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Author | Eshtehardi, H.A.; van 't Veer, K.; Delplancke, M.-P.; Reniers, F.; Bogaerts, A. | ||||
Title | Postplasma Catalytic Model for NO Production: Revealing the Underlying Mechanisms to Improve the Process Efficiency | Type | A1 Journal article | ||
Year | 2023 | Publication | ACS Sustainable Chemistry and Engineering | Abbreviated Journal | |
Volume | 11 | Issue | 5 | Pages | 1720-1733 |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Plasma catalysis is emerging for plasma-assisted gas conversion processes. However, the underlying mechanisms of plasma catalysis are poorly understood. In this work, we present a 1D heterogeneous catalysis model with axial dispersion (i.e., accounting for back-mixing and molecular diffusion of fluid elements in the process stream in the axial direction), for plasma-catalytic NO production from N2/O2 mixtures. We investigate the concentration and reaction rates of each species formed as a function of time and position across the catalyst, in order to determine the underlying mechanisms. To obtain insights into how the performance of the process can be further improved, we also study how changes in the postplasma gas flow composition entering the catalyst bed and in the operation conditions of the catalytic stage affect the performance of NO production. | ||||
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Language | Wos | 000926412800001 | Publication Date | 2023-02-06 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2168-0485 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 8.4 | Times cited | Open Access | OpenAccess | |
Notes | Fonds Wetenschappelijk Onderzoek, 30505023 GoF9618n ; Fonds De La Recherche Scientifique FNRS, 30505023 GoF9618n ; H2020 European Research Council, 810182 ; | Approved | Most recent IF: 8.4; 2023 IF: 5.951 | ||
Call Number | PLASMANT @ plasmant @c:irua:195377 | Serial | 7241 | ||
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Author | Eshtehardi, H.A.; Van ‘t Veer, K.; Delplancke, M.-P.; Reniers, F.; Bogaerts, A. | ||||
Title | Postplasma Catalytic Model for NO Production: Revealing the Underlying Mechanisms to Improve the Process Efficiency | Type | A1 Journal article | ||
Year | 2023 | Publication | ACS Sustainable Chemistry and Engineering | Abbreviated Journal | |
Volume | 11 | Issue | 5 | Pages | 1720-1733 |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Plasma catalysis is emerging for plasma-assisted gas conversion processes. However, the underlying mechanisms of plasma catalysis are poorly understood. In this work, we present a 1D heterogeneous catalysis model with axial dispersion (i.e., accounting for back-mixing and molecular diffusion of fluid elements in the process stream in the axial direction), for plasma-catalytic NO production from N2/O2 mixtures. We investigate the concentration and reaction rates of each species formed as a function of time and position across the catalyst, in order to determine the underlying mechanisms. To obtain insights into how the performance of the process can be further improved, we also study how changes in the postplasma gas flow composition entering the catalyst bed and in the operation conditions of the catalytic stage affect the performance of NO production. |
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Language | Wos | 000926412800001 | Publication Date | 2023-02-06 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2168-0485 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 8.4 | 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) and the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No. 810182 − SCOPE ERC Synergy project). The 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: 8.4; 2023 IF: 5.951 | ||
Call Number | PLASMANT @ plasmant @c:irua:195377 | Serial | 7257 | ||
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Author | Eshtehardi, H.A.; Van ‘t Veer, K.; Delplancke, M.-P.; Reniers, F.; Bogaerts, A. | ||||
Title | Postplasma Catalytic Model for NO Production: Revealing the Underlying Mechanisms to Improve the Process Efficiency | Type | A1 Journal article | ||
Year | 2023 | Publication | ACS Sustainable Chemistry and Engineering | Abbreviated Journal | |
Volume | 11 | Issue | 5 | Pages | 1720-1733 |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Plasma catalysis is emerging for plasma-assisted gas conversion processes. However, the underlying mechanisms of plasma catalysis are poorly understood. In this work, we present a 1D heterogeneous catalysis model with axial dispersion (i.e., accounting for back-mixing and molecular diffusion of fluid elements in the process stream in the axial direction), for plasma-catalytic NO production from N2/O2 mixtures. We investigate the concentration and reaction rates of each species formed as a function of time and position across the catalyst, in order to determine the underlying mechanisms. To obtain insights into how the performance of the process can be further improved, we also study how changes in the postplasma gas flow composition entering the catalyst bed and in the operation conditions of the catalytic stage affect the performance of NO production. |
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000926412800001 | Publication Date | 2023-02-06 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2168-0485 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 8.4 | Times cited | Open Access | OpenAccess | |
Notes | Fonds Wetenschappelijk Onderzoek, 30505023 GoF9618n ; Fonds De La Recherche Scientifique – FNRS, 30505023 GoF9618n ; H2020 European Research Council, 810182 ; | Approved | Most recent IF: 8.4; 2023 IF: 5.951 | ||
Call Number | PLASMANT @ plasmant @c:irua:195377 | Serial | 7258 | ||
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Author | Pattyn, C.; Maira, N.; Buddhadasa, M.; Vervloessem, E.; Iseni, S.; Roy, N.C.; Remy, A.; Delplancke, M.-P.; De Geyter, N.; Reniers, F. | ||||
Title | Disproportionation of nitrogen induced by DC plasma-driven electrolysis in a nitrogen atmosphere | Type | A1 Journal article | ||
Year | 2022 | Publication | Green Chemistry | Abbreviated Journal | Green Chem |
Volume | 24 | Issue | 18 | Pages | 7100-7112 |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Nitrogen disproportionation i.e. its simultaneous conversion to compounds of higher (NOx) and lower (NH3) oxidation states in a N-2 DC plasma-driven electrolysis process with a plasma cathode is investigated. This type of plasma-liquid interaction exhibits a growing interest for many applications, in particular nitrogen fixation where it represents a green alternative to the Haber-Bosch process. Optical emission spectroscopy, FTIR and electrochemical sensing systems are used to characterize the gas phase physico-chemistry while the liquid phase is analyzed via ionic chromatography and colorimetric assays. Experiments suggest that lowering the discharge current enhances nitrogen reduction and facilitates the transfer of nitrogen compounds to the liquid phase. Large amounts of water vapor appear to impact the gas discharge physico-chemistry and to favor the vibrational excitation of N-2, a key parameter for an energy-efficient nitrogen fixation. | ||||
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Language | Wos | 000847733600001 | Publication Date | 2022-08-30 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1463-9262; 1463-9270 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 9.8 | Times cited | Open Access | OpenAccess | |
Notes | Approved | Most recent IF: 9.8 | |||
Call Number | UA @ admin @ c:irua:190655 | Serial | 7145 | ||
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Author | van ‘t Veer, K.; van Alphen, S.; Remy, A.; Gorbanev, Y.; De Geyter, N.; Snyders, R.; Reniers, F.; Bogaerts, A. | ||||
Title | Spatially and temporally non-uniform plasmas: microdischarges from the perspective of molecules in a packed bed plasma reactor | Type | A1 Journal article | ||
Year | 2021 | Publication | Journal Of Physics D-Applied Physics | Abbreviated Journal | J Phys D Appl Phys |
Volume | 54 | Issue | 17 | Pages | 174002 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Dielectric barrier discharges (DBDs) typically operate in the filamentary regime and thus exhibit great spatial and temporal non-uniformity. In order to optimize DBDs for various applications, such as in plasma catalysis, more fundamental insight is needed. Here, we consider how the millions of microdischarges, characteristic for a DBD, influence individual gas molecules. We use a Monte Carlo approach to determine the number of microdischarges to which a single molecule would be exposed, by means of particle tracing simulations through a full-scale packed bed DBD reactor, as well as an empty DBD reactor. We find that the fraction of microdischarges to which the molecules are exposed can be approximated as the microdischarge volume over the entire reactor gas volume. The use of this concept provides good agreement between a plasma-catalytic kinetics model and experiments for plasma-catalytic NH3 synthesis. We also show that the concept of the fraction of microdischarges indicates the efficiency by which the plasma power is transferred to the gas molecules. This generalised concept is also applicable for other spatially and temporally non-uniform plasmas. | ||||
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Language | Wos | 000618776000001 | Publication Date | 2021-04-29 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0022-3727 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 2.588 | Times cited | Open Access | OpenAccess | |
Notes | Excellence of Science FWO-FNRS project, FWO grant ID GoF9618n ; Flemish Government, project P2C (HBC.2019.0108) ; H2020 European Research Council, grant agreement No 810182 – SCOPE ERC Synergy pr ; 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 by the Flemish Government through the Moonshot cSBO project P2C (HBC. 2019.0108). 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. The authors would also like to thank Hamid Ahmadi Eshtehardi for discussions on the plasma-kinetic DBD model and Yannick Engelmann for discussions on the surface kinetics model. | Approved | Most recent IF: 2.588 | ||
Call Number | PLASMANT @ plasmant @c:irua:175878 | Serial | 6674 | ||
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Author | van ‘t Veer, K.; Engelmann, Y.; Reniers, F.; Bogaerts, A. | ||||
Title | Plasma-Catalytic Ammonia Synthesis in a DBD Plasma: Role of Microdischarges and Their Afterglows | Type | A1 Journal article | ||
Year | 2020 | Publication | Journal Of Physical Chemistry C | Abbreviated Journal | J Phys Chem C |
Volume | 124 | Issue | 42 | Pages | 22871-22883 |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Movement Antwerp (MOVANT) | ||||
Abstract | Plasma-catalytic ammonia synthesis is receiving ever increasing attention, especially in packed bed dielectric barrier discharge (DBD) reactors. The latter typically operate in the filamentary regime when used for gas conversion applications. While DBDs are in principle well understood and already applied in the industry, the incorporation of packing materials and catalytic surfaces considerably adds to the complexity of the plasma physics and chemistry governing the ammonia formation. We employ a plasma kinetics model to gain insights into the ammonia formation mechanisms, paying special attention to the role of filamentary microdischarges and their afterglows. During the microdischarges, the synthesized ammonia is actually decomposed, but the radicals created upon electron impact dissociation of N2 and H2 and the subsequent catalytic reactions cause a net ammonia gain in the afterglows of the microdischarges. Under our plasma conditions, electron impact dissociation of N2 in the gas phase followed by the adsorption of N atoms is identified as a rate-limiting step, instead of dissociative adsorption of N2 on the catalyst surface. Both elementary Eley−Rideal and Langmuir−Hinshelwood reaction steps can be found important in plasma-catalytic NH3 synthesis. | ||||
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Language | Wos | 000585970300002 | Publication Date | 2020-10-22 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1932-7447 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 3.7 | Times cited | Open Access | OpenAccess | |
Notes | Fonds Wetenschappelijk Onderzoek, 30505023 GoF9618n ; Fonds De La Recherche Scientifique – FNRS, 30505023 GoF9618n ; H2020 European Research Council, 810182 ;This research was supported by the Excellence of Science FWOFNRS project (FWO grant ID GoF9618n, EOS ID 30505023) and by the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement no 810182-SCOPE ERC Synergy project). The 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. The authors would also like to thank Järi Van den Hoek and Dr. Yury Gorbanev for providing the experimentally measured electrical characteristics and Dr. Fatme Jardali for creating the TOC graphics. | Approved | Most recent IF: 3.7; 2020 IF: 4.536 | ||
Call Number | PLASMANT @ plasmant @c:irua:173587 | Serial | 6428 | ||
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Author | van ‘t Veer, K.; Reniers, F.; Bogaerts, A. | ||||
Title | Zero-dimensional modeling of unpacked and packed bed dielectric barrier discharges: the role of vibrational kinetics in ammonia synthesis | Type | A1 Journal article | ||
Year | 2020 | Publication | Plasma Sources Science & Technology | Abbreviated Journal | Plasma Sources Sci T |
Volume | 29 | Issue | 4 | Pages | 045020 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | We present a zero-dimensional plasma kinetics model, including both surface and gas phase kinetics, to determine the role of vibrationally excited states in plasma-catalytic ammonia synthesis. We defined a new method to systematically capture the conditions of dielectric barrier discharges (DBDs), including those found in packed bed DBDs. We included the spatial and temporal nature of such discharges by special consideration of the number of micro-discharges in the model. We introduce a parameter that assigns only a part of the plasma power to the microdischarges, to scale the model conditions from filamentary to uniform plasma. Because of the spatial and temporal behaviour of the micro-discharges, not all micro-discharges occurring in the plasma reactor during a certain gas residence time are affecting the molecules. The fraction of power considered in the model ranges from 0.005 %, for filamentary plasma, to 100 %, for uniform plasma. If vibrational excitation is included in the plasma chemistry, these different conditions, however, yield an ammonia density that is only varying within one order of magnitude. At only 0.05 % of the power put into the uniform plasma component, a model neglecting vibrational excitation clearly does not result in adequate amounts of ammonia. Thus, our new model, which accounts for the concept in which not all the power is deposited by the micro-discharges, but some part may also be distributed in between them, suggests that vibrational kinetic processes are really important in (packed bed) DBDs. Indeed, vibrational excitation takes place in both the uniform plasma between the micro-discharges and in the strong micro-discharges, and is responsible for an increased N2 dissociation rate. This is shown here for plasma-catalytic ammonia synthesis, but might also be valid for other gas conversion applications. | ||||
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Language | Wos | 000570241500001 | Publication Date | 2020-04-09 | |
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Series Volume | Series Issue | Edition | |||
ISSN | 1361-6595 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 3.8 | Times cited | Open Access | ||
Notes | This research was supported by the Excellence of Science FWO-FNRS project (FWO grant ID GoF9618n, EOS ID 30505023). 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. The authors would also like to thank Dr. Fatme Jardali for the discussions on plasma kinetic modelling and Dr. Jungmi Hong and Dr. Anthony B. Murphy for their aid in the calculation of the diffusion coefficients. | Approved | Most recent IF: 3.8; 2020 IF: 3.302 | ||
Call Number | PLASMANT @ plasmant @c:irua:168097 | Serial | 6359 | ||
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Author | Michielsen, I.; Uytdenhouwen, Y.; Pype, J.; Michielsen, B.; Mertens, J.; Reniers, F.; Meynen, V.; Bogaerts, A. | ||||
Title | CO 2 dissociation in a packed bed DBD reactor: First steps towards a better understanding of plasma catalysis | Type | A1 Journal article | ||
Year | 2017 | Publication | Chemical engineering journal | Abbreviated Journal | Chem Eng J |
Volume | 326 | Issue | 326 | Pages | 477-488 |
Keywords | A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Plasma catalysis is gaining increasing interest for CO2 conversion, but the interaction between the plasma and catalyst is still poorly understood. This is caused by limited systematic materials research, since most works combine a plasma with commercial supported catalysts and packings. In the present paper, we study the influence of specific material and reactor properties, as well as reactor/bead configuration, on the conversion and energy efficiency of CO2 dissociation in a packed bed dielectric barrier discharge (DBD) reactor. Of the various packing materials investigated, BaTiO3 yields the highest conversion and energy efficiency, i.e., 25% and 4.5%. Our results show that, when evaluating the influence of catalysts, the impact of the packing (support) material itself cannot be neglected, since it can largely affect the conversion and energy efficiency. This shows the large potential for further improvement of packed bed plasma reactors for CO2 conversion and other chemical conversion reactions by adjusting both packing (support) properties and catalytically active sites. Moreover, we clearly prove that comparison of results obtained in different reactor setups should be done with care, since there is a large effect of the reactor setup and reactor/bead configuration. |
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Language | Wos | 000406137200047 | Publication Date | 2017-06-01 | |
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ISSN | 1385-8947 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 6.216 | Times cited | 49 | Open Access | OpenAccess |
Notes | This research was carried out with financial support of the Institute for the Promotion of Innovation by Science and Technology in Flanders (IWT Flanders) for both I. Michielsen (IWT-141093) and J. Pype (IWT-131229) and of the Walloon region through the excellence programme FLYCOAT (nr. 1318147) for the profilometry measurements. The authors also acknowledge financial support from an IOF-SBO project from the University of Antwerp and from the Fund for Scientific Research (FWO; grant number: G.0254.14 N). This research was carried out in the framework of the network on Physical Chemistry of Plasma-Surface Interactions – Interuniversity Attraction Poles, phase VII (http://psi-iap7.ulb. ac.be/), and supported by the Belgian Science Policy Office (BELSPO). The authors would also like to thank Koen Van Laer for the discussions on this manuscript. | Approved | Most recent IF: 6.216 | ||
Call Number | PLASMANT @ plasmant @ c:irua:144802 | Serial | 4626 | ||
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Author | Ozkan, A.; Bogaerts, A.; Reniers, F. | ||||
Title | Routes to increase the conversion and the energy efficiency in the splitting of CO2by a dielectric barrier discharge | Type | A1 Journal article | ||
Year | 2017 | Publication | Journal of physics: D: applied physics | Abbreviated Journal | J Phys D Appl Phys |
Volume | 50 | Issue | 50 | Pages | 084004 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Here, we present routes to increase CO2 conversion into CO using an atmospheric pressure dielectric-barrier discharge. The change in conversion as a function of simple plasma parameters, such as power, flow rate, but also frequency, on-and-off power pulse, thickness and the chemical nature of the dielectric, wall and gas temperature, are described. By means of an in-depth electrical characterization of the discharge (effective plasma voltage, dielectric voltage, plasma current, number and lifetime of the microdischarges), combined with infrared analysis of the walls of the reactor, optical emission spectroscopy for the gas temperature, and mass spectrometry for the CO2 conversion, we propose a global interpretation of the effect of all the experimental parameters on the conversion and efficiency of the reaction. | ||||
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Language | Wos | 000395400700001 | Publication Date | 2017-01-30 | |
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Series Volume | Series Issue | Edition | |||
ISSN | 0022-3727 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 2.588 | Times cited | 28 | Open Access | OpenAccess |
Notes | The authors acknowledge financial support from the IAPVII/ 12, P7/34 (Interuniversity Attraction Pole) program PSIPhysical Chemistry of Plasma–Surface Interaction financially supported by the Belgian Federal Office for Science Policy (BELSPO). A Ozkan would like to thank the financial support given by the Fonds David et Alice Van Buuren. | Approved | Most recent IF: 2.588 | ||
Call Number | PLASMANT @ plasmant @ c:irua:140093 | Serial | 4415 | ||
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Author | Snoeckx, R.; Ozkan, A.; Reniers, F.; Bogaerts, A. | ||||
Title | The Quest for Value-Added Products from Carbon Dioxide and Water in a Dielectric Barrier Discharge: A Chemical Kinetics Study | Type | A1 Journal article | ||
Year | 2017 | Publication | Chemsuschem | Abbreviated Journal | Chemsuschem |
Volume | 10 | Issue | 10 | Pages | 409-424 |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Recycling of carbon dioxide by its conversion into value-added products has gained significant interest owing to the role it can play for use in an anthropogenic carbon cycle. The combined conversion with H2O could even mimic the natural photosynthesis process. An interesting gas conversion technique currently being considered in the field of CO2 conversion is plasma technology. To investigate whether it is also promising for this combined conversion, we performed a series of experiments and developed a chemical kinetics plasma chemistry model for a deeper understanding of the process. The main products formed were the syngas components CO and H2, as well as O2 and H2O2, whereas methanol formation was only observed in the parts-per-billion to parts-per-million range. The syngas ratio, on the other hand, could easily be controlled by varying both the water content and/or energy input. On the basis of the model, which was validated with experimental results, a chemical kinetics analysis was performed, which allowed the construction and investigation of the different pathways leading to the observed experimental results and which helped to clarify these results. This approach allowed us to evaluate this technology on the basis of its underlying chemistry and to propose solutions on how to further improve the formation of value-added products by using plasma technology. | ||||
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Language | Wos | 000394571900012 | Publication Date | 2016-11-25 | |
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ISSN | 1864-5631 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 7.226 | Times cited | 25 | Open Access | OpenAccess |
Notes | The authors acknowledge financial support from the Inter-university Attraction Pole (IAP; grant number IAP-VII/12, P7/34) program “PSI-Physical Chemistry of Plasma-Surface Interactions”, financially supported by the Belgian Federal Office for Science Policy (BELSPO), as well as the Fund for Scientific Research Flanders (FWO; grant number G.0066.12N). This work was performed in part using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen, a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the University of Antwerp. We also would like to thank the financial support given by “Fonds David et Alice Van Buuren”. Finally, we are very grateful to M. Kushner for providing the Global kin code, to T. Dufour for his support during the experiments, and to R. Aerts for his support during the model development. | Approved | Most recent IF: 7.226 | ||
Call Number | PLASMANT @ plasmant @ c:irua:139880 | Serial | 4412 | ||
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Author | Ozkan, A.; Dufour, T.; Silva, T.; Britun, N.; Snyders, R.; Reniers, F.; Bogaerts, A. | ||||
Title | DBD in burst mode: solution for more efficient CO2conversion? | Type | A1 Journal article | ||
Year | 2016 | Publication | Plasma sources science and technology | Abbreviated Journal | Plasma Sources Sci T |
Volume | 25 | Issue | 25 | Pages | 055005 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | CO2 conversion into value-added products has gained significant interest over the few last years, as the greenhouse gas concentrations constantly increase due to anthropogenic activities. Here we report on experiments for CO2 conversion by means of a cold atmospheric plasma using a cylindrical flowing dielectric barrier discharge (DBD) reactor. A detailed comparison of this DBD ignited in a so-called burst mode (i.e. where an AC voltage is applied during a limited amount of time) and pure AC mode is carried out to evaluate their effect on the conversion of CO2 as well as on the energy efficiency. Decreasing the duty cycle in the burst mode from 100% (i.e. corresponding to pure AC mode) to 40% leads to a rise in the conversion from 16–26% and to a rise in the energy efficiency from 15 to 23%. Based on a detailed electrical analysis, we show that the conversion correlates with the features of the microfilaments. Moreover, the root-mean-square voltage in the burst mode remains constant as a function of the process time for the duty cycles <70%, while a higher duty cycle or the usual pure AC mode leads to a clear voltage decay by more than 500 V, over approximately 90 s, before reaching a steady state regime. The higher plasma voltage in the burst mode yields a higher electric field. This causes the increasing the electron energy, and therefore their involvement in the CO2 dissociation process, which is an additional explanation for the higher CO2 conversion and energy efficiency in the burst mode. |
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Language | Wos | 000403945500005 | Publication Date | 2016-08-02 | |
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ISSN | 1361-6595 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 3.302 | Times cited | 17 | Open Access | |
Notes | The authors acknowledge financial support from the IAPVII/ 12, P7/34 (Inter-university Attraction Pole) program ‘PSI-Physical Chemistry of Plasma-Surface Interactions’, financially supported by the Belgian Federal Office for Science Policy (BELSPO). A. Ozkan would also like to thank financial support given by ‘Fonds David et Alice Van Buuren’. | Approved | Most recent IF: 3.302 | ||
Call Number | c:irua:134841 | Serial | 4107 | ||
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Author | Ozkan, A.; Dufour, T.; Bogaerts, A.; Reniers, F. | ||||
Title | How do the barrier thickness and dielectric material influence the filamentary mode and CO2conversion in a flowing DBD? | Type | A1 Journal article | ||
Year | 2016 | Publication | Plasma sources science and technology | Abbreviated Journal | Plasma Sources Sci T |
Volume | 25 | Issue | 25 | Pages | 045016 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Dielectric barrier discharges (DBDs) are commonly used to generate cold plasmas at atmospheric pressure. Whatever their configuration (tubular or planar), the presence of a dielectric barrier is mandatory to prevent too much charge build up in the plasma and the formation of a thermal arc. In this article, the role of the barrier thickness (2.0, 2.4 and 2.8 mm) and of the kind of dielectric material (alumina, mullite, pyrex, quartz) is investigated on the filamentary behavior in the plasma and on the CO2 conversion in a tubular flowing DBD, by means of mass spectrometry measurements correlated with electrical characterization and IR imaging. Increasing the barrier thickness decreases the capacitance, while preserving the electrical charge. As a result, the voltage over the dielectric increases and a larger number of microdischarges is generated, which enhances the CO2 conversion. Furthermore, changing the dielectric material of the barrier, while keeping the same geometry and dimensions, also affects the CO2 conversion. The highest CO2 conversion and energy efficiency are obtained for quartz and alumina, thus not following the trend of the relative permittivity. From the electrical characterization, we clearly demonstrate that the most important parameters are the somewhat higher effective plasma voltage (yielding a somewhat higher electric field and electron energy in the plasma) for quartz, as well as the higher plasma current (and thus larger electron density) and the larger number of microdischarge filaments (mainly for alumina, but also for quartz). The latter could be correlated to the higher surface roughness for alumina and to the higher voltage over the dielectric for quartz. |
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000380380200030 | Publication Date | 2016-06-30 | |
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Series Volume | Series Issue | Edition | |||
ISSN | 0963-0252 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 3.302 | Times cited | 24 | Open Access | |
Notes | The authors acknowledge financial support from the IAPVII/ 12, P7/34 (Inter-university Attraction Pole) program ‘PSI-Physical Chemistry of Plasma-Surface Interactions’, financially supported by the Belgian Federal Office for Science Policy (BELSPO). A. Ozkan would like to thank the financial support given by ‘Fonds David et Alice Van Buuren’. | Approved | Most recent IF: 3.302 | ||
Call Number | c:irua:134396 | Serial | 4100 | ||
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Author | Ozkan, A.; Dufour, T.; Silva, T.; Britun, N.; Snyders, R.; Bogaerts, A.; Reniers, F. | ||||
Title | The influence of power and frequency on the filamentary behavior of a flowing DBD—application to the splitting of CO2 | Type | A1 Journal article | ||
Year | 2016 | Publication | Plasma sources science and technology | Abbreviated Journal | Plasma Sources Sci T |
Volume | 25 | Issue | 25 | Pages | 025013 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | In this experimental study, a flowing dielectric barrier discharge operating at atmospheric pressure is used for the splitting of CO2 into O2 and CO. The influence of the applied frequency and plasma power on the microdischarge properties is investigated to understand their role on the CO2 conversion. Electrical measurements are carried out to explain the conversion trends and to characterize the microdischarges through their number, their lifetime, their intensity and the induced electrical charge. Their influence on the gas and electrode temperatures is also evidenced through optical emission spectroscopy and infrared imaging. It is shown that, in our configuration, the conversion depends mostly on the charge delivered in the plasma and not on the effective plasma voltage when the applied power is modified. Similarly, at constant total current, a better conversion is observed at low frequencies, where a less filamentary discharge regime with a higher effective plasma voltage than that at a higher frequency is obtained. |
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Language | Wos | 000372337900015 | Publication Date | 2016-02-25 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0963-0252 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 3.302 | Times cited | 40 | Open Access | |
Notes | The authors acknowledge financial support from the IAPVII/ 12, P7/34 (Inter-university Attraction Pole) program ‘PSI-Physical Chemistry of Plasma-Surface Interactions’, financially supported by the Belgian Federal Office for Science Policy (BELSPO). A Ozkan would like to thank the financial support given by ‘Fonds David et Alice Van Buuren’. N Britun is a postdoctoral researcher of the F.R.S.-FNRS, Belgium. | Approved | Most recent IF: 3.302 | ||
Call Number | c:irua:131904 | Serial | 4021 | ||
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Author | Ozkan, A.; Dufour, T.; Arnoult, G.; De Keyzer, P.; Bogaerts, A.; Reniers, F. | ||||
Title | CO2-CH4 conversion and syngas formation at atmospheric pressure using a multi-electrode dielectric barrier discharge | Type | A1 Journal article | ||
Year | 2015 | Publication | Journal of CO2 utilization | Abbreviated Journal | J Co2 Util |
Volume | 9 | Issue | 9 | Pages | 74-81 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | The conversion of CO2 and CH4 into value-added chemicals is studied in a new geometry of a dielectric barrier discharge (DBD) with multi-electrodes, dedicated to the treatment of high gas flow rates. Gas chromatography is used to define the CO2 and CH4 conversion as well as the yields of the products of decomposition (CO, O2 and H2) and of recombination (C2H4, C2H6 and CH2O). The influence of three parameters is investigated on the conversion: the CO2 and CH4 flow rates, the plasma power and the nature of the carrier gas (argon or helium). The energy efficiency of the CO2 conversion is estimated and compared with those of similar atmospheric plasma sources. Our DBD reactor shows a good compromise between a good energy efficiency and the treatment of a large CO2 flow rate. | ||||
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Language | Wos | 000350088700010 | Publication Date | 2015-01-28 | |
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ISSN | 2212-9820; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 4.292 | Times cited | 57 | Open Access | |
Notes | Approved | Most recent IF: 4.292; 2015 IF: 3.091 | |||
Call Number | c:irua:123029 | Serial | 3522 | ||
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Author | Dufour, T.; Minnebo, J.; Abou Rich, S.; Neyts, E.C.; Bogaerts, A.; Reniers, F. | ||||
Title | Understanding polyethylene surface functionalization by an atmospheric He/O2 plasma through combined experiments and simulations | Type | A1 Journal article | ||
Year | 2014 | Publication | Journal of physics: D: applied physics | Abbreviated Journal | J Phys D Appl Phys |
Volume | 47 | Issue | 22 | Pages | 224007 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | High density polyethylene surfaces were exposed to the atmospheric post-discharge of a radiofrequency plasma torch supplied in helium and oxygen. Dynamic water contact angle measurements were performed to evaluate changes in surface hydrophilicity and angle resolved x-ray photoelectron spectroscopy was carried out to identify the functional groups responsible for wettability changes and to study their subsurface depth profiles, up to 9 nm in depth. The reactions leading to the formation of CO, C = O and OC = O groups were simulated by molecular dynamics. These simulations demonstrate that impinging oxygen atoms do not react immediately upon impact but rather remain at or close to the surface before eventually reacting. The simulations also explain the release of gaseous species in the ambient environment as well as the ejection of low molecular weight oxidized materials from the surface. | ||||
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Publisher | Place of Publication | London | Editor | ||
Language | Wos | 000336207900008 | Publication Date | 2014-05-14 | |
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ISSN | 0022-3727;1361-6463; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 2.588 | Times cited | 13 | Open Access | |
Notes | Approved | Most recent IF: 2.588; 2014 IF: 2.721 | |||
Call Number | UA @ lucian @ c:irua:116919 | Serial | 3804 | ||
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Author | Maerivoet, S.; Tsonev, I.; Slaets, J.; Reniers, F.; Bogaerts, A. | ||||
Title | Coupled multi-dimensional modelling of warm plasmas: Application and validation for an atmospheric pressure glow discharge in CO2/CH4/O2 | Type | A1 Journal Article | ||
Year | 2024 | Publication | Chemical Engineering Journal | Abbreviated Journal | Chemical Engineering Journal |
Volume | 492 | Issue | Pages | 152006 | |
Keywords | A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | To support experimental research into gas conversion by warm plasmas, models should be developed to explain the experimental observations. These models need to describe all physical and chemical plasma properties in a coupled way. In this paper, we present a modelling approach to solve the complete set of assumed relevant equations, including gas flow, heat balance and species transport, coupled with a rather extensive chemistry set, consisting of 21 species, obtained by reduction of a more detailed chemistry set, consisting of 41 species. We apply this model to study the combined CO2 and CH4 conversion in the presence of O2, in a direct current atmospheric pressure glow discharge. Our model can predict the experimental trends, and can explain why higher O2 fractions result in higher CH4 conversion, namely due to the higher gas temperature, rather than just by additional chemical reactions. Indeed, our model predicts that when more O2 is added, the energy required to reach any set temperature (i.e., the enthalpy) drops, allowing the system to reach higher temperatures with similar amounts of energy. This is in turn related to the higher H2O fraction and lower H2 fraction formed in the plasma, as demonstrated by our model. Altogether, our new self-consistent model can capture the main physics and chemistry occurring in this warm plasma, which is an important step towards predictive modelling for plasma-based gas conversion. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2024-05-09 | ||
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ISSN | 1385-8947 | ISBN | Additional Links | ||
Impact Factor | 15.1 | Times cited | Open Access | ||
Notes | This research was supported by the Excellence of Science FWO-FNRS project (FWO grant ID G0I1822N; EOS ID 40007511) and the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No. 810182–SCOPE ERC Synergy project, and grant agreement No. 101081162–PREPARE ERC Proof of Concept project). computational resources and services used in this work were provided by the HPC core facility CalcUA of the Universiteit Antwerpen, and VSC (Flemish Supercomputer Center), funded by the Research Foundation – Flanders (FWO) and the Flemish Government. | Approved | Most recent IF: 15.1; 2024 IF: 6.216 | ||
Call Number | PLASMANT @ plasmant @ | Serial | 9132 | ||
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