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Author |
Belov, I.; Vermeiren, V.; Paulussen, S.; Bogaerts, A. |
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Title |
Carbon dioxide dissociation in a microwave plasma reactor operating in a wide pressure range and different gas inlet configurations |
Type |
A1 Journal article |
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Year  |
2018 |
Publication |
Journal of CO2 utilization |
Abbreviated Journal |
J Co2 Util |
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Volume |
24 |
Issue |
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Pages |
386-397 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
Microwave (MW) plasmas represent a promising solution for efficient CO2 dissociation. MW discharges are also very versatile and can be sustained at various pressure and gas flow regimes. To identify the most favorable conditions for the further scale-up of the CO2 decomposition reaction, a MW plasma reactor operating in pure CO2 in a wide pressure range (200 mbar–1 bar) is studied. Three different gas flow configurations are explored: a direct, reverse and a vortex regime. The CO2 conversion and energy efficiency drop almost linearly with increasing pressure, regardless of the gas flow regime. The results obtained in the direct flow configuration underline the importance of post-discharge cooling, as the exhaust of the MW plasma reactor in this regime expanded into the vacuum chamber without additional quenching. As a result, this system yields exhaust temperatures of up to 1000 K, which explains the lowest conversion (∼3.5% at 200 mbar and 2% at 1 bar). A post-discharge cooling step is introduced for the reverse gas inlet regime and allows the highest conversion to be achieved (∼38% at 200 mbar and 6.2% at 1 bar, with energy efficiencies of 23% and 3.7%). Finally, a tangential gas inlet is utilized in the vortex configuration to generate a swirl flow pattern. This results in the generation of a stable discharge in a broader range of CO2 flows (15–30 SLM) and the highest energy efficiencies obtained in this study (∼25% at 300 mbar and ∼13% at 1 bar, at conversions of 21% and 12%). The experimental results are complemented with computational fluid dynamics simulations and with the analysis of the latest literature to identify the further research directions. |
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Wos |
000428234500045 |
Publication Date |
2018-03-15 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2212-9820 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.292 |
Times cited |
8 |
Open Access |
Not_Open_Access: Available from 16.03.2020
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Notes |
The research leading to these results has received funding from the European Union Seventh Framework Programme (FP7-PEOPLE-2013- ITN) under Grant Agreement№606889 (R |
Approved |
Most recent IF: 4.292 |
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Call Number |
PLASMANT @ plasmant @c:irua:150874 |
Serial |
4955 |
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Author |
Belov, I.; Paulussen, S.; Bogaerts, A. |
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Title |
Pressure as an additional control handle for non-thermal atmospheric plasma processes |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
Plasma processes and polymers |
Abbreviated Journal |
Plasma Process Polym |
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Volume |
14 |
Issue |
11 |
Pages |
1700046 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
above atmospheric) pressure regimes (1–3.5 bar). It was demonstrated that these operational conditions significantly influence both the discharge dynamics and the process efficiencies of O2 and CO2 discharges. For the case of the O2 DBD, the pressure rise results in the amplification of the discharge current, the appearance of emission lines of the metal electrode material (Fe, Cr, Ni) in the optical emission spectrum and the formation of a granular film of the erosion products (10–300 nm iron oxide nanoparticles) on the reactor walls. Somewhat similar behavior was observed also for the CO2 DBD. The discharge current, the relative intensity of the CO Angstrom band measured by Optical Emission Spectroscopy (OES) and the CO2 conversion rates could be stimulated to some extent by the rise in pressure. The optimal conditions for the O2 DBD (P = 2 bar) and the CO2 DBD (P = 1.5 bar) are demonstrated. It can be argued that the dynamics of the microdischarges (MD) define the underlying process of this behavior. It could be
demonstrated that the pressure increase stimulates the formation of more intensive but fewer MDs. In this way, the operating pressure can represent an additional tool to manipulate the properties of the MDs in a DBD, and as a result also the discharge performance. |
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Wos |
000415339700011 |
Publication Date |
2017-06-07 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1612-8850 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
2.846 |
Times cited |
1 |
Open Access |
Not_Open_Access |
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Notes |
Seventh Framework Programme, Grant Agreement № 606889 (RAPID – Reactive Atmospheric Plasma processIng – Education Network) ; |
Approved |
Most recent IF: 2.846 |
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Call Number |
PLASMANT @ plasmant @c:irua:147024 |
Serial |
4763 |
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| Permanent link to this record |
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Author |
Belov, I.; Vanneste, J.; Aghaee, M.; Paulussen, S.; Bogaerts, A. |
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Title |
Synthesis of Micro- and Nanomaterials in CO2and CO Dielectric Barrier Discharges: Synthesis of Micro- and Nanomaterials… |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
Plasma processes and polymers |
Abbreviated Journal |
Plasma Process Polym |
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Volume |
14 |
Issue |
14 |
Pages |
1600065 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
Dielectric Barrier Discharges operating in CO and CO2 form solid products at atmospheric pressure. The main differences between both plasmas and their deposits were analyzed, at similar energy input. GC measurements revealed a mixture of CO2, CO, and O2 in the CO2 DBD exhaust, while no O2 was found in the CO plasma. A coating of nanoparticles composed of Fe, O, and C was produced by the CO2 discharge, whereas, a microscopic dendrite-like carbon structure was formed in the CO plasma. Fe3O4 and Fe crystalline phases were found in the CO2 sample. The CO
deposition was characterized as an amorphous structure, close to polymeric CO (p-CO). Interestingly, p-CO is not formed in the CO2 plasma, in spite of the significant amounts of CO produced (up to 30% in the reactor exhaust). |
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Wos |
000397476000007 |
Publication Date |
2016-07-29 |
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Series Editor |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1612-8850 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
2.846 |
Times cited |
10 |
Open Access |
Not_Open_Access |
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Notes |
European Union Seventh Framework Programme FP7-PEOPLE-2013-ITN, 606889 ; |
Approved |
Most recent IF: 2.846 |
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Call Number |
PLASMANT @ plasmant @ c:irua:141759 |
Serial |
4487 |
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Author |
Belov, I.; Paulussen, S.; Bogaerts, A. |
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Title |
Appearance of a conductive carbonaceous coating in a CO2dielectric barrier discharge and its influence on the electrical properties and the conversion efficiency |
Type |
A1 Journal article |
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Year |
2016 |
Publication |
Plasma sources science and technology |
Abbreviated Journal |
Plasma Sources Sci T |
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Volume |
25 |
Issue |
25 |
Pages |
015023 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
This work examines the properties of a dielectric barrier discharge (DBD) reactor, built for CO2 decomposition, by means of electrical characterization, optical emission spectroscopy and gas chromatography. The discharge, formed in an electronegative gas (such as CO2, but also O2), exhibits clearly different electrical characteristics, depending on the surface conductivity of the reactor walls. An asymmetric current waveform is observed in the metaldielectric (MD) configuration, with sparse high-current pulses in the positive half-cycle (HC) and a more uniform regime in the negative HC. This indicates that the discharge is operating in two alternating regimes with rather different properties. At high CO2 conversion regimes, a conductive coating is deposited on the dielectric. This so-called coated MD configuration yields a symmetric current waveform, with current peaks in both the positive and negative HCs. In a double-dielectric (DD) configuration, the current waveform is also symmetric, but without current peaks in both the positive and negative HC. Finally, the DD configuration with conductive coating on the inner surface of the outer dielectric, i.e. so-called coated DD, yields again an asymmetric current waveform, with current peaks in the negative HC. These different electrical characteristics are related to the presence of the conductive coating on the dielectric wall of the reactor and can be explained by an increase of the local barrier capacitance available for charge transfer. The different discharge regimes affect the CO2 conversion, more specifically, the CO2 conversion is lowest in the clean DD configuration. It is somewhat higher in the coated DD configuration, and still higher in the MD configuration. The clean and coated MD configuration, however, gave similar CO2 conversion. These results indicate that the conductivity of the dielectric reactor walls can highly promote the development of the high-amplitude discharge current pulses and subsequently the CO2 conversion. |
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Wos |
000370974800030 |
Publication Date |
2016-01-21 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0963-0252 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.302 |
Times cited |
25 |
Open Access |
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Notes |
The research leading to these results has received funding from the European Union Seventh Framework Programme (FP7-PEOPLE-2013-ITN) under Grant Agreement № 606889 (RAPID—Reactive Atmospheric Plasma processIng—eDucation network). |
Approved |
Most recent IF: 3.302 |
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Call Number |
c:irua:130790 |
Serial |
4006 |
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Author |
Belov, I.; Paulussen, S.; Bogaerts, A. |
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Title |
Analysis and comparison of the co2 and co dielectric barrier discharge solid products |
Type |
P1 Proceeding |
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Year |
2016 |
Publication |
Hakone Xv: International Symposium On High Pressure Low Temperature Plasma Chemistry: With Joint Cost Td1208 Workshop: Non-equilibrium Plasmas With Liquids For Water And Surface Treatment |
Abbreviated Journal |
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Volume |
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Pages |
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Keywords |
P1 Proceeding; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
The CO and CO2 Dielectric Barrier Discharges (DBD) and their solid products were analyzed keeping similar energy input regimes. Gas chromatography analysis revealed the presence of CO2, CO and O-2 mixture in the exhaust of the CO2 DBD, while no O-2 was found when CO was used as a feed gas. It was shown that the C-2 Swan lines observed with optical emission spectroscopy were distinct in the CO plasma while they were not observed in the CO2 emission spectrum. Also the solid products of the plasmas exhibited remarkable differences. Nanoparticles with a diameter between10 and 300 nm, composed of Fe, O and C (Fe: O: C similar to 13: 50: 30) were produced by the CO2 DBD, while microscopic dendrite-like carbon structure (C: O similar to 73: 27) were formed in the CO plasma. The growth rate in the CO2 and CO DBDs was evaluated to be on the level of 0.15 mg/min and 15 mg/min, respectively. The difference of the CO and CO2 discharges and their products might be attributed to the oxygen content in the latter (6.4 mol.% O-2 in the exhaust) and subsequent etching of the carbonaceous film. |
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Publisher |
Masarykova univ |
Place of Publication |
Brno |
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Wos |
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Publication Date |
0000-00-00 |
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Abbreviated Series Title |
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Edition |
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ISSN |
978-80-210-8318-9 |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
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Times cited |
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Open Access |
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Notes |
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Approved |
Most recent IF: NA |
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Call Number |
UA @ lucian @ c:irua:141554 |
Serial |
4516 |
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Author |
De Bie, C.; Verheyde, B.; Martens, T.; van Dijk, J.; Paulussen, S.; Bogaerts, A. |
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Title |
Fluid modeling of the conversion of methane into higher hydrocarbons in an atmospheric pressure dielectric barrier discharge |
Type |
A1 Journal article |
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Year |
2011 |
Publication |
Plasma processes and polymers |
Abbreviated Journal |
Plasma Process Polym |
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Volume |
8 |
Issue |
11 |
Pages |
1033-1058 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
A one-dimensional fluid model for a dielectric barrier discharge in methane, used as a chemical reactor for gas conversion, is developed. The model describes the gas phase chemistry governing the conversion process of methane to higher hydrocarbons. The spatially averaged densities of the various plasma species as a function of time are discussed. Besides, the conversion of methane and the yields of the reaction products as a function of the residence time in the reactor are shown and compared with experimental data. Higher hydrocarbons (C2Hy and C3Hy) and hydrogen gas are typically found to be important reaction products. Furthermore, the main underlying reaction pathways are determined. |
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Publisher |
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Place of Publication |
Weinheim |
Editor |
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Language |
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Wos |
000297745500005 |
Publication Date |
2011-07-11 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1612-8850; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
2.846 |
Times cited |
70 |
Open Access |
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Notes |
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Approved |
Most recent IF: 2.846; 2011 IF: 2.468 |
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Call Number |
UA @ lucian @ c:irua:92443 |
Serial |
1227 |
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Author |
De Bie, C.; Martens, T.; van Dijk, J.; Paulussen, S.; Verheyde, B.; Corthals, S.; Bogaerts, A. |
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Title |
Dielectric barrier discharges used for the conversion of greenhouse gases: modeling the plasma chemistry by fluid simulations |
Type |
A1 Journal article |
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Year |
2011 |
Publication |
Plasma sources science and technology |
Abbreviated Journal |
Plasma Sources Sci T |
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Volume |
20 |
Issue |
2 |
Pages |
024008,1-024008,11 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
The conversion of methane to value-added chemicals and fuels is considered to be one of the challenges of the 21st century. In this paper we study, by means of fluid modeling, the conversion of methane to higher hydrocarbons or oxygenates by partial oxidation with CO2 or O2 in a dielectric barrier discharge. Sixty-nine different plasma species (electrons, ions, molecules, radicals) are included in the model, as well as a comprehensive set of chemical reactions. The calculation results presented in this paper include the conversion of the reactants and the yields of the reaction products as a function of residence time in the reactor, for different gas mixing ratios. Syngas (i.e. H2 + CO) and higher hydrocarbons (C2Hx) are typically found to be important reaction products. |
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Publisher |
Institute of Physics |
Place of Publication |
Bristol |
Editor |
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Language |
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Wos |
000290719900009 |
Publication Date |
2011-04-02 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0963-0252;1361-6595; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.302 |
Times cited |
38 |
Open Access |
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Notes |
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Approved |
Most recent IF: 3.302; 2011 IF: 2.521 |
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Call Number |
UA @ lucian @ c:irua:87868 |
Serial |
689 |
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Author |
Philippaerts, A.; Paulussen, S.; Breesch, A.; Turner, S.; Lebedev, O.I.; Van Tendeloo, G.; Sels, B.; Jacobs, P. |
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Title |
Unprecedented shape selectivity in hydrogenation of triacylglycerol molecules with Pt/ZSM-5 zeolite |
Type |
A1 Journal article |
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Year |
2011 |
Publication |
Angewandte Chemie: international edition in English |
Abbreviated Journal |
Angew Chem Int Edit |
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Volume |
50 |
Issue |
17 |
Pages |
3947-3949 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Well tuned: ZSM-5 with platinum nanoparticles preferably hydrogenates trans fatty acids over cis isomers in model triacylglycerols for geometric reasons. The central fatty acid chain reacts faster, pointing to pore mouth adsorption in a tuning fork conformation (see picture). This conformation induces stepwise hydrogenation, resulting in fast removal of the unstable central triene, while formation of saturated chains is limited. |
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Place of Publication |
Weinheim |
Editor |
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Language |
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Wos |
000289514100025 |
Publication Date |
2011-03-18 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1433-7851; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
11.994 |
Times cited |
31 |
Open Access |
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Notes |
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Approved |
Most recent IF: 11.994; 2011 IF: 13.455 |
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Call Number |
UA @ lucian @ c:irua:88381 |
Serial |
3814 |
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Author |
Paulussen, S.; Verheyde, B.; Tu, X.; De Bie, C.; Martens, T.; Petrovic, D.; Bogaerts, A.; Sels, B. |
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Title |
Conversion of carbon dioxide to value-added chemicals in atmospheric pressure dielectric barrier discharges |
Type |
A1 Journal article |
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Year |
2010 |
Publication |
Plasma sources science and technology |
Abbreviated Journal |
Plasma Sources Sci T |
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Volume |
19 |
Issue |
3 |
Pages |
034015,1-034015,6 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
The aim of this work consists of the evaluation of atmospheric pressure dielectric barrier discharges for the conversion of greenhouse gases into useful compounds. Therefore, pure CO2 feed flows are administered to the discharge zone at varying discharge frequency, power input, gas temperature and feed flow rates, aiming at the formation of CO and O2. The discharge obtained in CO2 is characterized as a filamentary mode with a microdischarge zone in each half cycle of the applied voltage. It is shown that the most important parameter affecting the CO2-conversion levels is the gas flow rate. At low flow rates, both the conversion and the CO-yield are significantly higher. In addition, also an increase in the gas temperature and the power input give rise to higher conversion levels, although the effect on the CO-yield is limited. The optimum discharge frequency depends on the power input level and it cannot be unambiguously stated that higher frequencies give rise to increased conversion levels. A maximum CO2 conversion of 30% is achieved at a flow rate of 0.05 L min−1, a power density of 14.75 W cm−3 and a frequency of 60 kHz. The most energy efficient conversions are achieved at a flow rate of 0.2 L min−1, a power density of 11 W cm−3 and a discharge frequency of 30 kHz. |
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Publisher |
Institute of Physics |
Place of Publication |
Bristol |
Editor |
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Language |
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Wos |
000277982800016 |
Publication Date |
2010-05-22 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0963-0252;1361-6595; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.302 |
Times cited |
116 |
Open Access |
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Notes |
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Approved |
Most recent IF: 3.302; 2010 IF: 2.218 |
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Call Number |
UA @ lucian @ c:irua:82408 |
Serial |
512 |
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Author |
Philippaerts, A.; Paulussen, S.; Turner, S.; Lebedev, O.I.; Van Tendeloo, G.; Poelman, H.; Bulut, M.; de Clippel, F.; Smeets, P.; Sels, B.; Jacobs, P. |
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Title |
Selectivity in sorption and hydrogenation of methyl oleate and elaidate on MFI zeolites |
Type |
A1 Journal article |
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Year |
2010 |
Publication |
Journal of catalysis |
Abbreviated Journal |
J Catal |
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Volume |
270 |
Issue |
1 |
Pages |
172-184 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Different zeolites were tested for selective removal of methyl elaidate (trans isomer) from an equimolar mixture with methyl oleate (cis isomer). Sorption experiments of the geometric isomers show that only ZSM-5 samples with reduced Al content in the framework are able to discriminate among the bent cis and the linear trans fatty acid methyl esters. Hydrogenation experiments of equimolar methyl oleate and elaidate mixtures at low temperature (65 °C) and high hydrogen pressure (6.0 MPa), using Pt catalysts, confirm this result. Only with a Pt/NaZSM-5 catalyst outspoken selectivity for the hydrogenation of the trans isomer is obtained. In order to prepare a selective Pt/ZSM-5 catalyst, the influence of Pt addition (impregnation, ion-exchange and competitive ion-exchange) and Pt activation (different calcination and reduction temperatures) on the Pt-distribution and Pt particle size was investigated using SEM, bright-field and HR TEM, EDX, electron tomography, CO-chemisorption, XPS, XRD, and UVvis measurements. The best result in terms of hydrogenation activity and selectivity is obtained with a Pt/ZSM-5 catalyst, which is prepared via competitive ion-exchange, followed by slow calcination up to 350 °C under high O2 flow and a reduction up to 500 °C under H2. This preparation method leads to a Pt/ZSM-5 catalyst with the best Pt distribution and the smallest Pt clusters occluded in the zeolite structure. Finally, the influence of zeolite crystal size, morphology, and elemental composition of ZSM-5 on hydrogenation activity and selectivity was investigated in detail. |
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Publisher |
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Place of Publication |
San Diego, Calif. |
Editor |
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Language |
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Wos |
000275966100021 |
Publication Date |
2010-01-28 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0021-9517; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
6.844 |
Times cited |
24 |
Open Access |
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| |
Notes |
FWO; IAP-IV; Methusalem |
Approved |
Most recent IF: 6.844; 2010 IF: 5.415 |
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| |
Call Number |
UA @ lucian @ c:irua:82435 |
Serial |
2970 |
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| Permanent link to this record |
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| |
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Author |
Paulussen, S.; Sels, B.; Bogaerts, A.; Paul, J. |
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Title |
Een tweede leven voor broeikasgassen? |
Type |
A2 Journal article |
| |
Year |
2008 |
Publication |
Het ingenieursblad : maandblad van de Koninklijke Vlaamse Ingenieursvereniging KVIV |
Abbreviated Journal |
|
|
| |
Volume |
77 |
Issue |
3 |
Pages |
16-20 |
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| |
Keywords |
A2 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
Antwerpen |
Editor |
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Language |
|
Wos |
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Publication Date |
0000-00-00 |
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Series Editor |
|
Series Title |
|
Abbreviated Series Title |
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Series Volume |
|
Series Issue |
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Edition |
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ISSN |
0020-1235 |
ISBN |
|
Additional Links |
UA library record |
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Impact Factor |
|
Times cited |
|
Open Access |
|
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| |
Notes |
|
Approved |
Most recent IF: NA |
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| |
Call Number |
UA @ lucian @ c:irua:82308 |
Serial |
3765 |
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| Permanent link to this record |
