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Author Uytdenhouwen, Y.; Bal, Km.; Neyts, Ec.; Meynen, V.; Cool, P.; Bogaerts, A.
Title On the kinetics and equilibria of plasma-based dry reforming of methane Type A1 Journal article
Year 2021 Publication Chemical Engineering Journal Abbreviated Journal Chem Eng J
Volume 405 Issue Pages 126630
Keywords A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract Plasma reactors are interesting for gas-based chemical conversion but the fundamental relation between the plasma chemistry and selected conditions remains poorly understood. Apparent kinetic parameters for the loss and formation processes of individual components of gas conversion processes, can however be extracted by performing experiments in an extended residence time range (2–75 s) and fitting the gas composition to a firstorder kinetic model of the evolution towards partial chemical equilibrium (PCE). We specifically investigated the differences in kinetic characteristics and PCE state of the CO2 dissociation and CH4 reforming reactions in a dielectric barrier discharge reactor (DBD), how these are mutually affected when combining both gases in the dry reforming of methane (DRM) reaction, and how they change when a packing material (non-porous SiO2) is added to the reactor. We find that CO2 dissociation is characterized by a comparatively high reaction rate of 0.120 s−1 compared to CH4 reforming at 0.041 s−1; whereas CH4 reforming reaches higher equilibrium conversions, 82% compared to 53.6% for CO2 dissociation. Combining both feed gases makes the DRM reaction to proceed at a relatively high rate (0.088 s−1), and high conversion (75.4%) compared to CO2 dissociation, through accessing new chemical pathways between the products of CO2 and CH4. The addition of the packing material can also distinctly influence the conversion rate and position of the equilibrium, but its precise effect depends strongly on the gas composition. Comparing different CO2:CH4 ratios reveals the delicate balance of the combined chemistry. CO2 drives the loss reactions in DRM, whereas CH4 in the mixture suppresses back reactions. As a result, our methodology provides some of the insight necessary to systematically tune the conversion process.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000621197700003 Publication Date 2020-08-12
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.216 Times cited Open Access OpenAccess
Notes The authors 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), a TOP-BOF project and an IOF-SBO (SynCO2Chem) project from the University of Antwerp. Approved Most recent IF: 6.216
Call Number PLASMANT @ plasmant @c:irua:172458 Serial 6411
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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
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000623394200004 Publication Date 2021-01-09
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947 ISBN 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
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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
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000797716700002 Publication Date 0000-00-00
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 15.1 Times cited Open Access OpenAccess
Notes Horizon 2020 Marie Skłodowska-Curie Actions; European Research Council; This research was supported by the European Research Council (ERC) under the European Union’s Horizon 2020 Research and Innovation programme (grant agreement No 810182 – SCOPE ERC Synergy project) and the European Union’s Horizon 2020 Research and Inno­vation programme under the Marie Sklodowska-Curie grant agreement No 813393 (PIONEER). The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Approved Most recent IF: 15.1
Call Number PLASMANT @ plasmant @c:irua:188286 Serial 7052
Permanent link to this record
 

 
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
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000797716700002 Publication Date 0000-00-00
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 15.1 Times cited Open Access OpenAccess
Notes Horizon 2020 Marie Skłodowska-Curie Actions; European Research Council; This research was supported by the European Research Council (ERC) under the European Union’s Horizon 2020 Research and Innovation programme (grant agreement No 810182 – SCOPE ERC Synergy project) and the European Union’s Horizon 2020 Research and Inno­vation programme under the Marie Sklodowska-Curie grant agreement No 813393 (PIONEER). The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UAntwerpen), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Govern­ment (department EWI) and the UAntwerpen. We also thank R. De Meyer, K. Leyssens and S. Defossé for performing the charcoal characterizations. Approved Most recent IF: 15.1
Call Number PLASMANT @ plasmant @c:irua:188286 Serial 7053
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Author Van Alphen, S.; Ahmadi Eshtehardi, H.; O'Modhrain, C.; Bogaerts, J.; Van Poyer, H.; Creel, J.; Delplancke, M.-P.; Snyders, R.; Bogaerts, A.
Title Effusion nozzle for energy-efficient NOx production in a rotating gliding arc plasma reactor Type A1 Journal article
Year 2022 Publication Chemical Engineering Journal Abbreviated Journal Chem Eng J
Volume 443 Issue Pages 136529
Keywords A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract Plasma-based NOx production is of interest for sustainable N2 fixation, but more research is needed to improve its performance. One of the current limitations is recombination of NO back into N2 and O2 molecules immediately after the plasma reactor. Therefore, we developed a novel so-called “effusion nozzle”, to improve the perfor­mance of a rotating gliding arc plasma reactor for NOx production, but the same principle can also be applied to other plasma types. Experiments in a wide range of applied power, gas flow rates and N2/O2 ratios demonstrate an enhancement in NOx concentration by about 8%, and a reduction in energy cost by 22.5%. In absolute terms, we obtain NOx concentrations up to 5.9%, at an energy cost down to 2.1 MJ/mol, which are the best values reported to date in literature. In addition, we developed four complementary models to describe the gas flow, plasma temperature and plasma chemistry, aiming to reveal why the effusion nozzle yields better performance. Our simulations reveal that the effusion nozzle acts as very efficient heat sink, causing a fast drop in gas tem­perature when the gas molecules leave the plasma, hence limiting the recombination of NO back into N2 and O2. This yields an overall higher NOx concentration than without the effusion nozzle. This immediate quenching right at the end of the plasma makes our effusion nozzle superior to more conventional cooling options, like water cooling In addition, this higher NOx concentration can be obtained at a slightly lower power, because the effusion nozzle allows for the ignition and sustainment of the plasma at somewhat lower power. Hence, this also explains the lower energy cost. Overall, our experimental results and detailed modeling analysis will be useful to improve plasma-based NOx production in other plasma reactors as well.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000800010600003 Publication Date 0000-00-00
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 15.1 Times cited Open Access OpenAccess
Notes This research was supported by the Excellence of Science FWO-FNRS project (FWO grant ID GoF9618n, EOS ID 30505023), the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No 810182 – SCOPE ERC Synergy project), and through long-term structural funding (Methusalem). The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UAntwerpen), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (depart­ment EWI) and the UAntwerpen. Approved Most recent IF: 15.1
Call Number PLASMANT @ plasmant @c:irua:188283 Serial 7057
Permanent link to this record
 

 
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
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000830813300004 Publication Date 0000-00-00
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 15.1 Times cited Open Access OpenAccess
Notes This project received funding from the European Union’s Horizon 2020 research and innovation program under the Marie SklodowskaCurie grant agreement No. 813393. Approved Most recent IF: 15.1
Call Number PLASMANT @ plasmant @c:irua:189502 Serial 7100
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Author Andersen, Ja.; Holm, Mc.; van 't Veer, K.; Christensen, Jm.; Østberg, M.; Bogaerts, A.; Jensen, Ad.
Title Plasma-catalytic ammonia synthesis in a dielectric barrier discharge reactor: A combined experimental study and kinetic modeling Type A1 Journal article
Year 2023 Publication Chemical engineering journal Abbreviated Journal
Volume 457 Issue Pages 141294
Keywords A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract Plasma-catalytic ammonia synthesis in a dielectric barrier discharge reactor has emerged as a possible route for electrification of nitrogen fixation. In this study, we use a combination of experiments and a plasma kinetic model to investigate the ammonia synthesis from N2 and H2, both with and without a solid packing material in the plasma zone. The effect of plasma power, feed flow rate, N2:H2 feed ratio, gas residence time, temperature, and packing material (MgAl2O4 alone or impregnated with Co or Ru) on the ammonia synthesis rate were examined in the experiments. The kinetic model was employed to improve our understanding of the ammonia formation pathways and identify possible changes in these pathways when altering the N2:H2 feed ratio. A higher NH3 synthesis rate was achieved when increasing the feed flow rate, as well as when increasing the gas tem-perature from 100 to 200 ◦C when a packing material was present in the plasma. At the elevated temperature of 200 ◦C, an optimum in the NH3 synthesis rate was observed at an equimolar feed ratio (N2:H2 =1:1) for the plasma alone and MgAl2O4, while a N2-rich feed was favored for Ru/MgAl2O4 and Co/MgAl2O4. The optimum in the synthesis rate with the N2-rich feed, where high energy electrons are more likely to collide with N2, suggests that the rate-limiting step is the dissociation of N2 in the gas phase. This is supported by the kinetic model when packing material was used. However, for the plasma alone, the model found that the N2 dissociation is only rate limiting in H2-rich feeds, whereas the limited access to H in N2-rich feeds makes the hydrogenation of N species limiting.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001058978000001 Publication Date 2023-01-05
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 15.1 Times cited Open Access OpenAccess
Notes We thank Topsoe A/S for providing the catalytic materials used in the study, the research group PLASMANT (University of Antwerp) for sharing their plasma kinetic model and allocating time on their cluster for the calculations, and the Department of Chemical and Biochemical Engineering (Technical University of Denmark) for funding the project. Approved Most recent IF: 15.1; 2023 IF: 6.216
Call Number PLASMANT @ plasmant @c:irua:195877 Serial 7234
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Author Morais, E.; Delikonstantis, E.; Scapinello, M.; Smith, G.; Stefanidis, G.D.; Bogaerts, A.
Title Methane coupling in nanosecond pulsed plasmas: Correlation between temperature and pressure and effects on product selectivity Type A1 Journal article
Year 2023 Publication Chemical engineering journal Abbreviated Journal
Volume 462 Issue Pages 142227
Keywords A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract We present a zero-dimensional kinetic model to characterise specifically the gas-phase dynamics of methane

conversion in a nanosecond pulsed discharge (NPD) plasma reactor. The model includes a systematic approach to

capture the nanoscale power discharges and the rapid ensuing changes in electric field, gas and electron temperature,

as well as species densities. The effects of gas temperature and reactor pressure on gas conversion and

product selectivity are extensively investigated and validated against experimental work. We discuss the

important reaction pathways and provide an analysis of the dynamics of the heating and cooling mechanisms. H

radicals are found to be the most populous plasma species and they participate in hydrogenation and dehydrogenation

reactions, which are the dominant recombination reactions leading to C2H4 and C2H2 as main

products (depending on the pressure).
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000983631500001 Publication Date 2023-03-02
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 15.1 Times cited Open Access OpenAccess
Notes We gratefully acknowledge financial support by the Flemish Government through the Moonshot cSBO project “Power-to-Olefins” (P2O; HBC.2020.2620). Approved Most recent IF: 15.1; 2023 IF: 6.216
Call Number PLASMANT @ plasmant @c:irua:195881 Serial 7246
Permanent link to this record
 

 
Author Van Alphen, S.; Hecimovic, A.; Kiefer, C.K.; Fantz, U.; Snyders, R.; Bogaerts, A.
Title Modelling post-plasma quenching nozzles for improving the performance of CO2 microwave plasmas Type A1 Journal article
Year 2023 Publication Chemical engineering journal Abbreviated Journal
Volume 462 Issue Pages 142217
Keywords A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract Given the ecological problems associated to the CO2 emissions of fossil fuels, plasma technology has gained

interest for conversion of CO2 into value-added products. Microwave plasmas operating at atmospheric pressure

have proven to be especially interesting, due to the high gas temperatures inside the reactor (i.e. up to 6000 K)

allowing for efficient thermal dissociation of CO2 into CO and O2. However, the performance of these high

temperature plasmas is limited by recombination of CO back into CO2 once the gas cools down in the afterglow.

In this work, we computationally investigated several quenching nozzles, developed and experimentally tested

by Hecimovic et al., [1] for their ability to quickly cool the gas after the plasma, thereby quenching the CO

recombination reactions. Using a 3D computational fluid dynamics model and a quasi-1D chemical kinetics

model, we reveal that a reactor without nozzle lacks gas mixing between hot gas in the center and cold gas near

the reactor walls. Especially at low flow rates, where there is an inherent lack of convective cooling due to the

low gas flow velocity, the temperature in the afterglow remains high (between 2000 and 3000 K) for a relatively

long time (in the 0.1 s range). As shown by our quasi-1D chemical kinetics model, this results in a important loss

of CO due to recombination reactions. Attaching a nozzle in the effluent of the reactor induces fast gas quenching

right after the plasma. Indeed, it introduces (i) more convective cooling by forcing cool gas near the walls to mix

with hot gas in the center of the reactor, as well as (ii) more conductive cooling through the water-cooled walls of

the nozzle. Our model shows that gas quenching and the suppression of recombination reactions have more

impact at low flow rates, where recombination is the most limiting factor in the conversion process.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000962382600001 Publication Date 2023-03-03
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 15.1 Times cited Open Access OpenAccess
Notes This research was supported by the Excellence of Science FWO-FNRS project (FWO grant ID GoF9618n, EOS ID 30505023), the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No 810182 – SCOPE ERC Synergy project), and through long-term structural funding (Methusalem). The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UAntwerpen), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the UAntwerpen. Approved Most recent IF: 15.1; 2023 IF: 6.216
Call Number PLASMANT @ plasmant @c:irua:195889 Serial 7250
Permanent link to this record
 

 
Author Liu, R.; Hao, Y.; Wang, T.; Wang, L.; Bogaerts, A.; Guo, H.; Yi, Y.
Title Hybrid plasma-thermal system for methane conversion to ethylene and hydrogen Type A1 Journal article
Year 2023 Publication Chemical engineering journal Abbreviated Journal
Volume 463 Issue Pages 142442
Keywords A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract By combining dielectric barrier discharge plasma and external heating, we exploit a two-stage hybrid plasmathermal

system (HPTS), i.e., a plasma stage followed by a thermal stage, for direct non-oxidative coupling of

CH4 to C2H4 and H2, yielding a CH4 conversion of ca. 17 %. In the two-stage HPTS, the plasma first converts CH4

into C2H6 and C3H8, which in the thermal stage leads to a high C2H4 selectivity of ca. 63 % by pyrolysis, with H2

selectivity of ca. 64 %.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000953890500001 Publication Date 2023-03-16
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 15.1 Times cited Open Access OpenAccess
Notes This work was supported by the National Natural Science Foundation of China [22272015, 21503032], the Fundamental Research Funds for the Central Universities of China [DUT21JC40]. Approved Most recent IF: 15.1; 2023 IF: 6.216
Call Number PLASMANT @ plasmant @c:irua:195888 Serial 7253
Permanent link to this record
 

 
Author Van Alphen, S.; Hecimovic, A.; Kiefer, C.K.; Fantz, U.; Snyders, R.; Bogaerts, A.
Title Modelling post-plasma quenching nozzles for improving the performance of CO2 microwave plasmas Type A1 Journal article
Year 2023 Publication Chemical engineering journal Abbreviated Journal
Volume 462 Issue Pages 142217
Keywords A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract Given the ecological problems associated to the CO2 emissions of fossil fuels, plasma technology has gained

interest for conversion of CO2 into value-added products. Microwave plasmas operating at atmospheric pressure

have proven to be especially interesting, due to the high gas temperatures inside the reactor (i.e. up to 6000 K)

allowing for efficient thermal dissociation of CO2 into CO and O2. However, the performance of these high

temperature plasmas is limited by recombination of CO back into CO2 once the gas cools down in the afterglow.

In this work, we computationally investigated several quenching nozzles, developed and experimentally tested

by Hecimovic et al., [1] for their ability to quickly cool the gas after the plasma, thereby quenching the CO

recombination reactions. Using a 3D computational fluid dynamics model and a quasi-1D chemical kinetics

model, we reveal that a reactor without nozzle lacks gas mixing between hot gas in the center and cold gas near

the reactor walls. Especially at low flow rates, where there is an inherent lack of convective cooling due to the

low gas flow velocity, the temperature in the afterglow remains high (between 2000 and 3000 K) for a relatively

long time (in the 0.1 s range). As shown by our quasi-1D chemical kinetics model, this results in a important loss

of CO due to recombination reactions. Attaching a nozzle in the effluent of the reactor induces fast gas quenching

right after the plasma. Indeed, it introduces (i) more convective cooling by forcing cool gas near the walls to mix

with hot gas in the center of the reactor, as well as (ii) more conductive cooling through the water-cooled walls of

the nozzle. Our model shows that gas quenching and the suppression of recombination reactions have more

impact at low flow rates, where recombination is the most limiting factor in the conversion process.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000962382600001 Publication Date 2023-03-03
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 15.1 Times cited Open Access OpenAccess
Notes This research was supported by the Excellence of Science FWO-FNRS project (FWO grant ID GoF9618n, EOS ID 30505023), the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No 810182 – SCOPE ERC Synergy project), and through long-term structural funding (Methusalem). The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UAntwerpen), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the UAntwerpen. Approved Most recent IF: 15.1; 2023 IF: 6.216
Call Number PLASMANT @ plasmant @c:irua:195889 Serial 7259
Permanent link to this record
 

 
Author Wang, K.; Ceulemans, S.; Zhang, H.; Tsonev, I.; Zhang, Y.; Long, Y.; Fang, M.; Li, X.; Yan, J.; Bogaerts, A.
Title Inhibiting recombination to improve the performance of plasma-based CO2 conversion Type A1 Journal Article
Year 2024 Publication Chemical Engineering Journal Abbreviated Journal Chemical Engineering Journal
Volume 481 Issue Pages 148684
Keywords A1 Journal Article; Plasma-based CO2 splitting Recombination reactions In-situ gas sampling Fluid dynamics modeling Kinetics modeling Afterglow quenching; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Abstract Warm plasma offers a promising route for CO2 splitting into valuable CO, yet recombination reactions of CO with oxygen, forming again CO2, have recently emerged as critical limitation. This study combines experiments and fluid dynamics + chemical kinetics modelling to comprehensively analyse the recombination reactions upon CO2 splitting in an atmospheric plasmatron. We introduce an innovative in-situ gas sampling technique, enabling 2D spatial mapping of gas product compositions and temperatures, experimentally confirming for the first time the substantial limiting effect of CO recombination reactions in the afterglow region. Our results show that the CO mole fraction at a 5 L/min flow rate drops significantly from 11.9 % at a vertical distance of z = 20 mm in the afterglow region to 8.6 % at z = 40 mm. We constructed a comprehensive 2D model that allows for spatial reaction rates analysis incorporating crucial reactions, and we validated it to kinetically elucidate this phenomenon. CO2 +M⇌O+CO+M and CO2 +O⇌CO+O2 are the dominant reactions, with the forward reactions prevailing in the plasma region and the backward reactions becoming prominent in the afterglow region. These results allow us to propose an afterglow quenching strategy for performance enhancement, which is further demonstrated through a meticulously developed plasmatron reactor with two-stage cooling. Our approach substantially increases the CO2 conversion (e.g., from 6.6 % to 19.5 % at 3 L/min flow rate) and energy efficiency (from 13.5 % to 28.5 %, again at 3 L/min) and significantly shortens the startup time (from ~ 150 s to 25 s). Our study underscores the critical role of inhibiting recombination reactions in plasma-based CO2 conversion and offers new avenues for performance enhancement.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001168999200001 Publication Date 2024-01-10
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947 ISBN Additional Links UA library record; WoS full record
Impact Factor 15.1 Times cited Open Access Not_Open_Access
Notes Key Research and Development Program of Zhejiang Province, 2023C03129 ; Vlaamse regering; European Research Council; National Natural Science Foundation of China, 51976191 52276214 ; Horizon 2020 Framework Programme; Fonds De La Recherche Scientifique – FNRS; Fonds Wetenschappelijk Onderzoek, 1101524N ; Vlaams Supercomputer Centrum; Horizon 2020, 101081162 810182 ; European Research Council; Approved Most recent IF: 15.1; 2024 IF: 6.216
Call Number PLASMANT @ plasmant @c:irua:204352 Serial 8993
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Author De Meyer, R.; Gorbanev, Y.; Ciocarlan, R.-G.; Cool, P.; Bals, S.; Bogaerts, A.
Title Importance of plasma discharge characteristics in plasma catalysis: Dry reforming of methane vs. ammonia synthesis Type A1 Journal Article
Year 2024 Publication Chemical Engineering Journal Abbreviated Journal Chemical Engineering Journal
Volume 488 Issue Pages 150838
Keywords A1 Journal Article; Gas conversion Dry reforming of methane Ammonia Microdischarges Dielectric barrier discharge; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Abstract Plasma catalysis is a rapidly growing field, often employing a packed-bed dielectric barrier discharge plasma reactor. Such dielectric barrier discharges are complex, especially when a packing material (e.g., a catalyst) is introduced in the discharge volume. Catalysts are known to affect the plasma discharge, though the underlying mechanisms influencing the plasma physics are not fully understood. Moreover, the effect of the catalysts on the plasma discharge and its subsequent effect on the overall performance is often overlooked. In this work, we deliberately design and synthesize catalysts to affect the plasma discharge in different ways. These Ni or Co alumina-based catalysts are used in plasma-catalytic dry reforming of methane and ammonia synthesis. Our work shows that introducing a metal to the dielectric packing can affect the plasma discharge, and that the distribution of the metal is crucial in this regard. Further, the altered discharge can greatly influence the overall performance. In an atmospheric pressure dielectric barrier discharge reactor, this apparently more uniform plasma yields a significantly better performance for ammonia synthesis compared to the more conventional filamentary discharge, while it underperforms in dry reforming of methane. This study stresses the importance of analyzing the plasma discharge in plasma catalysis experiments. We hope this work encourages a more critical view on the plasma discharge characteristics when studying various catalysts in a plasma reactor.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos Publication Date 2024-03-30
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947 ISBN Additional Links UA library record
Impact Factor 15.1 Times cited Open Access
Notes This research was supported through long-term structural funding (Methusalem FFB15001C) and by the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme with grant agreement No 810182 (SCOPE ERC Synergy project) and with grant agreement No 815128 (REALNANO). We acknowledge the practical contribution of Senne Van Doorslaer. Approved Most recent IF: 15.1; 2024 IF: 6.216
Call Number PLASMANT @ plasmant @c:irua:205154 Serial 9115
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Author Maerivoet, S.; Tsonev, I.; Slaets, J.; Reniers, F.; Bogaerts, A.
Title Coupled multi-dimensional modelling of warm plasmas: Application and validation for an atmospheric pressure glow discharge in CO2/CH4/O2 Type A1 Journal Article
Year 2024 Publication Chemical Engineering Journal Abbreviated Journal Chemical Engineering Journal
Volume 492 Issue Pages 152006
Keywords A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Abstract To support experimental research into gas conversion by warm plasmas, models should be developed to explain the experimental observations. These models need to describe all physical and chemical plasma properties in a coupled way. In this paper, we present a modelling approach to solve the complete set of assumed relevant equations, including gas flow, heat balance and species transport, coupled with a rather extensive chemistry set, consisting of 21 species, obtained by reduction of a more detailed chemistry set, consisting of 41 species. We apply this model to study the combined CO2 and CH4 conversion in the presence of O2, in a direct current atmospheric pressure glow discharge. Our model can predict the experimental trends, and can explain why higher O2 fractions result in higher CH4 conversion, namely due to the higher gas temperature, rather than just by additional chemical reactions. Indeed, our model predicts that when more O2 is added, the energy required to reach any set temperature (i.e., the enthalpy) drops, allowing the system to reach higher temperatures with similar amounts of energy. This is in turn related to the higher H2O fraction and lower H2 fraction formed in the plasma, as demonstrated by our model. Altogether, our new self-consistent model can capture the main physics and chemistry occurring in this warm plasma, which is an important step towards predictive modelling for plasma-based gas conversion.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos Publication Date 2024-05-09
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947 ISBN Additional Links
Impact Factor 15.1 Times cited Open Access
Notes This research was supported by the Excellence of Science FWO-FNRS project (FWO grant ID G0I1822N; EOS ID 40007511) and the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No. 810182–SCOPE ERC Synergy project, and grant agreement No. 101081162–PREPARE ERC Proof of Concept project). computational resources and services used in this work were provided by the HPC core facility CalcUA of the Universiteit Antwerpen, and VSC (Flemish Supercomputer Center), funded by the Research Foundation – Flanders (FWO) and the Flemish Government. Approved Most recent IF: 15.1; 2024 IF: 6.216
Call Number PLASMANT @ plasmant @ Serial 9132
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Author Tytgat, T.; Hauchecorne, B.; Abakumov, A.M.; Smits, M.; Verbruggen, S.W.; Lenaerts, S.
Title Photocatalytic process optimisation for ethylene oxidation Type A1 Journal article
Year 2012 Publication Chemical engineering journal Abbreviated Journal Chem Eng J
Volume 209 Issue Pages 494-500
Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Sustainable Energy, Air and Water Technology (DuEL)
Abstract When studying photocatalysis it is important to consider, beside the chemical approach, the engineering part related to process optimisation. To achieve this a fixed bed photocatalytic set-up consisting of different catalyst placings, in order to vary catalyst distribution, is studied. The use of a fixed quantity of catalyst placed packed or randomly distributed in the reactor, results in an almost double degradation for the distributed catalyst. Applying this knowledge leads to an improved performance with limited use of catalyst. A reactor only half filled with catalyst leads to higher degradation performance compared to a completely filled reactor. Taking into account this simple process optimisation by better distributing the catalyst a more sustainable photocatalytic air purification process is achieved. (C) 2012 Elsevier B.V. All rights reserved.
Address
Corporate Author Thesis
Publisher Place of Publication Lausanne Editor
Language Wos 000311190500058 Publication Date 2012-08-22
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.216 Times cited 12 Open Access
Notes ; We are grateful for the delivered photocatalyst by Evonik as well as for the PhD grant (T. Tytgat) given by the Institute of Innovation by Science and Technology in Flanders (IWT). ; Approved Most recent IF: 6.216; 2012 IF: 3.473
Call Number UA @ lucian @ c:irua:105185 Serial 2609
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Author Smeulders, G.; van Oers, C.; Van Havenbergh, K.; Houthoofd, K.; Mertens, M.; Martens, J.A.; Bals, S.; Maes, B.U.W.; Meynen, V.; Cool, P.
Title Smart heating profiles for the synthesis of benzene bridged periodic mesoporous organosilicas Type A1 Journal article
Year 2011 Publication Chemical engineering journal Abbreviated Journal Chem Eng J
Volume 175 Issue Pages 585-591
Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Organic synthesis (ORSY)
Abstract In this study the effects of the heating rate and heating time on the formation of crystal-like benzene bridged periodic mesoporous organosilicas (PMOs) are investigated. The time needed to heat up an autoclave during the hydrothermal treatment has shown to be crucial in the synthesis of PMOs, while the total duration of heating gave rise to only minor differences. By choosing a smart heating profile, superior PMO materials can be obtained in a short time. Different heating profiles in a range from one minute to one hour are adopted by microwave equipment and compared with conventional heating methods. The heating rate has a large influence on the porosity characteristics and the uniformity of the obtained particles. Moreover, two new alternative synthetic strategies to adopt the smart heating profile are presented, in order to give some possible solutions for the expensive microwave equipment.
Address
Corporate Author Thesis
Publisher Place of Publication Lausanne Editor
Language Wos 000297875900069 Publication Date 2011-10-07
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.216 Times cited 7 Open Access
Notes Fwo; Goa-Bof Approved Most recent IF: 6.216; 2011 IF: 3.461
Call Number UA @ lucian @ c:irua:93630 Serial 3044
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Author Gholampour, N.; Chaemchuen, S.; Hu, Z.-Y.; Mousavi, B.; Van Tendeloo, G.; Verpoort, F.
Title Simultaneous creation of metal nanoparticles in metal organic frameworks via spray drying technique Type A1 Journal article
Year 2017 Publication Chemical engineering journal Abbreviated Journal Chem Eng J
Volume 322 Issue Pages 702-709
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
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.
Address
Corporate Author Thesis
Publisher Place of Publication Lausanne Editor
Language Wos 000401594200069 Publication Date 2017-04-19
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947; 0300-9467 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.216 Times cited 14 Open Access OpenAccess
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 Most recent IF: 6.216
Call Number UA @ lucian @ c:irua:144152 Serial 4686
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Author Zhang, H.; Wang, W.; Li, X.; Han, L.; Yan, M.; Zhong, Y.; Tu, X.
Title Plasma activation of methane for hydrogen production in a N2 rotating gliding arc warm plasma : a chemical kinetics study Type A1 Journal article
Year 2018 Publication Chemical engineering journal Abbreviated Journal Chem Eng J
Volume 345 Issue 345 Pages 67-78
Keywords A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
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.
Address
Corporate Author Thesis
Publisher Elsevier Sequoia Place of Publication Lausanne Editor
Language Wos 000430696500008 Publication Date 2018-03-24
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947; 1873-3212 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.216 Times cited 25 Open Access OpenAccess
Notes Approved Most recent IF: 6.216
Call Number UA @ lucian @ c:irua:151450 Serial 5036
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Author Trenchev, G.; Nikiforov, A.; Wang, W.; Kolev, S.; Bogaerts, A.
Title Atmospheric pressure glow discharge for CO2 conversion : model-based exploration of the optimum reactor configuration Type A1 Journal article
Year 2019 Publication Chemical engineering journal Abbreviated Journal Chem Eng J
Volume 362 Issue 362 Pages 830-841
Keywords A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract We investigate the performance of an atmospheric pressure glow discharge (APGD) reactor for CO2 conversion in three different configurations, through experiments and simulations. The first (basic) configuration utilizes the well-known pin-to-plate design, which offers a limited conversion. The second configuration improves the reactor performance by employing a vortex-flow generator. The third, “confined” configuration is a complete redesign of the reactor, which encloses the discharge in a limited volume, significantly surpassing the conversion rate of the other two designs. The plasma properties are investigated using an advanced plasma model.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000457863500084 Publication Date 2019-01-18
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947; 1873-3212 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.216 Times cited 4 Open Access Not_Open_Access: Available from 15.10.2019
Notes Approved Most recent IF: 6.216
Call Number UA @ admin @ c:irua:157459 Serial 5269
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Author Pauwels, D.; Hereijgers, J.; Verhulst, K.; De Wael, K.; Breugelmans, T.
Title Investigation of the electrosynthetic pathway of the aldol condensation of acetone Type A1 Journal article
Year 2016 Publication Chemical engineering journal Abbreviated Journal Chem Eng J
Volume 289 Issue Pages 554-561
Keywords A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Applied Electrochemistry & Catalysis (ELCAT)
Abstract The potential-controlled electrochemical aldol condensation of acetone to diacetone alcohol in a standard batch electrolysis set-up was studied in this work. It is confirmed that the reaction proceeds at the cathode and that, contrary to what is mentioned in earlier literature, water in the electrolyte has a disadvantageous effect on the reaction. Similar to the chemical reaction, the electrochemical reaction reaches a maximum yield when the equilibrium is reached. Separating the anode and cathode prevents cross-over and degradation of products, leading to a higher yield. Starting with pure acetone and support electrolyte, it was possible to obtain a diacetone alcohol concentration of 15 m% after two hours electrolysis in a divided set-up with a platinum electrode at -2.5 V. The concentration gradient throughout the electrolysis follows an exponential curve up to its equilibrium concentration.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000371559900061 Publication Date 2016-01-13
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947; 1873-3212 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.216 Times cited 6 Open Access
Notes ; ; Approved Most recent IF: 6.216
Call Number UA @ admin @ c:irua:130396 Serial 5675
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Author Verbruggen, S.W.; Lenaerts, S.; Denys, S.
Title Analytic versus CFD approach for kinetic modeling of gas phase photocatalysis Type A1 Journal article
Year 2015 Publication Chemical engineering journal Abbreviated Journal Chem Eng J
Volume 262 Issue Pages 1-8
Keywords A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Abstract In this work two methods for determining the LangmuirHinshelwood kinetic parameters for a slit-shaped flat bed photocatalytic reactor are compared: an analytic mass transfer based model adapted from literature and a computational fluid dynamics (CFD) approach that was used in conjunction with a simplex optimization routine. Despite the differences between both approaches, similar values for the kinetic parameters and similar trends in terms of their UV intensity dependence were found. Using an effectiveness-NTU (number of transfer units) approach, the analytic mass transfer based method could quantify the relative contributions of the rate limiting steps through a reaction effectiveness parameter. The numeric CFD approach on the other hand could yield the two kinetic parameters that determine the photocatalytic reaction rate simultaneously. Furthermore, it proved to be more accurate as it accounts for the spatial variation of flow rate, reaction rate and concentrations at the surface of the photocatalyst. We elaborate this dual kinetic analysis with regard to the photocatalytic degradation of acetaldehyde in air over a silicon wafer coated with a layer of TiO2 P25 (Evonik) and study the usefulness and limitations of both strategies.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000347577700001 Publication Date 2014-09-28
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947; 1873-3212 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.216 Times cited 30 Open Access
Notes ; S.W.V. acknowledges the Research Foundation of Flanders (FWO) for financial support. ; Approved Most recent IF: 6.216; 2015 IF: 4.321
Call Number UA @ admin @ c:irua:119724 Serial 5927
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Author Verbruggen, S.W.; Ribbens, S.; Tytgat, T.; Hauchecorne, B.; Smits, M.; Meynen, V.; Cool, P.; Martens, J.A.; Lenaerts, S.
Title The benefit of glass bead supports for efficient gas phase photocatalysis : case study of a commercial and a synthesised photocatalyst Type A1 Journal article
Year 2011 Publication Chemical engineering journal Abbreviated Journal Chem Eng J
Volume 174 Issue 1 Pages 318-325
Keywords A1 Journal article; Engineering sciences. Technology; Laboratory of adsorption and catalysis (LADCA); Sustainable Energy, Air and Water Technology (DuEL)
Abstract In the field of photocatalytic air purification, the immobilisation of catalyst particles on support surfaces without loss of photon efficiency is an important challenge. Therefore, an immobilisation method involving a one-step suspension coating of pre-synthesised photocatalysts on glass beads was applied. The various benefits are exemplified in the gas phase photodegradation of ethylene. Coating of glass beads is easy, fast, cheap and offers a more efficient alternative to bulk catalyst pellets. Furthermore, this coating procedure allows to use porous, pre-synthesised catalysts to their full potential, as the surface area and morphology of the initial powder is barely altered after coating, in strong contrast to pelletising. With this technique it became possible to study the gas phase photocatalytic activity of commercial titanium dioxide, trititanate nanotubes and mixed phase anatase/trititanate nanotubes in a packed bed reactor towards the degradation of ethylene without changing the catalyst properties. Coating of glass beads with the photocatalyst revealed the superior activity of the as-prepared nanotubes, compared to TiO2 Aerolyst® 7710 in gaseous phase.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000296950300041 Publication Date 2011-09-17
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947; 1873-3212 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.216 Times cited 39 Open Access
Notes ; The author wishes to acknowledge the Research Foundation of Flanders (FWO) for the financial support. Evonik is greatly thanked for supplying the TiO<INF>2</ INF> Aerolyst (R) 7710 pellets. ; Approved Most recent IF: 6.216; 2011 IF: 3.461
Call Number UA @ admin @ c:irua:93364 Serial 5929
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Author van Walsem, J.; Verbruggen, S.W.; Modde, B.; Lenaerts, S.; Denys, S.
Title CFD investigation of a multi-tube photocatalytic reactor in non-steady-state conditions Type A1 Journal article
Year 2016 Publication Chemical engineering journal Abbreviated Journal Chem Eng J
Volume 304 Issue Pages 808-816
Keywords A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Abstract A novel multi-tube photoreactor is presented with a high efficiency (over 90% conversion) toward the degradation of acetaldehyde in air under UV conditions with an incident intensity of 2.1 mW cm−2. A CFD model was developed to simulate the transient adsorption and photocatalytic degradation processes of acetaldehyde in this reactor design and to estimate the corresponding kinetic parameters through an optimization routine using the experimentally determined outlet concentration profiles. The CFD model takes into account the entire reactor geometry and all relevant flow parameters, in contrast to analytical methods that often oversimplify the physical and chemical process characteristics. Using CFD, we show that both adsorption and desorption rate constants increase by respectively one and two orders of magnitude when the UV light is switched on, which clearly affects the transient behavior. The agreement of the experimental and modelled concentration profiles is excellent as evidenced by a coefficient of determination of at least 0.965. To demonstrate the reliability and accuracy of all parameters obtained from the modelling approach, an ultimate validation test was performed using other conditions than the ones used for estimating the kinetic parameters. The model was able to accurately simulate simultaneous adsorption, desorption and photocatalytic degradation.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000384777200089 Publication Date 2016-07-08
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947; 1873-3212 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.216 Times cited 10 Open Access
Notes ; J.V.W. acknowledges the Agentschap Innoveren & Ondernemen for a PhD fellowship. S.W.V. acknowledges the Research Foundation – Flanders (FWO) for a postdoctoral fellowship. ; Approved Most recent IF: 6.216
Call Number UA @ admin @ c:irua:139620 Serial 5933
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Author Verbruggen, S.W.; Keulemans, M.; van Walsem, J.; Tytgat, T.; Lenaerts, S.; Denys, S.
Title CFD modeling of transient adsorption/desorption behavior in a gas phase photocatalytic fiber reactor Type A1 Journal article
Year 2016 Publication Chemical engineering journal Abbreviated Journal Chem Eng J
Volume 292 Issue Pages 42-50
Keywords A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Abstract We present the use of computational fluid dynamics (CFD) for accurately determining the adsorption parameters of acetaldehyde on photocatalytic fiber filter material, integrated in a continuous flow system. Unlike the traditional analytical analysis based on Langmuir adsorption, not only steady-state situations but also transient phenomena can be accounted for. Air displacement effects in the reactor and gas detection cell are investigated and inherently made part of the model. Incorporation of a surface aldol condensation reaction in the CFD analysis further improves the accuracy of the model which enables to extract precise, intrinsic adsorption parameters for situations in which analytical analysis would otherwise fail.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000373648000005 Publication Date 2016-02-09
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947; 1873-3212 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.216 Times cited 12 Open Access
Notes ; S.W.V. acknowledges the Research Foundation – Flanders (FWO) for a postdoctoral fellowship. M.K. acknowledges the IWT for a Ph.D. fellowship. Konstantina Kalafata and Ioanna Fasaki are greatly thanked for providing the NanoPhos suspension. Bioscience Engineering bachelor students M. Gerritsma, J. Helsen and Y. Riahi Drif are thanked for their assistance in performing the adsorption experiments. ; Approved Most recent IF: 6.216
Call Number UA @ admin @ c:irua:130876 Serial 5934
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Author van Walsem, J.; Roegiers, J.; Modde, B.; Lenaerts, S.; Denys, S.
Title Determination of intrinsic kinetic parameters in photocatalytic multi-tube reactors by combining the NTUm-method with radiation field modelling Type A1 Journal article
Year 2018 Publication Chemical engineering journal Abbreviated Journal Chem Eng J
Volume 354 Issue 354 Pages 1042-1049
Keywords A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Abstract In this work, we propose an adapted Number of Transfer Units (NTUm)-method as an effective tool to determine the Langmuir-Hinshelwood kinetic parameters for a photocatalytic multi-tube reactor. The Langmuir-Hinshelwood rate constant kLH and the Langmuir adsorption constant KL were determined from several experiments under different UV-irradiance conditions, resulting in irradiance depending values for kLH. In order to determine a unique, intrinsic empirical constant k0, valid for all irradiation conditions, we coupled the adapted NTUm-method with a radiation field model to predict UV-irradiance distribution inside the reactor. The final set of kinetic parameters were derived using a Generalized Reduced Gradient (GRG) nonlinear solving method in Matlab which minimizes the differences between model and experimental reactor outlet concentrations of acetaldehyde for various photocatalytic experiments under varying operating conditions, including inlet concentration, flow rate and UV-irradiance. An excellent agreement of the intrinsic empirical constant k0, derived from the coupled NTUm-radiation field model and an earlier published CFD approach was found, emphasizing its validity and reliability.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000445413900099 Publication Date 2018-08-03
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947; 1873-3212 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.216 Times cited 2 Open Access
Notes ; J.V.W. acknowledges the Agentschap Innoveren & Ondernemen for a PhD fellowship. ; Approved Most recent IF: 6.216
Call Number UA @ admin @ c:irua:154845 Serial 5940
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Author Van Hal, M.; Verbruggen, S.W.; Yang, X.-Y.; Lenaerts, S.; Tytgat, T.
Title Image analysis and in situ FTIR as complementary detection tools for photocatalytic soot oxidation Type A1 Journal article
Year 2019 Publication Chemical engineering journal Abbreviated Journal Chem Eng J
Volume 367 Issue 367 Pages 269-277
Keywords A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Abstract Air pollution, especially particulate matter (PM), is an increasingly urgent problem in urban environments, causing both short and long-term health problems, climate interference and aesthetical problems due to building fouling. Photocatalysis has been shown to be a possible solution to that end. In this work two complementary detection methods for photocatalytic soot oxidation are studied and their advantages and disadvantages are discussed. First, a colour-based digital image analysis method is drastically improved towards an accurate, detailed and straightforward detection tool, that enables simultaneous measurement of the degradation of different grades of soot fouling (for instance a shallow soot haze versus condensed soot deposits). In the next part, a second soot oxidation detection method is presented based on in situ FTIR spectroscopy. This method has the additional advantage of providing more insight into the photocatalytic soot degradation process by monitoring both gaseous and adsorbed intermediates as well as reaction products while the reactions are ongoing. As an illustration, the proposed detection strategies were applied on four different commercially available and synthesized photocatalytic materials. The digital image analysis showed that P25 (Evonik) is the fastest photocatalytic soot degrader of all studied materials for both a uniform soot haze as well as concentrated soot spots. Application of the in situ method showed that for all studied materials adsorbed formate-related surface species were formed and that commercially available ZnO nanopowder has the highest specificity towards complete mineralization into CO2. With this we aim to provide a set of complementary experimental tools for the convenient, reliable, realistic and standardised detection of photocatalytic soot degradation.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000461380400028 Publication Date 2019-02-23
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947; 1873-3212 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.216 Times cited 1 Open Access
Notes ; M.V.H. acknowledges the Research Foundation-Flanders (FWO) for a doctoral fellowship. M.V.H., S.W.V., S.L. and X-Y.Y. thank the FWO and the National Natural Science Foundation of China (NSFC) for funding an international collaboration project. Mr. M. Minjauw is greatly thanked for his help in the AFM measurements. ; Approved Most recent IF: 6.216
Call Number UA @ admin @ c:irua:157789 Serial 5958
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Author Smits, M.; Chan, C. kit; Tytgat, T.; Craeye, B.; Costarramone, N.; Lacombe, S.; Lenaerts, S.
Title Photocatalytic degradation of soot deposition : self-cleaning effect on titanium dioxide coated cementitious materials Type A1 Journal article
Year 2013 Publication Chemical engineering journal Abbreviated Journal Chem Eng J
Volume 222 Issue Pages 411-418
Keywords A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Abstract Diesel soot emissions deteriorate the appearance of architectural building materials by soot fouling. This soot deposition devalue the aesthetic value of the building. A solution to counteract this problem is applying titanium dioxide on building materials. TiO2 can provide air-purifying and self-cleaning properties due to its photocatalytic activity. In literature, photocatalytic soot oxidation is observed on glass or silicon substrates. However, degradation of soot by photocatalysis was not yet investigated on cementitious samples (mortar, concrete) although it is one of the most frequently used building materials. In this study, photocatalytic soot oxidation by means of TiO2 coated cementitious samples is addressed. The soot removal capacity of four types of TiO2 layers, coated on mortar samples, is evaluated by means of two detection methods. The first method is based on colorimetric measurements, while the second method uses digital image processing to calculate the area of soot coverage. The experimental data revealed that cementitious materials coated with commercially available TiO2 exhibited self-cleaning properties as it was found that all coated samples were able to remove soot. The P25 coating gave the best soot degradation performance, while the Eoxolit product showed the slowest soot degradation rate. In addition, gas chromatography measurements in a closed chamber experiment with P25 confirmed that complete mineralization of about 60% of the soot was obtained within 24 hours since CO2 was the sole observed oxidation product. Due to its realistic approach, this study proves that photocatalytic soot removal on TiO2 coated cementitious surfaces is possible in practice, which is an important step towards the practical application of self-cleaning building materials.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000319528900046 Publication Date 2013-03-05
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947; 1873-3212 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.216 Times cited 43 Open Access
Notes ; This work was supported by a PhD grant (M. Smits) from the University of Antwerp, a PhD grant (T. Tytgat) funded by the Institute of Innovation by Science and Technology in Flanders (IWT) and the exchange program Tournesol (Project T2012.05) financed by the Flemish government. ; Approved Most recent IF: 6.216; 2013 IF: 4.058
Call Number UA @ admin @ c:irua:106519 Serial 5979
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Author van Walsem, J.; Roegiers, J.; Modde, B.; Lenaerts, S.; Denys, S.
Title Proof of concept of an upscaled photocatalytic multi-tube reactor : a combined modelling and experimental study Type A1 Journal article
Year 2019 Publication Chemical engineering journal Abbreviated Journal Chem Eng J
Volume 378 Issue 378 Pages 122038
Keywords A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL)
Abstract Three upscaled multi-tube photocatalytic reactors designed for integration into HVAC (Heating, Ventilation and Air Conditioning) systems were proposed and evaluated using a CFD modelling approach, with emphasis on the flow, irradiation and concentration distribution in the reactor and hence, photocatalytic performance. Based on the obtained insights, the best reactor design was selected, further characterized and improved by an additional proof of concept study and eventually converted into practice. Subsequently, the scaled-up prototype was experimentally tested according to the CEN-EN-16846-1 standard (2017) for volatile organic compound (VOC) removal by an external scientific research center. The combined modelling and experimental approach used in this work, leads to essential insights into the design and assessment of photocatalytic reactors. Therefore, this study provides an essential step towards the optimization and commercialization of photocatalytic reactors for HVAC applications.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000487764800011 Publication Date 2019-06-22
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947; 1873-3212 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.216 Times cited Open Access
Notes ; J.V.W. acknowledges the Agentschap Innoveren & Ondernemen for a PhD fellowship. ; Approved Most recent IF: 6.216
Call Number UA @ admin @ c:irua:162190 Serial 5986
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Author Zhou, R.; Zhou, R.; Xian, Y.; Fang, Z.; Lu, X.; Bazaka, K.; Bogaerts, A.; Ostrikov, K.(K.)
Title Plasma-enabled catalyst-free conversion of ethanol to hydrogen gas and carbon dots near room temperature Type A1 Journal article
Year 2020 Publication Chemical Engineering Journal Abbreviated Journal Chem Eng J
Volume 382 Issue 382 Pages 122745
Keywords A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract Selective conversion of bio-renewable ethanol under mild conditions especially at room temperature remains a major challenge for sustainable production of hydrogen and valuable carbon-based materials. In this study, adaptive non-thermal plasma is applied to deliver pulsed energy to rapidly and selectively reform ethanol in the absence of a catalyst. Importantly, the carbon atoms in ethanol that would otherwise be released into the environment in the form of CO or CO2 are effectively captured in the form of carbon dots (CDs). Three modes of non-thermal spark plasma discharges, i.e. single spark mode (SSM), multiple spark mode (MSM) and gliding spark mode (GSM), provide additional flexibility in ethanol reforming by controlling the processes of energy transfer and distribution, thereby affecting the flow rate, gas content, and energy consumption in H-2 production. A favourable combination of low temperature (< 40 degrees C), attractive conversion rate (gas flow rate of similar to 120 mL/min), high hydrogen yield (H-2 content > 90%), low energy consumption (similar to 0.96 kWh/m(3) H-2) and the effective generation of photoluminescent CDs (which are applicable for bioimaging or biolabelling) in the MSM indicate that the proposed strategy may offer a new carbon-negative avenue for comprehensive utilization of alcohols and mitigating the increasingly severe energy and environmental issues.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000503381200200 Publication Date 2019-09-07
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947; 1873-3212 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 15.1 Times cited 20 Open Access
Notes ; ; Approved Most recent IF: 15.1; 2020 IF: 6.216
Call Number UA @ admin @ c:irua:165648 Serial 6318
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Author Lang, X.; Ouyang, Y.; Vandewalle, L.A.; Goshayeshi, B.; Chen, S.; Madanikashani, S.; Perreault, P.; Van Geem, K.M.; van Geem, K.M.
Title Gas-solid hydrodynamics in a stator-rotor vortex chamber reactor Type A1 Journal article
Year 2022 Publication Chemical engineering journal Abbreviated Journal Chem Eng J
Volume 446 Issue 5 Pages 137323-12
Keywords A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
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.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000833418100006 Publication Date 2022-06-01
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN (up) 1385-8947; 1873-3212 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 15.1 Times cited Open Access OpenAccess
Notes Approved Most recent IF: 15.1
Call Number UA @ admin @ c:irua:189283 Serial 7167
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