| Records |
| Author |
Blommaerts, N.; Hoeven, N.; Arenas Esteban, D.; Campos, R.; Mertens, M.; Borah, R.; Glisenti, A.; De Wael, K.; Bals, S.; Lenaerts, S.; Verbruggen, S.W.; Cool, P. |
| Title |
Tuning the turnover frequency and selectivity of photocatalytic CO2 reduction to CO and methane using platinum and palladium nanoparticles on Ti-Beta zeolites |
Type |
A1 Journal article |
| Year |
2021 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chem Eng J |
| Volume |
410 |
Issue |
|
Pages |
128234 |
| Keywords |
A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL); Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
| Abstract |
A Ti-Beta zeolite was used in gas phase photocatalytic CO2 reduction to reduce the charge recombination rate and increase the surface area compared to P25 as commercial benchmark, reaching 607 m2 g-1. By adding Pt nanoparticles, the selectivity can be tuned toward CO, reaching a value of 92% and a turnover frequency (TOF) of 96 µmol.gcat-1.h-1, nearly an order of magnitude higher in comparison with P25. By adding Pd nanoparticles the selectivity can be shifted from CO (70% for a bare Ti-Beta zeolite), toward CH4 as the prevalent species (60%). In this way, the selectivity toward CO or CH4 can be tuned by either using Pt or Pd. The TOF values obtained in this work outperform reported state-of-the-art values in similar research. The improved activity by adding the nanoparticles was attributed to an improved charge separation efficiency, together with a plasmonic contribution of the metal nanoparticles under the applied experimental conditions. |
| Address |
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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 |
000623394200004 |
Publication Date |
2021-01-09 |
| 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 |
| Impact Factor |
6.216 |
Times cited |
15 |
Open Access |
OpenAccess |
| Notes |
N.B., S.L., S.W.V. and P.C. wish to thank the Flemish government and Catalisti for financial support and coordination in terms of a sprint SBO in the context of the moonshot project D2M. N.H. thanks the Flanders Innovation and Entrepreneurship (VLAIO) for the financial support. The Systemic Physiological and Ecotoxicological Research (SPHERE) group, R. Blust, University of Antwerp is acknowledged for the ICP-MS measurements. |
Approved |
Most recent IF: 6.216 |
| Call Number |
EMAT @ emat @c:irua:174591 |
Serial |
6662 |
| Permanent link to this record |
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| Author |
Girard-Sahun, F.; Biondo, O.; Trenchev, G.; van Rooij, G.; Bogaerts, A. |
| Title |
Carbon bed post-plasma to enhance the CO2 conversion and remove O2 from the product stream |
Type |
A1 Journal article |
| Year |
2022 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chem Eng J |
| Volume |
442 |
Issue |
|
Pages |
136268 |
| Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
| Abstract |
CO2 conversion by plasma technology is gaining increasing interest. We present a carbon (charcoal) bed placed after a Gliding Arc Plasmatron (GAP) reactor, to enhance the CO2 conversion, promote O/O2 removal and in crease the CO fraction in the exhaust mixture. By means of an innovative (silo) system, the carbon is constantly supplied, to avoid carbon depletion upon reaction with O/O2. Using this carbon bed, the CO2 conversion is enhanced by almost a factor of two (from 7.6 to 12.6%), while the CO concentration even increases by a factor of three (from 7.2 to 21.9%), and O2 is completely removed from the exhaust mixture. Moreover, the energy ef ficiency of the conversion process drastically increases from 27.9 to 45.4%, and the energy cost significantly drops from 41.9 to 25.4 kJ.L− 1. We also present the temperature as a function of distance from the reactor outlet, as well as the CO2, CO and O2 concentrations and the temperature in the carbon bed as a function of time, which is important for understanding the underlying mechanisms. Indeed, these time-resolved measurements reveal that the initial enhancements in CO2 conversion and in CO concentration are not maintained in our current setup. Therefore, we present a model to study the gasification of carbon with different feed gases (i.e., O2, CO and CO2 separately), from which we can conclude that the oxygen coverage at the surface plays a key role in determining the product composition and the rate of carbon consumption. Indeed, our model insights indicate that the drop in CO2 conversion and in CO concentration after a few minutes is attributed to deactivation of the carbon bed, due to rapid formation of oxygen complexes at the surface. |
| Address |
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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 |
000797716700002 |
Publication Date |
0000-00-00 |
| 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 |
| Impact Factor |
15.1 |
Times cited |
|
Open Access |
OpenAccess |
| Notes |
Horizon 2020 Marie Skłodowska-Curie Actions; European Research Council; This research was supported by the European Research Council (ERC) under the European Union’s Horizon 2020 Research and Innovation programme (grant agreement No 810182 – SCOPE ERC Synergy project) and the European Union’s Horizon 2020 Research and Innovation programme under the Marie Sklodowska-Curie grant agreement No 813393 (PIONEER). The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit |
Approved |
Most recent IF: 15.1 |
| Call Number |
PLASMANT @ plasmant @c:irua:188286 |
Serial |
7052 |
| Permanent link to this record |
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| Author |
Girard-Sahun, F.; Biondo, O.; Trenchev, G.; van Rooij, G.; Bogaerts, A. |
| Title |
Carbon bed post-plasma to enhance the CO2 conversion and remove O2 from the product stream |
Type |
A1 Journal article |
| Year |
2022 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chem Eng J |
| Volume |
442 |
Issue |
|
Pages |
136268 |
| Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
| Abstract |
CO2 conversion by plasma technology is gaining increasing interest. We present a carbon (charcoal) bed placed after a Gliding Arc Plasmatron (GAP) reactor, to enhance the CO2 conversion, promote O/O2 removal and in crease the CO fraction in the exhaust mixture. By means of an innovative (silo) system, the carbon is constantly supplied, to avoid carbon depletion upon reaction with O/O2. Using this carbon bed, the CO2 conversion is enhanced by almost a factor of two (from 7.6 to 12.6%), while the CO concentration even increases by a factor of three (from 7.2 to 21.9%), and O2 is completely removed from the exhaust mixture. Moreover, the energy ef ficiency of the conversion process drastically increases from 27.9 to 45.4%, and the energy cost significantly drops from 41.9 to 25.4 kJ.L− 1. We also present the temperature as a function of distance from the reactor outlet, as well as the CO2, CO and O2 concentrations and the temperature in the carbon bed as a function of time, which is important for understanding the underlying mechanisms. Indeed, these time-resolved measurements reveal that the initial enhancements in CO2 conversion and in CO concentration are not maintained in our current setup. Therefore, we present a model to study the gasification of carbon with different feed gases (i.e., O2, CO and CO2 separately), from which we can conclude that the oxygen coverage at the surface plays a key role in determining the product composition and the rate of carbon consumption. Indeed, our model insights indicate that the drop in CO2 conversion and in CO concentration after a few minutes is attributed to deactivation of the carbon bed, due to rapid formation of oxygen complexes at the surface. |
| Address |
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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 |
000797716700002 |
Publication Date |
0000-00-00 |
| 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 |
| Impact Factor |
15.1 |
Times cited |
|
Open Access |
OpenAccess |
| Notes |
Horizon 2020 Marie Skłodowska-Curie Actions; European Research Council; This research was supported by the European Research Council (ERC) under the European Union’s Horizon 2020 Research and Innovation programme (grant agreement No 810182 – SCOPE ERC Synergy project) and the European Union’s Horizon 2020 Research and Innovation programme under the Marie Sklodowska-Curie grant agreement No 813393 (PIONEER). The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UAntwerpen), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the UAntwerpen. We also thank R. De Meyer, K. Leyssens and S. Defossé for performing the charcoal characterizations. |
Approved |
Most recent IF: 15.1 |
| Call Number |
PLASMANT @ plasmant @c:irua:188286 |
Serial |
7053 |
| 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. |
| Title |
Effusion nozzle for energy-efficient NOx production in a rotating gliding arc plasma reactor |
Type |
A1 Journal article |
| Year |
2022 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chem Eng J |
| Volume |
443 |
Issue |
|
Pages |
136529 |
| Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
| Abstract |
Plasma-based NOx production is of interest for sustainable N2 fixation, but more research is needed to improve its performance. One of the current limitations is recombination of NO back into N2 and O2 molecules immediately after the plasma reactor. Therefore, we developed a novel so-called “effusion nozzle”, to improve the performance of a rotating gliding arc plasma reactor for NOx production, but the same principle can also be applied to other plasma types. Experiments in a wide range of applied power, gas flow rates and N2/O2 ratios demonstrate an enhancement in NOx concentration by about 8%, and a reduction in energy cost by 22.5%. In absolute terms, we obtain NOx concentrations up to 5.9%, at an energy cost down to 2.1 MJ/mol, which are the best values reported to date in literature. In addition, we developed four complementary models to describe the gas flow, plasma temperature and plasma chemistry, aiming to reveal why the effusion nozzle yields better performance. Our simulations reveal that the effusion nozzle acts as very efficient heat sink, causing a fast drop in gas temperature when the gas molecules leave the plasma, hence limiting the recombination of NO back into N2 and O2. This yields an overall higher NOx concentration than without the effusion nozzle. This immediate quenching right at the end of the plasma makes our effusion nozzle superior to more conventional cooling options, like water cooling In addition, this higher NOx concentration can be obtained at a slightly lower power, because the effusion nozzle allows for the ignition and sustainment of the plasma at somewhat lower power. Hence, this also explains the lower energy cost. Overall, our experimental results and detailed modeling analysis will be useful to improve plasma-based NOx production in other plasma reactors as well. |
| Address |
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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 |
000800010600003 |
Publication Date |
0000-00-00 |
| 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 |
| Impact Factor |
15.1 |
Times cited |
|
Open Access |
OpenAccess |
| Notes |
This research was supported by the Excellence of Science FWO-FNRS project (FWO grant ID GoF9618n, EOS ID 30505023), the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No 810182 – SCOPE ERC Synergy project), and through long-term structural funding (Methusalem). The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UAntwerpen), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the UAntwerpen. |
Approved |
Most recent IF: 15.1 |
| Call Number |
PLASMANT @ plasmant @c:irua:188283 |
Serial |
7057 |
| Permanent link to this record |
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| Author |
Wang, Y.; Chen, Y.; Harding, J.; He, H.; Bogaerts, A.; Tu, X. |
| Title |
Catalyst-free single-step plasma reforming of CH4 and CO2 to higher value oxygenates under ambient conditions |
Type |
A1 Journal article |
| Year |
2022 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chem Eng J |
| Volume |
450 |
Issue |
|
Pages |
137860 |
| Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
| Abstract |
Direct conversion of CH4 and CO2 to liquid fuels and chemicals under mild conditions is appealing for biogas conversion and utilization but challenging due to the inert nature of both gases. Herein, we report a promising plasma process for the catalyst-free single-step conversion of CH4 and CO2 into higher value oxygenates (i.e., methanol, acetic acid, ethanol, and acetone) at ambient pressure and room temperature using a water-cooled dielectric barrier discharge (DBD) reactor, with methanol being the main liquid product. The distribution of liquid products could be tailored by tuning the discharge power, reaction temperature and residence time. Lower discharge powers (10–15 W) and reaction temperatures (5–20 ◦ C) were favourable for the production of liquid products, achieving the highest methanol selectivity of 43% at 5 ◦ C and 15 W. A higher discharge power and reaction temperature, on the other hand, produced more gaseous products, particularly H2 (up to 26% selectivity) and CO (up to 33% selectivity). In addition, varying these process parameters (discharge power, reaction temperature and residence time) resulted in a simultaneous change in key discharge properties, such as mean electron energy (Ee), electron density (ne) and specific energy input (SEI), all of which are essential determiners of plasma chemical reactions. According to the results of artificial neural network (ANN) models, the relative importance of these process parameters and key discharge indicators on reaction performance follows the order: discharge power > reaction temperature > residence time, and SEI > ne > Ee, respectively. This work provides new insights into the contributions and tuning mechanism of multiple parameters for optimizing the reaction performance (e.g., liquid production) in the plasma gas conversion process. |
| Address |
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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 |
000830813300004 |
Publication Date |
0000-00-00 |
| 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 |
| Impact Factor |
15.1 |
Times cited |
|
Open Access |
OpenAccess |
| Notes |
This project received funding from the European Union’s Horizon 2020 research and innovation program under the Marie SklodowskaCurie grant agreement No. 813393. |
Approved |
Most recent IF: 15.1 |
| Call Number |
PLASMANT @ plasmant @c:irua:189502 |
Serial |
7100 |
| Permanent link to this record |
