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Author | Vanraes, P.; Parayil Venugopalan, S.; Bogaerts, A. | ||||
Title | Multiscale modeling of plasma–surface interaction—General picture and a case study of Si and SiO2etching by fluorocarbon-based plasmas | Type | A1 Journal Article | ||
Year | 2021 | Publication | Applied Physics Reviews | Abbreviated Journal | Appl Phys Rev |
Volume | 8 | Issue | 4 | Pages | 041305 |
Keywords | A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | The physics and chemistry of plasma–surface interaction is a broad domain relevant to various applications and several natural processes, including plasma etching for microelectronics fabrication, plasma deposition, surface functionalization, nanomaterial synthesis, fusion reactors, and some astrophysical and meteorological phenomena. Due to their complex nature, each of these processes is generally investigated in separate subdomains, which are considered to have their own theoretical, modeling, and experimental challenges. In this review, however, we want to emphasize the overarching nature of plasma–surface interaction physics and chemistry, by focusing on the general strategy for its computational simulation. In the first half of the review, we provide a menu card with standard and less standardized computational methods to be used for the multiscale modeling of the underlying processes. In the second half, we illustrate the benefits and potential of the multiscale modeling strategy with a case study of Si and SiO2 etching by fluorocarbon plasmas and identify the gaps in knowledge still present on this intensely investigated plasma–material combination, both on a qualitative and quantitative level. Remarkably, the dominant etching mechanisms remain the least understood. The resulting new insights are of general relevance, for all plasmas and materials, including their various applications. We therefore hope to motivate computational and experimental scientists and engineers to collaborate more intensely on filling the existing gaps in knowledge. In this way, we expect that research will overcome a bottleneck stage in the development and optimization of multiscale models, and thus the fundamental understanding of plasma–surface interaction. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000754799700001 | Publication Date | 2021-10-07 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1931-9401 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 13.667 | Times cited | Open Access | OpenAccess | |
Notes | Asml; P. Vanraes acknowledges funding by ASML for the project “Computational simulation of plasma etching of trench structures.” 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. 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. S. P. Venugopalan wishes to thank Sander Wuister, Coen Verschuren, Michael Kubis, Mohammad Kamali, | Approved | Most recent IF: 13.667 | ||
Call Number | PLASMANT @ plasmant @c:irua:183287 | Serial | 6814 | ||
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Author | Neyts, E.C.; van Duin, A.C.T.; Bogaerts, A. | ||||
Title | Changing chirality during single-walled carbon nanotube growth : a reactive molecular dynamics/Monte Carlo study | Type | A1 Journal article | ||
Year | 2011 | Publication | Journal of the American Chemical Society | Abbreviated Journal | J Am Chem Soc |
Volume | 133 | Issue | 43 | Pages | 17225-17231 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | The growth mechanism and chirality formation of a single-walled carbon nanotube (SWNT) on a surface-bound nickel nanocluster are investigated by hybrid reactive molecular dynamics/force-biased Monte Carlo simulations. The validity of the interatomic potential used, the so-called ReaxFF potential, for simulating catalytic SWNT growth is demonstrated. The SWNT growth process was found to be in agreement with previous studies and observed to proceed through a number of distinct steps, viz., the dissolution of carbon in the metallic particle, the surface segregation of carbon with the formation of aggregated carbon clusters on the surface, the formation of graphitic islands that grow into SWNT caps, and finally continued growth of the SWNT. Moreover, it is clearly illustrated in the present study that during the growth process, the carbon network is continuously restructured by a metal-mediated process, thereby healing many topological defects. It is also found that a cap can nucleate and disappear again, which was not observed in previous simulations. Encapsulation of the nanoparticle is observed to be prevented by the carbon network migrating as a whole over the cluster surface. Finally, for the first time, the chirality of the growing SWNT cap is observed to change from (11,0) over (9,3) to (7,7). It is demonstrated that this change in chirality is due to the metal-mediated restructuring process. | ||||
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Publisher | Place of Publication | Washington, D.C. | Editor | ||
Language | Wos | 000297380900026 | Publication Date | 2011-10-06 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0002-7863;1520-5126; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 13.858 | Times cited | 116 | Open Access | |
Notes | Approved | Most recent IF: 13.858; 2011 IF: 9.907 | |||
Call Number | UA @ lucian @ c:irua:92043 | Serial | 309 | ||
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Author | Neyts, E.C.; van Duin, A.C.T.; Bogaerts, A. | ||||
Title | Insights in the plasma-assisted growth of carbon nanotubes through atomic scale simulations : effect of electric field | Type | A1 Journal article | ||
Year | 2012 | Publication | Journal of the American Chemical Society | Abbreviated Journal | J Am Chem Soc |
Volume | 134 | Issue | 2 | Pages | 1256-1260 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Carbon nanotubes (CNTs) are nowadays routinely grown in a thermal CVD setup. State-of-the-art plasma-enhanced CVD (PECVD) growth, however, offers advantages over thermal CVD. A lower growth temperature and the growth of aligned freestanding single-walled CNTs (SWNTs) makes the technique very attractive. The atomic scale growth mechanisms of PECVD CNT growth, however, remain currently entirely unexplored. In this contribution, we employed molecular dynamics simulations to focus on the effect of applying an electric field on the SWNT growth process, as one of the effects coming into play in PECVD. Using sufficiently strong fields results in (a) alignment of the growing SWNTs, (b) a better ordering of the carbon network, and (c) a higher growth rate relative to thermal growth rate. We suggest that these effects are due to the small charge transfer occurring in the Ni/C system. These simulations constitute the first study of PECVD growth of SWNTs on the atomic level. | ||||
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Publisher | Place of Publication | Washington, D.C. | Editor | ||
Language | Wos | 000301084300086 | Publication Date | 2011-11-30 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0002-7863;1520-5126; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 13.858 | Times cited | 56 | Open Access | |
Notes | Approved | Most recent IF: 13.858; 2012 IF: 10.677 | |||
Call Number | UA @ lucian @ c:irua:97163 | Serial | 1673 | ||
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Author | Neyts, E.C.; Shibuta, Y.; van Duin, A.C.T.; Bogaerts, A. | ||||
Title | Catalyzed growth of carbon nanotube with definable chirality by hybrid molecular dynamics-force biased Monte Carlo simulations | Type | A1 Journal article | ||
Year | 2010 | Publication | ACS nano | Abbreviated Journal | Acs Nano |
Volume | 4 | Issue | 11 | Pages | 6665-6672 |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Metal-catalyzed growth mechanisms of carbon nanotubes (CNTs) were studied by hybrid molecular dynamics−Monte Carlo simulations using a recently developed ReaxFF reactive force field. Using this novel approach, including relaxation effects, a CNT with definable chirality is obtained, and a step-by-step atomistic description of the nucleation process is presented. Both root and tip growth mechanisms are observed. The importance of the relaxation of the network is highlighted by the observed healing of defects. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000284438000043 | Publication Date | 2010-10-12 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1936-0851;1936-086X; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 13.942 | Times cited | 129 | Open Access | |
Notes | Approved | Most recent IF: 13.942; 2010 IF: 9.865 | |||
Call Number | UA @ lucian @ c:irua:84759 | Serial | 294 | ||
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Author | Girard-Sahun, F.; Biondo, O.; Trenchev, G.; van Rooij, G.; Bogaerts, A. | ||||
Title | Carbon bed post-plasma to enhance the CO2 conversion and remove O2 from the product stream | Type | A1 Journal article | ||
Year | 2022 | Publication | Chemical Engineering Journal | Abbreviated Journal | Chem Eng J |
Volume | 442 | Issue | Pages | 136268 | |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | CO2 conversion by plasma technology is gaining increasing interest. We present a carbon (charcoal) bed placed after a Gliding Arc Plasmatron (GAP) reactor, to enhance the CO2 conversion, promote O/O2 removal and in crease the CO fraction in the exhaust mixture. By means of an innovative (silo) system, the carbon is constantly supplied, to avoid carbon depletion upon reaction with O/O2. Using this carbon bed, the CO2 conversion is enhanced by almost a factor of two (from 7.6 to 12.6%), while the CO concentration even increases by a factor of three (from 7.2 to 21.9%), and O2 is completely removed from the exhaust mixture. Moreover, the energy ef ficiency of the conversion process drastically increases from 27.9 to 45.4%, and the energy cost significantly drops from 41.9 to 25.4 kJ.L− 1. We also present the temperature as a function of distance from the reactor outlet, as well as the CO2, CO and O2 concentrations and the temperature in the carbon bed as a function of time, which is important for understanding the underlying mechanisms. Indeed, these time-resolved measurements reveal that the initial enhancements in CO2 conversion and in CO concentration are not maintained in our current setup. Therefore, we present a model to study the gasification of carbon with different feed gases (i.e., O2, CO and CO2 separately), from which we can conclude that the oxygen coverage at the surface plays a key role in determining the product composition and the rate of carbon consumption. Indeed, our model insights indicate that the drop in CO2 conversion and in CO concentration after a few minutes is attributed to deactivation of the carbon bed, due to rapid formation of oxygen complexes at the surface. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000797716700002 | Publication Date | 0000-00-00 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1385-8947 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 15.1 | Times cited | Open Access | OpenAccess | |
Notes | Horizon 2020 Marie Skłodowska-Curie Actions; European Research Council; 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 European Union’s Horizon 2020 Research and Innovation programme under the Marie Sklodowska-Curie grant agreement No 813393 (PIONEER). The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit | Approved | Most recent IF: 15.1 | ||
Call Number | PLASMANT @ plasmant @c:irua:188286 | Serial | 7052 | ||
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Author | Girard-Sahun, F.; Biondo, O.; Trenchev, G.; van Rooij, G.; Bogaerts, A. | ||||
Title | Carbon bed post-plasma to enhance the CO2 conversion and remove O2 from the product stream | Type | A1 Journal article | ||
Year | 2022 | Publication | Chemical Engineering Journal | Abbreviated Journal | Chem Eng J |
Volume | 442 | Issue | Pages | 136268 | |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | CO2 conversion by plasma technology is gaining increasing interest. We present a carbon (charcoal) bed placed after a Gliding Arc Plasmatron (GAP) reactor, to enhance the CO2 conversion, promote O/O2 removal and in crease the CO fraction in the exhaust mixture. By means of an innovative (silo) system, the carbon is constantly supplied, to avoid carbon depletion upon reaction with O/O2. Using this carbon bed, the CO2 conversion is enhanced by almost a factor of two (from 7.6 to 12.6%), while the CO concentration even increases by a factor of three (from 7.2 to 21.9%), and O2 is completely removed from the exhaust mixture. Moreover, the energy ef ficiency of the conversion process drastically increases from 27.9 to 45.4%, and the energy cost significantly drops from 41.9 to 25.4 kJ.L− 1. We also present the temperature as a function of distance from the reactor outlet, as well as the CO2, CO and O2 concentrations and the temperature in the carbon bed as a function of time, which is important for understanding the underlying mechanisms. Indeed, these time-resolved measurements reveal that the initial enhancements in CO2 conversion and in CO concentration are not maintained in our current setup. Therefore, we present a model to study the gasification of carbon with different feed gases (i.e., O2, CO and CO2 separately), from which we can conclude that the oxygen coverage at the surface plays a key role in determining the product composition and the rate of carbon consumption. Indeed, our model insights indicate that the drop in CO2 conversion and in CO concentration after a few minutes is attributed to deactivation of the carbon bed, due to rapid formation of oxygen complexes at the surface. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000797716700002 | Publication Date | 0000-00-00 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1385-8947 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 15.1 | Times cited | Open Access | OpenAccess | |
Notes | Horizon 2020 Marie Skłodowska-Curie Actions; European Research Council; 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 European Union’s Horizon 2020 Research and Innovation programme under the Marie Sklodowska-Curie grant agreement No 813393 (PIONEER). The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UAntwerpen), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the UAntwerpen. We also thank R. De Meyer, K. Leyssens and S. Defossé for performing the charcoal characterizations. | Approved | Most recent IF: 15.1 | ||
Call Number | PLASMANT @ plasmant @c:irua:188286 | Serial | 7053 | ||
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Author | Van Alphen, S.; Ahmadi Eshtehardi, H.; O'Modhrain, C.; Bogaerts, J.; Van Poyer, H.; Creel, J.; Delplancke, M.-P.; Snyders, R.; Bogaerts, A. | ||||
Title | Effusion nozzle for energy-efficient NOx production in a rotating gliding arc plasma reactor | Type | A1 Journal article | ||
Year | 2022 | Publication | Chemical Engineering Journal | Abbreviated Journal | Chem Eng J |
Volume | 443 | Issue | Pages | 136529 | |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Plasma-based NOx production is of interest for sustainable N2 fixation, but more research is needed to improve its performance. One of the current limitations is recombination of NO back into N2 and O2 molecules immediately after the plasma reactor. Therefore, we developed a novel so-called “effusion nozzle”, to improve the performance of a rotating gliding arc plasma reactor for NOx production, but the same principle can also be applied to other plasma types. Experiments in a wide range of applied power, gas flow rates and N2/O2 ratios demonstrate an enhancement in NOx concentration by about 8%, and a reduction in energy cost by 22.5%. In absolute terms, we obtain NOx concentrations up to 5.9%, at an energy cost down to 2.1 MJ/mol, which are the best values reported to date in literature. In addition, we developed four complementary models to describe the gas flow, plasma temperature and plasma chemistry, aiming to reveal why the effusion nozzle yields better performance. Our simulations reveal that the effusion nozzle acts as very efficient heat sink, causing a fast drop in gas temperature when the gas molecules leave the plasma, hence limiting the recombination of NO back into N2 and O2. This yields an overall higher NOx concentration than without the effusion nozzle. This immediate quenching right at the end of the plasma makes our effusion nozzle superior to more conventional cooling options, like water cooling In addition, this higher NOx concentration can be obtained at a slightly lower power, because the effusion nozzle allows for the ignition and sustainment of the plasma at somewhat lower power. Hence, this also explains the lower energy cost. Overall, our experimental results and detailed modeling analysis will be useful to improve plasma-based NOx production in other plasma reactors as well. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000800010600003 | Publication Date | 0000-00-00 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1385-8947 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 15.1 | Times cited | Open Access | OpenAccess | |
Notes | This research was supported by the Excellence of Science FWO-FNRS project (FWO grant ID GoF9618n, EOS ID 30505023), the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No 810182 – SCOPE ERC Synergy project), and through long-term structural funding (Methusalem). The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UAntwerpen), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the UAntwerpen. | Approved | Most recent IF: 15.1 | ||
Call Number | PLASMANT @ plasmant @c:irua:188283 | Serial | 7057 | ||
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Author | Wang, Y.; Chen, Y.; Harding, J.; He, H.; Bogaerts, A.; Tu, X. | ||||
Title | Catalyst-free single-step plasma reforming of CH4 and CO2 to higher value oxygenates under ambient conditions | Type | A1 Journal article | ||
Year | 2022 | Publication | Chemical Engineering Journal | Abbreviated Journal | Chem Eng J |
Volume | 450 | Issue | Pages | 137860 | |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Direct conversion of CH4 and CO2 to liquid fuels and chemicals under mild conditions is appealing for biogas conversion and utilization but challenging due to the inert nature of both gases. Herein, we report a promising plasma process for the catalyst-free single-step conversion of CH4 and CO2 into higher value oxygenates (i.e., methanol, acetic acid, ethanol, and acetone) at ambient pressure and room temperature using a water-cooled dielectric barrier discharge (DBD) reactor, with methanol being the main liquid product. The distribution of liquid products could be tailored by tuning the discharge power, reaction temperature and residence time. Lower discharge powers (10–15 W) and reaction temperatures (5–20 ◦ C) were favourable for the production of liquid products, achieving the highest methanol selectivity of 43% at 5 ◦ C and 15 W. A higher discharge power and reaction temperature, on the other hand, produced more gaseous products, particularly H2 (up to 26% selectivity) and CO (up to 33% selectivity). In addition, varying these process parameters (discharge power, reaction temperature and residence time) resulted in a simultaneous change in key discharge properties, such as mean electron energy (Ee), electron density (ne) and specific energy input (SEI), all of which are essential determiners of plasma chemical reactions. According to the results of artificial neural network (ANN) models, the relative importance of these process parameters and key discharge indicators on reaction performance follows the order: discharge power > reaction temperature > residence time, and SEI > ne > Ee, respectively. This work provides new insights into the contributions and tuning mechanism of multiple parameters for optimizing the reaction performance (e.g., liquid production) in the plasma gas conversion process. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000830813300004 | Publication Date | 0000-00-00 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1385-8947 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 15.1 | Times cited | Open Access | OpenAccess | |
Notes | This project received funding from the European Union’s Horizon 2020 research and innovation program under the Marie SklodowskaCurie grant agreement No. 813393. | Approved | Most recent IF: 15.1 | ||
Call Number | PLASMANT @ plasmant @c:irua:189502 | Serial | 7100 | ||
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Author | Zhou, R.; Zhou, R.; Xian, Y.; Fang, Z.; Lu, X.; Bazaka, K.; Bogaerts, A.; Ostrikov, K.(K.) | ||||
Title | Plasma-enabled catalyst-free conversion of ethanol to hydrogen gas and carbon dots near room temperature | Type | A1 Journal article | ||
Year | 2020 | Publication | Chemical Engineering Journal | Abbreviated Journal | Chem Eng J |
Volume | 382 | Issue | 382 | Pages | 122745 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Selective conversion of bio-renewable ethanol under mild conditions especially at room temperature remains a major challenge for sustainable production of hydrogen and valuable carbon-based materials. In this study, adaptive non-thermal plasma is applied to deliver pulsed energy to rapidly and selectively reform ethanol in the absence of a catalyst. Importantly, the carbon atoms in ethanol that would otherwise be released into the environment in the form of CO or CO2 are effectively captured in the form of carbon dots (CDs). Three modes of non-thermal spark plasma discharges, i.e. single spark mode (SSM), multiple spark mode (MSM) and gliding spark mode (GSM), provide additional flexibility in ethanol reforming by controlling the processes of energy transfer and distribution, thereby affecting the flow rate, gas content, and energy consumption in H-2 production. A favourable combination of low temperature (< 40 degrees C), attractive conversion rate (gas flow rate of similar to 120 mL/min), high hydrogen yield (H-2 content > 90%), low energy consumption (similar to 0.96 kWh/m(3) H-2) and the effective generation of photoluminescent CDs (which are applicable for bioimaging or biolabelling) in the MSM indicate that the proposed strategy may offer a new carbon-negative avenue for comprehensive utilization of alcohols and mitigating the increasingly severe energy and environmental issues. | ||||
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Language | Wos | 000503381200200 | Publication Date | 2019-09-07 | |
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Series Volume | Series Issue | Edition | |||
ISSN | 1385-8947; 1873-3212 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 15.1 | Times cited | 20 | Open Access | |
Notes | ; ; | Approved | Most recent IF: 15.1; 2020 IF: 6.216 | ||
Call Number | UA @ admin @ c:irua:165648 | Serial | 6318 | ||
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Author | Andersen, Ja.; Christensen, Jm.; Østberg, M.; Bogaerts, A.; Jensen, Ad. | ||||
Title | Plasma-catalytic dry reforming of methane: Screening of catalytic materials in a coaxial packed-bed DBD reactor | Type | A1 Journal article | ||
Year | 2020 | Publication | Chemical Engineering Journal | Abbreviated Journal | Chem Eng J |
Volume | 397 | Issue | Pages | 125519 | |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | The combination of catalysis with non-thermal plasma is a promising alternative to thermal catalysis. A dielectric-barrier discharge reactor was used to study plasma-catalytic dry reforming of methane at ambient pressure and temperature and a fixed plasma power of 45 W. The effect of different catalytic packing materials was evaluated in terms of conversion, product selectivity, and energy efficiency. The conversion of CO2 (~22%) and CH4 (~33%) were found to be similar in plasma-only and when introducing packing materials in plasma. The main reason is the shorter residence time of the gas due to packing geometry, when compared at identical flow rates. H2, CO, C2-C4 hydrocarbons, and oxygenates were identified in the product gas. High selectivity towards H2 and CO were found for all catalysts and plasma-only, with a H2/CO molar ratio of ~0.9. The lowest syngas selectivity was obtained with Cu/Al2O3 (~66%), which instead, had the highest alcohol selectivity (~3.6%). | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000542296100011 | Publication Date | 2020-05-17 | |
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Series Volume | Series Issue | Edition | |||
ISSN | 1385-8947 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 15.1 | Times cited | Open Access | ||
Notes | Department of Chemical and Biochemical Engineering, Technical University of Denmark; We thank Haldor Topsoe A/S for providing all the catalytic materials used and the Department of Chemical and Biochemical Engineering, Technical University of Denmark, for funding this project. | Approved | Most recent IF: 15.1; 2020 IF: 6.216 | ||
Call Number | PLASMANT @ plasmant @c:irua:170613 | Serial | 6406 | ||
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Author | Wang, J.; Zhang, K.; Bogaerts, A.; Meynen, V. | ||||
Title | 3D porous catalysts for plasma-catalytic dry reforming of methane : how does the pore size affect the plasma-catalytic performance? | Type | A1 Journal article | ||
Year | 2023 | Publication | Chemical engineering journal | Abbreviated Journal | |
Volume | 464 | Issue | Pages | 142574-12 | |
Keywords | A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | The effect of pore size on plasma catalysis is crucial but still unclear. Studies have shown plasma cannot enter micropores and mesopores, so catalysts for traditional thermocatalysis may not fit plasma catalysis. Here, 3D porous Cu and CuO with different pore sizes were prepared using uniform silica particles (10–2000 nm) as templates, and compared in plasma-catalytic dry reforming. In most cases, the smaller the pore size, the higher the conversion of CH4 and CO2. Large pores reachable by more electrons did not improve the reaction efficiency. We attribute this to the small surface area and large crystallite size, as indicated by N2-sorption, mercury intrusion and XRD. While the smaller pores might not be reachable by electrons, due to the sheath formed in front of them, as predicted by modeling, they can still be reached by radicals formed in the plasma, and ions can even be attracted into these pores. An exception are the samples synthesized from 1 μm silica, which show better performance. We believe this is due to the electric field enhancement for pore sizes close to the Debye length. The performances of CuO and Cu with different pore sizes can provide references for future research on oxide supports and metal components of plasma catalysts. | ||||
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Language | Wos | 000966076400001 | Publication Date | 2023-03-21 | |
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Series Volume | Series Issue | Edition | |||
ISSN | 1385-8947; 1873-3212 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 15.1 | Times cited | Open Access | OpenAccess | |
Notes | Approved | Most recent IF: 15.1; 2023 IF: 6.216 | |||
Call Number | UA @ admin @ c:irua:194862 | Serial | 7262 | ||
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Author | Andersen, Ja.; Holm, Mc.; van 't Veer, K.; Christensen, Jm.; Østberg, M.; Bogaerts, A.; Jensen, Ad. | ||||
Title | Plasma-catalytic ammonia synthesis in a dielectric barrier discharge reactor: A combined experimental study and kinetic modeling | Type | A1 Journal article | ||
Year | 2023 | Publication | Chemical engineering journal | Abbreviated Journal | |
Volume | 457 | Issue | Pages | 141294 | |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Plasma-catalytic ammonia synthesis in a dielectric barrier discharge reactor has emerged as a possible route for electrification of nitrogen fixation. In this study, we use a combination of experiments and a plasma kinetic model to investigate the ammonia synthesis from N2 and H2, both with and without a solid packing material in the plasma zone. The effect of plasma power, feed flow rate, N2:H2 feed ratio, gas residence time, temperature, and packing material (MgAl2O4 alone or impregnated with Co or Ru) on the ammonia synthesis rate were examined in the experiments. The kinetic model was employed to improve our understanding of the ammonia formation pathways and identify possible changes in these pathways when altering the N2:H2 feed ratio. A higher NH3 synthesis rate was achieved when increasing the feed flow rate, as well as when increasing the gas tem-perature from 100 to 200 ◦C when a packing material was present in the plasma. At the elevated temperature of 200 ◦C, an optimum in the NH3 synthesis rate was observed at an equimolar feed ratio (N2:H2 =1:1) for the plasma alone and MgAl2O4, while a N2-rich feed was favored for Ru/MgAl2O4 and Co/MgAl2O4. The optimum in the synthesis rate with the N2-rich feed, where high energy electrons are more likely to collide with N2, suggests that the rate-limiting step is the dissociation of N2 in the gas phase. This is supported by the kinetic model when packing material was used. However, for the plasma alone, the model found that the N2 dissociation is only rate limiting in H2-rich feeds, whereas the limited access to H in N2-rich feeds makes the hydrogenation of N species limiting. | ||||
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Language | Wos | 001058978000001 | Publication Date | 2023-01-05 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1385-8947 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 15.1 | Times cited | Open Access | OpenAccess | |
Notes | We thank Topsoe A/S for providing the catalytic materials used in the study, the research group PLASMANT (University of Antwerp) for sharing their plasma kinetic model and allocating time on their cluster for the calculations, and the Department of Chemical and Biochemical Engineering (Technical University of Denmark) for funding the project. | Approved | Most recent IF: 15.1; 2023 IF: 6.216 | ||
Call Number | PLASMANT @ plasmant @c:irua:195877 | Serial | 7234 | ||
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Author | Morais, E.; Delikonstantis, E.; Scapinello, M.; Smith, G.; Stefanidis, G.D.; Bogaerts, A. | ||||
Title | Methane coupling in nanosecond pulsed plasmas: Correlation between temperature and pressure and effects on product selectivity | Type | A1 Journal article | ||
Year | 2023 | Publication | Chemical engineering journal | Abbreviated Journal | |
Volume | 462 | Issue | Pages | 142227 | |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | We present a zero-dimensional kinetic model to characterise specifically the gas-phase dynamics of methane conversion in a nanosecond pulsed discharge (NPD) plasma reactor. The model includes a systematic approach to capture the nanoscale power discharges and the rapid ensuing changes in electric field, gas and electron temperature, as well as species densities. The effects of gas temperature and reactor pressure on gas conversion and product selectivity are extensively investigated and validated against experimental work. We discuss the important reaction pathways and provide an analysis of the dynamics of the heating and cooling mechanisms. H radicals are found to be the most populous plasma species and they participate in hydrogenation and dehydrogenation reactions, which are the dominant recombination reactions leading to C2H4 and C2H2 as main products (depending on the pressure). |
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Language | Wos | 000983631500001 | Publication Date | 2023-03-02 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1385-8947 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 15.1 | Times cited | Open Access | OpenAccess | |
Notes | We gratefully acknowledge financial support by the Flemish Government through the Moonshot cSBO project “Power-to-Olefins” (P2O; HBC.2020.2620). | Approved | Most recent IF: 15.1; 2023 IF: 6.216 | ||
Call Number | PLASMANT @ plasmant @c:irua:195881 | Serial | 7246 | ||
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Author | Van Alphen, S.; Hecimovic, A.; Kiefer, C.K.; Fantz, U.; Snyders, R.; Bogaerts, A. | ||||
Title | Modelling post-plasma quenching nozzles for improving the performance of CO2 microwave plasmas | Type | A1 Journal article | ||
Year | 2023 | Publication | Chemical engineering journal | Abbreviated Journal | |
Volume | 462 | Issue | Pages | 142217 | |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Given the ecological problems associated to the CO2 emissions of fossil fuels, plasma technology has gained interest for conversion of CO2 into value-added products. Microwave plasmas operating at atmospheric pressure have proven to be especially interesting, due to the high gas temperatures inside the reactor (i.e. up to 6000 K) allowing for efficient thermal dissociation of CO2 into CO and O2. However, the performance of these high temperature plasmas is limited by recombination of CO back into CO2 once the gas cools down in the afterglow. In this work, we computationally investigated several quenching nozzles, developed and experimentally tested by Hecimovic et al., [1] for their ability to quickly cool the gas after the plasma, thereby quenching the CO recombination reactions. Using a 3D computational fluid dynamics model and a quasi-1D chemical kinetics model, we reveal that a reactor without nozzle lacks gas mixing between hot gas in the center and cold gas near the reactor walls. Especially at low flow rates, where there is an inherent lack of convective cooling due to the low gas flow velocity, the temperature in the afterglow remains high (between 2000 and 3000 K) for a relatively long time (in the 0.1 s range). As shown by our quasi-1D chemical kinetics model, this results in a important loss of CO due to recombination reactions. Attaching a nozzle in the effluent of the reactor induces fast gas quenching right after the plasma. Indeed, it introduces (i) more convective cooling by forcing cool gas near the walls to mix with hot gas in the center of the reactor, as well as (ii) more conductive cooling through the water-cooled walls of the nozzle. Our model shows that gas quenching and the suppression of recombination reactions have more impact at low flow rates, where recombination is the most limiting factor in the conversion process. |
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000962382600001 | Publication Date | 2023-03-03 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1385-8947 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 15.1 | Times cited | Open Access | OpenAccess | |
Notes | This research was supported by the Excellence of Science FWO-FNRS project (FWO grant ID GoF9618n, EOS ID 30505023), the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No 810182 – SCOPE ERC Synergy project), and through long-term structural funding (Methusalem). The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UAntwerpen), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the UAntwerpen. | Approved | Most recent IF: 15.1; 2023 IF: 6.216 | ||
Call Number | PLASMANT @ plasmant @c:irua:195889 | Serial | 7250 | ||
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Author | Liu, R.; Hao, Y.; Wang, T.; Wang, L.; Bogaerts, A.; Guo, H.; Yi, Y. | ||||
Title | Hybrid plasma-thermal system for methane conversion to ethylene and hydrogen | Type | A1 Journal article | ||
Year | 2023 | Publication | Chemical engineering journal | Abbreviated Journal | |
Volume | 463 | Issue | Pages | 142442 | |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | By combining dielectric barrier discharge plasma and external heating, we exploit a two-stage hybrid plasmathermal system (HPTS), i.e., a plasma stage followed by a thermal stage, for direct non-oxidative coupling of CH4 to C2H4 and H2, yielding a CH4 conversion of ca. 17 %. In the two-stage HPTS, the plasma first converts CH4 into C2H6 and C3H8, which in the thermal stage leads to a high C2H4 selectivity of ca. 63 % by pyrolysis, with H2 selectivity of ca. 64 %. |
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Language | Wos | 000953890500001 | Publication Date | 2023-03-16 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1385-8947 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 15.1 | Times cited | Open Access | OpenAccess | |
Notes | This work was supported by the National Natural Science Foundation of China [22272015, 21503032], the Fundamental Research Funds for the Central Universities of China [DUT21JC40]. | Approved | Most recent IF: 15.1; 2023 IF: 6.216 | ||
Call Number | PLASMANT @ plasmant @c:irua:195888 | Serial | 7253 | ||
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Author | Van Alphen, S.; Hecimovic, A.; Kiefer, C.K.; Fantz, U.; Snyders, R.; Bogaerts, A. | ||||
Title | Modelling post-plasma quenching nozzles for improving the performance of CO2 microwave plasmas | Type | A1 Journal article | ||
Year | 2023 | Publication | Chemical engineering journal | Abbreviated Journal | |
Volume | 462 | Issue | Pages | 142217 | |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Given the ecological problems associated to the CO2 emissions of fossil fuels, plasma technology has gained interest for conversion of CO2 into value-added products. Microwave plasmas operating at atmospheric pressure have proven to be especially interesting, due to the high gas temperatures inside the reactor (i.e. up to 6000 K) allowing for efficient thermal dissociation of CO2 into CO and O2. However, the performance of these high temperature plasmas is limited by recombination of CO back into CO2 once the gas cools down in the afterglow. In this work, we computationally investigated several quenching nozzles, developed and experimentally tested by Hecimovic et al., [1] for their ability to quickly cool the gas after the plasma, thereby quenching the CO recombination reactions. Using a 3D computational fluid dynamics model and a quasi-1D chemical kinetics model, we reveal that a reactor without nozzle lacks gas mixing between hot gas in the center and cold gas near the reactor walls. Especially at low flow rates, where there is an inherent lack of convective cooling due to the low gas flow velocity, the temperature in the afterglow remains high (between 2000 and 3000 K) for a relatively long time (in the 0.1 s range). As shown by our quasi-1D chemical kinetics model, this results in a important loss of CO due to recombination reactions. Attaching a nozzle in the effluent of the reactor induces fast gas quenching right after the plasma. Indeed, it introduces (i) more convective cooling by forcing cool gas near the walls to mix with hot gas in the center of the reactor, as well as (ii) more conductive cooling through the water-cooled walls of the nozzle. Our model shows that gas quenching and the suppression of recombination reactions have more impact at low flow rates, where recombination is the most limiting factor in the conversion process. |
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000962382600001 | Publication Date | 2023-03-03 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1385-8947 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 15.1 | Times cited | Open Access | OpenAccess | |
Notes | This research was supported by the Excellence of Science FWO-FNRS project (FWO grant ID GoF9618n, EOS ID 30505023), the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No 810182 – SCOPE ERC Synergy project), and through long-term structural funding (Methusalem). The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UAntwerpen), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the UAntwerpen. | Approved | Most recent IF: 15.1; 2023 IF: 6.216 | ||
Call Number | PLASMANT @ plasmant @c:irua:195889 | Serial | 7259 | ||
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Author | Wang, J.; Zhang, K.; Meynen, V.; Bogaerts, A. | ||||
Title | Dry reforming in a dielectric barrier discharge reactor with non-uniform discharge gap : effects of metal rings on the discharge behavior and performance | Type | A1 Journal article | ||
Year | 2023 | Publication | Chemical engineering journal | Abbreviated Journal | |
Volume | Issue | Pages | 142953-29 | ||
Keywords | A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | The application of dielectric barrier discharge (DBD) plasma reactors is promising in various environmental and energy processes, but is limited by their low energy yield. In this study, we put a number of stainless steel rings over the inner electrode rod of the DBD reactor to change the local discharge gap and electric field, and we studied the dry reforming performance. At 50 W supplied power, the metal rings mostly have a negative impact on the performance, which we attribute to the non-uniform spatial distribution of the discharges caused by the rings. However, at 30 W supplied power, the energy yield is higher than at 50 W and the placement of the rings improves the performance of the reactor. More rings and with a larger cross-sectional diameter can further improve the performance. The reactor with 20 rings with a 3.2 mm cross-sectional diameter exhibits the best performance in this study. Compared to the reactor without rings, it increases the CO2 conversion from 7% to 16 %, the CH4 conversion from 12% to 23%, and the energy yield from 0.05 mmol/kJ supplied power to 0.1 mmol/kJ (0.19 mmol/kJ if calculated from the plasma power), respectively. The presence of the rings increases the local electric field, the displaced charge and the discharge fraction, and also makes the discharge more stable and with more uniform intensity. It also slightly improves the selectivity to syngas. The performance improvement observed by placing stainless steel rings in this study may also be applicable to other plasma-based processes. | ||||
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Language | Wos | 000986051300001 | Publication Date | 2023-04-17 | |
Series Editor | Series Title | Abbreviated Series Title | |||
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ISSN | 1385-8947; 1873-3212 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 15.1 | Times cited | Open Access | OpenAccess | |
Notes | Approved | Most recent IF: 15.1; 2023 IF: 6.216 | |||
Call Number | UA @ admin @ c:irua:195603 | Serial | 7264 | ||
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Author | Wang, K.; Ceulemans, S.; Zhang, H.; Tsonev, I.; Zhang, Y.; Long, Y.; Fang, M.; Li, X.; Yan, J.; Bogaerts, A. | ||||
Title | Inhibiting recombination to improve the performance of plasma-based CO2 conversion | Type | A1 Journal Article | ||
Year | 2024 | Publication | Chemical Engineering Journal | Abbreviated Journal | Chemical Engineering Journal |
Volume | 481 | Issue | Pages | 148684 | |
Keywords | A1 Journal Article; Plasma-based CO2 splitting Recombination reactions In-situ gas sampling Fluid dynamics modeling Kinetics modeling Afterglow quenching; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | Warm plasma offers a promising route for CO2 splitting into valuable CO, yet recombination reactions of CO with oxygen, forming again CO2, have recently emerged as critical limitation. This study combines experiments and fluid dynamics + chemical kinetics modelling to comprehensively analyse the recombination reactions upon CO2 splitting in an atmospheric plasmatron. We introduce an innovative in-situ gas sampling technique, enabling 2D spatial mapping of gas product compositions and temperatures, experimentally confirming for the first time the substantial limiting effect of CO recombination reactions in the afterglow region. Our results show that the CO mole fraction at a 5 L/min flow rate drops significantly from 11.9 % at a vertical distance of z = 20 mm in the afterglow region to 8.6 % at z = 40 mm. We constructed a comprehensive 2D model that allows for spatial reaction rates analysis incorporating crucial reactions, and we validated it to kinetically elucidate this phenomenon. CO2 +M⇌O+CO+M and CO2 +O⇌CO+O2 are the dominant reactions, with the forward reactions prevailing in the plasma region and the backward reactions becoming prominent in the afterglow region. These results allow us to propose an afterglow quenching strategy for performance enhancement, which is further demonstrated through a meticulously developed plasmatron reactor with two-stage cooling. Our approach substantially increases the CO2 conversion (e.g., from 6.6 % to 19.5 % at 3 L/min flow rate) and energy efficiency (from 13.5 % to 28.5 %, again at 3 L/min) and significantly shortens the startup time (from ~ 150 s to 25 s). Our study underscores the critical role of inhibiting recombination reactions in plasma-based CO2 conversion and offers new avenues for performance enhancement. | ||||
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Language | Wos | 001168999200001 | Publication Date | 2024-01-10 | |
Series Editor | Series Title | Abbreviated Series Title | |||
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ISSN | 1385-8947 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 15.1 | Times cited | Open Access | Not_Open_Access | |
Notes | Key Research and Development Program of Zhejiang Province, 2023C03129 ; Vlaamse regering; European Research Council; National Natural Science Foundation of China, 51976191 52276214 ; Horizon 2020 Framework Programme; Fonds De La Recherche Scientifique – FNRS; Fonds Wetenschappelijk Onderzoek, 1101524N ; Vlaams Supercomputer Centrum; Horizon 2020, 101081162 810182 ; European Research Council; | Approved | Most recent IF: 15.1; 2024 IF: 6.216 | ||
Call Number | PLASMANT @ plasmant @c:irua:204352 | Serial | 8993 | ||
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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 | Chemical engineering journal | Abbreviated Journal | Chemical Engineering Journal |
Volume | 488 | Issue | Pages | 150838 | |
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 | 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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Language | Wos | 001221606600001 | Publication Date | 2024-03-30 | |
Series Editor | Series Title | Abbreviated Series Title | |||
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ISSN | 1385-8947 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 15.1 | Times cited | Open Access | ||
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 | ||
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Author | Maerivoet, S.; Tsonev, I.; Slaets, J.; Reniers, F.; Bogaerts, A. | ||||
Title | Coupled multi-dimensional modelling of warm plasmas: Application and validation for an atmospheric pressure glow discharge in CO2/CH4/O2 | Type | A1 Journal Article | ||
Year | 2024 | Publication | Chemical Engineering Journal | Abbreviated Journal | Chemical Engineering Journal |
Volume | 492 | Issue | Pages | 152006 | |
Keywords | A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | To support experimental research into gas conversion by warm plasmas, models should be developed to explain the experimental observations. These models need to describe all physical and chemical plasma properties in a coupled way. In this paper, we present a modelling approach to solve the complete set of assumed relevant equations, including gas flow, heat balance and species transport, coupled with a rather extensive chemistry set, consisting of 21 species, obtained by reduction of a more detailed chemistry set, consisting of 41 species. We apply this model to study the combined CO2 and CH4 conversion in the presence of O2, in a direct current atmospheric pressure glow discharge. Our model can predict the experimental trends, and can explain why higher O2 fractions result in higher CH4 conversion, namely due to the higher gas temperature, rather than just by additional chemical reactions. Indeed, our model predicts that when more O2 is added, the energy required to reach any set temperature (i.e., the enthalpy) drops, allowing the system to reach higher temperatures with similar amounts of energy. This is in turn related to the higher H2O fraction and lower H2 fraction formed in the plasma, as demonstrated by our model. Altogether, our new self-consistent model can capture the main physics and chemistry occurring in this warm plasma, which is an important step towards predictive modelling for plasma-based gas conversion. | ||||
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Language | Wos | Publication Date | 2024-05-09 | ||
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ISSN | 1385-8947 | ISBN | Additional Links | ||
Impact Factor | 15.1 | Times cited | Open Access | ||
Notes | This research was supported by the Excellence of Science FWO-FNRS project (FWO grant ID G0I1822N; EOS ID 40007511) and the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No. 810182–SCOPE ERC Synergy project, and grant agreement No. 101081162–PREPARE ERC Proof of Concept project). computational resources and services used in this work were provided by the HPC core facility CalcUA of the Universiteit Antwerpen, and VSC (Flemish Supercomputer Center), funded by the Research Foundation – Flanders (FWO) and the Flemish Government. | Approved | Most recent IF: 15.1; 2024 IF: 6.216 | ||
Call Number | PLASMANT @ plasmant @ | Serial | 9132 | ||
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Author | Lv, H.; Meng, S.; Cui, Z.; Li, S.; Li, D.; Gao, X.; Guo, H.; Bogaerts, A.; Yi, Y. | ||||
Title | Plasma-catalytic direct oxidation of methane to methanol over Cu-MOR: Revealing the zeolite-confined Cu2+ active sites | Type | A1 Journal Article | ||
Year | 2024 | Publication | Chemical Engineering Journal | Abbreviated Journal | Chemical Engineering Journal |
Volume | 496 | Issue | Pages | 154337 | |
Keywords | A1 Journal Article; Direct oxidation Methanol production Plasma catalysis Copper-mordenite catalysts; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | Efficient methane conversion to methanol remains a significant challenge in chemical industry. This study investigates the direct oxidation of methane to methanol under mild conditions, employing a synergy of nonthermal plasma and Cu-MOR (Copper-Mordenite) catalysts. Catalytic tests demonstrate that the Cu-MOR IE-3 catalyst (i.e., prepared by three cycles of ion exchange) exhibits superior catalytic performance (with 51 % methanol selectivity and 7.9 % methane conversion). Conversely, the Cu-MOR catalysts prepared via wetness impregnation tend to over-oxidize CH4 to CO and CO2. Through systematic catalyst characterizations (XRD, TPR, UV–Vis, HRTEM, XPS), we elucidate that ion exchange mainly leads to the formation of zeolite-confined Cu2+ species, while wetness impregnation predominantly results in CuO particles. Based on the catalytic performance, catalyst characterizations and in-situ FTIR spectra, we conclude that zeolite-confined Cu2+ species serve as the active sites for plasma-catalytic direct oxidation of methane to methanol. | ||||
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Language | Wos | Publication Date | 2024-08-02 | ||
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ISSN | 1385-8947 | ISBN | Additional Links | ||
Impact Factor | 15.1 | Times cited | Open Access | ||
Notes | PetroChina Innovation Foundation, 2018D-5007-0501 ; Fundamental Research Funds for the Central Universities, DUT21JC40 ; Fundamental Research Funds for the Central Universities; China Scholarship Council; National Natural Science Foundation of China, 22272015 ; | Approved | Most recent IF: 15.1; 2024 IF: 6.216 | ||
Call Number | PLASMANT @ plasmant @ | Serial | 9260 | ||
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Author | Sun, J.; Chen, Q.; Qin, W.; Wu, H.; Liu, B.; Li, S.; Bogaerts, A. | ||||
Title | Plasma-catalytic dry reforming of CH4: Effects of plasma-generated species on the surface chemistry | Type | A1 Journal Article | ||
Year | 2024 | Publication | Chemical Engineering Journal | Abbreviated Journal | Chemical Engineering Journal |
Volume | 498 | Issue | Pages | 155847 | |
Keywords | A1 Journal Article; Dry reforming of methane Plasma catalysis Plasma-enhanced surface chemistry Path flux and sensitivity analysis Coking kinetics; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | By means of steady-state experiments and a global model, we studied the effects of plasma-generated reactive species on the surface chemistry and coking in plasma-catalytic CH4/CO2 reforming at reduced pressure (8–40 kPa). We used a hybrid ZDPlasKin-CHEMKIN model to predict the species densities over time. The detailed plasma-catalytic mechanism consists of the plasma discharge scheme, a gas-phase chemistry set and a surface mechanism. Our experimental results show that the coupling of Ni/SiO2 catalyst with plasma is more effective in CH4/CO2 activation and conversion than unpacked DBD plasma, with syngas being the main products. The highest total conversion of 16 % was achieved at 8000 V and 473 K, with corresponding CO and H2 yields of 15 % and 12 %, respectively. The reactants conversion and product selectivity are well captured by the kinetic model. Our simulation results suggest that vibrational species and radicals can accelerate the dissociative adsorption and Eley-Rideal (E-R) reactions. Path flux analysis shows that E-R reactions dominate the surface reaction pathways, which differs from thermal catalysis, indicating that the coupling of non-equilibrium plasma and catalysis can effectively shift the formation and consumption pathways of important adsorbates. For instance, our model suggests that HCOO(s) is primarily generated through the E-R reaction CO2(v) + H(s) → HCOO(s), while the hydrogenation reaction HCOO(s) + H → HCOOH(s) is the main source of HCOOH(s). Carbon deposition on the catalyst surface is primarily formed through the stepwise dehydrogenation of CH4, while the E-R reactions enhanced by plasma-generated H and O atoms dominate the consumption of carbon deposition. This work provides new insights into the effects of reactive species on the surface chemistry in plasma-catalytic CH4/CO2 reforming. |
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Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2024-09-17 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1385-8947 | ISBN | Additional Links | ||
Impact Factor | 15.1 | Times cited | Open Access | ||
Notes | National Natural Science Foundation of China; | Approved | Most recent IF: 15.1; 2024 IF: 6.216 | ||
Call Number | PLASMANT @ plasmant @ | Serial | 9266 | ||
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Author | Fedirchyk, I.; Tsonev, I.; Quiroz Marnef, R.; Bogaerts, A. | ||||
Title | Plasma-assisted NH3 cracking in warm plasma reactors for green H2 production | Type | A1 Journal Article | ||
Year | 2024 | Publication | Chemical Engineering Journal | Abbreviated Journal | Chemical Engineering Journal |
Volume | 499 | Issue | Pages | 155946 | |
Keywords | A1 Journal Article; Plasma-assisted NH3 cracking Plasma reactors Warm plasma H2 production from NH3; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | renewable energy. Plasma technology is promising for this purpose, as it can crack NH3 without the need for a catalyst and is highly compatible with renewable electricity, reducing the environmental footprint of the cracking process. This work investigates the NH3 cracking performance of four different warm plasma reactors with different configurations and operating in a wide range of conditions. We show that the NH3 conversion in warm plasma reactors is primarily determined by the specific energy input, with the main difference observed in the energy cost (EC) of cracking. The lowest EC obtained is 146 kJ/mol but at a conversion of only 8 %. A more reasonable conversion of around 50 % yields an EC of around 200 kJ/mol in two of the reactors investigated. Plasma reactors operating at higher feed flow rates are more efficient and yield a higher H2 production rate. Our data indicate that NH3 cracking in these warm plasma reactors occurs mainly via thermal chemistry, with nonthermal plasma chemistry playing a less prominent role. NH3 decomposes not only inside the plasma core but also in a hot volume around it, which reduces the EC. Our study shows that warm plasmas are significantly more efficient for NH3 cracking than cold plasmas, even when the latter are combined with catalysts. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2024-09-19 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1385-8947 | ISBN | Additional Links | ||
Impact Factor | 15.1 | Times cited | Open Access | ||
Notes | Belgian Federal Government; European Commission Marie Sklodowska-Curie Actions; | Approved | Most recent IF: 15.1; 2024 IF: 6.216 | ||
Call Number | PLASMANT @ plasmant @ | Serial | 9267 | ||
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Author | Hollevoet, L.; Jardali, F.; Gorbanev, Y.; Creel, J.; Bogaerts, A.; Martens, J.A. | ||||
Title | Towards green ammonia synthesis through plasma-driven nitrogen oxidation and catalytic reduction | Type | A1 Journal article | ||
Year | 2020 | Publication | Angewandte Chemie-International Edition | Abbreviated Journal | Angew Chem Int Edit |
Volume | Issue | Pages | |||
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Ammonia is an industrial large-volume chemical, with its main application in fertilizer production. It also attracts increasing attention as a green-energy vector. Over the past century, ammonia production has been dominated by the Haber-Bosch process, in which a mixture of nitrogen and hydrogen gas is converted to ammonia at high temperatures and pressures. Haber-Bosch processes with natural gas as the source of hydrogen are responsible for a significant share of the global CO(2)emissions. Processes involving plasma are currently being investigated as an alternative for decentralized ammonia production powered by renewable energy sources. In this work, we present the PNOCRA process (plasma nitrogen oxidation and catalytic reduction to ammonia), combining plasma-assisted nitrogen oxidation and lean NO(x)trap technology, adopted from diesel-engine exhaust gas aftertreatment technology. PNOCRA achieves an energy requirement of 4.6 MJ mol(-1)NH(3), which is more than four times less than the state-of-the-art plasma-enabled ammonia synthesis from N(2)and H(2)with reasonable yield (>1 %). | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000580489400001 | Publication Date | 2020-09-21 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1433-7851; 0570-0833 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 16.6 | Times cited | 1 | Open Access | |
Notes | ; We gratefully acknowledge the financial support by the Flemish Government through the Moonshot cSBO project P2C (HBC.2019.0108). J.A.M. and A.B. acknowledge the Flemish Government for long-term structural funding (Methusalem). ; | Approved | Most recent IF: 16.6; 2020 IF: 11.994 | ||
Call Number | UA @ admin @ c:irua:173589 | Serial | 6634 | ||
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Author | Živanić, M.; Espona‐Noguera, A.; Verswyvel, H.; Smits, E.; Bogaerts, A.; Lin, A.; Canal, C. | ||||
Title | Injectable Plasma‐Treated Alginate Hydrogel for Oxidative Stress Delivery to Induce Immunogenic Cell Death in Osteosarcoma | Type | A1 Journal article | ||
Year | 2023 | Publication | Advanced functional materials | Abbreviated Journal | Adv Funct Materials |
Volume | Issue | Pages | |||
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Center for Oncological Research (CORE) | ||||
Abstract | Cold atmospheric plasma (CAP) is a source of cell‐damaging oxidant molecules that may be used as low‐cost cancer treatment with minimal side effects. Liquids treated with cold plasma and enriched with oxidants are a modality for non‐invasive treatment of internal tumors with cold plasma via injection. However, liquids are easily diluted with body fluids which impedes high and localized delivery of oxidants to the target. As an alternative, plasma‐treated hydrogels (PTH) emerge as vehicles for the precise delivery of oxidants. This study reports an optimal protocol for the preparation of injectable alginate PTH that ensures the preservation of plasma‐generated oxidants. The generation, storage, and release of oxidants from the PTH are assessed. The efficacy of the alginate PTH in cancer treatment is demonstrated in the context of cancer cell cytotoxicity and immunogenicity–release of danger signals and phagocytosis by immature dendritic cells, up to now unexplored for PTH. These are shown in osteosarcoma, a hard‐to‐treat cancer. The study aims to consolidate PTH as a novel cold plasma treatment modality for non‐invasive or postoperative tumor treatment. The results offer a rationale for further exploration of alginate‐based PTHs as a versatile platform in biomedical engineering. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 001129424500001 | Publication Date | 2023-12-21 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1616-301X | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 19 | Times cited | Open Access | ||
Notes | Fonds Wetenschappelijk Onderzoek, 1S67621N ; European Cooperation in Science and Technology, COST Action CA20114 ; Agència de Gestió d'Ajuts Universitaris i de Recerca, SGR2022‐1368 ; Agencia Estatal de Investigación, PID2019‐ 103892RB‐I00/AEI/10.13039/501100011033 ; Instituto de Salud Carlos III, IHRC22/00003 ; | Approved | Most recent IF: 19; 2023 IF: 12.124 | ||
Call Number | PLASMANT @ plasmant @c:irua:202030 | Serial | 8979 | ||
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Author | Vanraes, P.; Bogaerts, A. | ||||
Title | The essential role of the plasma sheath in plasma–liquid interaction and its applications—A perspective | Type | A1 Journal Article | ||
Year | 2021 | Publication | Journal Of Applied Physics | Abbreviated Journal | J Appl Phys |
Volume | 129 | Issue | 22 | Pages | 220901 |
Keywords | A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | Based on the current knowledge, a plasma–liquid interface looks and behaves very differently from its counterpart at a solid surface. Local processes characteristic to most liquids include a stronger evaporation, surface deformations, droplet ejection, possibly distinct mechanisms behind secondary electron emission, the formation of an electric double layer, and an ion drift-mediated liquid resistivity. All of them can strongly influence the interfacial charge distribution. Accordingly, the plasma sheath at a liquid surface is most likely unique in its own way, both with respect to its structure and behavior. However, insights into these properties are still rather scarce or uncertain, and more studies are required to further disclose them. In this Perspective, we argue why more research on the plasma sheath is not only recommended but also crucial to an accurate understanding of the plasma–liquid interaction. First, we analyze how the sheath regulates various elementary processes at the plasma–liquid interface, in terms of the electrical coupling, the bidirectional mass transport, and the chemistry between plasma and liquid phase. Next, these three regulatory functions of the sheath are illustrated for concrete applications. Regarding the electrical coupling, a great deal of attention is paid to the penetration of fields into biological systems due to their relevance for plasma medicine, plasma agriculture, and food processing. Furthermore, we illuminate the role of the sheath in nuclear fusion, nanomaterial synthesis, and chemical applications. As such, we hope to motivate the plasma community for more fundamental research on plasma sheaths at liquid surfaces. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000681700000013 | Publication Date | 2021-06-14 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0021-8979 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 2.068 | Times cited | Open Access | OpenAccess | |
Notes | P.V. thanks Dr. Angela Privat Maldonado (University of Antwerp) for the fruitful discussions on Sec. III and Professor Mark J. Kushner (University of Michigan) for the interesting discussion on Ref. 198. | Approved | Most recent IF: 2.068 | ||
Call Number | PLASMANT @ plasmant @c:irua:178814 | Serial | 6794 | ||
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Author | Bruggeman, P.J.; Bogaerts, A.; Pouvesle, J.M.; Robert, E.; Szili, E.J. | ||||
Title | Plasma–liquid interactions | Type | A1 Journal Article | ||
Year | 2021 | Publication | Journal Of Applied Physics | Abbreviated Journal | J Appl Phys |
Volume | 130 | Issue | 20 | Pages | 200401 |
Keywords | A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2021-11-28 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0021-8979 | ISBN | Additional Links | UA library record | |
Impact Factor | 2.068 | Times cited | Open Access | OpenAccess | |
Notes | Approved | Most recent IF: 2.068 | |||
Call Number | PLASMANT @ plasmant @c:irua:184245 | Serial | 6830 | ||
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Author | Bogaerts, A.; Gijbels, R.; Vlcek, J. | ||||
Title | Collisional-radiative model for an argon glow discharge | Type | A1 Journal article | ||
Year | 1998 | Publication | Journal of applied physics | Abbreviated Journal | J Appl Phys |
Volume | 84 | Issue | Pages | 121-136 | |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
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Publisher | American Institute of Physics | Place of Publication | New York, N.Y. | Editor | |
Language | Wos | 000075258100015 | Publication Date | 2002-07-26 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0021-8979; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 2.068 | Times cited | 138 | Open Access | |
Notes | Approved | Most recent IF: 2.068; 1998 IF: 1.729 | |||
Call Number | UA @ lucian @ c:irua:19614 | Serial | 387 | ||
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Author | Bogaerts, A.; Yan, M.; Gijbels, R.; Goedheer, W. | ||||
Title | Modeling of ionization of argon in an analytical capacitively coupled radio-frequency glow discharge | Type | A1 Journal article | ||
Year | 1999 | Publication | Journal of applied physics | Abbreviated Journal | J Appl Phys |
Volume | 86 | Issue | 6 | Pages | 2990-3001 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
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Publisher | American Institute of Physics | Place of Publication | New York, N.Y. | Editor | |
Language | Wos | 000082232400010 | Publication Date | 2002-07-26 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0021-8979; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 2.068 | Times cited | 18 | Open Access | |
Notes | Approved | Most recent IF: 2.068; 1999 IF: 2.275 | |||
Call Number | UA @ lucian @ c:irua:28320 | Serial | 2127 | ||
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Author | Bogaerts, A.; Gijbels, R. | ||||
Title | Role of Ar2+ and Ar+2 ions in a direct current argon glow discharge: a numerical description | Type | A1 Journal article | ||
Year | 1999 | Publication | Journal of applied physics | Abbreviated Journal | J Appl Phys |
Volume | 86 | Issue | 8 | Pages | 4124-4133 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
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Publisher | American Institute of Physics | Place of Publication | New York, N.Y. | Editor | |
Language | Wos | 000082840300009 | Publication Date | 2002-07-26 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0021-8979; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 2.068 | Times cited | 50 | Open Access | |
Notes | Approved | Most recent IF: 2.068; 1999 IF: 2.275 | |||
Call Number | UA @ lucian @ c:irua:28322 | Serial | 2923 | ||
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