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Author |
Girard-Sahun, F.; Biondo, O.; Trenchev, G.; van Rooij, G.; Bogaerts, A. |
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Title |
Carbon bed post-plasma to enhance the CO2 conversion and remove O2 from the product stream |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chem Eng J |
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Volume |
442 |
Issue |
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Pages |
136268 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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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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Wos |
000797716700002 |
Publication Date |
0000-00-00 |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1385-8947 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
OpenAccess |
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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 ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 15.1 |
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Call Number |
PLASMANT @ plasmant @c:irua:188286 |
Serial |
7052 |
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Permanent link to this record |
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Author |
Girard-Sahun, F.; Biondo, O.; Trenchev, G.; van Rooij, G.; Bogaerts, A. |
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Title |
Carbon bed post-plasma to enhance the CO2 conversion and remove O2 from the product stream |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chem Eng J |
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Volume |
442 |
Issue |
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Pages |
136268 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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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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000797716700002 |
Publication Date |
0000-00-00 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1385-8947 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
OpenAccess |
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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 ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 15.1 |
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Call Number |
PLASMANT @ plasmant @c:irua:188286 |
Serial |
7053 |
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Permanent link to this record |
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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. |
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Title |
Effusion nozzle for energy-efficient NOx production in a rotating gliding arc plasma reactor |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chem Eng J |
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Volume |
443 |
Issue |
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Pages |
136529 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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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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Wos |
000800010600003 |
Publication Date |
0000-00-00 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1385-8947 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
OpenAccess |
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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 ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 15.1 |
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Call Number |
PLASMANT @ plasmant @c:irua:188283 |
Serial |
7057 |
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Permanent link to this record |
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Author |
Wang, Y.; Chen, Y.; Harding, J.; He, H.; Bogaerts, A.; Tu, X. |
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Title |
Catalyst-free single-step plasma reforming of CH4 and CO2 to higher value oxygenates under ambient conditions |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chem Eng J |
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Volume |
450 |
Issue |
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Pages |
137860 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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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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Wos |
000830813300004 |
Publication Date |
0000-00-00 |
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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 |
1385-8947 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
OpenAccess |
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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 ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 15.1 |
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Call Number |
PLASMANT @ plasmant @c:irua:189502 |
Serial |
7100 |
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Permanent link to this record |
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Author |
Lang, X.; Ouyang, Y.; Vandewalle, L.A.; Goshayeshi, B.; Chen, S.; Madanikashani, S.; Perreault, P.; Van Geem, K.M.; van Geem, K.M. |
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Title |
Gas-solid hydrodynamics in a stator-rotor vortex chamber reactor |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Chemical engineering journal |
Abbreviated Journal |
Chem Eng J |
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Volume |
446 |
Issue |
5 |
Pages |
137323-12 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL) |
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Abstract |
The gas-solid vortex reactor (GSVR) has enormous process intensification potential. However the huge gas consumption can be a serious disadvantage for the GSVR in some applications such as fast pyrolysis. In this work, we demonstrate a recent novel design, where a stator-rotor vortex chamber (STARVOC) is driven by the fluid's kinetic energy, to decouple the solids bed rotation and gas. Gas-solid fluidization by using air and monosized aluminum balls was performed to investigate the hydrodynamics. A constructed fluidization flow regime map for a fixed solids loading of 100 g shows that the bed can only be fluidized for a rotation speed between 200 and 400 RPM. Below 200 RPM, particles settle down on the bottom plate and cannot form a stable bed due to inertia and friction. Above 400 RPM, the bed cannot be fluidized with superficial velocities up to 1.8 m/s (air flow rate of 90 Nm(3)/h). The bed thickness shows some non-uniformities, being smaller at the top of the bed than at the bottom counterpart. However by increasing the air flow rate or rotation speed the axial nonuniformity can be resolved. The bed pressure drop first increases with increasing gas flow rate and then levels off, showing similar characteristics as conventional fluidized beds. Theoretical pressure drops calculated from mathematical models such as Kao et al. model agree well with experimental measurements. Particle velocity discrepancies between the top and bottom particles reveal that the impact of gravity cannot be completely neglected. Design guidelines and possible applications for further development of STARVOC concept are proposed based on fundamental data provided in this work. |
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Wos |
000833418100006 |
Publication Date |
2022-06-01 |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1385-8947; 1873-3212 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 15.1 |
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Call Number |
UA @ admin @ c:irua:189283 |
Serial |
7167 |
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Permanent link to this record |
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Author |
Brienza, F.; Van Aelst, K.; Devred, F.; Magnin, D.; Tschulkow, M.; Nimmegeers, P.; Van Passel, S.; Sels, B.F.; Gerin, P.; Debecker, D.P.; Cybulska, I. |
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Title |
Unleashing lignin potential through the dithionite-assisted organosolv fractionation of lignocellulosic biomass |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chem Eng J |
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Volume |
450 |
Issue |
3 |
Pages |
138179-14 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Engineering Management (ENM); Intelligence in PRocesses, Advanced Catalysts and Solvents (iPRACS) |
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Abstract |
The development of biomass pretreatment approaches that, next to (hemi)cellulose valorization, aim at the conversion of lignin to chemicals is essential for the long-term success of a biorefinery. Herein, we discuss a dithionite-assisted organosolv fractionation (DAOF) of lignocellulose in n-butanol and water to produce cellulosic pulp and mono-/oligo-aromatics. The study frames the technicalities of this biorefinery process and relates them to the features of the obtained product streams. We comprehensively identify and quantify all products of interest: solid pulp (acid hydrolysis-HPLC, ATR-FTIR, XRD, SEM, enzymatic hydrolysis-HPLC), lignin derivatives (GPC, GC-MS/FID, 1H-13C HSQC NMR, ICP-AES), and carbohydrate derivatives (HPLC). These results were used for inspecting the economic feasibility of DAOF. In the best process configuration, a high yield of monophenolics was reached (~20%, based on acid insoluble lignin in birch sawdust). Various other lignocellulosic feedstocks were also explored, showing that DAOF is particularly effective on hardwood and herbaceous biomass. Overall, this study demonstrates that DAOF is a viable fractionation method for the sustainable upgrading of lignocellulosic biomass. |
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Wos |
000888204900005 |
Publication Date |
2022-07-20 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1385-8947; 1873-3212 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 15.1 |
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Call Number |
UA @ admin @ c:irua:189322 |
Serial |
7373 |
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Permanent link to this record |
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Author |
Zhou, R.; Zhou, R.; Xian, Y.; Fang, Z.; Lu, X.; Bazaka, K.; Bogaerts, A.; Ostrikov, K.(K.) |
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Title |
Plasma-enabled catalyst-free conversion of ethanol to hydrogen gas and carbon dots near room temperature |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chem Eng J |
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Volume |
382 |
Issue |
382 |
Pages |
122745 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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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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Wos |
000503381200200 |
Publication Date |
2019-09-07 |
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Series Issue |
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Edition |
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ISSN |
1385-8947; 1873-3212 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15.1 |
Times cited |
20 |
Open Access |
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Notes |
; ; |
Approved ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 15.1; 2020 IF: 6.216 |
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Call Number |
UA @ admin @ c:irua:165648 |
Serial |
6318 |
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Permanent link to this record |
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Author |
Andersen, Ja.; Christensen, Jm.; Østberg, M.; Bogaerts, A.; Jensen, Ad. |
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Title |
Plasma-catalytic dry reforming of methane: Screening of catalytic materials in a coaxial packed-bed DBD reactor |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chem Eng J |
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Volume |
397 |
Issue |
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Pages |
125519 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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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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Wos |
000542296100011 |
Publication Date |
2020-05-17 |
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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 |
1385-8947 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
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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 ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 15.1; 2020 IF: 6.216 |
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Call Number |
PLASMANT @ plasmant @c:irua:170613 |
Serial |
6406 |
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Author |
Ma, Z.; Perreault, P.; Pelegrin, D.C.; Boffito, D.C.; Patience, G.S. |
![goto web page (via DOI) doi](http://nano.uantwerpen.be/nanorefs/img/doi.gif)
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Title |
Thermodynamically unconstrained forced concentration cycling of methane catalytic partial oxidation over CeO2FeCralloy catalysts |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chem Eng J |
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Volume |
380 |
Issue |
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Pages |
122470-11 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL) |
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Abstract |
Converting waste associated natural gas from oil fields is uneconomic with current gas-to-liquid technology. Micro Gas-to-Liquids technology ( GtL) combines process intensification and numbering up economics to reduce capital costs to convert flared and vented natural gas to value-added synthetic fuel: Milli-second contact times in the catalytic partial oxidation of methane (CPOX) integrated with a tandem Fischer-Tropsch (FT) step meets the economic constraints together with remote process control. FeCralloy knitted fibres with high thermal conductivity and low pressure drop, resist thermal and mechanical stresses in the high pressure CPOX step. The FeCralloy catalysts are free of pre-reduction treatments. We deposited Pt and/or CeO2 over the fibre surface via solution combustion synthesis. Methane conversion was higher at ambient pressure compared to 2 MPa while the Pt/CeO2 FeCralloy was relatively inert from 0.1 MPa to 2 MPa. However, both catalysts demonstrated high activity in quasi-chemical looping partial oxidation of methane: during the reduction step while feeding methane, an on-line mass spectrometer only detected H2 while in the oxidation step it detected predominantly CO. Kinetic modeling of the oxidation-reduction cycles suggests that the reaction follows a direct mechanism to produce CO and H2 rather than an indirect mechanism that first produces CO2 and H2O followed by reforming. |
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Publication Date |
2019-08-14 |
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ISSN |
1385-8947; 1873-3212 |
ISBN |
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Additional Links |
UA library record |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
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Approved ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 15.1; 2020 IF: 6.216 |
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Call Number |
UA @ admin @ c:irua:162119 |
Serial |
8665 |
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Permanent link to this record |
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Author |
Wang, J.; Zhang, K.; Bogaerts, A.; Meynen, V. |
![goto web page url](http://nano.uantwerpen.be/nanorefs/img/www.gif)
![find record details (via OpenURL) openurl](img/xref.gif)
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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 |
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Year |
2023 |
Publication |
Chemical engineering journal |
Abbreviated Journal |
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Volume |
464 |
Issue |
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Pages |
142574-12 |
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Keywords |
A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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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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Wos |
000966076400001 |
Publication Date |
2023-03-21 |
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ISSN |
1385-8947; 1873-3212 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 15.1; 2023 IF: 6.216 |
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Call Number |
UA @ admin @ c:irua:194862 |
Serial |
7262 |
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Permanent link to this record |
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Author |
Andersen, Ja.; Holm, Mc.; van 't Veer, K.; Christensen, Jm.; Østberg, M.; Bogaerts, A.; Jensen, Ad. |
![goto web page (via DOI) doi](http://nano.uantwerpen.be/nanorefs/img/doi.gif)
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Title |
Plasma-catalytic ammonia synthesis in a dielectric barrier discharge reactor: A combined experimental study and kinetic modeling |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Chemical engineering journal |
Abbreviated Journal |
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Volume |
457 |
Issue |
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Pages |
141294 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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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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Wos |
001058978000001 |
Publication Date |
2023-01-05 |
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ISSN |
1385-8947 |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
OpenAccess |
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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 ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 15.1; 2023 IF: 6.216 |
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Call Number |
PLASMANT @ plasmant @c:irua:195877 |
Serial |
7234 |
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Permanent link to this record |
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Author |
Morais, E.; Delikonstantis, E.; Scapinello, M.; Smith, G.; Stefanidis, G.D.; Bogaerts, A. |
![goto web page url](http://nano.uantwerpen.be/nanorefs/img/www.gif)
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Title |
Methane coupling in nanosecond pulsed plasmas: Correlation between temperature and pressure and effects on product selectivity |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Chemical engineering journal |
Abbreviated Journal |
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Volume |
462 |
Issue |
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Pages |
142227 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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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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Wos |
000983631500001 |
Publication Date |
2023-03-02 |
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Edition |
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ISSN |
1385-8947 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
OpenAccess |
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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). |
Approved ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 15.1; 2023 IF: 6.216 |
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Call Number |
PLASMANT @ plasmant @c:irua:195881 |
Serial |
7246 |
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Permanent link to this record |
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Author |
Van Alphen, S.; Hecimovic, A.; Kiefer, C.K.; Fantz, U.; Snyders, R.; Bogaerts, A. |
![goto web page url](http://nano.uantwerpen.be/nanorefs/img/www.gif)
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Title |
Modelling post-plasma quenching nozzles for improving the performance of CO2 microwave plasmas |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Chemical engineering journal |
Abbreviated Journal |
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Volume |
462 |
Issue |
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Pages |
142217 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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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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Wos |
000962382600001 |
Publication Date |
2023-03-03 |
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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 |
1385-8947 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
OpenAccess |
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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 ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 15.1; 2023 IF: 6.216 |
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Call Number |
PLASMANT @ plasmant @c:irua:195889 |
Serial |
7250 |
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Permanent link to this record |
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Author |
Liu, R.; Hao, Y.; Wang, T.; Wang, L.; Bogaerts, A.; Guo, H.; Yi, Y. |
![goto web page url](http://nano.uantwerpen.be/nanorefs/img/www.gif)
![find record details (via OpenURL) openurl](img/xref.gif)
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Title |
Hybrid plasma-thermal system for methane conversion to ethylene and hydrogen |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Chemical engineering journal |
Abbreviated Journal |
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Volume |
463 |
Issue |
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Pages |
142442 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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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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Wos |
000953890500001 |
Publication Date |
2023-03-16 |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1385-8947 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
OpenAccess |
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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 ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 15.1; 2023 IF: 6.216 |
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Call Number |
PLASMANT @ plasmant @c:irua:195888 |
Serial |
7253 |
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Permanent link to this record |
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Author |
Van Alphen, S.; Hecimovic, A.; Kiefer, C.K.; Fantz, U.; Snyders, R.; Bogaerts, A. |
![goto web page url](http://nano.uantwerpen.be/nanorefs/img/www.gif)
![find record details (via OpenURL) openurl](img/xref.gif)
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Title |
Modelling post-plasma quenching nozzles for improving the performance of CO2 microwave plasmas |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Chemical engineering journal |
Abbreviated Journal |
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Volume |
462 |
Issue |
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Pages |
142217 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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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 |
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Thesis |
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Place of Publication |
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Editor |
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Wos |
000962382600001 |
Publication Date |
2023-03-03 |
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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 |
1385-8947 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
OpenAccess |
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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 ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 15.1; 2023 IF: 6.216 |
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Call Number |
PLASMANT @ plasmant @c:irua:195889 |
Serial |
7259 |
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Permanent link to this record |
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Author |
Wang, J.; Zhang, K.; Meynen, V.; Bogaerts, A. |
![goto web page url](http://nano.uantwerpen.be/nanorefs/img/www.gif)
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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 |
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Year |
2023 |
Publication |
Chemical engineering journal |
Abbreviated Journal |
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Volume |
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Issue |
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Pages |
142953-29 |
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Keywords |
A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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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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Wos |
000986051300001 |
Publication Date |
2023-04-17 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1385-8947; 1873-3212 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 15.1; 2023 IF: 6.216 |
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Call Number |
UA @ admin @ c:irua:195603 |
Serial |
7264 |
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Permanent link to this record |
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Author |
Orozco-Jimenez, A.J.; Pinilla-Fernandez, D.A.; Pugliese, V.; Bula, A.; Perreault, P.; Gonzalez-Quiroga, A. |
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Title |
Angular momentum based-analysis of gas-solid fluidized beds in vortex chambers |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Chemical engineering journal |
Abbreviated Journal |
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Volume |
457 |
Issue |
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Pages |
141222-21 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL) |
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Abstract |
Gas-solid vortex chambers are a promising alternative for reactive and non-reactive processes requiring enhanced heat and mass transfer rates and order-of-milliseconds contact time. The conservation of angular momentum is instrumental in understanding how the interactions between gas, particulate solids, and chamber walls influence the formation of a rotating solids bed. Therefore, this work applies the conservation of angular momentum to derive a model that gives the average angular velocity of solids in terms of gas injection velocity, wall-solids bed drag coefficient, gas and particle properties, and chamber geometry. Three datasets from published studies, comprising 1 g-Geldart B- and d-type particles in different vortex chambers, validate the model results. Using a sensitivity analysis, we assessed the effect of input variables on the average angular velocity of solids, average void fraction, and average bed height. Results indicate that the top and bottom end-wall boundaries exert the most significant braking effect on the rotating solids bed compared with the cylindrical outer wall and gas injection boundaries. The wall-solids bed drag coefficient appears independent of the gas injection velocity for a wide range of operating conditions. The proposed model is a valuable tool for analyzing and comparing gas–solid vortex typologies, unraveling improvement opportunities, and scale-up. |
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Wos |
000951011600001 |
Publication Date |
2022-12-29 |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1385-8947; 1873-3212 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 15.1; 2023 IF: 6.216 |
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Call Number |
UA @ admin @ c:irua:192868 |
Serial |
7282 |
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Permanent link to this record |
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Author |
Ag, K.R.; Minja, A.C.; Ninakanti, R.; Van Hal, M.; Dingenen, F.; Borah, R.; Verbruggen, S.W. |
![goto web page url](http://nano.uantwerpen.be/nanorefs/img/www.gif)
![find record details (via OpenURL) openurl](img/xref.gif)
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Title |
Impact of soot deposits on waste gas-to-electricity conversion in a TiO₂/WO₃-based photofuel cell |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Chemical engineering journal |
Abbreviated Journal |
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Volume |
470 |
Issue |
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Pages |
144390-13 |
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Keywords |
A1 Journal article; Engineering sciences. Technology |
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Abstract |
An unbiased photo-fuel cell (PFC) is a device that integrates the functions of a photoanode and a cathode to achieve simultaneous light-driven oxidation and dark reduction reactions. As such, it generates electricity while degrading pollutants like volatile organic compounds (VOCs). The photoanode is excited by light to generate electron-hole pairs, which give rise to a photocurrent, and are utilized to oxidise organic pollutants simultaneously. Here we have systematically studied various TiO2/WO3 photoanodes towards their photocatalytic soot degradation performance, PFC performance in the presence of VOCs, and the combination of both. The latter thus mimics an urban environment where VOCs and soot are present simultaneously. The formation of a type-II heterojunction after the addition of a thin TiO2 top layer over a dense WO3 bottom layer, improved both soot oxidation efficiency as well as photocurrent generation, thus paving the way towards low-cost PFC technology for energy recovery from real polluted air. |
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Wos |
001030456200001 |
Publication Date |
2023-06-25 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1385-8947; 1873-3212 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
Not_Open_Access: Available from 29.12.2023 |
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Notes |
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Approved ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 15.1; 2023 IF: 6.216 |
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Call Number |
UA @ admin @ c:irua:197222 |
Serial |
8882 |
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Permanent link to this record |
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Author |
Zhang, K.; Wang, J.; Ninakanti, R.; Verbruggen, S.W. |
![goto web page url](http://nano.uantwerpen.be/nanorefs/img/www.gif)
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Title |
Solvothermal synthesis of mesoporous TiO2 with tunable surface area, crystal size and surface hydroxylation for efficient photocatalytic acetaldehyde degradation |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Chemical engineering journal |
Abbreviated Journal |
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Volume |
474 |
Issue |
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Pages |
145188-14 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Laboratory of adsorption and catalysis (LADCA) |
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Abstract |
Photocatalytic acetaldehyde degradation exhibits satisfactory performance only at relatively low acetaldehyde flow rates, predominately below 10 × 10-3 mL/min, leaving ample room for improvement. Therefore, it is necessary to prepare more efficient photocatalysts for acetaldehyde degradation. Moreover, the impact of the interaction strength between the titania surface and surface water on the photocatalytic acetaldehyde efficiency is poorly understood. To address these issues, in this work a series of (0 0 1)-faceted anatase titania samples with various surface properties and structures were synthesized via a solvothermal method and tested at high acetaldehyde flow rates under UV light irradiation. With increasing solvothermal time, the pore volume, surface area, and the abundance of surface OH groups all increased, while the crystallite size decreased. These were all identified to be beneficial to promote the degradation performance. When the solvothermal temperature was 180 ℃ and the reaction time was 5 h, the prepared sample displayed the most efficient performance at 19.25× 10-3 mL/min of acetaldehyde (conversion of (74 ± 1)% versus (29 ± 1)% for P25), and achieved a 100 % conversion at 16 × 10-3 mL/min. A weaker interaction strength between surface water and the titania surface was found to improve the acetaldehyde adsorption capacity, thereby promoting the acetaldehyde degradation efficiency. The stability of the best performing sample was tested over 48 h, demonstrating a highly stable performance with no signs of deactivation. Even at a relative humidity of 30 %, the acetaldehyde conversion retains 82% of its efficiency in a dry atmosphere, highlighting its potential in practical applications. |
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Wos |
001144928800001 |
Publication Date |
2023-08-05 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1385-8947; 1873-3212 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
Not_Open_Access: Available from 06.02.2024 |
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Notes |
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Approved ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 15.1; 2023 IF: 6.216 |
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Call Number |
UA @ admin @ c:irua:198652 |
Serial |
8933 |
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Permanent link to this record |
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Author |
Vingerhoets, R.; Brienza, C.; Sigurnjak, I.; Buysse, J.; Vlaeminck, S.E.; Spiller, M.; Meers, E. |
![goto web page (via DOI) doi](http://nano.uantwerpen.be/nanorefs/img/doi.gif)
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Title |
Ammonia stripping and scrubbing followed by nitrification and denitrification saves costs for manure treatment based on a calibrated model approach |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Chemical engineering journal |
Abbreviated Journal |
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Volume |
477 |
Issue |
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Pages |
146984-14 |
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Keywords |
A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL) |
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Abstract |
Resource-efficient nitrogen management is of high environmental and economic interest, and manure represents the major nutrient flow in livestock-intensive regions. Ammonia stripping/scrubbing (SS) is an appealing nitrogen recovery route from manure, yet its real-life implementation has been limited thus far. In nutrient surplus regions like Flanders, treatment of the liquid fraction (LF) of (co–)digested manure typically consists of nitrification/denitrification (NDN) removing most N as nitrogen gas. Integrating SS before NDN in existing plants would expand treatment capacity and recover N while maintaining low N effluent values, yet cost estimations of this novel approach after process optimisation are not yet available. A programming model was developed and calibrated to minimise the treatment costs of this approach and find the balance between N recovery versus N removal. Four crucial operational parameters (CO2 stripping time, NH3 stripping time, temperature and NaOH addition) were optimised for 18 scenarios which were different in terms of technical set-up, influent characteristics and scrubber acid. The model shows that SS before NDN can decrease the costs by 1 to 56% under optimal conditions compared to treatment with NDN only, with 1 to 8% reduction for the LF of manure (22–29% recovered of N treated), and 11 to 56% reduction for the LF of co-digested manure (42–67% recovered of N treated), primarily dependent on resource pricing. This study shows the power of modelling for minimum-cost design and operation of manure treatment yielding savings while producing useful N recovery products with SS followed by NDN. |
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Wos |
001108935900001 |
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 |
1385-8947; 1873-3212 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
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Notes |
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Approved ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 15.1; 2023 IF: 6.216 |
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Call Number |
UA @ admin @ c:irua:200649 |
Serial |
9003 |
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Permanent link to this record |
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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. |
![goto web page url](http://nano.uantwerpen.be/nanorefs/img/www.gif)
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Title |
Inhibiting recombination to improve the performance of plasma-based CO2 conversion |
Type |
A1 Journal Article |
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Year |
2024 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chemical Engineering Journal |
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Volume |
481 |
Issue |
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Pages |
148684 |
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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) ; |
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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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Wos |
001168999200001 |
Publication Date |
2024-01-10 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1385-8947 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
Not_Open_Access |
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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 ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 15.1; 2024 IF: 6.216 |
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Call Number |
PLASMANT @ plasmant @c:irua:204352 |
Serial |
8993 |
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Permanent link to this record |
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Author |
De Meyer, R.; Gorbanev, Y.; Ciocarlan, R.-G.; Cool, P.; Bals, S.; Bogaerts, A. |
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Title |
Importance of plasma discharge characteristics in plasma catalysis: Dry reforming of methane vs. ammonia synthesis |
Type |
A1 Journal Article |
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Year |
2024 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chemical Engineering Journal |
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Volume |
488 |
Issue |
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Pages |
150838 |
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Keywords |
A1 Journal Article; Gas conversion Dry reforming of methane Ammonia Microdischarges Dielectric barrier discharge; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
Plasma catalysis is a rapidly growing field, often employing a packed-bed dielectric barrier discharge plasma reactor. Such dielectric barrier discharges are complex, especially when a packing material (e.g., a catalyst) is introduced in the discharge volume. Catalysts are known to affect the plasma discharge, though the underlying mechanisms influencing the plasma physics are not fully understood. Moreover, the effect of the catalysts on the plasma discharge and its subsequent effect on the overall performance is often overlooked. In this work, we deliberately design and synthesize catalysts to affect the plasma discharge in different ways. These Ni or Co alumina-based catalysts are used in plasma-catalytic dry reforming of methane and ammonia synthesis. Our work shows that introducing a metal to the dielectric packing can affect the plasma discharge, and that the distribution of the metal is crucial in this regard. Further, the altered discharge can greatly influence the overall performance. In an atmospheric pressure dielectric barrier discharge reactor, this apparently more uniform plasma yields a significantly better performance for ammonia synthesis compared to the more conventional filamentary discharge, while it underperforms in dry reforming of methane. This study stresses the importance of analyzing the plasma discharge in plasma catalysis experiments. We hope this work encourages a more critical view on the plasma discharge characteristics when studying various catalysts in a plasma reactor. |
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Wos |
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Publication Date |
2024-03-30 |
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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 |
1385-8947 |
ISBN |
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Additional Links |
UA library record |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
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Notes |
This research was supported 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 ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 15.1; 2024 IF: 6.216 |
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Call Number |
PLASMANT @ plasmant @c:irua:205154 |
Serial |
9115 |
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Permanent link to this record |
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Author |
Maerivoet, S.; Tsonev, I.; Slaets, J.; Reniers, F.; Bogaerts, A. |
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Title |
Coupled multi-dimensional modelling of warm plasmas: Application and validation for an atmospheric pressure glow discharge in CO2/CH4/O2 |
Type |
A1 Journal Article |
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Year |
2024 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chemical Engineering Journal |
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Volume |
492 |
Issue |
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Pages |
152006 |
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Keywords |
A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
To support experimental research into gas conversion by warm plasmas, models should be developed to explain the experimental observations. These models need to describe all physical and chemical plasma properties in a coupled way. In this paper, we present a modelling approach to solve the complete set of assumed relevant equations, including gas flow, heat balance and species transport, coupled with a rather extensive chemistry set, consisting of 21 species, obtained by reduction of a more detailed chemistry set, consisting of 41 species. We apply this model to study the combined CO2 and CH4 conversion in the presence of O2, in a direct current atmospheric pressure glow discharge. Our model can predict the experimental trends, and can explain why higher O2 fractions result in higher CH4 conversion, namely due to the higher gas temperature, rather than just by additional chemical reactions. Indeed, our model predicts that when more O2 is added, the energy required to reach any set temperature (i.e., the enthalpy) drops, allowing the system to reach higher temperatures with similar amounts of energy. This is in turn related to the higher H2O fraction and lower H2 fraction formed in the plasma, as demonstrated by our model. Altogether, our new self-consistent model can capture the main physics and chemistry occurring in this warm plasma, which is an important step towards predictive modelling for plasma-based gas conversion. |
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Wos |
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Publication Date |
2024-05-09 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1385-8947 |
ISBN |
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Additional Links |
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Impact Factor |
15.1 |
Times cited |
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Open Access |
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Notes |
This research was supported by the Excellence of Science FWO-FNRS project (FWO grant ID G0I1822N; EOS ID 40007511) and the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No. 810182–SCOPE ERC Synergy project, and grant agreement No. 101081162–PREPARE ERC Proof of Concept project). computational resources and services used in this work were provided by the HPC core facility CalcUA of the Universiteit Antwerpen, and VSC (Flemish Supercomputer Center), funded by the Research Foundation – Flanders (FWO) and the Flemish Government. |
Approved ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 15.1; 2024 IF: 6.216 |
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Call Number |
PLASMANT @ plasmant @ |
Serial |
9132 |
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Permanent link to this record |
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Author |
Blommaerts, N.; Asapu, R.; Claes, N.; Bals, S.; Lenaerts, S.; Verbruggen, S.W. |
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Title |
Gas phase photocatalytic spiral reactor for fast and efficient pollutant degradation |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
Chemical engineering journal |
Abbreviated Journal |
Chem Eng J |
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Volume |
316 |
Issue |
316 |
Pages |
850-856 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Sustainable Energy, Air and Water Technology (DuEL) |
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Abstract |
Photocatalytic reactors for the degradation of gaseous organic pollutants often suffer from major limitations such as small reaction area, sub-optimal irradiation conditions and thus limited reaction rate. In this work, an alternative solution is presented that involves a glass tube coated on the inside with (silvermodified) TiO2 and spiraled around a UVA lamp. First, the spiral reactor is coated from the inside with TiO2 using an experimentally verified procedure that is optimized toward UV light transmission. This procedure is kept as simple as possible and involves a single casting step of a 1 wt% suspension of TiO2 in ethanol through the spiral. This results in a coated tube that absorbs nearly all incident UV light under the experimental conditions used. The optimized coated spiral reactor is then benchmarked to a conventional annular photoreactor of the same outer dimensions and total catalyst loading over a broad range of experimental conditions. Although residence time distribution experiments indicate slightly longer dwelling of molecules in the spiral reactor, no significant difference in by-passing of gas between the spiral reactor and the annular reactor can be claimed. Acetaldehyde degradation efficiency of 100% is obtained with the spiral reactor for a residence time as low as 60 s, whereas the annular reactor could not achieve full degradation even at 1000 s residence time. In a final case study, addition of long-term stable silver nanoparticles, protected by an ultra-thin polymer shell applied via the layer-by-layer (LbL) method, to the spiral reactor coating is shown to double the degradation efficiency and provides an interesting strategy to cope with higher pollutant concentrations without changing the overall dimensions. |
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Wos |
000398985200089 |
Publication Date |
2017-02-08 |
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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 |
1385-8947 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
6.216 |
Times cited |
30 |
Open Access |
OpenAccess |
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Notes |
N.B. wishes to thank the University of Antwerp – Belgium for financial support. N.C. and S.B. acknowledge financial support from European Research Council (ERC Starting Grant #335078- COLOURATOM). S.W.V. acknowledges the Research Foundation – Flanders (FWO) for a postdoctoral fellowship. (ROMEO:green; preprint:; postprint:can ; pdfversion:cannot); ecas_sara |
Approved ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 6.216 |
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Call Number |
EMAT @ emat @ c:irua:140925UA @ admin @ c:irua:140925 |
Serial |
4481 |
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Permanent link to this record |
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Author |
Wang, W.; Mei, D.; Tu, X.; Bogaerts, A. |
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Title |
Gliding arc plasma for CO 2 conversion: Better insights by a combined experimental and modelling approach |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
Chemical engineering journal |
Abbreviated Journal |
Chem Eng J |
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Volume |
330 |
Issue |
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Pages |
11-25 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
A gliding arc plasma is a potential way to convert CO2 into CO and O2, due to its non-equilibrium character, but little is known about the underlying mechanisms. In this paper, a self-consistent two-dimensional (2D) gliding arc model is developed, with a detailed non-equilibrium CO2 plasma chemistry, and validated with experiments. Our calculated values of the electron number density in the plasma, the CO2 conversion and energy efficiency show reasonable agreement with the experiments, indicating that the model can provide a realistic picture of the plasma chemistry. Comparison of the results with classical thermal conversion, as well as other plasma-based technologies for CO2 conversion reported in literature, demonstrates the non-equilibrium character of the gliding arc, and indicates that the gliding arc is a promising plasma reactor for CO2 conversion. However, some process modifications should be exploited to further improve its performance. As the model provides a realistic picture of the plasma behaviour, we use it first to investigate the plasma characteristics in a whole gliding arc cycle, which is necessary to understand the underlying mechanisms. Subsequently, we perform a chemical kinetics analysis, to investigate the different pathways for CO2 loss and formation. Based on the revealed discharge properties and the underlying CO2 plasma chemistry, the model allows us to propose solutions on how to further improve the
CO2 conversion and energy efficiency by a gliding arc plasma. |
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Wos |
000414083300002 |
Publication Date |
2017-07-22 |
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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 |
1385-8947 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
6.216 |
Times cited |
38 |
Open Access |
OpenAccess |
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Notes |
This research was supported by the European Marie Skłodowska- Curie Individual Fellowship “GlidArc” within Horizon 2020 (Grant No. 657304) and by the FWO project (grant G.0383.16N). The support of this experimental work by the EPSRC CO2Chem Seedcorn Grant and the FWO travel grant for study abroad (Grant K2.128.17N) is gratefully acknowledged. 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 ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 6.216 |
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Call Number |
PLASMANT @ plasmant @c:irua:145033 |
Serial |
4636 |
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Permanent link to this record |
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Author |
Michielsen, I.; Uytdenhouwen, Y.; Pype, J.; Michielsen, B.; Mertens, J.; Reniers, F.; Meynen, V.; Bogaerts, A. |
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Title |
CO 2 dissociation in a packed bed DBD reactor: First steps towards a better understanding of plasma catalysis |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
Chemical engineering journal |
Abbreviated Journal |
Chem Eng J |
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Volume |
326 |
Issue |
326 |
Pages |
477-488 |
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Keywords |
A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
Plasma catalysis is gaining increasing interest for CO2 conversion, but the interaction between the plasma and catalyst is still poorly understood. This is caused by limited systematic materials research, since most works combine a plasma with commercial supported catalysts and packings. In the present paper, we study the influence of specific material and reactor properties, as well as reactor/bead configuration, on the conversion and energy efficiency of CO2 dissociation in a packed bed dielectric barrier discharge (DBD) reactor. Of the various packing materials investigated, BaTiO3 yields the highest conversion and energy efficiency, i.e., 25% and 4.5%.
Our results show that, when evaluating the influence of catalysts, the impact of the packing (support) material itself cannot be neglected, since it can largely affect the conversion and energy efficiency. This shows the large potential for further improvement of packed bed plasma reactors for CO2 conversion and other chemical conversion reactions by adjusting both packing (support) properties and catalytically active sites. Moreover, we clearly prove that comparison of results obtained in different reactor setups should be done with care, since there is a large effect of the reactor setup and reactor/bead configuration. |
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Place of Publication |
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Language |
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Wos |
000406137200047 |
Publication Date |
2017-06-01 |
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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 |
1385-8947 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
6.216 |
Times cited |
49 |
Open Access |
OpenAccess |
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Notes |
This research was carried out with financial support of the Institute for the Promotion of Innovation by Science and Technology in Flanders (IWT Flanders) for both I. Michielsen (IWT-141093) and J. Pype (IWT-131229) and of the Walloon region through the excellence programme FLYCOAT (nr. 1318147) for the profilometry measurements. The authors also acknowledge financial support from an IOF-SBO project from the University of Antwerp and from the Fund for Scientific Research (FWO; grant number: G.0254.14 N). This research was carried out in the framework of the network on Physical Chemistry of Plasma-Surface Interactions – Interuniversity Attraction Poles, phase VII (http://psi-iap7.ulb. ac.be/), and supported by the Belgian Science Policy Office (BELSPO). The authors would also like to thank Koen Van Laer for the discussions on this manuscript. |
Approved ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 6.216 |
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Call Number |
PLASMANT @ plasmant @ c:irua:144802 |
Serial |
4626 |
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Permanent link to this record |
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Author |
Gholampour, N.; Chaemchuen, S.; Hu, Z.-Y.; Mousavi, B.; Van Tendeloo, G.; Verpoort, F. |
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Title |
Simultaneous creation of metal nanoparticles in metal organic frameworks via spray drying technique |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
Chemical engineering journal |
Abbreviated Journal |
Chem Eng J |
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Volume |
322 |
Issue |
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Pages |
702-709 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
In-situ fabrication of palladium(0) nanoparticles inside zeolitic imidazolate frameworks (ZIF-8) has been established via one-step facile spray-dry technique. Crystal structures and morphologies of the Pd@ZIF-8 samples are investigated by powder XRD, TEM, SAED, STEM, and EDX techniques. High angle annular dark field scanning transmission electron microscopy (HAAD-STEM) and 3D tomographic analysis confirm the presence of palladium nanoparticles inside the ZIF-8 structure. The porosity, surface area and N-2 physisorption properties are evaluated for Pd@ZIF-8 with various palladium contents. Furthermore, Pd@ZIF-8 samples are effectively applied as heterogeneous catalysts in alkenes hydrogenation. This straightforward method is able to speed up the synthesis of encapsulation of metal nanoparticles in metal organic frameworks. (C) 2017 Elsevier B.V. All rights reserved. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
Lausanne |
Editor |
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Language |
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Wos |
000401594200069 |
Publication Date |
2017-04-19 |
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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 |
1385-8947; 0300-9467 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
6.216 |
Times cited |
14 |
Open Access |
OpenAccess |
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Notes |
; The authors would like to express their deep accolade to “State Key Laboratory of Advanced Technology for Materials Synthesis and Processing” for financial support. S.C. appreciates of the National Natural Science Foundation of China (303-41150231), the Fundamental Research Funds for the Central Universities (WUT: 2016IVA092) and the Research Fund for the Doctoral Program of Higher Education of China (471-40120222). N.G. thanks the Chinese Scholarship Council (CSC) for her Ph.D. study grant 2013GXZ985. Z.-Y. H and G. V.T. acknowledge the support from the EC Framework 7 program ESTEEM2 (Reference 312483). ; |
Approved ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 6.216 |
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Call Number |
UA @ lucian @ c:irua:144152 |
Serial |
4686 |
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Permanent link to this record |
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Author |
Wang, W.; Kim, H.-H.; Van Laer, K.; Bogaerts, A. |
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Title |
Streamer propagation in a packed bed plasma reactor for plasma catalysis applications |
Type |
A1 Journal article |
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Year |
2018 |
Publication |
Chemical engineering journal |
Abbreviated Journal |
Chem Eng J |
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Volume |
334 |
Issue |
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Pages |
2467-2479 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
A packed bed dielectric barrier discharge (DBD) is widely used for plasma catalysis applications, but the exact plasma characteristics in between the packing beads are far from understood. Therefore, we study here these plasma characteristics by means of fluid modelling and experimental observations using ICCD imaging, for packing materials with different dielectric constants. Our study reveals that a packed bed DBD reactor in dry air at atmospheric pressure may show three types of discharges, i.e. positive restrikes, filamentary microdischarges, which can also be localized between two packing beads, and surface discharges (so-called surface ionization
waves). Restrikes between the dielectric surfaces result in the formation of filamentary microdischarges, while surface charging creates electric field components parallel to the dielectric surfaces, leading to the formation of surface discharges. A transition in discharge mode occurs from surface discharges to local filamentary discharges between the packing beads when the dielectric constant of the packing rises from 5 to 1000. This may have implications for the efficiency of plasma catalytic gas treatment, because the catalyst activation may be limited by constraining the discharge to the contact points of the beads. The production of reactive species occurs most in the positive restrikes, the surface discharges and the local microdischarges in between the beads, and is less significant in the longer filamentary microdischarges. The faster streamer propagation and discharge development with higher dielectric constant of the packing beads leads to a faster production of reactive species. This study is of great interest for plasma catalysis, where packing beads with different dielectric constants are often used as supports for the catalytic materials. It allows us to better understand how different packing materials can influence the performance of packed bed plasma reactors for environmental applications. |
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Place of Publication |
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Language |
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Wos |
000418533400246 |
Publication Date |
2017-11-23 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1385-8947 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
6.216 |
Times cited |
36 |
Open Access |
Not_Open_Access: Available from 10.01.2020
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Notes |
We acknowledge financial support from the Fund for Scientific Research Flanders (FWO) (grant nos G.0217.14 N, G.0254.14 N and G.0383.16 N), the TOP-BOF project of the University of Antwerp, the European Marie Skłodowska-Curie Individual Fellowship “GlidArc” within Horizon2020 (Grant No. 657304) and the Institute for the Promotion of Innovation by Science and Technology in Flanders (IWT Flanders). This research was carried out in the framework of the network on Physical Chemistry of Plasma-Surface Interactions – Interuniversity Attraction Poles, phase VII (http://psi-iap7.ulb.ac.be/), and supported by the Belgian Science Policy Office (BELSPO). The calculations were carried out 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 ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 6.216 |
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Call Number |
PLASMANT @ plasmant @c:irua:147864 |
Serial |
4800 |
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Permanent link to this record |
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Author |
Uytdenhouwen, Y.; Van Alphen, S.; Michielsen, I.; Meynen, V.; Cool, P.; Bogaerts, A. |
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Title |
A packed-bed DBD micro plasma reactor for CO 2 dissociation: Does size matter? |
Type |
A1 Journal article |
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Year |
2018 |
Publication |
Chemical engineering journal |
Abbreviated Journal |
Chem Eng J |
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Volume |
348 |
Issue |
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Pages |
557-568 |
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Keywords |
A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
DBD plasma reactors are of great interest for environmental and energy applications, such as CO2 conversion, but they suffer from limited conversion and especially energy efficiency. The introduction of packing materials has been a popular subject of investigation in order to increase the reactor performance. Reducing the discharge gap of the reactor below one millimetre can enhance the plasma performance as well. In this work, we combine both effects and use a packed-bed DBD micro plasma reactor to investigate the influence of gap size reduction, in combination with a packing material, on the conversion and efficiency of CO2 dissociation. Packing materials used in this work were SiO2, ZrO2, and Al2O3 spheres as well as glass wool. The results are compared to a regular size reactor as a benchmark. Reducing the discharge gap can greatly increase the CO2 conversion, although at a lower energy efficiency. Adding a packing material further increases the conversion when keeping a constant residence time, but is greatly dependent on the material composition, gap and sphere size used. Maximum conversions of 50–55% are obtained for very long residence times (30 s and higher) in an empty reactor or with certain packing material combinations, suggesting a balance in CO2 dissociation and recombination reactions. The maximum energy efficiency achieved is 4.3%, but this is for the regular sized reactor at a short residence time (7.5 s). Electrical characterization is performed to reveal some trends in the electrical behaviour of the plasma upon reduction of the discharge gap and addition of a packing material. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000434467000055 |
Publication Date |
2018-05-03 |
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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 |
1385-8947 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
6.216 |
Times cited |
22 |
Open Access |
Not_Open_Access: Available from 03.05.2020
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Notes |
We acknowledge financial support from the European Fund for Regional Development through the cross-border collaborative Interreg V program Flanders-the Netherlands (project EnOp), the Fund for Scientific Research (FWO; Grant Number: G.0254.14N) and an IOF-SBO (SynCO2Chem) project from the University of Antwerp. |
Approved ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 6.216 |
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Call Number |
PLASMANT @ plasmant @c:irua:151238 |
Serial |
4956 |
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Permanent link to this record |
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Author |
Zhang, H.; Wang, W.; Li, X.; Han, L.; Yan, M.; Zhong, Y.; Tu, X. |
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Title |
Plasma activation of methane for hydrogen production in a N2 rotating gliding arc warm plasma : a chemical kinetics study |
Type |
A1 Journal article |
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Year |
2018 |
Publication |
Chemical engineering journal |
Abbreviated Journal |
Chem Eng J |
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Volume |
345 |
Issue |
345 |
Pages |
67-78 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
In this work, a chemical kinetics study on methane activation for hydrogen production in a warm plasma, i.e., N-2 rotating gliding arc (RGA), was performed for the first time to get new insights into the underlying reaction mechanisms and pathways. A zero-dimensional chemical kinetics model was developed, which showed a good agreement with the experimental results in terms of the conversion of CH4 and product selectivities, allowing us to get a better understanding of the relative significance of various important species and their related reactions to the formation and loss of CH4, H-2, and C2H2 etc. An overall reaction scheme was obtained to provide a realistic picture of the plasma chemistry. The results reveal that the electrons and excited nitrogen species (mainly N-2(A)) play a dominant role in the initial dissociation of CH4. However, the H atom induced reaction CH4+ H -> CH3+ H-2, which has an enhanced reaction rate due to the high gas temperature (over 1200 K), is the major contributor to both the conversion of CH4 and H-2 production, with its relative contributions of > 90% and > 85%, respectively, when only considering the forward reactions. The coexistence and interaction of thermochemical and plasma chemical processes in the rotating gliding arc warm plasma significantly enhance the process performance. The formation of C-2 hydrocarbons follows a nearly one-way path of C2H6 -> C2H4 -> C2H2, explaining why the selectivities of C-2 products decreased in the order of C2H2 > C2H4 > C2H6. |
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Corporate Author |
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Thesis |
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Publisher |
Elsevier Sequoia |
Place of Publication |
Lausanne |
Editor |
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Language |
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Wos |
000430696500008 |
Publication Date |
2018-03-24 |
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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 |
1385-8947; 1873-3212 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
6.216 |
Times cited |
25 |
Open Access |
OpenAccess |
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Notes |
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Approved ![sorted by Approved field, ascending order (up)](img/sort_asc.gif) |
Most recent IF: 6.216 |
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Call Number |
UA @ lucian @ c:irua:151450 |
Serial |
5036 |
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Permanent link to this record |