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Author Zhang, L.; Heijkers, S.; Wang, W.; Martini, L.M.; Tosi, P.; Yang, D.; Fang, Z.; Bogaerts, A.
Title Dry reforming of methane in a nanosecond repetitively pulsed discharge: chemical kinetics modeling Type A1 Journal article
Year (down) 2022 Publication Plasma Sources Science & Technology Abbreviated Journal Plasma Sources Sci T
Volume 31 Issue 5 Pages 055014
Keywords A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract Nanosecond pulsed discharge plasma shows a high degree of non-equilibrium, and exhibits relatively high conversions in the dry reforming of methane. To further improve the application, a good insight of the underlying mechanisms is desired. We developed a chemical kinetics model to explore the underlying plasma chemistry in nanosecond pulsed discharge. We compared the calculated conversions and product selectivities with experimental results, and found reasonable agreement in a wide range of specific energy input. Hence, the chemical kinetics model is able to provide insight in the underlying plasma chemistry. The modeling results predict that the most important dissociation reaction of CO<sub>2</sub>and CH<sub>4</sub>is electron impact dissociation. C<sub>2</sub>H<sub>2</sub>is the most abundant hydrocarbon product, and it is mainly formed upon reaction of two CH<sub>2</sub>radicals. Furthermore, the vibrational excitation levels of CO<sub>2</sub>contribute for 85% to the total dissociation of CO<sub>2</sub>.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000797660000001 Publication Date 2022-05-01
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0963-0252 ISBN Additional Links UA library record; WoS full record
Impact Factor 3.8 Times cited Open Access OpenAccess
Notes China Scholarship Council; National Natural Science Foundation of China, 11965018 ; This work is supported by the National Natural Science Foundation of China (Grant Nos. 52077026, 11965018), L Zhang was also supported by the China Scholarship Council (CSC). Data availability statement The data that support the findings of this study are available upon reasonable request from the authors. Approved Most recent IF: 3.8
Call Number PLASMANT @ plasmant @c:irua:188537 Serial 7069
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Author Heijkers, S.; Martini, L.M.; Dilecce, G.; Tosi, P.; Bogaerts, A.
Title Nanosecond Pulsed Discharge for CO2Conversion: Kinetic Modeling To Elucidate the Chemistry and Improve the Performance Type A1 Journal article
Year (down) 2019 Publication The journal of physical chemistry: C : nanomaterials and interfaces Abbreviated Journal J Phys Chem C
Volume 123 Issue 19 Pages 12104-12116
Keywords A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract We study the mechanisms of CO2 conversion in a nanosecond repetitively pulsed (NRP) discharge, by means of a chemical kinetics model. The calculated conversions and energy efficiencies are in reasonable agreement with experimental results over a wide range of specific energy input values, and the same applies to the evolution of gas temperature and CO2 conversion as a function of time in the afterglow, indicating that our model provides a realistic picture of the underlying mechanisms in the NRP discharge and can be used to identify its limitations and thus to suggest further improvements. Our model predicts that vibrational excitation is very important in the NRP discharge, explaining why this type of plasma yields energy-efficient CO2 conversion. A significant part of the CO2 dissociation occurs by electronic excitation from the lower vibrational levels toward repulsive electronic states, thus resulting in dissociation. However, vibration−translation (VT) relaxation (depopulating the higher vibrational levels) and CO + O recombination (CO + O + M → CO2 + M), as well as mixing of the converted gas with fresh gas entering the plasma in between the pulses, are limiting factors for the conversion and energy efficiency. Our model predicts that extra cooling, slowing down the rate of VT relaxation and of the above recombination reaction, thus enhancing the contribution of the highest vibrational levels to the overall CO2 dissociation, can further improve the performance of the NRP discharge for energy-efficient CO2 conversion.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000468368800009 Publication Date 2019-05-16
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 4.536 Times cited 4 Open Access Not_Open_Access: Available from 26.04.2020
Notes Fonds Wetenschappelijk Onderzoek, G.0383.16N ; The authors acknowledge financial support from the Fund for Scientific Research, Flanders (FWO; Grant no. G.0383.16N). Approved Most recent IF: 4.536
Call Number PLASMANT @ plasmant @UA @ admin @ c:irua:159976 Serial 5174
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