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Wanten, B.; Vertongen, R.; De Meyer, R.; Bogaerts, A. |
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Title |
Plasma-based CO2 conversion: How to correctly analyze the performance? |
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A1 journal article |
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Year |
2023 |
Publication |
Journal of Energy Chemistry |
Abbreviated Journal |
Journal of Energy Chemistry |
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Volume |
86 |
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Pages |
180-196 |
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A1 journal article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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001070885000001 |
Publication Date |
2023-07-22 |
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ISSN |
2095-4956 |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.1 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
We acknowledge financial support from the Fund for Scientific Research (FWO) Flanders (Grant ID 110221N), the European Research Council (ERC) under the European Union’s Horizon 2020 Research and Innovation Program (grant agreement No 810182 – SCOPE ERC Synergy project), and the Methusalem funding of the University of Antwerp. We acknowledge the icons from the graphical abstract made by dDara, geotatah, Spashicons and Freepik on www.flaticon.com. We also thank Stein Maerivoet, Joachim Slaets, Elizabeth Mercer, Colín Ó’Modráin, Joran Van Turnhout, Pepijn Heirman, dr. Yury Gorbanev, dr. Fanny Girard-Sahun and dr. Sean Kelly for the interesting discussions and feedback. |
Approved |
Most recent IF: 13.1; 2023 IF: 2.594 |
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Call Number |
PLASMANT @ plasmant @c:irua:198709 |
Serial |
8816 |
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Author |
Pedrazo-Tardajos, A.; Claes, N.; Wang, D.; Sánchez-Iglesias, A.; Nandi, P.; Jenkinson, K.; De Meyer, R.; Liz-Marzán, L.M.; Bals, S. |
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Title |
Direct visualization of ligands on gold nanoparticles in a liquid environment |
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A1 Journal Article |
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Year |
2024 |
Publication |
Nature Chemistry |
Abbreviated Journal |
Nat. Chem. |
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A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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Abstract |
The interaction among Au nanoparticles, their surface ligands and the solvent critically influences the properties of nanoparticles. Despite employing spectroscopic and scattering techniques to investigate their ensemble structure, a comprehensive understanding at the nanoscale remains elusive. Electron microscopy enables characterization of the local structure and composition but is limited by insufficient contrast, electron beam sensitivity and ultra-high vacuum, which prevent the investigation of dynamic aspects. Here we show that, by exploiting high-quality graphene liquid cells, we can overcome these limitations and investigate the structure of the ligand shell around the Au nanoparticles, as well as the ligand-Au interface in a liquid environment. Using this graphene liquid cell, we visualize the anisotropy, composition and dynamics of ligand distribution at the Au nanorod surface. Our results indicate a micellar model for the surfactant organisation. This work opens up a reliable and direct visualization of ligand distribution around colloidal nanoparticles. |
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https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=brocade2&SrcAuth=WosAPI&KeyUT=WOS:001257 |
Publication Date |
2024-06-27 |
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Edition |
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ISSN |
1755-4330 |
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Additional Links |
UA library record; WoS full record; WoS citing articles; WoS full record |
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Impact Factor |
21.8 |
Times cited |
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Open Access |
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Notes |
S.B., and A.P.-T. acknowledge financial support from the European Commission under the Horizon 2020 Programme by grant no. 731019 (EUSMI) and ERC Consolidator grant no. 815128 (REALNANO). D.W. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (Grant 894254 SuprAtom). L.L.-M. acknowledges financial support from the European Research Council (ERC Advanced Grant 787510, 4DbioSERS) and the Spanish State Research Agency (Project PID2020-117779RB-I00 and MDM-2017-0720). The authors acknowledge Dr. J. Mosquera and Dr. Jimenez de Aberasturi for provision of samples and useful discussions. |
Approved |
Most recent IF: 21.8; 2024 IF: 25.87 |
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Call Number |
EMAT @ emat @c:irua:207062 |
Serial |
9256 |
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Permanent link to this record |
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Author |
Maerivoet, S.; Wanten, B.; De Meyer, R.; Van Hove, M.; Van Alphen, S.; Bogaerts, A. |
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Title |
Effect of O2on Plasma-Based Dry Reforming of Methane: Revealing the Optimal Gas Composition via Experiments and Modeling of an Atmospheric Pressure Glow Discharge |
Type |
A1 Journal Article |
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Year |
2024 |
Publication |
ACS Sustainable Chemistry & Engineering |
Abbreviated Journal |
ACS Sustainable Chem. Eng. |
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Volume |
12 |
Issue |
30 |
Pages |
11419-11434 |
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Keywords |
A1 Journal Article; plasma-based conversion, thermal plasma, syngas production, CO2 conversion, CH4 conversio; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
Plasma technology is gaining increasing interest for the conversion of greenhouse gases, such as CO2 and CH4, into value-added chemicals using (renewable) electricity. In this paper, we study the effect of O2 addition to the combined conversion of CO2 and CH4 in an atmospheric pressure glow discharge plasma. This process is called “oxidative CO2 reforming of methane”, and we search for the optimal gas mixing ratio in terms of conversion, energy cost, product output and plasma stability. A mixing ratio of 42.5:42.5:15 CO2/CH4/O2 yields the best performance, with a CO2 and CH4 conversion of 50 and 74%, respectively, and an energy cost as low as 2 eV molecule−1 (corresponding to 7.9 kJ L−1 and 190 kJ mol−1), i.e., clearly below the target defined to be competitive with other technologies. The syngas components (CO and H2) are the most important products, with a syngas ratio, H2/CO, being 0.8. Plasma destabilization at high CH4 fractions due to solid carbon formation is the limiting factor for further improving this syngas ratio. The solid carbon material is found to be contaminated with steel particles originating from the electrode material, rendering it unappealing as a side product. Therefore, O2 addition helps to remove the carbon formation. Besides the experiments, we developed a 2D axisymmetric fluid dynamics model, which can successfully predict the experimental trends in conversion, product composition and temperatures, while providing unique insights in the formation of CxHy species. |
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https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=brocade2&SrcAuth=WosAPI&KeyUT=WOS:001280 |
Publication Date |
2024-07-29 |
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ISSN |
2168-0485 |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
8.4 |
Times cited |
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Notes |
Universiteit Antwerpen; Fonds Wetenschappelijk Onderzoek, 40007511 G0I1822N ; H2020 European Research Council, 810182 ; |
Approved |
Most recent IF: 8.4; 2024 IF: 5.951 |
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Call Number |
PLASMANT @ plasmant @c:irua:207488 |
Serial |
9257 |
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Author |
Khaletskaya, K.; Turner, S.; Tu, M.; Wannapaiboon, S.; Schneemann, A.; Meyer, R.; Ludwig, A.; Van Tendeloo, G.; Fischer, R.A. |
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Title |
Self-directed localization of ZIF-8 thin film formation by conversion of ZnO nanolayers |
Type |
A1 Journal article |
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Year |
2014 |
Publication |
Advanced functional materials |
Abbreviated Journal |
Adv Funct Mater |
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Volume |
24 |
Issue |
30 |
Pages |
4804-4811 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Control of localized metal-organic framework (MOF) thin film formation is a challenge. Zeolitic imidazolate frameworks (ZIFs) are an important sub-class of MOFs based on transition metals and imidazolate linkers. Continuous coatings of intergrown ZIF crystals require high rates of heterogeneous nucleation. In this work, substrates coated with zinc oxide layers are used, obtained by atomic layer deposition (ALD) or by magnetron sputtering, to provide the Zn2+ ions required for nucleation and localized growth of ZIF-8 films ([Zn(mim)(2)]; Hmim = 2-methylimidazolate). The obtained ZIF-8 films reveal the expected microporosity, as deduced from methanol adsorption studies using an environmentally controlled quartz crystal microbalance (QCM) and comparison with bulk ZIF-8 reference data. The concept is transferable to other MOFs, and is applied to the formation of [Al(OH)(1,4-ndc)](n) (ndc = naphtalenedicarboxylate) thin films derived from Al2O3 nanolayers. |
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Weinheim |
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Wos |
000340549900010 |
Publication Date |
2014-05-07 |
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ISSN |
1616-301X; |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
12.124 |
Times cited |
77 |
Open Access |
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Notes |
312483 Esteem2; Fwo; esteem2_ta |
Approved |
Most recent IF: 12.124; 2014 IF: 11.805 |
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Call Number |
UA @ lucian @ c:irua:119215 |
Serial |
2975 |
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Permanent link to this record |
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Author |
De Meyer, R.; Albrecht, W.; Bals, S. |
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Title |
Effectiveness of reducing the influence of CTAB at the surface of metal nanoparticles during in situ heating studies by TEM |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Micron |
Abbreviated Journal |
Micron |
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Volume |
144 |
Issue |
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Pages |
103036 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
In situ TEM is a valuable technique to offer novel insights in the behavior of nanomaterials under various conditions. However, interpretation of in situ experiments is not straightforward since the electron beam can impact the outcome of such measurements. For example, ligands surrounding metal nanoparticles transform into a protective carbon layer upon electron beam irradiation and may impact the apparent thermal stability during in situ heating experiments. In this work, we explore the effect of different treatments typically proposed to remove such ligands. We found that plasma treatment prior to heating experiments for Au nanorods and nanostars increased the apparent thermal stability of the nanoparticles, while an activated carbon treatment resulted in a decrease of the observed thermal stability. Treatment with HCl barely changed the experimental outcome. These results demonstrate the importance of carefully selecting pre-treatments procedures during in situ heating experiments. |
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Wos |
000632282600002 |
Publication Date |
2021-02-19 |
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ISSN |
0968-4328 |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
1.98 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
H2020; European Research Council; This work was supported by the European Union’s Horizon 2020 research and innovation program [grant agreement No 823717 (ESTEEM3) and No 815128 (REALNANO)]; We acknowledge Prof. Luis M. Liz-Marzán and co-workers of the Bionanoplasmonics Laboratory, CICbiomaGUNE, Spain for providing the Au nanoparticles.; sygma; esteem3jra; esteem3reported |
Approved |
Most recent IF: 1.98 |
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Call Number |
EMAT @ emat @c:irua:175874 |
Serial |
6677 |
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Permanent link to this record |
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Author |
Kelly, S.; Mercer, E.; De Meyer, R.; Ciocarlan, R.-G.; Bals, S.; Bogaerts, A. |
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Title |
Microwave plasma-based dry reforming of methane: Reaction performance and carbon formation |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Journal of CO2 utilization |
Abbreviated Journal |
Journal of CO2 Utilization |
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Volume |
75 |
Issue |
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Pages |
102564 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
e investigate atmospheric pressure microwave (MW) plasma (2.45 GHz) conversion in CO2 and CH4 mixtures (i.e., dry reforming of methane, DRM) focusing on reaction performance and carbon formation. Promising energy costs of ~2.8–3.0 eV/molecule or ~11.1–11.9 kJ/L are amongst the best performance to date considering the current state-of-the-art for plasma-based DRM for all types of plasma. The conversion is in the range of ~46–49% and ~55–67% for CO2 and CH4, respectively, producing primarily syngas (i.e., H2 and CO) with H2/CO ratios of ~0.6–1 at CH4 fractions ranging from 30% to 45%. Water is the largest byproduct with levels ranging ~7–14% in the exhaust. Carbon particles visibly impact the plasma at higher CH4 fractions (> 30%), where they become heated and incandescent. Particle luminosity increases with increasing CH4 fractions, with the plasma becoming unstable near a 1:1 mixture (i.e., > 45% CH4). Electron microscopy of the carbon material reveals an agglomerated morphology of pure carbon nanoparticles. The mean particle size is determined as ~20 nm, free of any metal contamination, consistent with the electrode-less MW design. |
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001065310000001 |
Publication Date |
2023-08-10 |
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ISSN |
2212-9820 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7.7 |
Times cited |
6 |
Open Access |
OpenAccess |
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Notes |
We acknowledge financial support by a European Space Agency (ESA) Open Science Innovation Platform study (contract no. 4000137001/21/NL/GLC/ov), the European Marie Skłodowska-Curie Individual Fellowship ‘‘PENFIX’’ within Horizon 2020 (grant no. 838181), the European Research Council (ERC) under the European Union’s Horizon 2020 Research and Innovation Program (grant no. 810182; SCOPE ERC Synergy project), the Excellence of Science FWOFNRS PLASyntH2 project (FWO grant no. G0I1822N and EOS no. 4000751) and the Methusalem project of the University of Antwerp |
Approved |
Most recent IF: 7.7; 2023 IF: 4.292 |
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Call Number |
PLASMANT @ plasmant @c:irua:198155 |
Serial |
8807 |
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Author |
Ndayirinde, C.; Gorbanev, Y.; Ciocarlan, R.-G.; De Meyer, R.; Smets, A.; Vlasov, E.; Bals, S.; Cool, P.; Bogaerts, A. |
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Title |
Plasma-catalytic ammonia synthesis : packed catalysts act as plasma modifiers |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Catalysis today |
Abbreviated Journal |
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Volume |
419 |
Issue |
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Pages |
114156-12 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
We studied the plasma-catalytic production of NH3 from H2 and N2 in a dielectric barrier discharge plasma reactor using five different Co-based catalysts supported on Al2O3, namely Co/Al2O3, CoCe/Al2O3, CoLa/Al2O3, CoCeLa/Al2O3 and CoCeMg/Al2O3. The catalysts were characterized via several techniques, including SEM-EDX, and their performance was compared. The best performing catalyst was found to be CoLa/Al2O3, but the dif-ferences in NH3 concentration, energy consumption and production rate between the different catalysts were limited under the same conditions (i.e. feed gas, flow rate and ratio, and applied power). At the same time, the plasma properties, such as the plasma power and current profile, varied significantly depending on the catalyst. Taken together, these findings suggest that in the production of NH3 by plasma catalysis, our catalysts act as plasma modifiers, i.e., they change the discharge properties and hence the gas phase plasma chemistry. Importantly, this effect dominates over the direct catalytic effect (as e.g. in thermal catalysis) defined by the chemistry on the catalyst surface. |
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000987221300001 |
Publication Date |
2023-04-10 |
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ISSN |
0920-5861 |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
5.3 |
Times cited |
3 |
Open Access |
OpenAccess |
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Notes |
This research was supported by the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation programme (grant agreement No 810182 – SCOPE ERC Synergy project) and the Methusalem project of the University of Antwerp. We also gratefully acknowledge the NH3-TPD analysis performed by Sander Bossier. |
Approved |
Most recent IF: 5.3; 2023 IF: 4.636 |
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Call Number |
UA @ admin @ c:irua:197268 |
Serial |
8917 |
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Grünewald, L.; Chezganov, D.; De Meyer, R.; Orekhov, A.; Van Aert, S.; Bogaerts, A.; Bals, S.; Verbeeck, J. |
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Title |
In Situ Plasma Studies Using a Direct Current Microplasma in a Scanning Electron Microscope |
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A1 Journal article |
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Year |
2024 |
Publication |
Advanced Materials Technologies |
Abbreviated Journal |
Adv Materials Technologies |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Microplasmas can be used for a wide range of technological applications and to improve the understanding of fundamental physics. Scanning electron microscopy, on the other hand, provides insights into the sample morphology and chemistry of materials from the mm‐ down to the nm‐scale. Combining both would provide direct insight into plasma‐sample interactions in real‐time and at high spatial resolution. Up till now, very few attempts in this direction have been made, and significant challenges remain. This work presents a stable direct current glow discharge microplasma setup built inside a scanning electron microscope. The experimental setup is capable of real‐time in situ imaging of the sample evolution during plasma operation and it demonstrates localized sputtering and sample oxidation. Further, the experimental parameters such as varying gas mixtures, electrode polarity, and field strength are explored and experimental<italic>V</italic>–<italic>I</italic>curves under various conditions are provided. These results demonstrate the capabilities of this setup in potential investigations of plasma physics, plasma‐surface interactions, and materials science and its practical applications. The presented setup shows the potential to have several technological applications, for example, to locally modify the sample surface (e.g., local oxidation and ion implantation for nanotechnology applications) on the µm‐scale. |
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001168639900001 |
Publication Date |
2024-02-25 |
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ISSN |
2365-709X |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
6.8 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
L.G., S.B., and J.V. acknowledge support from the iBOF-21-085 PERsist research fund. D.C., S.V.A., and J.V. acknowledge funding from a TOPBOF project of the University of Antwerp (FFB 170366). R.D.M., A.B., and J.V. acknowledge funding from the Methusalem project of the University of Antwerp (FFB 15001A, FFB 15001C). A.O. and J.V. acknowledge funding from the Research Foundation Flanders (FWO, Belgium) project SBO S000121N. |
Approved |
Most recent IF: 6.8; 2024 IF: NA |
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EMAT @ emat @c:irua:204363 |
Serial |
8995 |
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Grünewald, L.; Chezganov, D.; De Meyer, R.; Orekhov, A.; Van Aert, S.; Bogaerts, A.; Bals, S.; Verbeeck, J. |
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Supplementary Information for “In-situ Plasma Studies using a Direct Current Microplasma in a Scanning Electron Microscope” |
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2023 |
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Dataset; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Supplementary information for the article “In-situ Plasma Studies using a Direct Current Microplasma in a Scanning Electron Microscope” containing the videos of in-situ SEM imaging (mp4 files), raw data/images, and Jupyter notebooks (ipynb files) for data treatment and plots. Link to the preprint: https://doi.org/10.48550/arXiv.2308.15123 Explanation of the data files can be found in the Information.pdf file. The Videos folder contains the in-situ SEM image series mentioned in the paper. If there are any questions/bugs, feel free to contact me at lukas.grunewaldatuantwerpen.be |
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Most recent IF: NA |
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Call Number |
UA @ admin @ c:irua:203389 |
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9100 |
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Author |
De Meyer, R.; Gorbanev, Y.; Ciocarlan, R.-G.; Cool, P.; Bals, S.; Bogaerts, A. |
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Title |
Importance of plasma discharge characteristics in plasma catalysis: Dry reforming of methane vs. ammonia synthesis |
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A1 Journal article |
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Year |
2024 |
Publication |
Chemical engineering journal |
Abbreviated Journal |
Chemical Engineering Journal |
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Volume |
488 |
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Pages |
150838 |
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A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
Plasma catalysis is a rapidly growing field, often employing a packed-bed dielectric barrier discharge plasma reactor. Such dielectric barrier discharges are complex, especially when a packing material (e.g., a catalyst) is introduced in the discharge volume. Catalysts are known to affect the plasma discharge, though the underlying mechanisms influencing the plasma physics are not fully understood. Moreover, the effect of the catalysts on the plasma discharge and its subsequent effect on the overall performance is often overlooked. In this work, we deliberately design and synthesize catalysts to affect the plasma discharge in different ways. These Ni or Co alumina-based catalysts are used in plasma-catalytic dry reforming of methane and ammonia synthesis. Our work shows that introducing a metal to the dielectric packing can affect the plasma discharge, and that the distribution of the metal is crucial in this regard. Further, the altered discharge can greatly influence the overall performance. In an atmospheric pressure dielectric barrier discharge reactor, this apparently more uniform plasma yields a significantly better performance for ammonia synthesis compared to the more conventional filamentary discharge, while it underperforms in dry reforming of methane. This study stresses the importance of analyzing the plasma discharge in plasma catalysis experiments. We hope this work encourages a more critical view on the plasma discharge characteristics when studying various catalysts in a plasma reactor. |
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001221606600001 |
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2024-03-30 |
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1385-8947 |
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UA library record; WoS full record |
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Impact Factor |
15.1 |
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Notes |
This research was supported through long-term structural funding (Methusalem FFB15001C) and by the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme with grant agreement No 810182 (SCOPE ERC Synergy project) and with grant agreement No 815128 (REALNANO). We acknowledge the practical contribution of Senne Van Doorslaer. |
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Most recent IF: 15.1; 2024 IF: 6.216 |
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PLASMANT @ plasmant @c:irua:205154 |
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9115 |
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