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Records |
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Author |
Bercx, M.; Mayda, S.; Depla, D.; Partoens, B.; Lamoen, D. |
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Title |
Plasmonic effects in the neutralization of slow ions at a metallic surface |
Type |
A1 Journal Article |
| |
Year |
2023 |
Publication |
Contributions to Plasma Physics |
Abbreviated Journal |
Contrib. Plasma Phys |
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Volume |
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Issue |
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Pages |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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Abstract |
Secondary electron emission is an important process that plays a significant role in several plasma‐related applications. As measuring the secondary electron yield experimentally is very challenging, quantitative modelling of this process to obtain reliable yield data is critical as input for higher‐scale simulations. Here, we build upon our previous work combining density functional theory calculations with a model originally developed by Hagstrum to extend its application to metallic surfaces. As plasmonic effects play a much more important role in the secondary electron emission mechanism for metals, we introduce an approach based on Poisson point processes to include both surface and bulk plasmon excitations to the process. The resulting model is able to reproduce the yield spectra of several available experimental results quite well but requires the introduction of global fitting parameters, which describe the strength of the plasmon interactions. Finally, we use an in‐house developed workflow to calculate the electron yield for a list of elemental surfaces spanning the periodic table to produce an extensive data set for the community and compare our results with more simplified approaches from the literature. |
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Wos |
001067651300001 |
Publication Date |
2023-09-16 |
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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 |
0863-1042 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
1.6 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
We acknowledge the financial support of FWO-Vlaanderen through project G.0216.14N. The computational resources and services used in this work were provided by the VSC (Flemish Supercomputer Center) and the HPC infrastructure of the University of Antwerp (CalcUA), both funded by the FWO-Vlaanderen and the Flemish Government-department EWI. |
Approved |
Most recent IF: 1.6; 2023 IF: 1.44 |
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Call Number |
EMAT @ emat @c:irua:200330 |
Serial |
8962 |
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Author |
Van Gordon, K.; Baúlde, S.; Mychinko, M.; Heyvaert, W.; Obelleiro-Liz, M.; Criado, A.; Bals, S.; Liz-Marzán, L.M.; Mosquera, J. |
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Title |
Tuning the Growth of Chiral Gold Nanoparticles Through Rational Design of a Chiral Molecular Inducer |
Type |
A1 Journal Article |
| |
Year |
2023 |
Publication |
Nano Letters |
Abbreviated Journal |
Nano Lett. |
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Volume |
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Issue |
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Pages |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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Abstract |
The bottom-up production of chiral gold nanomaterials holds great potential for the advancement of biosensing and nano-optics, among other applications. Reproducible preparations of colloidal nanomaterials with chiral morphology have been reported, using cosurfactants or chiral inducers such as thiolated amino acids. However, the underlying growth mechanisms for these nanomaterials remain insufficiently understood. We introduce herein a purposely devised chiral inducer, a cysteine modified with a hydrophobic chain, as a versatile chiral inducer. The amphiphilic and chiral features of this molecule provide control over the chiral morphology and the chiroptical signature of the obtained nanoparticles by simply varying the concentration of chiral inducer. These results are supported by circular dichroism and electromagnetic modeling as well as electron tomography to analyze structural evolution at the facet scale. Our observations suggest complex roles for the factors involved in chiral synthesis: the chemical nature of the chiral inducers and the influence of cosurfactants. |
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Wos |
001092787000001 |
Publication Date |
2023-10-25 |
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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 |
1530-6984 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
10.8 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
J.M. Taboada and F. Obelleiro are thanked for support with electromagnetic simulations. The authors acknowledge financial support by the European Research Council (ERC CoG No. 815128 REALNANO to S. Bals; ERC AdG No. 787510, 4DbioSERS to L.M.L.-M.) and from MCIN/AEI/10.13039/501100011033 and “ESF Investing in your future” (Grant PID2020-117779RB-I00 to L.M.L.-M., Grant RYC2020-030183-I to A.C., and Grants RYC2019-027842-I, PID2020-117885GA-I00 to J.M.). |
Approved |
Most recent IF: 10.8; 2023 IF: 12.712 |
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Call Number |
EMAT @ emat @c:irua:200590 |
Serial |
8963 |
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| Permanent link to this record |
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Author |
Li, S.; Sun, J.; Gorbanev, Y.; van’t Veer, K.; Loenders, B.; Yi, Y.; Kenis, T.; Chen, Q.; Bogaerts, A. |
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Title |
Plasma-Assisted Dry Reforming of CH4: How Small Amounts of O2Addition Can Drastically Enhance the Oxygenate Production─Experiments and Insights from Plasma Chemical Kinetics Modeling |
Type |
A1 Journal Article |
| |
Year |
2023 |
Publication |
ACS Sustainable Chemistry & Engineering |
Abbreviated Journal |
ACS Sustainable Chem. Eng. |
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| |
Volume |
11 |
Issue |
42 |
Pages |
15373-15384 |
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| |
Keywords |
A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
Plasma-based dry reforming of methane (DRM) into
high-value-added oxygenates is an appealing approach to enable
otherwise thermodynamically unfavorable chemical reactions at
ambient pressure and near room temperature. However, it suffers
from coke deposition due to the deep decomposition of CH4. In this
work, we assess the DRM performance upon O2 addition, as well as
varying temperature, CO2/CH4 ratio, discharge power, and gas
residence time, for optimizing oxygenate production. By adding O2,
the main products can be shifted from syngas (CO + H2) toward
oxygenates. Chemical kinetics modeling shows that the improved
oxygenate production is due to the increased concentration of
oxygen-containing radicals, e.g., O, OH, and HO2, formed by electron
impact dissociation [e + O2 → e + O + O/O(1D)] and subsequent
reactions with H atoms. Our study reveals the crucial role of oxygen-coupling in DRM aimed at oxygenates, providing practical
solutions to suppress carbon deposition and at the same time enhance the oxygenates production in plasma-assisted DRM. |
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Place of Publication |
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Wos |
001082603900001 |
Publication Date |
2023-10-23 |
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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 |
2168-0485 |
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 |
Not_Open_Access |
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Notes |
Fonds Wetenschappelijk Onderzoek, S001619N ; China Scholarship Council, 202006060029 ; National Natural Science Foundation of China, 21975018 ; H2020 European Research Council, 810182 ; |
Approved |
Most recent IF: 8.4; 2023 IF: 5.951 |
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Call Number |
PLASMANT @ plasmant @c:irua:201013 |
Serial |
8966 |
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| Permanent link to this record |
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Author |
de la Croix, T.; Claes, N.; Eyley, S.; Thielemans, W.; Bals, S.; De Vos, D. |
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Title |
Heterogeneous Pt-catalyzed transfer dehydrogenation of long-chain alkanes with ethylene |
Type |
A1 Journal Article |
| |
Year |
2023 |
Publication |
Catalysis Science & Technology |
Abbreviated Journal |
Catal. Sci. Technol. |
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Volume |
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Issue |
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Pages |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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Abstract |
The dehydrogenation of long-chain alkanes to olefins and alkylaromatics is a challenging endothermic reaction, typically requiring harsh conditions which can lead to low selectivity and coking. More favorable thermodynamics can be achieved by using a hydrogen acceptor, such as ethylene. In this work, the potential of heterogeneous platinum catalysts for the transfer dehydrogenation of long-chain alkanes is investigated, using ethylene as a convenient hydrogen acceptor. Pt/C and Pt–Sn/C catalysts were prepared<italic>via</italic>a simple polyol method and characterized with CO pulse chemisorption, HAADF-STEM, and EDX measurements. Conversion of ethylene was monitored<italic>via</italic>gas-phase FTIR, and distribution of liquid products was analyzed<italic>via</italic>GC-FID, GC-MS, and 1H-NMR. Compared to unpromoted Pt/C, Sn-promoted catalysts show lower initial reaction rates, but better resistance to catalyst deactivation, while increasing selectivity towards alkylaromatics. Both reaction products and ethylene were found to inhibit the reaction significantly. At 250 °C for 22 h, TON up to 28 and 86 mol per mol Pt were obtained for Pt/C and PtSn<sub>2</sub>/C, respectively, with olefin selectivities of 94% and 53%. The remaining products were mainly unbranched alkylaromatics. These findings show the potential of simple heterogeneous catalysts in alkane transfer dehydrogenation, for the preparation of valuable olefins and alkylaromatics, or as an essential step in various tandem reactions. |
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Wos |
001104905100001 |
Publication Date |
2023-11-09 |
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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 |
2044-4753 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
5 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
T. de la Croix gratefully acknowledges the support of the Flanders Research Foundation (FWO) under project 11F6622N. D. De Vos is grateful to FWO for support of project G0D3721N, and to KU Leuven for the iBOF project 21/016/C3. S. Bals and N. Claes acknowledge funding from the European Research Council under the European Union’s Horizon 2020 research and innovation program (ERC Consolidator Grant No. 815128- REALNANO). W. Thielemans and S. Eyley thank KU Leuven (grant C14/18/061) and FWO (G0A1219N) for financial support. |
Approved |
Most recent IF: 5; 2023 IF: 5.773 |
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Call Number |
EMAT @ emat @c:irua:201010 |
Serial |
8968 |
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| Permanent link to this record |
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Author |
Claes, J.; Partoens, B.; Lamoen, D. |
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Title |
Decoupled DFT-1/2 method for defect excitation energies |
Type |
A1 Journal Article |
| |
Year |
2023 |
Publication |
Physical Review B |
Abbreviated Journal |
Phys. Rev. B |
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| |
Volume |
108 |
Issue |
12 |
Pages |
125306 |
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Keywords |
A1 Journal Article; Condensed Matter Theory (CMT) ; |
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Abstract |
The DFT-1/2 method is a band-gap correction with GW precision at a density functional theory (DFT) computational cost. The method was also extended to correct the gap between defect levels, allowing for the calculation of optical transitions. However, this method fails when the atomic character of the occupied and unoccupied defect levels is similar as we illustrate by two examples, the tetrahedral hydrogen interstitial and the negatively charged vacancy in diamond. We solve this problem by decoupling the effect of the occupied and unoccupied defect levels and call this the decoupled DFT-1/2 method for defects. |
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Wos |
001089302800003 |
Publication Date |
2023-09-25 |
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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 |
2469-9950 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
3.7 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
This work was supported by the FWO (Research Foundation-Flanders), Project No. G0D1721N. This work was performed in part using HPC resources from the VSC (Flemish Supercomputer Center) and the HPC infrastructure of the University of Antwerp (CalcUA), both funded by the FWO-Vlaanderen and the Flemish Government department EWI (Economie, Wetenschap & Innovatie). |
Approved |
Most recent IF: 3.7; 2023 IF: 3.836 |
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Call Number |
CMT @ cmt @c:irua:201287 |
Serial |
8976 |
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| Permanent link to this record |
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Author |
Bogaerts, A. |
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Title |
Special Issue on “Dielectric Barrier Discharges and their Applications” in Commemoration of the 20th Anniversary of Dr. Ulrich Kogelschatz’s Work |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
Plasma Chemistry and Plasma Processing |
Abbreviated Journal |
Plasma Chem Plasma Process |
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Volume |
43 |
Issue |
6 |
Pages |
1281-1285 |
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Keywords |
A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
n/a |
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Address |
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Corporate Author |
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Place of Publication |
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Wos |
001110371000001 |
Publication Date |
2023-11-30 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0272-4324 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
3.6 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
n/a |
Approved |
Most recent IF: 3.6; 2023 IF: 2.355 |
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Call Number |
PLASMANT @ plasmant @c:irua:201387 |
Serial |
8969 |
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Author |
Lin, A.; Gromov, M.; Nikiforov, A.; Smits, E.; Bogaerts, A. |
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Title |
Characterization of Non-Thermal Dielectric Barrier Discharges for Plasma Medicine: From Plastic Well Plates to Skin Surfaces |
Type |
A1 Journal Article |
| |
Year |
2023 |
Publication |
Plasma Chemistry and Plasma Processing |
Abbreviated Journal |
Plasma Chem Plasma Process |
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Volume |
43 |
Issue |
6 |
Pages |
1587-1612 |
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Keywords |
A1 Journal Article; Non-thermal plasma · Plasma medicine · Dielectric barrier discharge · Plasma diagnostics · Plasma surface interaction · In situ plasma monitoring; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
technologies have been expanding, and one of the most exciting and rapidly growing
applications is in biology and medicine. Most biomedical studies with DBD plasma systems are performed in vitro, which include cells grown on the surface of plastic well plates, or in vivo, which include animal research models (e.g. mice, pigs). Since many DBD systems use the biological target as the secondary electrode for direct plasma generation and treatment, they are sensitive to the surface properties of the target, and thus can be altered based on the in vitro or in vivo system used. This could consequently affect biological response from plasma treatment. Therefore, in this study, we investigated the DBD plasma behavior both in vitro (i.e. 96-well flat bottom plates, 96-well U-bottom plates, and 24-well flat bottom plates), and in vivo (i.e. mouse skin). Intensified charge coupled device (ICCD) imaging was performed and the plasma discharges were visually distinguishable between the different systems. The geometry of the wells did not affect DBD plasma generation for low application distances (≤ 2 mm), but differentially affected plasma uniformity on the bottom of the well at greater distances. Since DBD plasma treatment in vitro is rarely performed in dry wells for plasma medicine experiments, the effect of well wetness was also investigated. In all in vitro cases, the uniformity of the DBD plasma was affected when comparing wet versus dry wells, with the plasma in the wide-bottom wells appearing the most similar to plasma generated on mouse skin. Interestingly, based on quantification of ICCD images, the DBD plasma intensity per surface area demonstrated an exponential one-phase decay with increasing application distance, regardless of the in vitro or in vivo system. This trend is similar to that of the energy per pulse of plasma, which is used to determine the total plasma treatment energy for biological systems. Optical emission spectroscopy performed on the plasma revealed similar trends in radical species generation between the plastic well plates and mouse skin. Therefore, taken together, DBD plasma intensity per surface area may be a valuable parameter to be used as a simple method for in situ monitoring during biological treatment and active plasma treatment control, which can be applied for in vitro and in vivo systems. |
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Wos |
001072607700001 |
Publication Date |
2023-09-27 |
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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 |
0272-4324 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.6 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
This work was partially funded by the Research Foundation—Flanders (FWO) and supported by the following Grants: 12S9221N (A. L.), G044420N (A. L. and A. B.), and G033020N (A.B.). We would also like to thank several patrons, as part of this research was funded by donations from different donors, including Dedert Schilde vzw, Mr Willy Floren, and the Vereycken family. We would also like to acknowledge the support from the European Cooperation in Science & Technology (COST) Action on “Therapeutical applications of Cold Plasmas” (CA20114; PlasTHER). |
Approved |
Most recent IF: 3.6; 2023 IF: 2.355 |
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Call Number |
PLASMANT @ plasmant @c:irua:200285 |
Serial |
8970 |
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Author |
Bhatia, H.; Keshavarz, M.; Martin, C.; Van Gaal, L.; Zhang, Y.; de Coen, B.; Schrenker, N.J.; Valli, D.; Ottesen, M.; Bremholm, M.; Van de Vondel, J.; Bals, S.; Hofkens, J.; Debroye, E. |
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Title |
Achieving High Moisture Tolerance in Pseudohalide Perovskite Nanocrystals for Light-Emitting Diode Application |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
ACS Applied Optical Materials |
Abbreviated Journal |
ACS Appl. Opt. Mater. |
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Volume |
1 |
Issue |
6 |
Pages |
1184-1191 |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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Abstract |
The addition of potassium thiocyanate (KSCN) to the FAPbBr3 structure and subsequent post-treatment of nanocrystals (NCs) lead to high quantum confinement, resulting in a photoluminescent quantum yield (PLQY) approaching unity and microsecond decay times. This synergistic approach demonstrated exceptional stability under humid conditions, retaining 70% of the PLQY for over a month, while the untreated NCs degrade within 24 h. Additionally, the devices incorporating the post-treated NCs displayed 1.5% external quantum efficiency (EQE), a 5-fold improvement over untreated devices. These results provide promising opportunities for the use of perovskites in moisture-stable optoelectronics. |
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Wos |
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Publication Date |
2023-06-23 |
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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 |
2771-9855 |
ISBN |
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Additional Links |
UA library record |
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Impact Factor |
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Times cited |
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Open Access |
OpenAccess |
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Notes |
Hercules Foundation, HER/11/14 ; European Commission; Ministerio de Ciencia e Innovaci?n, PID2021-128761OA-C22 ; European Regional Development Fund; Vlaamse regering, CASAS2 Meth/15/04 ; Fonds Wetenschappelijk Onderzoek, 1238622N 1514220N 1S45223N G.0B39.15 G.0B49.15 G098319N S002019N ZW15_09-GOH6316 ; Onderzoeksraad, KU Leuven, C14/19/079 db/21/006/bm iBOF-21-085 STG/21/010 ; Junta de Comunidades de Castilla-La Mancha, SBPLY/21/180501/000127 ; H2020 European Research Council, 642196 815128 ; |
Approved |
Most recent IF: NA |
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Call Number |
EMAT @ emat @c:irua:201011 |
Serial |
8975 |
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Author |
Delfino, C.L.; Hao, Y.; Martin, C.; Minoia, A.; Gopi, E.; Mali, K.S.; Van der Auweraer, M.; Geerts, Y.H.; Van Aert, S.; Lazzaroni, R.; De Feyter, S. |
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Title |
Conformation-Dependent Monolayer and Bilayer Structures of an Alkylated TTF Derivative Revealed using STM and Molecular Modeling |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
The Journal of Physical Chemistry C |
Abbreviated Journal |
J. Phys. Chem. C |
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Volume |
127 |
Issue |
47 |
Pages |
23023-23033 |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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Abstract |
In this study, the multi-layer self-assembled molecular network formation of an alkylated tetrathiafulvalene compound is studied at the liquid-solid interface between 1-phenyloctane and graphite. A combined theoretical/experimental approach associating force-field and quantum-chemical calculations with scanning tunnelling microscopy is used to determine the two-dimensional self-assembly beyond the monolayer, but also to further the understanding of the molecular adsorption conformation and its impact on the molecular packing within the assemblies at the monolayer and bilayer level. |
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Corporate Author |
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Place of Publication |
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Wos |
001111637100001 |
Publication Date |
2023-11-30 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
3.7 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
Financial support from the Research Foundation-Flanders (FWO G081518N, G0A3220N) and KU Leuven–Internal Funds (C14/19/079) is acknowledged. This work was in part supported by FWO and F. R. S.-FNRS under the Excellence of Science EOS program (project 30489208 and 40007495). C.M. acknowledges the financial support: Grants PID2021-128761OA-C22 and CNS2022-136052 funded by MCIN/AEI/10.13039/501100011033 by the “European Union” and SBPLY/21/180501/000127 funded by JCCM and by the EU through “Fondo Europeo de Desarollo Regional” (FEDER). Research in Mons is also supported by the Belgian National Fund for Scientific Research (FRS-FNRS) within the Consortium des Équipements de Calcul Intensif – CÉCI, under Grant 2.5020.11, and by the Walloon Region (ZENOBE Tier-1 supercomputer, under grant 1117545). |
Approved |
Most recent IF: 3.7; 2023 IF: 4.536 |
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Call Number |
EMAT @ emat @c:irua:201671 |
Serial |
8974 |
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Author |
Gerrits, N.; Jackson, B.; Bogaerts, A. |
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Title |
Accurate Reaction Probabilities for Translational Energies on Both Sides of the Barrier of Dissociative Chemisorption on Metal Surfaces |
Type |
A1 Journal Article |
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Year |
2024 |
Publication |
The Journal of Physical Chemistry Letters |
Abbreviated Journal |
J. Phys. Chem. Lett. |
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Volume |
15 |
Issue |
9 |
Pages |
2566-2572 |
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Keywords |
A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
Molecular dynamics simulations are essential for a better understanding of dissociative chemisorption on metal surfaces, which is often the rate-controlling step in heterogeneous and plasma catalysis. The workhorse quasi-classical trajectory approach ubiquitous in molecular dynamics is able to accurately predict reactivity only for high translational and low vibrational energies. In contrast, catalytically relevant conditions generally involve low translational and elevated vibrational energies. Existing quantum dynamics approaches are intractable or approximate as a result of the large number of degrees of freedom present in molecule−metal surface reactions. Here, we extend a ring polymer molecular dynamics approach to fully include, for the first time, the degrees of freedom of a moving metal surface. With this approach, experimental sticking probabilities for the dissociative chemisorption of methane on Pt(111) are reproduced for a large range of translational and vibrational energies by including nuclear quantum effects and employing full-dimensional simulations. |
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Wos |
001177959900001 |
Publication Date |
2024-03-07 |
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ISSN |
1948-7185 |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
5.7 |
Times cited |
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Open Access |
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Notes |
Nick Gerrits has been financially supported through a Dutch Research Council (NWO) Rubicon grant (019.202EN.012). The computational resources and services used in this work were provided by the high performance computing (HPC) core facility CalcUA of the Universiteit Antwerpen and the Flemish Supercomputer Center (VSC) funded by the Research Foundation−Flanders (FWO) and the Flemish Government. The authors thank Mark Somers for useful discussions. |
Approved |
Most recent IF: 5.7; 2024 IF: 9.353 |
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Call Number |
PLASMANT @ plasmant @c:irua:204818 |
Serial |
9114 |
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Author |
Faraji, F.; Neyts, E.C.; Milošević, M.V.; Peeters, F.M. |
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Title |
Comment on “Misinterpretation of the Shuttleworth equation” |
Type |
A1 Journal Article |
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Year |
2024 |
Publication |
Scripta Materialia |
Abbreviated Journal |
Scripta Materialia |
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Volume |
250 |
Issue |
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Pages |
116186 |
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Keywords |
A1 Journal Article; CMT |
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Wos |
001252293900001 |
Publication Date |
2024-05-24 |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1359-6462 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
6 |
Times cited |
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Open Access |
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Notes |
Research Foundation Flanders; |
Approved |
Most recent IF: 6; 2024 IF: 3.747 |
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Call Number |
UA @ lucian @ CMTc:irua:206327 |
Serial |
9116 |
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Author |
Gorbanev, Y.; Fedirchyk, I.; Bogaerts, A. |
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Title |
Plasma catalysis in ammonia production and decomposition: Use it, or lose it? |
Type |
A1 Journal Article |
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Year |
2024 |
Publication |
Current Opinion in Green and Sustainable Chemistry |
Abbreviated Journal |
Current Opinion in Green and Sustainable Chemistry |
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Volume |
47 |
Issue |
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Pages |
100916 |
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Keywords |
A1 Journal Article; Plasma Nitrogen fixation Ammonia Plasma catalysis Production and decomposition; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
The combination of plasma with catalysis for the synthesis and decomposition of NH3 is an attractive route to the production of carbon-neutral fertiliser and energy carriers and its conversion into H2. Recent years have seen fast developments in the field of plasma-catalytic NH3 life cycle. This work summarises the most recent advances in plasma-catalytic and related NH3-focussed processes, identifies some of the most important discoveries, and addresses plausible strategies for future developments in plasma-based NH3 technology. |
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Wos |
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Publication Date |
2024-03-29 |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2452-2236 |
ISBN |
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Additional Links |
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Impact Factor |
9.3 |
Times cited |
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Open Access |
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Notes |
The work was supported by the Fund for Scientific Research (FWO) Flanders Bioeconomy project (grant G0G2322N) funded by the European Union-NextGe- nerationEU, the HyPACT project funded by the Belgian Energy Transition Fund, and the MSCA4Ukraine project 1233629 funded by the European Union. |
Approved |
Most recent IF: 9.3; 2024 IF: NA |
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Call Number |
PLASMANT @ plasmant @ |
Serial |
9117 |
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Author |
Vlasov, E.; Heyvaert, W.; Ni, B.; Van Gordon, K.; Girod, R.; Verbeeck, J.; Liz-Marzán, L.M.; Bals, S. |
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Title |
High-Throughput Morphological Chirality Quantification of Twisted and Wrinkled Gold Nanorods |
Type |
A1 Journal Article |
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Year |
2024 |
Publication |
ACS Nano |
Abbreviated Journal |
ACS Nano |
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Volume |
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Issue |
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Pages |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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Abstract |
Chirality in gold nanostructures offers an exciting opportunity to tune their differential optical response to left- and right-handed circularly polarized light, as well as their interactions with biomolecules and living matter. However, tuning and understanding such interactions demands quantification of the structural features that are responsible for the chiral behavior. Electron tomography (ET) enables structural characterization at the single-particle level and has been used to quantify the helicity of complex chiral nanorods. However, the technique is time-consuming and consequently lacks statistical value. To address this issue, we introduce herein a high-throughput methodology that combines images acquired by secondary electron-based electron beam-induced current (SEEBIC) with quantitative image analysis. As a result, the geometric chirality of hundreds of nanoparticles can be quantified in less than 1 h. When combining the drastic gain in data collection efficiency of SEEBIC with a limited number of ET data sets, a better understanding of how the chiral structure of individual chiral nanoparticles translates into the ensemble chiroptical response can be reached. |
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Wos |
001227683500001 |
Publication Date |
2024-04-26 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
17.1 |
Times cited |
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Open Access |
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Notes |
The authors acknowledge financial support by the European Research Council (ERC CoG No. 815128 REALNANO to S.B.) and from MCIN/AEI/10.13039/501100011033 (Grant PID2020-117779RB-I00 to L.M.L.-M and FPI Fellowship PRE2021-097588 to K.V.G.). Funded by the European Union under Project 101131111 − DELIGHT, JV acknowledges the eBEAM project supported by the European Union’s Horizon 2020 research and innovation program FETPROACT-EIC-07- 2020: emerging paradigms and communities. |
Approved |
Most recent IF: 17.1; 2024 IF: 13.942 |
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Call Number |
EMAT @ emat @c:irua:206329 |
Serial |
9121 |
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Author |
Zhou, R.; Neek-Amal, M.; Peeters, F.M.; Bai, B.; Sun, C. |
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Title |
Interlink between Abnormal Water Imbibition in Hydrophilic and Rapid Flow in Hydrophobic Nanochannels |
Type |
A1 Journal Article |
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Year |
2024 |
Publication |
Physical Review Letters |
Abbreviated Journal |
Phys. Rev. Lett. |
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Volume |
132 |
Issue |
18 |
Pages |
184001 |
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Keywords |
A1 Journal Article; CMT |
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Abstract |
Nanoscale extension and refinement of the Lucas-Washburn model is presented with a detailed analysis of recent experimental data and extensive molecular dynamics simulations to investigate rapid water flow and water imbibition within nanocapillaries. Through a comparative analysis of capillary rise in hydrophilic nanochannels, an unexpected reversal of the anticipated trend, with an abnormal peak, of imbibition length below the size of 3 nm was discovered in hydrophilic nanochannels, surprisingly sharing the same physical origin as the well-known peak observed in flow rate within hydrophobic nanochannels. The extended imbibition model is applicable across diverse spatiotemporal scales and validated against simulation results and existing experimental data for both hydrophilic and hydrophobic |
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Wos |
001224703200013 |
Publication Date |
2024-04-30 |
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Series Issue |
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ISSN |
0031-9007 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
8.6 |
Times cited |
1 |
Open Access |
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Notes |
We gratefully acknowledge the financial support pro- vided by the National Natural Science Foundation of China (Projects No. 52488201 and No. 52222606). Part of this project was supported by the Flemish Science Foundations (FWO-Vl) and the Iranian National Science Foundation (No. 4025061 and No. 4021261). |
Approved |
Most recent IF: 8.6; 2024 IF: 8.462 |
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Call Number |
UA @ lucian @c:irua:206319 |
Serial |
9122 |
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Author |
Faraji, F.; Neyts, E.C.; Milošević, M.V.; Peeters, F.M. |
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Title |
Capillary Condensation of Water in Graphene Nanocapillaries |
Type |
A1 Journal Article |
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Year |
2024 |
Publication |
Nano Letters |
Abbreviated Journal |
Nano Lett. |
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Volume |
24 |
Issue |
18 |
Pages |
5625-5630 |
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Keywords |
A1 Journal Article; CMT |
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Abstract |
Recent experiments have revealed that the macroscopic Kelvin equation remains surprisingly accurate even for nanoscale capillaries. This phenomenon was so far explained by the oscillatory behavior of the solid−liquid interfacial free energy. We here demonstrate thermodynamic and capillarity inconsistencies with this explanation. After revising the Kelvin equation, we ascribe its validity at nanoscale confinement to the effect of disjoining pressure.
To substantiate our hypothesis, we employed molecular dynamics simulations to evaluate interfacial heat transfer and wetting properties. Our assessments unveil a breakdown in a previously established proportionality between the work of adhesion and the Kapitza conductance at capillary heights below 1.3 nm, where the dominance of the work of adhesion shifts primarily from energy to entropy. Alternatively, the peak density of the initial water layer can effectively probe the work of adhesion. Unlike under bulk conditions, high confinement renders the work of adhesion entropically unfavorable. |
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Wos |
001227815000001 |
Publication Date |
2024-05-08 |
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Series Issue |
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Edition |
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ISSN |
1530-6984 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
10.8 |
Times cited |
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Open Access |
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Notes |
This work was supported by Research Foundation-Flanders (FWO, project No. G099219N). The computational resources used in this work were provided by the HPC core facility CalcUA of the University of Antwerp, and the Flemish Supercomputer Center (VSC), funded by FWO and the Flemish Government. |
Approved |
Most recent IF: 10.8; 2024 IF: 12.712 |
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Call Number |
UA @ lucian @c:irua:206331 |
Serial |
9123 |
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Author |
Cai, Y.; Mei, D.; Chen, Y.; Bogaerts, A.; Tu, X. |
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Title |
Machine learning-driven optimization of plasma-catalytic dry reforming of methane |
Type |
A1 Journal Article |
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Year |
2024 |
Publication |
Journal of Energy Chemistry |
Abbreviated Journal |
Journal of Energy Chemistry |
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Volume |
96 |
Issue |
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Pages |
153-163 |
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Keywords |
A1 Journal Article; Plasma catalysis Machine learning Process optimization Dry reforming of methane Syngas production; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
This study investigates the dry reformation of methane (DRM) over Ni/Al2O3 catalysts in a dielectric barrier discharge (DBD) non-thermal plasma reactor. A novel hybrid machine learning (ML) model is developed to optimize the plasma-catalytic DRM reaction with limited experimental data. To address the non-linear and complex nature of the plasma-catalytic DRM process, the hybrid ML model integrates three well-established algorithms: regression trees, support vector regression, and artificial neural networks. A genetic algorithm (GA) is then used to optimize the hyperparameters of each algorithm within the hybrid ML model. The ML model achieved excellent agreement with the experimental data, demonstrating its efficacy in accurately predicting and optimizing the DRM process. The model was subsequently used to investigate the impact of various operating parameters on the plasma-catalytic DRM performance. We found that the optimal discharge power (20 W), CO2/CH4 molar ratio (1.5), and Ni loading (7.8 wt%) resulted in the maximum energy yield at a total flow rate of 51 mL/min. Furthermore, we investigated the relative significance of each operating parameter on the performance of the plasmacatalytic DRM process. The results show that the total flow rate had the greatest influence on the conversion, with a significance exceeding 35% for each output, while the Ni loading had the least impact on the overall reaction performance. This hybrid model demonstrates a remarkable ability to extract valuable insights from limited datasets, enabling the development and optimization of more efficient and selective plasma-catalytic chemical processes. |
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Wos |
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Publication Date |
2024-04-25 |
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Edition |
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ISSN |
2095-4956 |
ISBN |
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Impact Factor |
13.1 |
Times cited |
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Open Access |
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Notes |
This project received funding from the European Union’s Hori- zon 2020 research and innovation program under the Marie Sklodowska-Curie grant agreement No. 813393. |
Approved |
Most recent IF: 13.1; 2024 IF: 2.594 |
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Call Number |
PLASMANT @ plasmant @ |
Serial |
9124 |
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Author |
Albrechts, M.; Tsonev, I.; Bogaerts, A. |
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Title |
Investigation of O atom kinetics in O2plasma and its afterglow |
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A1 Journal Article |
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Year |
2024 |
Publication |
Plasma Sources Science and Technology |
Abbreviated Journal |
Plasma Sources Sci. Technol. |
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Volume |
33 |
Issue |
4 |
Pages |
045017 |
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Keywords |
A1 Journal Article; oxygen plasma, pseudo-1D plug-flow kinetic model, O atoms, low-pressure validation, atmospheric pressure microwave torch; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
We have developed a comprehensive kinetic model to study the O atom kinetics in an O<sub>2</sub>plasma and its afterglow. By adopting a pseudo-1D plug-flow formalism within the kinetic model, our aim is to assess how far the O atoms travel in the plasma afterglow, evaluating its potential as a source of O atoms for post-plasma gas conversion applications. Since we could not find experimental data for pure O<sub>2</sub>plasma at atmospheric pressure, we first validated our model at low pressure (1–10 Torr) where very good experimental data are available. Good agreement between our model and experiments was achieved for the reduced electric field, gas temperature and the densities of the dominant neutral species, i.e. O<sub>2</sub>(a), O<sub>2</sub>(b) and O. Subsequently, we confirmed that the chemistry set is consistent with thermodynamic equilibrium calculations at atmospheric pressure. Finally, we investigated the O atom densities in the O<sub>2</sub>plasma and its afterglow, for which we considered a microwave O<sub>2</sub>plasma torch, operating at a pressure between 0.1 and 1 atm, for a flow rate of 20 slm and an specific energy input of 1656 kJ mol<sup>−1</sup>. Our results show that for both pressure conditions, a high dissociation degree of ca. 92% is reached within the discharge. However, the O atoms travel much further in the plasma afterglow for<italic>p</italic>= 0.1 atm (9.7 cm) than for<italic>p</italic>= 1 atm (1.4 cm), attributed to the longer lifetime (3.8 ms at 0.1 atm vs 1.8 ms at 1 atm) resulting from slower three-body recombination kinetics, as well as a higher volumetric flow rate. |
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Wos |
001209453500001 |
Publication Date |
2024-04-01 |
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Edition |
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ISSN |
0963-0252 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
3.8 |
Times cited |
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Open Access |
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Notes |
This research was supported by the Horizon Europe Framework Program ‘Research and Innovation Actions’ (RIA), Project CANMILK (Grant No. 101069491). |
Approved |
Most recent IF: 3.8; 2024 IF: 3.302 |
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Call Number |
PLASMANT @ plasmant @c:irua:205920 |
Serial |
9125 |
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Author |
Guerrero, R.M.; Lemir, I.D.; Carrasco, S.; Fernández-Ruiz, C.; Kavak, S.; Pizarro, P.; Serrano, D.P.; Bals, S.; Horcajada, P.; Pérez, Y. |
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Title |
Scaling-Up Microwave-Assisted Synthesis of Highly Defective Pd@UiO-66-NH2Catalysts for Selective Olefin Hydrogenation under Ambient Conditions |
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A1 Journal Article |
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Year |
2024 |
Publication |
ACS Applied Materials & Interfaces |
Abbreviated Journal |
ACS Appl. Mater. Interfaces |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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Abstract |
The need to develop green and cost-effective industrial catalytic processes has led to growing interest in preparing more robust, efficient, and selective heterogeneous catalysts at a large scale. In this regard, microwave-assisted synthesis is a fast method for fabricating heterogeneous catalysts (including metal oxides, zeolites, metal–organic frameworks, and supported metal nanoparticles) with enhanced catalytic properties, enabling synthesis scale-up. Herein, the synthesis of nanosized UiO-66-NH2 was optimized via a microwave-assisted hydrothermal method to obtain defective matrices essential for the stabilization of metal nanoparticles, promoting catalytically active sites for hydrogenation reactions (760 kg·m–3·day–1 space time yield, STY). Then, this protocol was scaled up in a multimodal microwave reactor, reaching 86% yield (ca. 1 g, 1450 kg·m–3·day–1 STY) in only 30 min. Afterward, Pd nanoparticles were formed in situ decorating the nanoMOF by an effective and fast microwave-assisted hydrothermal method, resulting in the formation of Pd@UiO-66-NH2 composites. Both the localization and oxidation states of Pd nanoparticles (NPs) in the MOF were achieved using high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and X-ray photoelectron spectroscopy (XPS), respectively. The optimal composite, loaded with 1.7 wt % Pd, exhibited an extraordinary catalytic activity (>95% yield, 100% selectivity) under mild conditions (1 bar H2, 25 °C, 1 h reaction time), not only in the selective hydrogenation of a variety of single alkenes (1-hexene, 1-octene, 1-tridecene, cyclohexene, and tetraphenyl ethylene) but also in the conversion of a complex mixture of alkenes (i.e., 1-hexene, 1-tridecene, and anethole). The results showed a powerful interaction and synergy between the active phase (Pd NPs) and the catalytic porous scaffold (UiO-66-NH2), which are essential for the selectivity and recyclability. |
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Wos |
001227929100001 |
Publication Date |
2024-04-26 |
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Edition |
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ISSN |
1944-8244 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.5 |
Times cited |
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Open Access |
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Notes |
The authors gratefully acknowledge financial support from “Comunidad de Madrid” and European Regional Development Fund-FEDER through the project HUB MADRID+CIRCULAR; the State Research Agency (MCIN/AEI /10.13039/501100011033) through the grant with reference number CEX2019-000931-M received in the 2019 call for “Severo Ochoa Centres of Excellence” and “María de Maeztu Units of Excellence” of the State Programme for Knowledge Generation and Scientific and Technological Strengthening of the R&D&I System; and MICIU through the project “NAPOLION” (PID2022-139956OB-I00). S.K. acknowledges the Flemish Fund for Scientific Research (FWO Vlaanderen) through a PhD research grant (1181124N). |
Approved |
Most recent IF: 9.5; 2024 IF: 7.504 |
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Call Number |
EMAT @ emat @c:irua:206322 |
Serial |
9126 |
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Author |
Xu, W.; Van Alphen, S.; Galvita, V.V.; Meynen, V.; Bogaerts, A. |
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Title |
Effect of Gas Composition on Temperature and CO2Conversion in a Gliding Arc Plasmatron reactor: Insights for Post‐Plasma Catalysis from Experiments and Computation |
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A1 Journal Article |
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Year |
2024 |
Publication |
ChemSusChem |
Abbreviated Journal |
ChemSusChem |
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Keywords |
A1 Journal Article; CO2 conversion · Plasma · Gliding arc plasmatron · Temperature profiles · Computational modelling; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
Plasma‐based CO<sub>2</sub>conversion has attracted increasing interest. However, to understand the impact of plasma operation on post‐plasma processes, we studied the effect of adding N<sub>2</sub>, N<sub>2</sub>/CH<sub>4</sub>and N<sub>2</sub>/CH<sub>4</sub>/H<sub>2</sub>O to a CO<sub>2</sub>gliding arc plasmatron (GAP) to obtain valuable insights into their impact on exhaust stream composition and temperature, which will serve as feed gas and heat for post‐plasma catalysis (PPC). Adding N<sub>2</sub>improves the CO<sub>2</sub>conversion from 4 % to 13 %, and CH<sub>4</sub>addition further promotes it to 44 %, and even to 61 % at lower gas flow rate (6 L/min), allowing a higher yield of CO and hydrogen for PPC. The addition of H<sub>2</sub>O, however, reduces the CO<sub>2</sub>conversion from 55 % to 22 %, but it also lowers the energy cost, from 5.8 to 3 kJ/L. Regarding the temperature at 4.9 cm post‐plasma, N<sub>2</sub>addition increases the temperature, while the CO<sub>2</sub>/CH<sub>4</sub>ratio has no significant effect on temperature. We also calculated the temperature distribution with computational fluid dynamics simulations. The obtained temperature profiles (both experimental and calculated) show a decreasing trend with distance to the exhaust and provide insights in where to position a PPC bed. |
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Wos |
001200297300001 |
Publication Date |
2024-04-11 |
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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 |
We acknowledge the VLAIO Catalisti Moonshot project D2M and the VLAIO Catalisti transition project CO2PERATE (HBC.2017.0692) for financial support. We acknowledge Gilles Van Loon for his help to make the quartz and steel devices for the reactor. Vladimir V. Galvita also acknowledges a personal grant from the Research Fund of Ghent University (BOF; 01N16319). |
Approved |
Most recent IF: 8.4; 2024 IF: 7.226 |
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Call Number |
PLASMANT @ plasmant @c:irua:205101 |
Serial |
9128 |
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Author |
Van Gordon, K.; Ni, B.; Girod, R.; Mychinko, M.; Bevilacqua, F.; Bals, S.; Liz‐Marzán, L.M. |
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Title |
Single Crystal and Pentatwinned Gold Nanorods Result in Chiral Nanocrystals with Reverse Handedness |
Type |
A1 Journal Article |
| |
Year |
2024 |
Publication |
Angewandte Chemie International Edition |
Abbreviated Journal |
Angew Chem Int Ed |
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Volume |
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Issue |
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Pages |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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Abstract |
Handedness is an essential attribute of chiral nanocrystals, having a major influence on their properties. During chemical growth, the handedness of nanocrystals is usually tuned by selecting the corresponding enantiomer of chiral molecules involved in asymmetric growth, often known as chiral inducers. We report that, even using the same chiral inducer enantiomer, the handedness of chiral gold nanocrystals can be reversed by using Au nanorod seeds with either single crystalline or pentatwinned structure. This effect holds for chiral growth induced both by amino acids and by chiral micelles. Although it was challenging to discern the morphological handedness for<italic>L</italic>‐cystine‐directed particles, even using electron tomography, both cases showed circular dichroism bands of opposite sign, with nearly mirrored chiroptical signatures for chiral micelle‐directed growth, along with quasi‐helical wrinkles of inverted handedness. These results expand the chiral growth toolbox with an effect that might be exploited to yield a host of interesting morphologies with tunable optical properties. |
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Wos |
001230287700001 |
Publication Date |
2024-05-24 |
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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 |
1433-7851 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
16.6 |
Times cited |
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Open Access |
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Notes |
Ana Sánchez-Iglesias is acknowledged for support in the synthesis of pentatwinned gold nanorods. The authors acknowledge financial support by the European Research Council (ERC CoG No. 815128 REALNANO to S.B.), from MCIN/AEI/10.13039/501100011033 (Grant PID2020- 117779RB-I00 to L.M.L.-M and FPI Fellowship PRE2021- 097588 to K.V.G.), and by KU Leuven (C14/22/085). This work has been funded by the European Union under Project 101131111—DELIGHT. Funding for open access charge: Universidade de Vigo/ CRUE-CISUG. |
Approved |
Most recent IF: 16.6; 2024 IF: 11.994 |
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Call Number |
EMAT @ emat @c:irua:206328 |
Serial |
9129 |
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Author |
Xu, W.; Buelens, L.C.; Galvita, V.V.; Bogaerts, A.; Meynen, V. |
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Title |
Improving the performance of gliding arc plasma-catalytic dry reforming via a new post-plasma tubular catalyst bed |
Type |
A1 Journal Article |
| |
Year |
2024 |
Publication |
Journal of CO2 Utilization |
Abbreviated Journal |
Journal of CO2 Utilization |
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Volume |
83 |
Issue |
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Pages |
102820 |
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Keywords |
A1 Journal Article; Dry reforming Gliding arc plasma Plasma catalytic DRM Ni-based mixed oxide Post-plasma catalysis; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
A combination of a gliding arc plasmatron (GAP) reactor and a newly designed tubular catalyst bed (N-bed) was applied to investigate the post-plasma catalytic (PPC) effect for dry reforming of methane (DRM). As comparison, a traditional plasma catalyst bed (T-bed) was also utilized. The post-plasma catalytic effect of a Ni-based mixed oxide (Ni/MO) catalyst with a thermal catalytic performance of 77% CO2 and 86% CH4 conversion at 700 ℃ was studied. Although applying the T-bed had little effect on plasma based CO2 and CH4 conversion, an increase in selectivity to H2 was obtained with a maximum value of 89% at a distance of 2 cm. However, even when only α-Al2O3 packing material was used in the N-bed configuration, compared to the plasma alone and the T-bed, an increase of the CO2 and CH4 conversion from 53% and 53% to 69% and 69% to 83% was achieved. Addition of the Ni/MO catalyst further enhanced the DRM reaction, resulting in conversions of 79% for CO2 and 91% for
CH4. Hence, although no insulation nor external heating was applied to the N-bed post plasma, it provides a slightly better conversion than the thermal catalytic performance with the same catalyst, while being fully electrically driven. In addition, an enhanced CO selectivity to 96% was obtained and the energy cost was reduced from ~ 6 kJ/L (plasma alone) to 4.3 kJ/L. To our knowledge, it is the first time that a post-plasma catalytic system achieves this excellent catalytic performance for DRM without extra external heating or insulation. |
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Wos |
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Publication Date |
2024-05-25 |
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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 |
2212-9820 |
ISBN |
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Additional Links |
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Impact Factor |
7.7 |
Times cited |
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Open Access |
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Notes |
Wencong Xu, Vladimir V. Galvita, Annemie Bogaerts, and Vera Meynen would like to acknowledge the VLAIO Catalisti Moonshot project D2M and the VLAIO Catalisti transition project CO2PERATE (HBC.2017.0692). Lukas C. Buelens acknowledges financial support from the Fund for Scientific Research Flanders (FWO Flanders) through a postdoctoral fellowship grant 12E5623N. Vladimir V. Galvita also acknowledges a personal grant from the Research Fund of Ghent University (BOF; 01N16319). |
Approved |
Most recent IF: 7.7; 2024 IF: 4.292 |
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Call Number |
PLASMANT @ plasmant @ |
Serial |
9131 |
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Author |
Maerivoet, S.; Tsonev, I.; Slaets, J.; Reniers, F.; Bogaerts, A. |
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Title |
Coupled multi-dimensional modelling of warm plasmas: Application and validation for an atmospheric pressure glow discharge in CO2/CH4/O2 |
Type |
A1 Journal Article |
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Year |
2024 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chemical Engineering Journal |
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Volume |
492 |
Issue |
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Pages |
152006 |
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Keywords |
A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
To support experimental research into gas conversion by warm plasmas, models should be developed to explain the experimental observations. These models need to describe all physical and chemical plasma properties in a coupled way. In this paper, we present a modelling approach to solve the complete set of assumed relevant equations, including gas flow, heat balance and species transport, coupled with a rather extensive chemistry set, consisting of 21 species, obtained by reduction of a more detailed chemistry set, consisting of 41 species. We apply this model to study the combined CO2 and CH4 conversion in the presence of O2, in a direct current atmospheric pressure glow discharge. Our model can predict the experimental trends, and can explain why higher O2 fractions result in higher CH4 conversion, namely due to the higher gas temperature, rather than just by additional chemical reactions. Indeed, our model predicts that when more O2 is added, the energy required to reach any set temperature (i.e., the enthalpy) drops, allowing the system to reach higher temperatures with similar amounts of energy. This is in turn related to the higher H2O fraction and lower H2 fraction formed in the plasma, as demonstrated by our model. Altogether, our new self-consistent model can capture the main physics and chemistry occurring in this warm plasma, which is an important step towards predictive modelling for plasma-based gas conversion. |
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Publication Date |
2024-05-09 |
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Edition |
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ISSN |
1385-8947 |
ISBN |
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Additional Links |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
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Notes |
This research was supported by the Excellence of Science FWO-FNRS project (FWO grant ID G0I1822N; EOS ID 40007511) 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, and grant agreement No. 101081162–PREPARE ERC Proof of Concept project). computational resources and services used in this work were provided by the HPC core facility CalcUA of the Universiteit Antwerpen, and VSC (Flemish Supercomputer Center), funded by the Research Foundation – Flanders (FWO) and the Flemish Government. |
Approved |
Most recent IF: 15.1; 2024 IF: 6.216 |
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Call Number |
PLASMANT @ plasmant @ |
Serial |
9132 |
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Author |
Tong, J.; Fu, Y.; Domaretskiy, D.; Della Pia, F.; Dagar, P.; Powell, L.; Bahamon, D.; Huang, S.; Xin, B.; Costa Filho, R.N.; Vega, L.F.; Grigorieva, I.V.; Peeters, F.M.; Michaelides, A.; Lozada-Hidalgo, M. |
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Title |
Control of proton transport and hydrogenation in double-gated graphene |
Type |
A1 Journal Article |
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Year |
2024 |
Publication |
Nature |
Abbreviated Journal |
Nature |
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Volume |
630 |
Issue |
8017 |
Pages |
619-624 |
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Keywords |
A1 Journal Article; Condensed Matter Theory (CMT) ; |
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Abstract |
The basal plane of graphene can function as a selective barrier that is permeable to protons but impermeable to all ions and gases, stimulating its use in applications such as membranes, catalysis and isotope separation. Protons can chemically adsorb on graphene and hydrogenate it, inducing a conductor–insulator transition that has been explored intensively in graphene electronic devices. However, both processes face energy barriersand various strategies have been proposed to accelerate proton transport, for example by introducing vacancies, incorporating catalytic metalsor chemically functionalizing the lattice. But these techniques can compromise other properties, such as ion selectivity or mechanical stability. Here we show that independent control of the electric field,<italic>E</italic>, at around 1 V nm<sup>−1</sup>, and charge-carrier density,<italic>n</italic>, at around 1 × 10<sup>14</sup> cm<sup>−2</sup>, in double-gated graphene allows the decoupling of proton transport from lattice hydrogenation and can thereby accelerate proton transport such that it approaches the limiting electrolyte current for our devices. Proton transport and hydrogenation can be driven selectively with precision and robustness, enabling proton-based logic and memory graphene devices that have on–off ratios spanning orders of magnitude. Our results show that field effects can accelerate and decouple electrochemical processes in double-gated 2D crystals and demonstrate the possibility of mapping such processes as a function of<italic>E</italic>and<italic>n</italic>, which is a new technique for the study of 2D electrode–electrolyte interfaces. |
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Wos |
https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=brocade2&SrcAuth=WosAPI&KeyUT=WOS:001262 |
Publication Date |
2024-06-20 |
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Abbreviated Series Title |
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Edition |
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ISSN |
0028-0836 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
64.8 |
Times cited |
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Open Access |
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Notes |
This work was supported by UKRI (EP/X017745: M.L.-H; EP/X035891: A.M.), the Directed Research Projects Program of the Research and Innovation Center for Graphene and 2D Materials at Khalifa University (RIC2D-D001: M.L.-H., L.F.V. and D.B.), The Royal Society (URF\R1\201515: M.L.-H.) and the European Research Council (101071937: A.M.). Part of this work was supported by the Flemish Science Foundation (FWO-Vl, G099219N). A.M. acknowledges access to the UK national high-performance computing service (ARCHER2). |
Approved |
Most recent IF: 64.8; 2024 IF: 40.137 |
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Call Number |
CMT @ cmt @c:irua:206402 |
Serial |
9247 |
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Author |
Cai, Y.; Michiels, R.; De Luca, F.; Neyts, E.; Tu, X.; Bogaerts, A.; Gerrits, N. |
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Title |
Improving Molecule–Metal Surface Reaction Networks Using the Meta-Generalized Gradient Approximation: CO2Hydrogenation |
Type |
A1 Journal Article |
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Year |
2024 |
Publication |
The Journal of Physical Chemistry C |
Abbreviated Journal |
J. Phys. Chem. C |
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Volume |
128 |
Issue |
21 |
Pages |
8611-8620 |
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Keywords |
A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
Density functional theory is widely used to gain insights into molecule−metal surface reaction networks, which is important for a better understanding of catalysis. However, it is well-known that generalized gradient approximation (GGA)
density functionals (DFs), most often used for the study of reaction networks, struggle to correctly describe both gas-phase molecules and metal surfaces. Also, GGA DFs typically underestimate reaction barriers due to an underestimation of the selfinteraction energy. Screened hybrid GGA DFs have been shown to reduce this problem but are currently intractable for wide usage. In this work, we use a more affordable meta-GGA (mGGA) DF in combination with a nonlocal correlation DF for the first time to study and gain new insights into a catalytically important surface
reaction network, namely, CO2 hydrogenation on Cu. We show that the mGGA DF used, namely, rMS-RPBEl-rVV10, outperforms typical GGA DFs by providing similar or better predictions for metals and molecules, as well as molecule−metal surface adsorption
and activation energies. Hence, it is a better choice for constructing molecule−metal surface reaction networks. |
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Wos |
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Publication Date |
2024-05-30 |
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Abbreviated Series Title |
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Series Issue |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
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Impact Factor |
3.7 |
Times cited |
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Open Access |
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Notes |
H2020 Marie Sklodowska-Curie Actions, 813393 ; Fonds Wetenschappelijk Onderzoek, 1114921N ; H2020 European Research Council, 810182 ; Nederlandse Organisatie voor Wetenschappelijk Onderzoek, 019.202EN.012 ; |
Approved |
Most recent IF: 3.7; 2024 IF: 4.536 |
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Call Number |
PLASMANT @ plasmant @ |
Serial |
9248 |
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Author |
Arts, I.; Saniz, R.; Baldinozzi, G.; Leinders, G.; Verwerft, M.; Lamoen, D. |
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Title |
Ab initio study of the adsorption of O, O2, H2O and H2O2 on UO2 surfaces using DFT+U and non-collinear magnetism |
Type |
A1 Journal Article |
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Year |
2024 |
Publication |
Journal of Nuclear Materials |
Abbreviated Journal |
Journal of Nuclear Materials |
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Volume |
599 |
Issue |
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Pages |
155249 |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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Abstract |
In order to model correctly the corrosion of spent nuclear fuel under disposal conditions, it is important to understand its behavior in the presence of oxidants. To advance in this direction, we consider the oxidation of UO2. We investigate computationally the adsorption of various species on its three most stable surfaces: (111), (110), and (100), with emphasis on incorporating a full non-collinear PBE+U approach. Various species, namely O, O2, H2O and H2O2 are considered due to their relevance for the oxidation of UO2. The dissociation energy and an estimate for the dissociation barrier for O2 were obtained, using the preferred adsorption configurations of O and O2. The adsorption configurations for H2O in our study compare well with previous studies that used collinear approximations, both in terms of relative stability of configurations and bond lengths. Differences in adsorption energies were found, which may be important for reaction kinetics. Dissociative reactions in which the water molecule splits in hydrogen and hydroxyl occur only on one of the three surfaces. The hydrogen further reacts with a surface oxygen to also form a hydroxyl group. Not surprisingly, we find that H2O2 binds more strongly to the three surfaces than water (lower formation energy), and similar to H2O adsorption, dissociative reactions may occur. The dissociated hydrogen reacts with a surface oxygen to form a hydroxyl group and the hydroperoxyl molecule binds with a surface uranium. Our study, which includes a detailed study of electron transfer, magnetic structure and the preferred adsorption configurations, gives insight into the uranium oxidation states and the influence of surface geometry on adsorption. The findings contribute to a more comprehensive understanding of the early stages of UO2 oxidation. |
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https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=brocade2&SrcAuth=WosAPI&KeyUT=WOS:001262 |
Publication Date |
2024-06-25 |
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ISSN |
0022-3115 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS full record |
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Impact Factor |
3.1 |
Times cited |
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Open Access |
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Notes |
Financial support for this research was provided by the Energy Transition Fund of the Belgian FPS Economy (Project SF-CORMOD: Spent Fuel – Corrosion modeling). This work was performed using HPC resources from the VSC (Flemish Supercomputer Center) and the HPC infrastructure of the University of Antwerp (CalcUA), both funded by the FWO-Vlaanderen and the Flemish Government department EWI (Economie, Wetenschap & Innovatie). |
Approved |
Most recent IF: 3.1; 2024 IF: 2.048 |
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Call Number |
EMAT @ emat @c:irua:207055 |
Serial |
9249 |
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Author |
Ding, Y.; Wang, C.; Bandaru, S.; Pei, L.; Zheng, R.; Hau Ng, Y.; Arenas Esteban, D.; Bals, S.; Zhong, J.; Hofkens, J.; Van Tendeloo, G.; Roeffaers, M.B.J.; Chen, L.-H.; Su, B.-L. |
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Title |
Cs3Bi2Br9 nanoparticles decorated C3N4 nanotubes composite photocatalyst for highly selective oxidation of benzylic alcohol |
Type |
A1 Journal Article |
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Year |
2024 |
Publication |
Journal of Colloid and Interface Science |
Abbreviated Journal |
Journal of Colloid and Interface Science |
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Volume |
672 |
Issue |
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Pages |
600-609 |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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Abstract |
Solar-light driven oxidation of benzylic alcohols over photocatalysts endows significant prospects in value-added organics evolution owing to its facile, inexpensive and sustainable process. However, the unsatisfactory performance of actual photocatalysts due to the inefficient charge separation, low photoredox potential and sluggish surface reaction impedes the practical application of this process. Herein, we developed an innovative Z-Scheme Cs3BiBr9 nanoparticles@porous C3N4 tubes (CBB-NP@P-tube-CN) heterojunction photocatalyst for highly selective benzyl alcohol oxidation. Such composite combining increased photo-oxidation potential, Z-Scheme charge migration route as well as the structural advantages of porous tubular C3N4 ensures the accelerated mass and ions diffusion kinetics, the fast photoinduced carriers dissociation and sufficient photoredox potentials. The CBB-NP@P-tube-CN photocatalyst demonstrates an exceptional performance for selective photo-oxidation of benzylic alcohol into benzaldehyde with 19, 14 and 3 times higher benzylic alcohols conversion rate than those of C3N4 nanotubes, Cs3Bi2Br9 and Cs3Bi2Br9@bulk C3N4 photocatalysts, respectively. This work offers a sustainable photocatalytic system based on lead-free halide perovskite toward large scale solar-light driven value-added chemicals production. |
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001251644100001 |
Publication Date |
2024-06-05 |
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Edition |
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ISSN |
0021-9797 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.9 |
Times cited |
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Open Access |
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Notes |
This work is financially supported by the Zhejiang Provincial Natural Science Foundation of China (No. LQ24E020011), and National Natural Science Foundation of China (No. 12374372, 52072101)., Program for Changjiang Scholars and Innovative Research Team in University (IRT_15R52) of the Chinese Ministry of Education and Program of Introducing Talents of Discipline to Universities-Plan 111 (Grant No. B20002) from the Ministry of Science and Technology and the Ministry of Education of China. This research is also supported by the European Commission Interreg V France-Wallonie-Vlaanderen project “DepollutAir”. |
Approved |
Most recent IF: 9.9; 2024 IF: 4.233 |
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Call Number |
EMAT @ emat @c:irua:206675 |
Serial |
9250 |
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Author |
Michiels, R.; Gerrits, N.; Neyts, E.; Bogaerts, A. |
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Title |
Plasma Catalysis Modeling: How Ideal Is Atomic Hydrogen for Eley–Rideal? |
Type |
A1 Journal Article |
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Year |
2024 |
Publication |
The Journal of Physical Chemistry C |
Abbreviated Journal |
J. Phys. Chem. C |
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Volume |
128 |
Issue |
27 |
Pages |
11196-11209 |
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Keywords |
A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
Plasma catalysis is an emerging technology, but a lot of questions about the underlying surface mechanisms remain unanswered. One of these questions is how important Eley−Rideal (ER) reactions are, next to Langmuir−Hinshelwood reactions. Most plasma catalysis kinetic models predict ER reactions to be important and sometimes even vital for the surface chemistry. In this work, we take a critical look at how ER reactions involving H radicals are incorporated in kinetic models describing CO2 hydrogenation and NH3 synthesis. To this end, we construct potential energy surface (PES) intersections, similar to elbow plots constructed for dissociative chemisorption. The results of the PES intersections are in agreement with ab initio molecular dynamics (AIMD) findings in literature while being computationally much cheaper. We find that, for the reactions studied here, adsorption is more probable than a reaction via the hot atom (HA) mechanism, which in turn is more probable than a reaction via the ER mechanism. We also conclude that kinetic models of plasma-catalytic systems tend to overestimate the importance if ER reactions. Furthermore, as opposed to what is often assumed in kinetic models, the choice of catalyst will influence the ER reaction probability. Overall, the description of ER reactions is too much “ideal” in models. Based on our indings, we make a number of recommendations on how to incorporate ER reactions in kinetic models to avoid overestimation of their importance. |
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Publication Date |
2024-07-11 |
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ISSN |
1932-7447 |
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Impact Factor |
3.7 |
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Notes |
Fonds Wetenschappelijk Onderzoek, 1114921N ; Horizon 2020 Framework Programme, 810182 ; |
Approved |
Most recent IF: 3.7; 2024 IF: 4.536 |
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PLASMANT @ plasmant @ |
Serial |
9251 |
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Author |
Jeong, Y.; Han, B.; Tamayo, A.; Claes, N.; Bals, S.; Samorì, P. |
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Title |
Defect Engineering of MoTe2via Thiol Treatment for Type III van der Waals Heterojunction Phototransistor |
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A1 Journal Article |
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Year |
2024 |
Publication |
ACS Nano |
Abbreviated Journal |
ACS Nano |
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18 |
Issue |
28 |
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18334-18343 |
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A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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Molybdenum ditelluride (MoTe2) nanosheets have displayed intriguing physicochemical properties and opto-electric characteristics as a result of their tunable and
small band gap (Eg ∼ 1 eV), facilitating concurrent electron and hole transport. Despite the numerous efforts devoted to the development of p-type MoTe2 field-effect transistors (FETs), the presence of tellurium (Te) point vacancies has caused serious reliability issues. Here, we overcome this major
limitation by treating the MoTe2 surface with thiolated molecules to heal Te vacancies. Comprehensive materials and electrical characterizations provided unambiguous evidence for the efficient chemisorption of butanethiol. Our thiol-treated MoTe2 FET exhibited a 10-fold increase in hole current and a positive threshold voltage shift of 25 V, indicative of efficient hole carrier doping. We demonstrated that our powerful molecular engineering strategy can be extended to the controlled formation of van der Waals heterostructures by developing an n-SnS2/thiol-MoTe2 junction FET (thiol-JFET). Notably, the thiol-JFET exhibited a significant negative photoresponse with a responsivity of 50 A W−1 and a fast response time of 80 ms based on band-to-band tunneling. More interestingly, the
thiol-JFET displayed a gate tunable trimodal photodetection comprising two photoactive modes (positive and negative photoresponse) and one photoinactive mode. These findings underscore the potential of molecular engineering approaches in
enhancing the performance and functionality of MoTe2-based nanodevices as key components in advanced 2D-based optoelectronics. |
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https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=brocade2&SrcAuth=WosAPI&KeyUT=WOS:001264 |
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2024-07-16 |
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1936-0851 |
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UA library record; WoS full record; WoS citing articles; WoS full record |
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Impact Factor |
17.1 |
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The authors acknowledge the financial support from the FLAG-ERA project MULTISPIN funded by the Agence Nationale de la Recherche (ANR-21-GRF1-0003-01). We also acknowledge funding from the European Union’s Horizon Europe research and innovation programme through the project HYPERSONIC (GA-101129613) and the ERC project SUPRA2DMAT (GA-833707) as well as the ANR through the Interdisciplinary Thematic Institute SysChem via the IdEx Unistra (ANR-10-IDEX-0002) within the program Investissement d’Avenir, the Foundation Jean-Marie Lehn and the Institut Universitaire de France (IUF). This work was also supported by National Research Foundation of Korea (NRF) grant funded by Korea government (MSIT) (No. RS-2023- 00251360). |
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Most recent IF: 17.1; 2024 IF: 13.942 |
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EMAT @ emat @c:irua:207002 |
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9252 |
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Manaigo, F.; Chatterjee, A.; Bogaerts, A.; Snyders, R. |
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Title |
Insight in NO synthesis in a gliding arc plasma via gas temperature and density mapping by laser-induced fluorescence |
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A1 Journal Article |
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2024 |
Publication |
Plasma Sources Science and Technology |
Abbreviated Journal |
Plasma Sources Sci. Technol. |
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33 |
Issue |
7 |
Pages |
075005 |
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Keywords |
A1 Journal Article; plasma nitrogen fixation, gliding arc plasmatron, laser-induced fluorescence, afterglow rotational temperature, afterglow NO concentration; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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A gliding arc (GA) plasma, operating at atmospheric pressure in a gas mixture of 50% N<sub>2</sub>and 50% O<sub>2</sub>, is studied using laser-induced fluorescence spectroscopy. The main goal is to determine the two-dimensional distribution of both the gas temperature and the NO ground state density in the afterglow. As GA plasma discharges at atmospheric pressure normally produce rather high NO<sub><italic>x</italic></sub>densities, the high concentration of relevant absorbers, such as NO, may impose essential restrictions for the use of ‘classical’ laser-induced fluorescence methods (dealing with excitation in the bandhead vicinity), as the laser beam would be strongly absorbed along its propagation in the afterglow. Since this was indeed the case for the studied discharge, an approach dealing with laser-based excitation of separate rotational lines is proposed. In this case, due to a non-saturated absorption regime, simultaneous and reliable measurements of both the NO density and the gas temperature (using a reference fitting spectrum) are possible. The proposed method is applied to provide a two-dimensional map for both the NO density and the gas temperature at different plasma conditions. The results show that the input gas flow rate strongly alters the plasma shape, which appears as an elongated column at low input gas flow rate and spreads laterally as the flow rate increases. Finally, based on temperature map analysis, a clear correlation between the gas temperature and NO concentration is found. The proposed method may be interesting for the plasma-chemical analysis of discharges with high molecular production yields, where knowledge of both molecular concentration and gas temperature is required. |
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2024-07-01 |
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ISSN |
0963-0252 |
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Impact Factor |
3.8 |
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Notes |
Fonds De La Recherche Scientifique – FNRS, EOS O005118F ; |
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Most recent IF: 3.8; 2024 IF: 3.302 |
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PLASMANT @ plasmant @ |
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9253 |
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Wanten, B.; Gorbanev, Y.; Bogaerts, A. |
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Title |
Plasma-based conversion of CO2 and CH4 into syngas: A dive into the effect of adding water |
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A1 Journal Article |
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2024 |
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Fuel |
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Fuel |
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374 |
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132355 |
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A1 Journal Article; Plasma Bi-reforming of methane Atmospheric pressure glow discharge Hydrogen-rich syngas; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Plasma technology can play a vital role in the electrification and decarbonization of chemical processes. In this work, we carried out the bi-reforming of methane (BRM), producing syngas out of H2O vapor and the greenhouse gases CO2 and CH4, in an atmospheric pressure glow discharge reactor. Compared to dry reforming of methane (DRM), the addition of H2O helps in counteracting soot formation, and thus avoids severe destabilization of the generated plasma. A mixture of 14–41-45 vol% (CO2-CH4-H2O) leads to the overall best results in terms of stable plasma and performance metrics. We obtained a CO2 and CH4 conversion of 49 % and 74 %, respectively, at a SEI of 210 kJ/mol. The energy cost is 390 kJ/mol converted reactants, which is below the target defined for plasmabased syngas production to be competitive with other technologies. Moreover, we reached CO and H2 yields of
59 % and 49 %, and a syngas ratio (SR) of 2, which is ideal for further methanol synthesis. |
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Publication Date |
2024-07-15 |
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0016-2361 |
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Impact Factor |
7.4 |
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This project has received funding from the BlueApp Proof-of-Concept project “Optanic”, the VLAIO-Catalisti ICON project “BluePlasma” (grant ID HBC.2022.0445), and the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (grant agreement no. 810182─SCOPE ERC Synergy project). |
Approved |
Most recent IF: 7.4; 2024 IF: 4.601 |
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Call Number |
PLASMANT @ plasmant @ |
Serial |
9254 |
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