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Author |
Wang, J.; Zhang, K.; Mertens, M.; Bogaerts, A.; Meynen, V. |
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Title |
Plasma-based dry reforming of methane in a dielectric barrier discharge reactor: Importance of uniform (sub)micron packings/catalysts to enhance the performance |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
APPLIED CATALYSIS B-ENVIRONMENTAL |
Abbreviated Journal |
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Volume |
337 |
Issue |
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Pages |
122977 |
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Keywords |
A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
This study presents new insights on the effect of (sub)micrometer particle sized materials in plasma-based CO2-
CH4 reforming by investigating the performance of SiO2 spheres (with/without supported metal) of varying
particle sizes. (Sub)micron particles synthesized through the St¨ober method were used instead of (sub)millimeter
particles employed in previous studies. Increasing particle size (from 120 nm to 2390 nm) was found to first
increase and then decrease conversion and energy yield, with optimal performance achieved using 740 nm 5 wt%
Ni loaded SiO2, which improved CO2 and CH4 conversion, and energy yield to 44%, 55%, and 0.271 mmol/kJ,
respectively, compared to 20%, 27%, and 0.116 mmol/kJ in an empty reactor at the same flow rate. This is the
first to achieve significant performance improvement in a fully packed reactor, highlighting the importance of
selecting a suitable particle size. The findings can offer guidance towards rational design of catalysts for plasmabased
reactions. |
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Wos |
001056527600001 |
Publication Date |
2023-06-09 |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0926-3373 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
22.1 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
This work is supported by the China Scholarship Council (No. 201806060123); and the VLAIO Catalisti transition project CO2PERATE (HBC.2017.0692). K.Z acknowledges the EASiCHEM project funded by the Flemish Strategic Basic Research Program of the Catalisti cluster and Flanders Innovation & Entrepreneurship (HBC.2018.0484). |
Approved |
Most recent IF: 22.1; 2023 IF: 9.446 |
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Call Number |
PLASMANT @ plasmant @c:irua:196955 |
Serial |
8798 |
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Permanent link to this record |
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Author |
Vertongen, R.; Bogaerts, A. |
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Title |
How important is reactor design for CO2 conversion in warm plasmas? |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
Journal of CO2 Utilization |
Abbreviated Journal |
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Volume |
72 |
Issue |
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Pages |
102510 |
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Keywords |
A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
In this work, we evaluated several new electrode configurations for CO2 conversion in a gliding arc plasmatron
(GAP) reactor. Although the reactor design influences the performance, the best results give only slightly higher
CO2 conversion than the basic GAP reactor design, which indicates that this reactor may have reached its performance
limits. Moreover, we compared our results to those of four completely different plasma reactors, also
operating at atmospheric pressure and with contact between the plasma and the electrodes. Surprisingly, the
performance of all these warm plasmas is very similar (CO2 conversion around 10 % for an energy efficiency
around 30 %). In view of these apparent performance limits regarding the reactor design, we believe further
improvements should focus on other aspects, such as the post-plasma-region where the implementation of
nozzles or a carbon bed are promising. We summarize the performance of our GAP reactor by comparing the
energy efficiency and CO2 conversion for all different plasma reactors reported in literature. We can conclude
that the GAP is not the best plasma reactor, but its operation at atmospheric pressure makes it appealing for
industrial application. We believe that future efforts should focus on process design, techno-economic assessments
and large-scale demonstrations: these will be crucial to assess the real industrial potential of this warm
plasma technology |
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Wos |
001024970900001 |
Publication Date |
2023-06-16 |
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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 |
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Impact Factor |
7.7 |
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) and the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreements No 810182 – SCOPE ERC Synergy project and No. 101081162 — “PREPARE” ERC Proof of Concept project). We also thank I. Tsonev, P. Heirman, F. Girard-Sahun and G. Trenchev for the interesting discussions and practical help with the experiments, as well as J. Creel for his ideas on the inserted anode designs. |
Approved |
Most recent IF: 7.7; 2023 IF: 4.292 |
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Call Number |
PLASMANT @ plasmant @c:irua:197044 |
Serial |
8799 |
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Permanent link to this record |
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Author |
Adhami Sayad Mahaleh, M.; Narimisa, M.; Nikiforov, A.; Gromov, M.; Gorbanev, Y.; Bitar, R.; Morent, R.; De Geyter, N. |
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Title |
Nitrogen Oxidation in a Multi-Pin Plasma System in the Presence and Absence of a Plasma/Liquid Interface |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
Applied Sciences |
Abbreviated Journal |
Applied Sciences |
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Volume |
13 |
Issue |
13 |
Pages |
7619 |
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Keywords |
A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
The recent energy crisis revealed that there is a strong need to replace hydrocarbon-fueled industrial nitrogen fixation processes by alternative, more sustainable methods. In light of this, plasma-based nitrogen fixation remains one of the most promising options, considering both theoretical and experimental aspects. Lately, plasma interacting with water has received considerable attention in nitrogen fixation applications as it can trigger a unique gas- and liquid-phase chemistry. Within this context, a critical exploration of plasma-assisted nitrogen fixation with or without water presence is of great interest with an emphasis on energy costs, particularly in plasma reactors which have potential for large-scale industrial application. In this work, the presence of water in a multi-pin plasma system on nitrogen oxidation is experimentally investigated by comparing two pulsed negative DC voltage plasmas in metal–metal and metal–liquid electrode configurations. The plasma setups are designed to create similar plasma properties, including plasma power and discharge regime in both configurations. The system energy cost is calculated, considering nitrogen-containing species generated in gas and liquid phases as measured by a gas analyzer, nitrate sensor, and a colorimetry method. The energy cost profile as a function of specific energy input showed a strong dependency on the plasma operational frequency and the gas flow rate, as a result of different plasma operation regimes and initiated reverse processes. More importantly, the presence of the plasma/liquid interface increased the energy cost up to 14 ± 8%. Overall, the results showed that the presence of water in the reaction zone has a negative impact on the nitrogen fixation process. |
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Wos |
001031217300001 |
Publication Date |
2023-06-28 |
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Edition |
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ISSN |
2076-3417 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
2.7 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
NITROPLASM FWO-FNRS Excellence of Science, 30505023 ; European Union-NextGenerationEU, G0G2322N ; |
Approved |
Most recent IF: 2.7; 2023 IF: 1.679 |
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Call Number |
PLASMANT @ plasmant @c:irua:198153 |
Serial |
8802 |
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Permanent link to this record |
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Author |
Abduvokhidov, D.; Yusupov, M.; Shahzad, A.; Attri, P.; Shiratani, M.; Oliveira, M.C.; Razzokov, J. |
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Title |
Unraveling the Transport Properties of RONS across Nitro-Oxidized Membranes |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
Biomolecules |
Abbreviated Journal |
Biomolecules |
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Volume |
13 |
Issue |
7 |
Pages |
1043 |
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Keywords |
A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
The potential of cold atmospheric plasma (CAP) in biomedical applications has received significant interest, due to its ability to generate reactive oxygen and nitrogen species (RONS). Upon exposure to living cells, CAP triggers alterations in various cellular components, such as the cell membrane. However, the permeation of RONS across nitrated and oxidized membranes remains understudied. To address this gap, we conducted molecular dynamics simulations, to investigate the permeation capabilities of RONS across modified cell membranes. This computational study investigated the translocation processes of less hydrophilic and hydrophilic RONS across the phospholipid bilayer (PLB), with various degrees of oxidation and nitration, and elucidated the impact of RONS on PLB permeability. The simulation results showed that less hydrophilic species, i.e., NO, NO2, N2O4, and O3, have a higher penetration ability through nitro-oxidized PLB compared to hydrophilic RONS, i.e., HNO3, s-cis-HONO, s-trans-HONO, H2O2, HO2, and OH. In particular, nitro-oxidation of PLB, induced by, e.g., cold atmospheric plasma, has minimal impact on the penetration of free energy barriers of less hydrophilic species, while it lowers these barriers for hydrophilic RONS, thereby enhancing their translocation across nitro-oxidized PLB. This research contributes to a better understanding of the translocation abilities of RONS in the field of plasma biomedical applications and highlights the need for further analysis of their role in intracellular signaling pathways. |
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Wos |
001035160000001 |
Publication Date |
2023-06-27 |
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Abbreviated Series Title |
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Series Issue |
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Edition |
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ISSN |
2218-273X |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
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Times cited |
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Open Access |
Not_Open_Access |
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Notes |
This research was funded by the Innovative Development Agency of the Republic of Uzbekistan, grant number FZ-2020092817. |
Approved |
Most recent IF: NA |
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Call Number |
PLASMANT @ plasmant @c:irua:198154 |
Serial |
8803 |
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Permanent link to this record |
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Author |
Loenders, B.; Michiels, R.; Bogaerts, A. |
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Title |
Is a catalyst always beneficial in plasma catalysis? Insights from the many physical and chemical interactions |
Type |
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 |
85 |
Issue |
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Pages |
501-533 |
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Keywords |
A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
Plasma-catalytic dry reforming of CH4 (DRM) is promising to convert the greenhouse gasses CH4 and CO2 into value-added chemicals, thus simultaneously providing an alternative to fossil resources as feedstock for the chemical industry. However, while many experiments have been dedicated to plasma-catalytic DRM, there is no consensus yet in literature on the optimal choice of catalyst for targeted products, because the underlying mechanisms are far from understood. Indeed, plasma catalysis is very complex, as it encompasses various chemical and physical interactions between plasma and catalyst, which depend on many parameters. This complexity hampers the comparison of experimental results from different studies, which, in our opinion, is an important bottleneck in the further development of this promising research field. Hence, in this perspective paper, we describe the important physical and chemical effects that should be accounted for when designing plasma-catalytic experiments in general, highlighting the need for standardized experimental setups, as well as careful documentation of packing properties and reaction conditions, to further advance this research field. On the other hand, many parameters also create many windows of opportunity for further optimizing plasma-catalytic systems. Finally, various experiments also reveal the lack of improvement in plasma catalysis compared to plasma-only, specifically for DRM, but the underlying mechanisms are unclear. Therefore, we present our newly developed coupled plasma-surface kinetics model for DRM, to provide more insight in the underlying reasons. Our model illustrates that transition metal catalysts can adversely affect plasmacatalytic DRM, if radicals dominate the plasma-catalyst interactions. Thus, we demonstrate that a good understanding of the plasma-catalyst interactions is crucial to avoiding conditions at which these interactions negatively affect the results, and we provide some recommendations for improvement. For instance, we believe that plasma-catalytic DRM may benefit more from higher reaction temperatures, at which vibrational excitation can enhance the surface reactions. |
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Wos |
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Publication Date |
2023-06-30 |
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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 |
2095-4956 |
ISBN |
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Additional Links |
UA library record |
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Impact Factor |
13.1 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
This research was supported by the FWO-SBO project PlasMa- CatDESIGN (FWO grant ID S001619N), the FWO fellowship of R. Michiels (FWO grant ID 1114921N), 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). The 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: 13.1; 2023 IF: 2.594 |
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Call Number |
PLASMANT @ plasmant @c:irua:198159 |
Serial |
8806 |
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Author |
Vanraes, P.; Parayil Venugopalan, S.; Besemer, M.; Bogaerts, A. |
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Title |
Assessing neutral transport mechanisms in aspect ratio dependent etching by means of experiments and multiscale plasma modeling |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
Plasma Sources Science and Technology |
Abbreviated Journal |
Plasma Sources Sci. Technol. |
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Volume |
32 |
Issue |
6 |
Pages |
064004 |
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Keywords |
A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
Since the onset of pattern transfer technologies for chip manufacturing, various strategies have been developed to circumvent or overcome aspect ratio dependent etching (ARDE). These methods have, however, their own limitations in terms of etch non-idealities, throughput or costs. Moreover, they have mainly been optimized for individual in-device features and die-scale patterns, while occasionally ending up with poor patterning of metrology marks, affecting the alignment and overlay in lithography. Obtaining a better understanding of the underlying mechanisms of ARDE and how to mitigate them therefore remains a relevant challenge to date, for both marks and advanced nodes. In this work, we accordingly assessed the neutral transport mechanisms in ARDE by means of experiments and multiscale modeling for SiO<sub>2</sub>etching with CHF<sub>3</sub>/Ar and CF<sub>4</sub>/Ar plasmas. The experiments revealed a local maximum in the etch rate for an aspect ratio around unity, i.e. the simultaneous occurrence of regular and inverse reactive ion etching lag for a given etch condition. We were able to reproduce this ARDE trend in the simulations without taking into account charging effects and the polymer layer thickness, suggesting shadowing and diffuse reflection of neutrals as the primary underlying mechanisms. Subsequently, we explored four methods with the simulations to regulate ARDE, by varying the incident plasma species fluxes, the amount of polymer deposition, the ion energy and angular distribution and the initial hardmask sidewall angle, for which the latter was found to be promising in particular. Although our study focusses on feature dimensions characteristic to metrology marks and back-end-of-the-line integration, the obtained insights have a broader relevance, e.g. to the patterning of advanced nodes. Additionally, this work supports the insight that physisorption may be more important in plasma etching at room temperature than originally thought, in line with other recent studies, a topic on which we recommend further research. |
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Wos |
001021250100001 |
Publication Date |
2023-06-01 |
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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 |
0963-0252 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.8 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
P Vanraes acknowledges funding by ASML for the project ‘Computational simulation of plasma etching of trench structures’. P Vanraes and A Bogaerts want to express their gratitude to Mark J Kushner (University of Michigan) for the sharing of the HPEM and MCFPM codes, and for the interesting exchange of views. P Vanraes wishes to thank Violeta Georgieva and Stefan Tinck for the fruitful discussions on the HPEM code, Yu-Ru Zhang for an example of the CCP reactor code and Karel Venken for his technical help with the server maintenance and use. S P Venugopalan and M Besemer wish to thank Luigi Scaccabarozzi, Sander Wuister, Coen Verschuren, Michael Kubis, Kuan-Ming Chen, Ruben Maas, Huaichen Zhang and Julien Mailfert (ASML) for the insightful discussions. |
Approved |
Most recent IF: 3.8; 2023 IF: 3.302 |
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Call Number |
PLASMANT @ plasmant @c:irua:197760 |
Serial |
8811 |
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Permanent link to this record |
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Author |
Tampieri, F.; Gorbanev, Y.; Sardella, E. |
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Title |
Plasma‐treated liquids in medicine: Let's get chemical |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
Plasma Processes and Polymers |
Abbreviated Journal |
Plasma Processes & Polymers |
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Volume |
20 |
Issue |
9 |
Pages |
e2300077 |
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Keywords |
A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
Fundamental and applied research on plasma‐treated liquids for biomedical applications was boosted in the last few years, dictated by their advantages with respect to direct treatments. However, often, the lack of consistent analysis at a molecular level of these liquids, and of the processes used to produce them, have raised doubts of their usefulness in the clinic. The aim of this article is to critically discuss some basic aspects related to the use of plasma‐treated liquids in medicine, with a focus on their chemical composition. We analyze the main liquids used in the field, how they are affected by non‐thermal plasmas, and the possibility to replicate them without plasma treatment. |
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Wos |
001005060700001 |
Publication Date |
2023-06-08 |
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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 |
1612-8850 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.5 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
We thank COST Actions CA20114 (Therapeutical Applications of Cold Plasmas) and CA19110 (Plasma Applications for Smart and Sustainable Agriculture) for the stimulating environment provided. Francesco Tampieri wishes to thank Dr. Cristina Canal for the helpful discussion during the planning stage of this paper. |
Approved |
Most recent IF: 3.5; 2023 IF: 2.846 |
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Call Number |
PLASMANT @ plasmant @c:irua:197386 |
Serial |
8814 |
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Permanent link to this record |
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Author |
Wanten, B.; Vertongen, R.; De Meyer, R.; Bogaerts, A. |
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Title |
Plasma-based CO2 conversion: How to correctly analyze the performance? |
Type |
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 |
Issue |
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Pages |
180-196 |
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Keywords |
A1 journal article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Wos |
001070885000001 |
Publication Date |
2023-07-22 |
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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 |
2095-4956 |
ISBN |
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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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Permanent link to this record |
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Author |
Morais, E.; Bogaerts, A. |
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Title |
Modelling the dynamics of hydrogen synthesis from methane in nanosecond‐pulsed plasmas |
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A1 Journal Article |
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Year |
2024 |
Publication |
Plasma Processes and Polymers |
Abbreviated Journal |
Plasma Processes & Polymers |
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Volume |
21 |
Issue |
1 |
Pages |
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Keywords |
A1 Journal Article; chemical kinetics model, hydrogen, methane, nanosecond pulsed discharges, reaction mechanism; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
A chemical kinetics model was developed to characterise the gas‐phase dynamics of H<sub>2</sub>production in nanosecond‐pulsed CH<sub>4</sub>plasmas. Pulsed behaviour was observed in the calculated electric field, electron temperature and species densities at all pressures. The model agrees reasonably with experimental results, showing CH<sub>4</sub>conversion at 30% and C<sub>2</sub>H<sub>2</sub>and H<sub>2</sub>as major products. The underlying mechanisms in CH<sub>4</sub>dissociation and H<sub>2</sub>formation were analysed, highlighting the large contribution of vibrationally excited CH<sub>4</sub>and H<sub>2</sub>to coupling energy from the plasma into gas‐phase heating, and revealing that H<sub>2</sub>synthesis is not affected by applied pressure, with selectivity remaining unchanged at ~42% in the 1–5 bar range. |
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Wos |
001091258700001 |
Publication Date |
2023-10-27 |
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Abbreviated Series Title |
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Series Volume |
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Edition |
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ISSN |
1612-8850 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.5 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
We gratefully acknowledge financial support by the Flemish Government through the Moonshot cSBO project “Power‐to‐Olefins” (P2O; HBC.2020.2620) and funding from the Independent Research Fund Denmark (project nr. 0217‐00231B). |
Approved |
Most recent IF: 3.5; 2024 IF: 2.846 |
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Call Number |
PLASMANT @ plasmant @c:irua:201192 |
Serial |
8983 |
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Permanent link to this record |
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Author |
Ghasemitarei, M.; Ghorbi, T.; Yusupov, M.; Zhang, Y.; Zhao, T.; Shali, P.; Bogaerts, A. |
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Title |
Effects of Nitro-Oxidative Stress on Biomolecules: Part 1—Non-Reactive Molecular Dynamics Simulations |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
Biomolecules |
Abbreviated Journal |
Biomolecules |
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Volume |
13 |
Issue |
9 |
Pages |
1371 |
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Keywords |
A1 Journal Article; plasma medicine; reactive oxygen and; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
Plasma medicine, or the biomedical application of cold atmospheric plasma (CAP), is an expanding field within plasma research. CAP has demonstrated remarkable versatility in diverse biological applications, including cancer treatment, wound healing, microorganism inactivation, and skin disease therapy. However, the precise mechanisms underlying the effects of CAP remain incompletely understood. The therapeutic effects of CAP are largely attributed to the generation of reactive oxygen and nitrogen species (RONS), which play a crucial role in the biological responses induced by CAP. Specifically, RONS produced during CAP treatment have the ability to chemically modify cell membranes and membrane proteins, causing nitro-oxidative stress, thereby leading to changes in membrane permeability and disruption of cellular processes. To gain atomic-level insights into these interactions, non-reactive molecular dynamics (MD) simulations have emerged as a valuable tool. These simulations facilitate the examination of larger-scale system dynamics, including protein-protein and protein-membrane interactions. In this comprehensive review, we focus on the applications of non-reactive MD simulations in studying the effects of CAP on cellular components and interactions at the atomic level, providing a detailed overview of the potential of CAP in medicine. We also review the results of other MD studies that are not related to plasma medicine but explore the effects of nitro-oxidative stress on cellular components and are therefore important for a broader understanding of the underlying processes. |
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Wos |
001071356400001 |
Publication Date |
2023-09-11 |
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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 |
2218-273X |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
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Times cited |
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Open Access |
Not_Open_Access |
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Notes |
This research received no external funding. |
Approved |
Most recent IF: NA |
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Call Number |
PLASMANT @ plasmant @c:irua:200380 |
Serial |
8958 |
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Permanent link to this record |
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Author |
Meng, S.; Wu, L.; Liu, M.; Cui, Z.; Chen, Q.; Li, S.; Yan, J.; Wang, L.; Wang, X.; Qian, J.; Guo, H.; Niu, J.; Bogaerts, A.; Yi, Y. |
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Title |
Plasma‐driven<scp>CO2</scp>hydrogenation to<scp>CH3OH</scp>over<scp>Fe2O3</scp>/<scp>γ‐Al2O3</scp>catalyst |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
AIChE Journal |
Abbreviated Journal |
AIChE Journal |
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Volume |
69 |
Issue |
10 |
Pages |
e18154 |
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Keywords |
A1 Journal Article; chemisorbed oxygen, CO2 hydrogenation, iron-based catalyst, methanol production, plasma catalysis; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
We report a plasma‐assisted CO<sub>2</sub>hydrogenation to CH<sub>3</sub>OH over Fe<sub>2</sub>O<sub>3</sub>/γ‐Al<sub>2</sub>O<sub>3</sub>catalysts, achieving 12% CO<sub>2</sub>conversion and 58% CH<sub>3</sub>OH selectivity at a temperature of nearly 80°C atm pressure. We investigated the effect of various supports and loadings of the Fe‐based catalysts, as well as optimized reaction conditions. We characterized catalysts by X‐ray powder diffraction (XRD), hydrogen temperature programmed reduction (H<sub>2</sub>‐TPR), CO<sub>2</sub>and CO temperature programmed desorption (CO<sub>2</sub>/CO‐TPD), high‐resolution transmission electron microscopy (HRTEM), scanning transmission electron microscopy (STEM), x‐ray photoelectron spectroscopy (XPS), Mössbauer, and Fourier transform infrared<bold>(</bold>FTIR). The XPS results show that the enhanced CO<sub>2</sub>conversion and CH<sub>3</sub>OH selectivity are attributed to the chemisorbed oxygen species on Fe<sub>2</sub>O<sub>3</sub>/γ‐Al<sub>2</sub>O<sub>3</sub>. Furthermore, the diffuse reflectance infrared Fourier transform spectroscopy (DRIFTs) and TPD results illustrate that the catalysts with stronger CO<sub>2</sub>adsorption capacity exhibit a higher reaction performance.<italic>In situ</italic>DRIFTS gain insight into the specific reaction pathways in the CO<sub>2</sub>/H<sub>2</sub>plasma. This study reveals the role of chemisorbed oxygen species as a key intermediate, and inspires to design highly efficient catalysts and expand the catalytic systems for CO<sub>2</sub>hydrogenation to CH<sub>3</sub>OH. |
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Publisher |
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Place of Publication |
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Wos |
001022420000001 |
Publication Date |
2023-07-07 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0001-1541 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.7 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
Fundamental Research Funds for the Central Universities, DUT18JC42 ; National Natural Science Foundation of China, 21908016 21978032 ; |
Approved |
Most recent IF: 3.7; 2023 IF: 2.836 |
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Call Number |
PLASMANT @ plasmant @c:irua:197829 |
Serial |
8959 |
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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 |
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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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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 |
Meng, S.; Li, S.; Sun, S.; Bogaerts, A.; Liu, Y.; Yi, Y. |
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Title |
NH3 decomposition for H2 production by thermal and plasma catalysis using bimetallic catalysts |
Type |
A1 Journal Article |
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Year |
2024 |
Publication |
Chemical Engineering Science |
Abbreviated Journal |
Chemical Engineering Science |
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Volume |
283 |
Issue |
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Pages |
119449 |
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Keywords |
A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
Plasma catalysis has emerged as a promising approach for driving thermodynamically unfavorable chemical
reactions. Nevertheless, comprehending the mechanisms involved remains a challenge, leading to uncertainty
about whether the optimal catalyst in plasma catalysis aligns with that in thermal catalysis. In this research, we
explore this question by studying monometallic catalysts (Fe, Co, Ni and Mo) and bimetallic catalysts (Fe-Co, Mo-
Co, Fe-Ni and Mo-Ni) in both thermal catalytic and plasma catalytic NH3 decomposition. Our findings reveal that
the Fe-Co bimetallic catalyst exhibits the highest activity in thermal catalysis, the Fe-Ni bimetallic catalyst
outperforms others in plasma catalysis, indicating a discrepancy between the optimal catalysts for the two
catalytic modes in NH3 decomposition. Comprehensive catalyst characterization, kinetic analysis, temperature
program surface reaction experiments and plasma diagnosis are employed to discuss the key factors influencing
NH3 decomposition performance. |
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Wos |
001105312500001 |
Publication Date |
2023-10-28 |
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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 |
0009-2509 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
4.7 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
Universiteit Antwerpen, 32249 ; National Natural Science Foundation of China, 21503032 ; PetroChina Innovation Foundation, 2018D-5007-0501 ; |
Approved |
Most recent IF: 4.7; 2024 IF: 2.895 |
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Call Number |
PLASMANT @ plasmant @c:irua:201009 |
Serial |
8967 |
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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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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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Permanent link to this record |
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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 |
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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 |
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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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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Permanent link to this record |
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Author |
Slaets, J.; Loenders, B.; Bogaerts, A. |
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Title |
Plasma-based dry reforming of CH4: Plasma effects vs. thermal conversion |
Type |
A1 Journal Article |
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Year |
2024 |
Publication |
Fuel |
Abbreviated Journal |
Fuel |
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Volume |
360 |
Issue |
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Pages |
130650 |
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Keywords |
A1 Journal Article; Plasma kinetics Computer modelling Dry reforming of methane; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
In this work we evaluate the chemical kinetics of dry reforming of methane in warm plasmas (1000–4000 K) using modelling with a newly developed chemistry set, for a broad range of parameters (temperature, power density and CO2/CH4 ratio). We compare the model against thermodynamic equilibrium concentrations, serving as validation of the thermal chemical kinetics. Our model reveals that plasma-specific reactions (i.e., electron impact collisions) accelerate the kinetics compared to thermal conversion, rather than altering the overall kinetics pathways and intermediate products, for gas temperatures below 2000 K. For higher temperatures, the kinetics are dominated by heavy species collisions and are strictly thermal, with negligible influence of the electrons and ions on the overall kinetics. When studying the effects of different gas mixtures on the kinetics, we identify important intermediate species, side reactions and side products. The use of excess CO2 leads to H2O formation, at the expense of H2 formation, and the CO2 conversion itself is limited, only approaching full conversion near 4000 K. In contrast, full conversion of both reactants is only kinetically limited for mixtures with excess CH4, which also gives rise to the formation of C2H2, alongside syngas. Within the given parameter space, our model predicts the 30/70 ratio of CO2/CH4 to be the most optimal for syngas formation with a H2/CO ratio of 2. |
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Wos |
001138077700001 |
Publication Date |
2023-12-15 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0016-2361 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
7.4 |
Times cited |
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Open Access |
Not_Open_Access |
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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), the Catalisti-ICON project BluePlasma (Project No. HBC.2022.0445), the FWO-SBO project PlasMaCatDESIGN (FWO Grant ID S001619N), the Independent Research Fund Denmark (Project No. 0217-00231B) and through long-term structural funding (Methusalem). The 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. We also thank Bart Wanten, Roel Michiels, Pepijn Heirman, Claudia Verheyen, dr. Senne Van Alphen, dr. Elise Vervloessem, dr. Kevin van ’t Veer, dr. Joshua Boothroyd, dr. Omar Biondo and dr. Eduardo Morais for their expertise and feedback regarding the kinetics scheme. |
Approved |
Most recent IF: 7.4; 2024 IF: 4.601 |
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Call Number |
PLASMANT @ plasmant @c:irua:201669 |
Serial |
8973 |
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Permanent link to this record |