Records |
Author |
Kummamuru, N.B.; Ciocarlan, R.-G.; Houlleberghs, M.; Martens, J.; Breynaert, E.; Verbruggen, S.W.; Cool, P.; Perreault, P. |
Title |
Surface modification of mesostructured cellular foam to enhance hydrogen storage in binary THF/H₂ clathrate hydrate |
Type |
A1 Journal article |
Year |
2024 |
Publication ![sorted by Publication field, descending order (down)](img/sort_desc.gif) |
Sustainable energy & fuels |
Abbreviated Journal |
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Volume |
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Issue |
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Pages |
1-15 |
Keywords |
A1 Journal article; Engineering sciences. Technology; Laboratory of adsorption and catalysis (LADCA) |
Abstract |
This study introduces solid-state tuning of a mesostructured cellular foam (MCF) to enhance hydrogen (H-2) storage in clathrate hydrates. Grafting of promoter-like molecules (e.g., tetrahydrofuran) at the internal surface of the MCF resulted in a substantial improvement in the kinetics of formation of binary H-2-THF clathrate hydrate. Identification of the confined hydrate as sII clathrate hydrate and enclathration of H-2 in its small cages was performed using XRD and high-pressure H-1 NMR spectroscopy respectively. Experimental findings show that modified MCF materials exhibit a similar to 1.3 times higher H-2 storage capacity as compared to non-modified MCF under the same conditions (7 MPa, 265 K, 100% pore volume saturation with a 5.56 mol% THF solution). The enhancement in H-2 storage is attributed to the hydrophobicity originating from grafting organic molecules onto pristine MCF, thereby influencing water interactions and fostering an environment conducive to H-2 enclathration. Gas uptake curves indicate an optimal tuning point for higher H-2 storage, favoring a lower density of carbon per nm(2). Furthermore, a direct correlation emerges between higher driving forces and increased H-2 storage capacity, culminating at 0.52 wt% (46.77 mmoles of H-2 per mole of H2O and 39.78% water-to-hydrate conversions) at 262 K for the modified MCF material with fewer carbons per nm(2). Notably, the substantial H-2 storage capacity achieved without energy-intensive processes underscores solid-state tuning's potential for H-2 storage in the synthesized hydrates. This study evaluated two distinct kinetic models to describe hydrate growth in MCF. The multistage kinetic model showed better predictive capabilities for experimental data and maintained a low average absolute deviation. This research provides valuable insights into augmenting H-2 storage capabilities and holds promising implications for future advancements. |
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Wos |
001208396000001 |
Publication Date |
2024-04-15 |
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 |
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ISBN |
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Additional Links |
UA library record; WoS full record |
Impact Factor |
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Times cited |
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Open Access |
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Notes |
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Approved |
Most recent IF: NA |
Call Number |
UA @ admin @ c:irua:205764 |
Serial |
9232 |
Permanent link to this record |
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Author |
Kelly, S.; Mercer, E.; De Meyer, R.; Ciocarlan, R.-G.; Bals, S.; Bogaerts, A. |
Title |
Microwave plasma-based dry reforming of methane: Reaction performance and carbon formation |
Type |
A1 Journal article |
Year |
2023 |
Publication ![sorted by Publication field, descending order (down)](img/sort_desc.gif) |
Journal of CO2 utilization |
Abbreviated Journal |
Journal of CO2 Utilization |
Volume |
75 |
Issue |
|
Pages |
102564 |
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) |
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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Place of Publication |
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Language |
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Wos |
001065310000001 |
Publication Date |
2023-08-10 |
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 |
2212-9820 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
7.7 |
Times cited |
6 |
Open Access |
OpenAccess |
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 |
Call Number |
PLASMANT @ plasmant @c:irua:198155 |
Serial |
8807 |
Permanent link to this record |
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Author |
Ciocarlan, R.-G.; Seftel, E.M.; Gavrila, R.; Suchea, M.; Batuk, M.; Mertens, M.; Hadermann, J.; Cool, P. |
Title |
Spinel nanoparticles on stick-like Freudenbergite nanocomposites as effective smart-removal photocatalysts for the degradation of organic pollutants under visible light |
Type |
A1 Journal article |
Year |
2020 |
Publication ![sorted by Publication field, descending order (down)](img/sort_desc.gif) |
Journal Of Alloys And Compounds |
Abbreviated Journal |
J Alloy Compd |
Volume |
820 |
Issue |
|
Pages |
153403 |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA) |
Abstract |
A series of mixed nanocomposite materials was synthetized, containing a Ferrite phase type Zn1-xNixFe2O4 and a Freudenbergite phase type Na2Fe2Ti6O16, where x = 0; 0.2; 0.4; 0.6; 0.8; 1. The choice for this combination is based on the good adsorption properties of Freudenbergite for dye molecules, and the small bandgap energy of Ferrite spinel, allowing activation of the catalysts under visible light irradiation. A two steps synthesis protocol was used to obtain the smart-removal nanocomposites. Firstly, the spinel structure was obtained via the co-precipitation route followed by the addition of the Ti-source and formation of the Freudenbergite system. The role of cations on the formation mechanism and an interesting interchange of cations between spinel and Freudenbergite structures was clarified by a TEM study. Part of the Ti4+ penetrated the spinel structure and, at the same time, part of the Fe3+ formed the Freudenbergite system. The photocatalytic activity was studied under visible light, reaching for the best catalysts a 67% and 40% mineralization degree for methylene blue and rhodamine 6G respectively, after 6 h of irradiation. In the same conditions, the well-known commercial P25 (Degussa) managed to mineralize only 12% and 3% of methylene blue and rhodamine 6G, respectively. Due to the remarkable magnetic properties of Ferrites, a convenient recovery and reuse of the catalysts is possible after the photocatalytic tests. Based on the excellent catalytic performance of the nanocomposites under visible light and their ease of separation out of the solution after the catalytic reaction, the newly developed composite catalysts are considered very effective for wastewater treatment. |
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Place of Publication |
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Editor |
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Language |
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Wos |
000507854700130 |
Publication Date |
2019-12-15 |
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 |
0925-8388 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
6.2 |
Times cited |
|
Open Access |
OpenAccess |
Notes |
The authors acknowledge the FWO-Flanders (project nr. G038215N) for financial support. |
Approved |
Most recent IF: 6.2; 2020 IF: 3.133 |
Call Number |
EMAT @ emat @c:irua:166447 |
Serial |
6342 |
Permanent link to this record |
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Author |
Kummamuru, N.B.; Watson, G.; Ciocarlan, R.-G.; Verbruggen, S.W.; Cool, P.; Van Der Voort, P.; Perreault, P. |
Title |
Accelerated methane storage in clathrate hydrates using mesoporous (Organo-) silica materials |
Type |
A1 Journal article |
Year |
2023 |
Publication ![sorted by Publication field, descending order (down)](img/sort_desc.gif) |
Fuel |
Abbreviated Journal |
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Volume |
354 |
Issue |
|
Pages |
129403-129418 |
Keywords |
A1 Journal article; Engineering sciences. Technology; Laboratory of adsorption and catalysis (LADCA) |
Abstract |
Methane (CH4) clathrate hydrates have gained much attention in the ever-growing search for novel energy storage methods; however, they are currently limited due to their poor water-to-hydrate conversions and slow formation kinetics. To surmount these bottlenecks, significant research has been centered on the design of novel methods (porous media). In this vein, the present work explores two hydrophobic mesoporous solids, an alkyl-grafted mesoporous silica (SBA-15 C8) and a periodic mesoporous organosilica (Ring-PMO), in their ability to promote CH4 clathrates. Both materials have shown to facilitate CH4 clathrate formation at mild operating conditions (6 MPa and 269–276 K). The study revealed that the maximal CH4 storage capacities are strongly linked to the critical/optimal quantity of water in the system which was determined to be at 130% and 200% of the pore volume for SBA-15 C8 and Ring-PMO, respectively. Up to 90% and 95% of the maximum water-to-hydrate conversions were achieved in 90 min at the lowest experimental temperature and critical water content for SBA-15 C8 and Ring-PMO, respectively. At these conditions, SBA-15 C8 and Ring-PMO showed a maximum gas uptake of 98.2 and 101.2 mmol CH4/mol H2O, respectively. Both the materials exhibited no chemical or morphological changes post-clathrate formations (characterized using FT-IR, N2 sorption, XRD, and TEM), inferring their viability as clathrate promoters for multiple cycles. An integrated multistep model was considered adequate for representing the hydrate crystallization kinetics and fits well with the experimental kinetic data with a low average absolute deviation in water-to-hydrate conversions among the three distinct kinetic models analyzed. Overall, the results from this study demonstrate hydrophobic porous materials as effective promoters of CH4 clathrates, which could make clathrate-based CH4 storage and transport technology industrially viable. |
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Place of Publication |
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Language |
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Wos |
001059413200001 |
Publication Date |
2023-08-07 |
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 |
0016-2361 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
7.4 |
Times cited |
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Open Access |
Not_Open_Access: Available from 07.02.2024 |
Notes |
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Approved |
Most recent IF: 7.4; 2023 IF: 4.601 |
Call Number |
UA @ admin @ c:irua:197987 |
Serial |
8829 |
Permanent link to this record |
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Author |
Gupta, A.; Baron, G.V.; Perreault, P.; Lenaerts, S.; Ciocarlan, R.-G.; Cool, P.; Mileo, P.G.M.; Rogge, S.; Van Speybroeck, V.; Watson, G.; Van Der Voort, P.; Houlleberghs, M.; Breynaert, E.; Martens, J.; Denayer, J.F.M. |
Title |
Hydrogen clathrates : next generation hydrogen storage materials |
Type |
A1 Journal article |
Year |
2021 |
Publication ![sorted by Publication field, descending order (down)](img/sort_desc.gif) |
Energy Storage Materials |
Abbreviated Journal |
|
Volume |
41 |
Issue |
|
Pages |
69-107 |
Keywords |
A1 Journal article; Engineering sciences. Technology; Laboratory of adsorption and catalysis (LADCA); Sustainable Energy, Air and Water Technology (DuEL) |
Abstract |
Extensive research has been carried on the molecular adsorption in high surface area materials such as carbonaceous materials and MOFs as well as atomic bonded hydrogen in metals and alloys. Clathrates stand among the ones to be recently suggested for hydrogen storage. Although, the simulations predict lower capacity than the expected by the DOE norms, the additional benefits of clathrates such as low production and operational cost, fully reversible reaction, environmentally benign nature, low risk of flammability make them one of the most promising materials to be explored in the next decade. The inherent ability to tailor the properties of clathrates using techniques such as addition of promoter molecules, use of porous supports and formation of novel reverse micelles morphology provide immense scope customisation and growth. As rapidly evolving materials, clathrates promise to get as close as possible in the search of “holy grail” of hydrogen storage. This review aims to provide the audience with the background of the current developments in the solid-state hydrogen storage materials, with a special focus on the hydrogen clathrates. The in-depth analysis of the hydrogen clathrates will be provided beginning from their discovery, various additives utilised to enhance their thermodynamic and kinetic properties, challenges in the characterisation of hydrogen in clathrates, theoretical developments to justify the experimental findings and the upscaling opportunities presented by this system. The review will present state of the art in the field and also provide a global picture for the path forward. |
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Wos |
000685118300009 |
Publication Date |
2021-06-08 |
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 |
2405-8297 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
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Times cited |
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Open Access |
OpenAccess |
Notes |
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Approved |
Most recent IF: NA |
Call Number |
UA @ admin @ c:irua:178744 |
Serial |
8045 |
Permanent link to this record |
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Author |
Ciocarlan, R.-G.; Blommaerts, N.; Lenaerts, S.; Cool, P.; Verbruggen, S.W. |
Title |
Recent trends in plasmon‐assisted photocatalytic CO₂ reduction |
Type |
A1 Journal article |
Year |
2023 |
Publication ![sorted by Publication field, descending order (down)](img/sort_desc.gif) |
Chemsuschem |
Abbreviated Journal |
|
Volume |
16 |
Issue |
5 |
Pages |
e202201647-25 |
Keywords |
A1 Journal article; Engineering sciences. Technology; Laboratory of adsorption and catalysis (LADCA) |
Abstract |
Direct photocatalytic reduction of CO2 has become an highly active field of research. It is thus of utmost importance to maintain an overview of the various materials used to sustain this process, find common trends, and, in this way, eventually improve the current conversions and selectivities. In particular, CO2 photoreduction using plasmonic photocatalysts under solar light has gained tremendous attention, and a wide variety of materials has been developed to reduce CO2 towards more practical gases or liquid fuels (CH4, CO, CH3OH/CH3CH2OH) in this manner. This Review therefore aims at providing insights in current developments of photocatalysts consisting of only plasmonic nanoparticles and semiconductor materials. By classifying recent studies based on product selectivity, this Review aims to unravel common trends that can provide effective information on ways to improve the photoreduction yield or possible means to shift the selectivity towards desired products, thus generating new ideas for the way forward. |
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Publisher |
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Place of Publication |
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Language |
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Wos |
000926901300001 |
Publication Date |
2023-01-10 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1864-5631 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
8.4 |
Times cited |
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Open Access |
OpenAccess |
Notes |
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Approved |
Most recent IF: 8.4; 2023 IF: 7.226 |
Call Number |
UA @ admin @ c:irua:193633 |
Serial |
7335 |
Permanent link to this record |
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Author |
De Meyer, R.; Gorbanev, Y.; Ciocarlan, R.-G.; Cool, P.; Bals, S.; Bogaerts, A. |
Title |
Importance of plasma discharge characteristics in plasma catalysis: Dry reforming of methane vs. ammonia synthesis |
Type |
A1 Journal Article |
Year |
2024 |
Publication ![sorted by Publication field, descending order (down)](img/sort_desc.gif) |
Chemical Engineering Journal |
Abbreviated Journal |
Chemical Engineering Journal |
Volume |
488 |
Issue |
|
Pages |
150838 |
Keywords |
A1 Journal Article; Gas conversion Dry reforming of methane Ammonia Microdischarges Dielectric barrier discharge; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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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Publisher |
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Place of Publication |
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Language |
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Wos |
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Publication Date |
2024-03-30 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1385-8947 |
ISBN |
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Additional Links |
UA library record |
Impact Factor |
15.1 |
Times cited |
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Open Access |
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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. |
Approved |
Most recent IF: 15.1; 2024 IF: 6.216 |
Call Number |
PLASMANT @ plasmant @c:irua:205154 |
Serial |
9115 |
Permanent link to this record |
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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. |
Title |
Plasma-catalytic ammonia synthesis : packed catalysts act as plasma modifiers |
Type |
A1 Journal article |
Year |
2023 |
Publication ![sorted by Publication field, descending order (down)](img/sort_desc.gif) |
Catalysis today |
Abbreviated Journal |
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Volume |
419 |
Issue |
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Pages |
114156-12 |
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) |
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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Thesis |
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Publisher |
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Place of Publication |
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Language |
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Wos |
000987221300001 |
Publication Date |
2023-04-10 |
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 |
0920-5861 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
5.3 |
Times cited |
3 |
Open Access |
OpenAccess |
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 |
Call Number |
UA @ admin @ c:irua:197268 |
Serial |
8917 |
Permanent link to this record |
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Author |
Van Everbroeck, T.; Wu, J.; Arenas-Esteban, D.; Ciocarlan, R.-G.; Mertens, M.; Bals, S.; Dujardin, C.; Granger, P.; Seftel, E.M.; Cool, P. |
Title |
ZnAl layered double hydroxide based catalysts (with Cu, Mn, Ti) used as noble metal-free three-way catalysts |
Type |
A1 Journal article |
Year |
2022 |
Publication ![sorted by Publication field, descending order (down)](img/sort_desc.gif) |
Applied clay science |
Abbreviated Journal |
Appl Clay Sci |
Volume |
217 |
Issue |
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Pages |
106390 |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA) |
Abstract |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000795870100004 |
Publication Date |
2022-01-02 |
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 |
0169-1317 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
5.6 |
Times cited |
6 |
Open Access |
OpenAccess |
Notes |
The authors acknowledge financial support by theEuropean Union’s Horizon 2020 Project Partial-PGMs (H2020-NMP-686086). R-G C. and P.C. acknowledge the FWO-Flanders (project no. G038215N) for financial support. S⋅B and D.A.E thank the financial support of the European Research Council (ERC-CoG-2019 815128). The authors are grateful to Johnson Matthey, UK, for supplying the commercial benchmark catalysts; realnano; sygmaSB |
Approved |
Most recent IF: 5.6 |
Call Number |
EMAT @ emat @c:irua:186956 |
Serial |
6955 |
Permanent link to this record |
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Author |
Asapu, R.; Claes, N.; Ciocarlan, R.-G.; Minjauw, M.; Detavernier, C.; Cool, P.; Bals, S.; Verbruggen, S.W. |
Title |
Electron Transfer and Near-Field Mechanisms in Plasmonic Gold-Nanoparticle-Modified TiO2Photocatalytic Systems |
Type |
A1 Journal article |
Year |
2019 |
Publication ![sorted by Publication field, descending order (down)](img/sort_desc.gif) |
ACS applied nano materials |
Abbreviated Journal |
ACS Appl. Nano Mater. |
Volume |
2 |
Issue |
2 |
Pages |
4067-4074 |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Sustainable Energy, Air and Water Technology (DuEL) |
Abstract |
The major mechanism responsible for plasmonic enhancement of titanium dioxide photocatalysis using gold nanoparticles is still under contention. This work introduces an experimental strategy to disentangle the significance of the charge transfer and near-field mechanisms in plasmonic photocatalysis. By controlling the thickness and conductive nature of a nanoparticle shell that acts as a spacer layer separating the plasmonic metal core from the TiO2 surface, field enhancement or charge transfer effects can be selectively repressed or evoked. Layer-by-layer and in situ polymerization methods are used to synthesize gold core–polymer shell nanoparticles with shell thickness control up to the sub-nanometer level. Detailed optical and electrical characterization supported by near-field simulation models corroborate the trends in photocatalytic activity of the different systems. This approach mainly points at an important contribution of the enhanced near field. |
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Place of Publication |
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Language |
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Wos |
000477917700006 |
Publication Date |
2019-05-31 |
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 |
2574-0970 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
|
Times cited |
32 |
Open Access |
OpenAccess |
Notes |
This work was supported by Research Foundation Flanders (FWO). P.C. and R-G.C. acknowledge financial support from FWO (Project No. G038215N). N.C. and S.B. acknowledge financial support from the European Research Council (ERC Starting Grant No. 335078-COLOURATOM). |
Approved |
Most recent IF: NA |
Call Number |
EMAT @ emat @UA @ admin @ c:irua:160579 |
Serial |
5184 |
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Author |
Pacquets, L.; Van den Hoek, J.; Arenas Esteban, D.; Ciocarlan, R.-G.; Cool, P.; Baert, K.; Hauffman, T.; Daems, N.; Bals, S.; Breugelmans, T. |
Title |
Use of nanoscale carbon layers on Ag-based gas diffusion electrodes to promote CO production |
Type |
A1 Journal article |
Year |
2022 |
Publication ![sorted by Publication field, descending order (down)](img/sort_desc.gif) |
ACS applied nano materials |
Abbreviated Journal |
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Volume |
5 |
Issue |
6 |
Pages |
7723-7732 |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Applied Electrochemistry & Catalysis (ELCAT) |
Abstract |
A promising strategy for the inhibition of the hydrogen evolution reaction along with the stabilization of the electrocatalyst in electrochemical CO2 reduction cells involves the application of a nanoscale amorphous carbon layer on top of the active catalyst layer in a gas diffusion electrode. Without modifying the chemical nature of the electrocatalyst itself, these amorphous carbon layers lead to the stabilization of the electrocatalyst, and a significant improvement with respect to the inhibition of the hydrogen evolution reaction was also obtained. The faradaic efficiencies of hydrogen could be reduced from 31.4 to 2.1% after 1 h of electrolysis with a 5 nm thick carbon layer. Furthermore, the impact of the carbon layer thickness (5–30 nm) on this inhibiting effect was investigated. We determined an optimal thickness of 15 nm where the hydrogen evolution reaction was inhibited and a decent stability was obtained. Next, a thickness of 15 nm was selected for durability measurements. Interestingly, these durability measurements revealed the beneficial impact of the carbon layer already after 6 h by suppressing the hydrogen evolution such that an increase of only 37.9% exists compared to 56.9% without the use of an additional carbon layer, which is an improvement of 150%. Since carbon is only applied afterward, it reveals its great potential in terms of electrocatalysis in general. |
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Wos |
000818507900001 |
Publication Date |
2022-05-19 |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2574-0970 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
5.9 |
Times cited |
3 |
Open Access |
OpenAccess |
Notes |
L.P. was supported through a Ph.D. fellowship strategic basic research (1S56920N) of the Research Foundation-Flanders (FWO). S.B. acknowledges financial support from ERC Consolidator Grant Number 815128 REALNANO. This research was financed by the Research Council of the University of Antwerp (BOF-GOA 33928). P.C. and R.-G.C. acknowledge financial support by FWO Flanders (project no. G038215N). The authors recognize the contribution of S. Pourbabak and T. Derez for the assistance with the Ag and carbon coating, Indah Prihatiningtyas and Bart Van der Bruggen for the assistance with the contact angle measurements, Daniel Choukroun for the use of the in-house-made hybrid flow cell, and Stijn Van den Broeck for his assistance with the FIB measurements. |
Approved |
Most recent IF: 5.9 |
Call Number |
UA @ admin @ c:irua:188887 |
Serial |
7099 |
Permanent link to this record |
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Author |
Asapu, R.; Ciocarlan, R.-G.; Claes, N.; Blommaerts, N.; Minjauw, M.; Ahmad, T.; Dendooven, J.; Cool, P.; Bals, S.; Denys, S.; Detavernier, C.; Lenaerts, S.; Verbruggen, S.W. |
Title |
Plasmonic Near-Field Localization of Silver Core–Shell Nanoparticle Assemblies via Wet Chemistry Nanogap Engineering |
Type |
A1 Journal article |
Year |
2017 |
Publication ![sorted by Publication field, descending order (down)](img/sort_desc.gif) |
ACS applied materials and interfaces |
Abbreviated Journal |
Acs Appl Mater Inter |
Volume |
9 |
Issue |
9 |
Pages |
41577-41585 |
Keywords |
A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL) |
Abstract |
Silver nanoparticles are widely used in the field of plasmonics because of their unique optical properties. The wavelength-dependent surface plasmon resonance gives rise to a strongly enhanced electromagnetic field, especially at so-called hot spots located in the nanogap in-between metal nanoparticle assemblies. Therefore, the interparticle distance is a decisive factor in plasmonic applications, such as surface-enhanced Raman spectroscopy (SERS). In this study, the aim is to engineer this interparticle distance for silver nanospheres using a convenient wet-chemical approach and to predict and quantify the corresponding enhancement factor using both theoretical and experimental tools. This was done by building a tunable ultrathin polymer shell around the nanoparticles using the layer-by-layer method, in which the polymer shell acts as the separating interparticle spacer layer. Comparison of different theoretical approaches and corroborating the results with SERS analytical experiments using silver and silver−polymer core−shell nanoparticle clusters as SERS substrates was also done. Herewith, an approach is provided to estimate the extent of plasmonic near-field enhancement both theoretically as well as experimentally. |
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Wos |
000417005900057 |
Publication Date |
2017-11-29 |
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 |
1944-8244 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
7.504 |
Times cited |
29 |
Open Access |
OpenAccess |
Notes |
financial support through a research fellowship. C.D. wishes to thank the Hercules foundation for the financial support (SPINAL). P.C. and R.-G.C. acknowledge financial support by FWO Vlaanderen (project no. G038215N). N.C. and S.B. acknowledge the financial support from the European Research Council (ERC starting grant #335078-COLOURATOM). (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); saraecas; ECAS_Sara; |
Approved |
Most recent IF: 7.504 |
Call Number |
EMAT @ emat @c:irua:147243 |
Serial |
4804 |
Permanent link to this record |