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| Author | Bogaerts, A.; Wang, W.; Berthelot, A.; Guerra, V. | ||||
| Title | Modeling plasma-based CO2conversion: crucial role of the dissociation cross section | Type | A1 Journal article | ||
| Year | 2016 | Publication | Plasma sources science and technology | Abbreviated Journal | Plasma Sources Sci T |
| Volume | 25 | Issue | 25 | Pages | 055016 |
| Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Plasma-based CO2 conversion is gaining increasing interest worldwide. A large research effort is devoted to improving the energy efficiency. For this purpose, it is very important to understand the underlying mechanisms of the CO2 conversion. The latter can be obtained by computer modeling, describing in detail the behavior of the various plasma species and all relevant chemical processes. However, the accuracy of the modeling results critically depends on the accuracy of the assumed input data, like cross sections. This is especially true for the cross section of electron impact dissociation, as the latter process is believed to proceed through electron impact excitation, but it is not clear from the literature which excitation channels effectively lead to dissociation. Therefore, the present paper discusses the effect of different electron impact dissociation cross sections reported in the literature on the calculated CO2 conversion, for a dielectric barrier discharge (DBD) and a microwave (MW) plasma. Comparison is made to experimental data for the DBD case, to elucidate which cross section might be the most realistic. This comparison reveals that the cross sections proposed by Itikawa and by Polak and Slovetsky both seem to underestimate the CO2 conversion. The cross sections recommended by Phelps with thresholds of 7 eV and 10.5 eV yield a CO2 conversion only slightly lower than the experimental data, but the sum of both cross sections overestimates the values, indicating that these cross sections represent dissociation, but most probably also include other (pure excitation) channels. Our calculations indicate that the choice of the electron impact dissociation cross section is crucial for the DBD, where this process is the dominant mechanism for CO2 conversion. In the MW plasma, it is only significant at pressures up to 100 mbar, while it is of minor importance for higher pressures, when dissociation proceeds mainly through collisions of CO2 with heavy particles. |
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| Language | Wos | 000384030600001 | Publication Date | 2016-08-31 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 1361-6595 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 3.302 | Times cited  |
57 | Open Access | |
| Notes | The authors would like to thank R Snoeckx and S Heijkers for the interesting discussions. This research was supported by the European Union’s Seventh Framework Programme for research, technological development and demonstration under grant agreement no. 606889, the European Marie Skłodowska-Curie Individual Fellowship project ‘GlidArc’ within Horizon2020, the FWO project (grant G.0383.16N), and the Network on Physical Chemistry of Plasma-Surface Interactions—Interuniversity Attraction Poles, phase VII (PSI-IAP7), supported by the Belgian Science Policy Office (BELSPO). The computational work was carried out using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UA), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the UA. VG was partially supported by the Portuguese FCT— Fundação para a Ci | Approved | Most recent IF: 3.302 | ||
| Call Number | c:irua:135070 | Serial | 4111 | ||
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| Author | Ramakers, M.; Michielsen, I.; Aerts, R.; Meynen, V.; Bogaerts, A. | ||||
| Title | Effect of argon or helium on the CO2 conversion in a dielectric barrier discharge | Type | A1 Journal article | ||
| Year | 2015 | Publication | Plasma processes and polymers | Abbreviated Journal | Plasma Process Polym |
| Volume | 12 | Issue | 12 | Pages | 755-763 |
| Keywords | A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | This paper demonstrates that the CO2 conversion in a dielectric barrier discharge rises drastically upon addition of Ar or He, and the effect is more pronounced for Ar than for He. The effective CO2 conversion, on the other hand, drops upon addition of Ar or He, which is logical due to the lower CO2 content in the gas mixture, and the same is true for the energy efficiency, because a considerable fraction of the energy is then consumed into ionization/excitation of Ar or He atoms. The higher absolute CO2 conversion upon addition of Ar or He can be explained by studying in detail the Lissajous plots and the current profiles. The breakdown voltage is lower in the CO2/Ar and CO2/He mixtures, and the discharge gap is more filled with plasma, which enhances the possibility for CO2 conversion. The rates of electron impact excitationdissociation of CO2, estimated from the electron densities and mean electron energies, are indeed higher in the CO2/Ar and (to a lower extent) in the CO2/He mixtures, compared to the pure CO2 plasma. Moreover, charge transfer between Ar+ or Ar2+ ions and CO2, followed by electron-ion dissociative recombination of the CO2+ ions, might also contribute to, or even be dominant for the CO2 dissociation. All these effects can explain the higher CO2 conversion, especially upon addition of Ar, but also upon addition of He. | ||||
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| Publisher | Place of Publication | Weinheim | Editor | ||
| Language | Wos | 000359672400007 | Publication Date | 2015-02-12 | |
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| Series Volume | Series Issue | Edition | |||
| ISSN | 1612-8850; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 2.846 | Times cited |
63 | Open Access | |
| Notes | Approved | Most recent IF: 2.846; 2015 IF: 2.453 | |||
| Call Number | c:irua:126822 | Serial | 799 | ||
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| Author | Neyts, E.C. | ||||
| Title | Plasma-Surface Interactions in Plasma Catalysis | Type | A1 Journal article | ||
| Year | 2016 | Publication | Plasma chemistry and plasma processing | Abbreviated Journal | Plasma Chem Plasma P |
| Volume | 36 | Issue | 36 | Pages | 185-212 |
| Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | In this paper the various elementary plasma—surface interaction processes occurring in plasma catalysis are critically evaluated. Specifically, plasma catalysis at atmospheric pressure is considered. The importance of the various processes is analyzed for the most common plasma catalysis sources, viz. the dielectric barrier discharge and the gliding arc. The role and importance of surface chemical reactions (including adsorption, surface-mediated association and dissociation reactions, and desorption), plasma-induced surface modification, photocatalyst activation, heating, charging, surface discharge formation and electric field enhancement are discussed in the context of plasma catalysis. Numerous examples are provided to demonstrate the importance of the various processes. | ||||
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| Language | Wos | 000370720800011 | Publication Date | 2015-10-16 | |
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| Series Volume | Series Issue | Edition | |||
| ISSN | 0272-4324 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 2.355 | Times cited |
66 | Open Access | |
| Notes | The author is indebted to many colleagues for fruitful discussions. In particular discussions with A. Bogaerts (University of Antwerp, Belgium), H.-H. Kim (AIST, Japan), J. C. Whitehead (University of Manchester, UK) and T. Nozaki (Tokyo Institute of Technology, Japan) are greatfully acknowledged and appreciated. | Approved | Most recent IF: 2.355 | ||
| Call Number | c:irua:130742 | Serial | 4004 | ||
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| Author | De Bie, C.; Verheyde, B.; Martens, T.; van Dijk, J.; Paulussen, S.; Bogaerts, A. | ||||
| Title | Fluid modeling of the conversion of methane into higher hydrocarbons in an atmospheric pressure dielectric barrier discharge | Type | A1 Journal article | ||
| Year | 2011 | Publication | Plasma processes and polymers | Abbreviated Journal | Plasma Process Polym |
| Volume | 8 | Issue | 11 | Pages | 1033-1058 |
| Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| 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 | Place of Publication | Weinheim | Editor | ||
| Language | Wos | 000297745500005 | Publication Date | 2011-07-11 | |
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| ISSN | 1612-8850; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 2.846 | Times cited |
70 | Open Access | |
| Notes | Approved | Most recent IF: 2.846; 2011 IF: 2.468 | |||
| Call Number | UA @ lucian @ c:irua:92443 | Serial | 1227 | ||
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| Author | de Bleecker, K.; Bogaerts, A.; Gijbels, R.; Goedheer, W. | ||||
| Title | Numerical investigation of particle formation mechanisms in silane discharges | Type | A1 Journal article | ||
| Year | 2004 | Publication | Physical review : E : statistical physics, plasmas, fluids, and related interdisciplinary topics | Abbreviated Journal | Phys Rev E |
| Volume | 69 | Issue | Pages | 056409,1-16 | |
| Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
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| Publisher | Place of Publication | Lancaster, Pa | Editor | ||
| Language | Wos | 000221813400085 | Publication Date | 2004-05-26 | |
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| Series Volume | Series Issue | Edition | |||
| ISSN | 1539-3755;1550-2376; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 2.366 | Times cited |
74 | Open Access | |
| Notes | Approved | Most recent IF: 2.366; 2004 IF: NA | |||
| Call Number | UA @ lucian @ c:irua:45497 | Serial | 2396 | ||
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| Author | de Bleecker, K.; Bogaerts, A.; Goedheer, W. | ||||
| Title | Detailed modeling of hydrocarbon nanoparticle nucleation in acetylene discharges | Type | A1 Journal article | ||
| Year | 2006 | Publication | Physical review : E : statistical physics, plasmas, fluids, and related interdisciplinary topics | Abbreviated Journal | Phys Rev E |
| Volume | 73 | Issue | 2 | Pages | 026405,1-16 |
| Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | The initial stage of nanoparticle formation and growth in radiofrequency acetylene (C2H2) plasmas is investigated by means of a self-consistent one-dimensional fluid model. A detailed chemical kinetic scheme, containing electron impact, ion-neutral, and neutral-neutral reactions, has been developed in order to predict the underlying dust growth mechanisms and the most important dust precursors. The model considers 41 different species (neutrals, radicals, ions, and electrons) describing hydrocarbons (CnHm) containing up to 12 carbon atoms. Possible routes for particle growth are discussed. Both positive and negative ion reaction pathways are considered, as consecutive anion- and cation-molecule reactions seem to lead to a fast build up of the carbon skeleton. | ||||
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| Publisher | Place of Publication | Lancaster, Pa | Editor | ||
| Language | Wos | 000235667700086 | Publication Date | 2006-03-10 | |
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| ISSN | 1539-3755;1550-2376; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 2.366 | Times cited |
89 | Open Access | |
| Notes | Approved | Most recent IF: 2.366; 2006 IF: 2.438 | |||
| Call Number | UA @ lucian @ c:irua:56337 | Serial | 666 | ||
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| Author | Georgieva, V.; Bogaerts, A.; Gijbels, R. | ||||
| Title | Numerical investigation of ion energy distribution functions in single and dual frequency capacitively coupled plasma reactors | Type | A1 Journal article | ||
| Year | 2004 | Publication | Physical review : E : statistical physics, plasmas, fluids, and related interdisciplinary topics | Abbreviated Journal | Phys Rev E |
| Volume | 69 | Issue | Pages | 026406 | |
| Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
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| Publisher | Place of Publication | Lancaster, Pa | Editor | ||
| Language | Wos | 000220255500058 | Publication Date | 2004-02-24 | |
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| Series Volume | Series Issue | Edition | |||
| ISSN | 1539-3755;1550-2376; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 2.366 | Times cited |
97 | Open Access | |
| Notes | Approved | Most recent IF: 2.366; 2004 IF: NA | |||
| Call Number | UA @ lucian @ c:irua:44025 | Serial | 2395 | ||
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| Author | Kozák, T.; Bogaerts, A. | ||||
| Title | Evaluation of the energy efficiency of CO2 conversion in microwave discharges using a reaction kinetics model | Type | A1 Journal article | ||
| Year | 2015 | Publication | Plasma sources science and technology | Abbreviated Journal | Plasma Sources Sci T |
| Volume | 24 | Issue | 24 | Pages | 015024 |
| Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | We use a zero-dimensional reaction kinetics model to simulate CO2 conversion in microwave discharges where the excitation of the vibrational levels plays a significant role in the dissociation kinetics. The model includes a description of the CO2 vibrational kinetics, taking into account state-specific VT and VV relaxation reactions and the effect of vibrational excitation on other chemical reactions. The model is used to simulate a general tubular microwave reactor, where a stream of CO2 flows through a plasma column generated by microwave radiation. We study the effects of the internal plasma parameters, namely the reduced electric field, electron density and the total specific energy input, on the CO2 conversion and its energy efficiency. We report the highest energy efficiency (up to 30%) for a specific energy input in the range 0.41.0 eV/molecule and a reduced electric field in the range 50100 Td and for high values of the electron density (an ionization degree greater than 10−5). The energy efficiency is mainly limited by the VT relaxation which contributes dominantly to the vibrational energy losses and also contributes significantly to the heating of the reacting gas. The model analysis provides useful insight into the potential and limitations of CO2 conversion in microwave discharges. | ||||
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| Publisher | Institute of Physics | Place of Publication | Bristol | Editor | |
| Language | Wos | 000348298200025 | Publication Date | 2014-12-23 | |
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| Series Volume | Series Issue | Edition | |||
| ISSN | 0963-0252;1361-6595; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 3.302 | Times cited |
100 | Open Access | |
| Notes | Approved | Most recent IF: 3.302; 2015 IF: 3.591 | |||
| Call Number | c:irua:122243 | Serial | 1087 | ||
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| Author | Paulussen, S.; Verheyde, B.; Tu, X.; De Bie, C.; Martens, T.; Petrovic, D.; Bogaerts, A.; Sels, B. | ||||
| Title | Conversion of carbon dioxide to value-added chemicals in atmospheric pressure dielectric barrier discharges | Type | A1 Journal article | ||
| Year | 2010 | Publication | Plasma sources science and technology | Abbreviated Journal | Plasma Sources Sci T |
| Volume | 19 | Issue | 3 | Pages | 034015,1-034015,6 |
| Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| 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 | |
| Language | Wos | 000277982800016 | Publication Date | 2010-05-22 | |
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| Series Volume | Series Issue | Edition | |||
| ISSN | 0963-0252;1361-6595; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 3.302 | Times cited |
116 | Open Access | |
| Notes | Approved | Most recent IF: 3.302; 2010 IF: 2.218 | |||
| Call Number | UA @ lucian @ c:irua:82408 | Serial | 512 | ||
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| Author | Kozák, T.; Bogaerts, A. | ||||
| Title | Splitting of CO2 by vibrational excitation in non-equilibrium plasmas : a reaction kinetics model | Type | A1 Journal article | ||
| Year | 2014 | Publication | Plasma sources science and technology | Abbreviated Journal | Plasma Sources Sci T |
| Volume | 23 | Issue | 4 | Pages | 045004 |
| Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | We present a zero-dimensional kinetic model of CO2 splitting in non-equilibrium plasmas. The model includes a description of the CO2 vibrational kinetics (25 vibrational levels up to the dissociation limit of the molecule), taking into account state-specific VT and VV relaxation reactions and the effect of vibrational excitation on other chemical reactions. The model is applied to study the reaction kinetics of CO2 splitting in an atmospheric-pressure dielectric barrier discharge (DBD) and in a moderate-pressure microwave discharge. The model results are in qualitative agreement with published experimental works. We show that the CO2 conversion and its energy efficiency are very different in these two types of discharges, which reflects the important dissociation mechanisms involved. In the microwave discharge, excitation of the vibrational levels promotes efficient dissociation when the specific energy input is higher than a critical value (2.0 eV/molecule under the conditions examined). The calculated energy efficiency of the process has a maximum of 23%. In the DBD, vibrationally excited levels do not contribute significantly to the dissociation of CO2 and the calculated energy efficiency of the process is much lower (5%). | ||||
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| Publisher | Institute of Physics | Place of Publication | Bristol | Editor | |
| Language | Wos | 000345761500014 | Publication Date | 2014-06-17 | |
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| Series Volume | Series Issue | Edition | |||
| ISSN | 0963-0252;1361-6595; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 3.302 | Times cited |
170 | Open Access | |
| Notes | Approved | Most recent IF: 3.302; 2014 IF: 3.591 | |||
| Call Number | UA @ lucian @ c:irua:117398 | Serial | 3108 | ||
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| Author | Bruggeman, P.J.; Kushner, M.J.; Locke, B.R.; Gardeniers, J.G.E.; Graham, W.G.; Graves, D.B.; Hofman-Caris, R.C.H.M.; Maric, D.; Reid, J.P.; Ceriani, E.; Fernandez Rivas, D.; Foster, J.E.; Garrick, S.C.; Gorbanev, Y.; Hamaguchi, S.; Iza, F.; Jablonowski, H.; Klimova, E.; Kolb, J.; Krcma, F.; Lukes, P.; Machala, Z.; Marinov, I.; Mariotti, D.; Mededovic Thagard, S.; Minakata, D.; Neyts, E.C.; Pawlat, J.; Petrovic, Z.L.; Pflieger, R.; Reuter, S.; Schram, D.C.; Schröter, S.; Shiraiwa, M.; Tarabová, B.; Tsai, P.A.; Verlet, J.R.R.; von Woedtke, T.; Wilson, K.R.; Yasui, K.; Zvereva, G. | ||||
| Title | Plasma–liquid interactions: a review and roadmap | Type | A1 Journal article | ||
| Year | 2016 | Publication | Plasma sources science and technology | Abbreviated Journal | Plasma Sources Sci T |
| Volume | 25 | Issue | 5 | Pages | 053002 |
| Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Plasma–liquid interactions represent a growing interdisciplinary area of research involving plasma science, fluid dynamics, heat and mass transfer, photolysis, multiphase chemistry and aerosol science. This review provides an assessment of the state-of-the-art of this multidisciplinary area and identifies the key research challenges. The developments in diagnostics, modeling and further extensions of cross section and reaction rate databases that are necessary to address these challenges are discussed. The review focusses on nonequilibrium plasmas. | ||||
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| Language | Wos | 000384715400001 | Publication Date | 2016-09-30 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 1361-6595 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 3.302 | Times cited |
460 | Open Access | |
| Notes | This manuscript originated from discussions at the Lorentz Center Workshop ‘Gas/Plasma–Liquid Interface: Transport, Chemistry and Fundamental Data’ that took place at the Lorentz Center, Leiden University in the Netherlands from August 4, through August 8, 2014, and follow-up discussions since the workshop. All authors acknowledge the support of the Lorentz Center, the COST action TD1208 (Electrical Discharges with Liquids for Future Applications) and the Royal Dutch Academy of Sciences for their financial support. PJB, MJK, DBG and JEF acknowledge the support of the ‘Center on Control of Plasma Kinetics’ of the United States Department of Energy Office of Fusion Energy Science (DE-SC0001319). In addition, PJB and BRL acknowledge the support of the National Science Foundation (PHY 1500135 and CBET 1236225, respectively). In addition the enormous help of Mrs. Victoria Piorek (University of Minnesota) in the formatting of the final document including the references is gratefully acknowledged. | Approved | Most recent IF: 3.302 | ||
| Call Number | PLASMANT @ plasmant @ c:irua:144654 | Serial | 4628 | ||
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