.536 |
| |
Call Number |
UA @ admin @ c:irua:178393 |
Serial |
7729 |
| Permanent link to this record |
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Author |
Nematollahi, P.; Ma, H.; Schneider, W.F.; Neyts, E.C. |
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Title |
DFT and microkinetic comparison of ru-doped porphyrin-like graphene and nanotubes toward catalytic formic acid decomposition and formation |
Type |
A1 Journal article |
| |
Year |
2021 |
Publication |
Journal Of Physical Chemistry C |
Abbreviated Journal |
J Phys Chem C |
| |
Volume |
125 |
Issue |
34 |
Pages |
18673-18683 |
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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 |
Immobilization of single metal atoms on a solid host opens numerous possibilities for catalyst designs. If that host is a two-dimensional sheet, sheet curvature becomes a design parameter potentially complementary to host and metal composition. Here, we use a combination of density functional theory calculations and microkinetic modeling to compare the mechanisms and kinetics of formic acid decomposition and formation, chosen for their relevance as a potential hydrogen storage medium, over single Ru atoms anchored to pyridinic nitrogen in a planar graphene flake (RuN4-G) and curved carbon nanotube (RuN4-CNT). Activation barriers are lowered and the predicted turnover frequencies are increased over RuN4-CNT relative to RuN4-CNT. The results highlight the potential of curvature control as a means to achieve high performance and robust catalysts. |
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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 |
000693413400013 |
Publication Date |
2021-08-22 |
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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; 1932-7455 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
| |
Impact Factor |
4.536 |
Times cited |
|
Open Access |
OpenAccess |
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Notes |
|
Approved |
Most recent IF: 4.536 |
| |
Call Number |
UA @ admin @ c:irua:181538 |
Serial |
7805 |
| Permanent link to this record |
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Author |
Verbruggen, S.W.; Ribbens, S.; Tytgat, T.; Hauchecorne, B.; Smits, M.; Meynen, V.; Cool, P.; Martens, J.A.; Lenaerts, S. |
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Title |
The benefit of glass bead supports for efficient gas phase photocatalysis : case study of a commercial and a synthesised photocatalyst |
Type |
A1 Journal article |
| |
Year |
2011 |
Publication |
Chemical engineering journal |
Abbreviated Journal |
Chem Eng J |
| |
Volume |
174 |
Issue |
1 |
Pages |
318-325 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Laboratory of adsorption and catalysis (LADCA); Sustainable Energy, Air and Water Technology (DuEL) |
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Abstract |
In the field of photocatalytic air purification, the immobilisation of catalyst particles on support surfaces without loss of photon efficiency is an important challenge. Therefore, an immobilisation method involving a one-step suspension coating of pre-synthesised photocatalysts on glass beads was applied. The various benefits are exemplified in the gas phase photodegradation of ethylene. Coating of glass beads is easy, fast, cheap and offers a more efficient alternative to bulk catalyst pellets. Furthermore, this coating procedure allows to use porous, pre-synthesised catalysts to their full potential, as the surface area and morphology of the initial powder is barely altered after coating, in strong contrast to pelletising. With this technique it became possible to study the gas phase photocatalytic activity of commercial titanium dioxide, trititanate nanotubes and mixed phase anatase/trititanate nanotubes in a packed bed reactor towards the degradation of ethylene without changing the catalyst properties. Coating of glass beads with the photocatalyst revealed the superior activity of the as-prepared nanotubes, compared to TiO2 Aerolyst® 7710 in gaseous phase. |
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Place of Publication |
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Wos |
000296950300041 |
Publication Date |
2011-09-17 |
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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 |
|
| |
ISSN |
1385-8947; 1873-3212 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
| |
Impact Factor |
6.216 |
Times cited |
39 |
Open Access |
|
| |
Notes |
; The author wishes to acknowledge the Research Foundation of Flanders (FWO) for the financial support. Evonik is greatly thanked for supplying the TiO<INF>2</ INF> Aerolyst (R) 7710 pellets. ; |
Approved |
Most recent IF: 6.216; 2011 IF: 3.461 |
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Call Number |
UA @ admin @ c:irua:93364 |
Serial |
5929 |
| Permanent link to this record |
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Author |
Uytdenhouwen, Y.; Hereijgers, J.; Breugelmans, T.; Cool, P.; Bogaerts, A. |
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Title |
How gas flow design can influence the performance of a DBD plasma reactor for dry reforming of methane |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chem Eng J |
| |
Volume |
405 |
Issue |
|
Pages |
126618 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
DBD plasma reactors are commonly used in a static ‘one inlet – one outlet’ design that goes against reactor design principles for multi-component reactions, such as dry reforming of methane (DRM). Therefore, in this paper we have developed a novel reactor design, and investigated how the shape and size of the reaction zone, as well as gradual gas addition, and the method of mixing CO2 and CH4 can influence the conversion and product com position of DRM. Even in the standard ‘one inlet – one outlet’ design, the direction of the gas flow (i.e. short or long path through the reactor, which defines the gas velocity at fixed residence time), as well as the dimensions of the reaction zone and the power delivery to the reactor, largely affect the performance. Using gradual gas addition and separate plasma activation zones for the individual gases give increased conversions within the same operational parameters, by optimising mixing ratios and kinetics. The choice of the main (pre-activated) gas and the direction of gas flow largely affect the conversion and energy cost, while the gas inlet position during separate addition only influences the product distribution. |
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Place of Publication |
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Language |
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Wos |
000626511800005 |
Publication Date |
2020-08-12 |
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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 |
|
| |
ISSN |
1385-8947 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
| |
Impact Factor |
6.216 |
Times cited |
|
Open Access |
OpenAccess |
| |
Notes |
Interreg; Flanders; FWO; University of Antwerp; The authors acknowledge financial support from the European Fund for Regional Development through the cross-border collaborative Interreg V program Flanders-the Netherlands (project EnOp), the Fund 13 for Scientific Research (FWO; grant number: G.0254.14N), and an IOFSBO (SynCO2Chem) project from the University of Antwerp. |
Approved |
Most recent IF: 6.216 |
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Call Number |
PLASMANT @ plasmant @c:irua:170609 |
Serial |
6410 |
| Permanent link to this record |
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Author |
Kovács, A.; Billen, P.; Cornet, I.; Wijnants, M.; Neyts, E.C. |
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Title |
Modeling the physicochemical properties of natural deep eutectic solvents : a review |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Chemsuschem |
Abbreviated Journal |
Chemsuschem |
| |
Volume |
13 |
Issue |
15 |
Pages |
3789-3804 |
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Intelligence in PRocesses, Advanced Catalysts and Solvents (iPRACS); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Biochemical Wastewater Valorization & Engineering (BioWaVE) |
| |
Abstract |
Natural deep eutectic solvents (NADES) are mixtures of naturally derived compounds with a significantly decreased melting point due to the specific interactions among the constituents. NADES have benign properties (low volatility, flammability, toxicity, cost) and tailorable physicochemical properties (by altering the type and molar ratio of constituents), hence they are often considered as a green alternative to common organic solvents. Modeling the relation between their composition and properties is crucial though, both for understanding and predicting their behavior. Several efforts were done to this end, yet this review aims at structuring the present knowledge as an outline for future research. First, we reviewed the key properties of NADES and relate them to their structure based on the available experimental data. Second, we reviewed available modeling methods applicable to NADES. At the molecular level, density functional theory and molecular dynamics allow interpreting density differences and vibrational spectra, and computation of interaction energies. Additionally, properties at the level of the bulk media can be explained and predicted by semi-empirical methods based on ab initio methods (COSMO-RS) and equation of state models (PC-SAFT). Finally, methods based on large datasets are discussed; models based on group contribution methods and machine learning. A combination of bulk media and dataset modeling allows qualitative prediction and interpretation of phase equilibria properties on the one hand, and quantitative prediction of melting point, density, viscosity, surface tension and refractive indices on the other hand. In our view, multiscale modeling, combining the molecular and macroscale methods, will strongly enhance the predictability of NADES properties and their interaction with solutes, yielding truly tailorable solvents to accommodate (bio)chemical reactions. |
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Wos |
000541499100001 |
Publication Date |
2020-05-07 |
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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 |
1864-5631 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
8.4 |
Times cited |
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Open Access |
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Notes |
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Approved |
Most recent IF: 8.4; 2020 IF: 7.226 |
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Call Number |
UA @ admin @ c:irua:168851 |
Serial |
6770 |
| Permanent link to this record |
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Author |
Brienza, F.; Van Aelst, K.; Devred, F.; Magnin, D.; Tschulkow, M.; Nimmegeers, P.; Van Passel, S.; Sels, B.F.; Gerin, P.; Debecker, D.P.; Cybulska, I. |
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Title |
Unleashing lignin potential through the dithionite-assisted organosolv fractionation of lignocellulosic biomass |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chem Eng J |
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Volume |
450 |
Issue |
3 |
Pages |
138179-14 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Engineering Management (ENM); Intelligence in PRocesses, Advanced Catalysts and Solvents (iPRACS) |
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Abstract |
The development of biomass pretreatment approaches that, next to (hemi)cellulose valorization, aim at the conversion of lignin to chemicals is essential for the long-term success of a biorefinery. Herein, we discuss a dithionite-assisted organosolv fractionation (DAOF) of lignocellulose in n-butanol and water to produce cellulosic pulp and mono-/oligo-aromatics. The study frames the technicalities of this biorefinery process and relates them to the features of the obtained product streams. We comprehensively identify and quantify all products of interest: solid pulp (acid hydrolysis-HPLC, ATR-FTIR, XRD, SEM, enzymatic hydrolysis-HPLC), lignin derivatives (GPC, GC-MS/FID, 1H-13C HSQC NMR, ICP-AES), and carbohydrate derivatives (HPLC). These results were used for inspecting the economic feasibility of DAOF. In the best process configuration, a high yield of monophenolics was reached (~20%, based on acid insoluble lignin in birch sawdust). Various other lignocellulosic feedstocks were also explored, showing that DAOF is particularly effective on hardwood and herbaceous biomass. Overall, this study demonstrates that DAOF is a viable fractionation method for the sustainable upgrading of lignocellulosic biomass. |
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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 |
000888204900005 |
Publication Date |
2022-07-20 |
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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 |
1385-8947; 1873-3212 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 15.1 |
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Call Number |
UA @ admin @ c:irua:189322 |
Serial |
7373 |
| Permanent link to this record |
