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Author | Oliveira, M.C.; Yusupov, M.; Bogaerts, A.; Cordeiro, R.M. | ||||
Title | Lipid Oxidation: Role of Membrane Phase-Separated Domains | Type | A1 Journal Article | ||
Year | 2021 | Publication | Journal Of Chemical Information And Modeling | Abbreviated Journal | J Chem Inf Model |
Volume | 61 | Issue | 6 | Pages | 2857-2868 |
Keywords | A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | Lipid oxidation is associated with several inflammatory and neurodegenerative diseases, but many questions to unravel its effects on biomembranes are still open due to the complexity of the topic. For instance, recent studies indicated that phase-separated domains can have a significant effect on membrane function. It is reported that domain interfaces are “hot spots” for pore formation, but the underlying mechanisms and the effect of oxidation-induced phase separation on membranes remain elusive. Thus, to evaluate the permeability of the membrane coexisting of liquid-ordered (Lo) and liquid-disordered (Ld) domains, we performed atomistic molecular dynamics simulations. Specifically, we studied the membrane permeability of nonoxidized or oxidized homogeneous membranes (single-phase) and at the Lo/Ld domain interfaces of heterogeneous membranes, where the Ld domain is composed of either oxidized or nonoxidized lipids. Our simulation results reveal that the addition of only 1.5% of lipid aldehyde molecules at the Lo/Ld domain interfaces of heterogeneous membranes increases the membrane permeability, whereas their addition at homogeneous membranes does not have any effect. This study is of interest for a better understanding of cancer treatment methods based on oxidative stress (causing among others lipid oxidation), such as plasma medicine and photodynamic therapy. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000669541400034 | Publication Date | 2021-06-28 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1549-9596 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 3.76 | Times cited | Open Access | OpenAccess | |
Notes | Fonds Wetenschappelijk Onderzoek, 1200219N ; Coordenação de Aperfeiçoamento de Pessoal de NÃvel Superior; We thank Universidade Federal do ABC for providing the computational resources needed for completion of this work and CAPES for the scholarship granted. M.Y. acknowledges the Flanders Research Foundation (grant 1200219N) for financial support. | Approved | Most recent IF: 3.76 | ||
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PLASMANT @ plasmant @c:irua:179766 | Serial | 6806 | ||
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Author | Aghaei, M.; Bogaerts, A. | ||||
Title | Flowing Atmospheric Pressure Afterglow for Ambient Ionization: Reaction Pathways Revealed by Modeling | Type | A1 Journal article | ||
Year | 2021 | Publication | Analytical Chemistry | Abbreviated Journal | Anal Chem |
Volume | 93 | Issue | 17 | Pages | 6620-6628 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | We describe the plasma chemistry in a helium flowing atmospheric pressure afterglow (FAPA) used for analytical spectrometry, by means of a quasione-dimensional (1D) plasma chemical kinetics model. We study the effect of typical impurities present in the feed gas, as well as the afterglow in ambient humid air. The model provides the species density profiles in the discharge and afterglow regions and the chemical pathways. We demonstrate that H, N, and O atoms are formed in the discharge region, while the dominant reactive neutral species in the afterglow are O3 and NO. He* and He2* are responsible for Penning ionization of O2, N2, H2O, H2, and N, and especially O and H atoms. Besides, He2+ also contributes to ionization of N2, O2, H2O, and O through charge transfer reactions. From the pool of ions created in the discharge, NO+ and (H2O)3H+ are the dominant ions in the afterglow. Moreover, negatively charged clusters, such as NO3H2O− and NO2H2O−, are formed and their pathway is discussed as well. Our model predictions are in line with earlier observations in the literature about the important reagent ions and provide a comprehensive overview of the underlying pathways. The model explains in detail why helium provides a high analytical sensitivity because of high reagent ion formation by both Penning ionization and charge transfer. Such insights are very valuable for improving the analytical performance of this (and other) ambient desorption/ionization source(s). | ||||
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Language | Wos | 000648505900008 | Publication Date | 2021-05-04 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0003-2700 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 6.32 | Times cited | Open Access | OpenAccess | |
Notes | Fonds Wetenschappelijk Onderzoek, 6713 ; The authors gratefully acknowledge financial support from the Fonds voor Wetenschappelijk Onderzoek (FWO) grant number 6713. 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. The authors also thank J. T. Shelley for providing experimental data for the gas velocity behind the anode disk and before the mass spectrometer interface, to validate our model. | Approved | Most recent IF: 6.32 | ||
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PLASMANT @ plasmant @c:irua:178126 | Serial | 6762 | ||
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Author | Izadi, M.E.; Bal, K.M.; Maghari, A.; Neyts, E.C. | ||||
Title | Reaction mechanisms of C(3PJ) and C+(2PJ) with benzene in the interstellar medium from quantum mechanical molecular dynamics simulations | Type | A1 Journal article | ||
Year | 2021 | Publication | Physical Chemistry Chemical Physics | Abbreviated Journal | Phys Chem Chem Phys |
Volume | 23 | Issue | 7 | Pages | 4205-4216 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | While spectroscopic data on small hydrocarbons in interstellar media in combination with crossed molecular beam (CMB) experiments have provided a wealth of information on astrochemically relevant species, much of the underlying mechanistic pathways of their formation remain elusive. Therefore, in this work, the chemical reaction mechanisms of C(<sup>3</sup>P<sub>J</sub>) + C<sub>6</sub>H<sub>6</sub>and C<sup>+</sup>(<sup>2</sup>P) + C<sub>6</sub>H<sub>6</sub>systems using the quantum mechanical molecular dynamics (QMMD) technique at the PBE0-D3(BJ) level of theory is investigated, mimicking a CMB experiment. Both the dynamics of the reactions as well as the electronic structure for the purpose of the reaction network are evaluated. The method is validated for the first reaction by comparison to the available experimental data. The reaction scheme for the C(<sup>3</sup>P<sub>J</sub>) + C<sub>6</sub>H<sub>6</sub>system covers the literature data,<italic>e.g.</italic>the major products are the 1,2-didehydrocycloheptatrienyl radical (C<sub>7</sub>H<sub>5</sub>) and benzocyclopropenyl radical (C<sub>6</sub>H<sub>5</sub>–CH), and it reveals the existence of less common pathways for the first time. The chemistry of the C<sup>+</sup>(<sup>2</sup>P<sub>J</sub>) + C<sub>6</sub>H<sub>6</sub>system is found to be much richer, and we have found that this is because of more exothermic reactions in this system in comparison to those in the C(<sup>3</sup>P<sub>J</sub>) + C<sub>6</sub>H<sub>6</sub>system. Moreover, using the QMMD simulation, a number of reaction paths have been revealed that produce three distinct classes of reaction products with different ring sizes. All in all, at all the collision energies and orientations, the major product is the heptagon molecular ion for the ionic system. It is also revealed that the collision orientation has a dominant effect on the reaction products in both systems, while the collision energy mostly affects the charged system. These simulations both prove the applicability of this approach to simulate crossed molecular beams, and provide fundamental information on reactions relevant for the interstellar medium. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000621595300016 | Publication Date | 2021-01-18 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1463-9076 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 4.123 | Times cited | Open Access | OpenAccess | |
Notes | Fonds Wetenschappelijk Onderzoek, 12ZI420N ; Ministry of Science Research and Technology; Universiteit Antwerpen; The financial support from the Iran Ministry of Science, Research and Technology and PLASMANT Research Group University of Antwerp is highly acknowledged by the authors. K.M.B. was funded as a junior postdoctoral fellow of the FWO (Research Foundation – Flanders), Grant 12ZI420N. The 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 FWO and the Flemish Government. | Approved | Most recent IF: 4.123 | ||
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PLASMANT @ plasmant @c:irua:176672 | Serial | 6742 | ||
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Author | Jardali, F.; Van Alphen, S.; Creel, J.; Ahmadi Eshtehardi, H.; Axelsson, M.; Ingels, R.; Snyders, R.; Bogaerts, A. | ||||
Title | NOxproduction in a rotating gliding arc plasma: potential avenue for sustainable nitrogen fixation | Type | A1 Journal article | ||
Year | 2021 | Publication | Green Chemistry | Abbreviated Journal | Green Chem |
Volume | 23 | Issue | 4 | Pages | 1748-1757 |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | The fast growing world population demands food to survive, and nitrogen-based fertilizers are essential to ensure sufficient food production. Today, fertilizers are mainly produced from non-sustainable fossil fuels<italic>via</italic>the Haber–Bosch process, leading to serious environmental problems. We propose here a novel rotating gliding arc plasma, operating in air, for direct NO<sub>x</sub>production, which can yield high nitrogen content organic fertilizers without pollution associated with ammonia emission. We explored the efficiency of NO<sub>x</sub>production in a wide range of feed gas ratios, and for two arc modes: rotating and steady. When the arc is in steady mode, record-value NO<sub>x</sub>concentrations up to 5.5% are achieved which are 1.7 times higher than the maximum concentration obtained by the rotating arc mode, and with an energy consumption of 2.5 MJ mol<sup>−1</sup>(or<italic>ca.</italic>50 kW h kN<sup>−1</sup>);<italic>i.e.</italic>the lowest value so far achieved by atmospheric pressure plasma reactors. Computer modelling, using a combination of five different complementary approaches, provides a comprehensive picture of NO<sub>x</sub>formation in both arc modes; in particular, the higher NO<sub>x</sub>production in the steady arc mode is due to the combined thermal and vibrationally-promoted Zeldovich mechanisms. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000629630600021 | Publication Date | 2021-01-28 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1463-9262 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 9.125 | Times cited | Open Access | OpenAccess | |
Notes | Fonds Wetenschappelijk Onderzoek, GoF9618n 30505023 ; H2020 European Research Council, 810182 ; This research was supported by a Bilateral Project with N2 Applied, the Excellence of Science FWO-FNRS 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. We also thank J.-L. Liu for the RGA design, L. Van ‘t dack and K. Leyssens for MS calibration and practical support, and K. Van ‘t Veer for the fruitful discussions on plasma kinetic modelling and for calculating the electron energy losses. | Approved | Most recent IF: 9.125 | ||
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PLASMANT @ plasmant @c:irua:176022 | Serial | 6678 | ||
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Author | Loenders, B.; Engelmann, Y.; Bogaerts, A. | ||||
Title | Plasma-Catalytic Partial Oxidation of Methane on Pt(111): A Microkinetic Study on the Role of Different Plasma Species | Type | A1 Journal article | ||
Year | 2021 | Publication | Journal Of Physical Chemistry C | Abbreviated Journal | J Phys Chem C |
Volume | 125 | Issue | 5 | Pages | 2966-2983 |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Movement Antwerp (MOVANT) | ||||
Abstract | We use microkinetic modeling to examine the potential of plasma-catalytic partial oxidation (POX) of CH4 as a promising new approach to produce oxygenates. We study how different plasma species affect POX of CH4 on the Pt(111) surface, and we discuss the associated kinetic and mechanistic changes. We discuss the effect of vibrationally excited CH4 and O2, as well as plasma-generated radicals and stable intermediates. Our results show that vibrational excitation enhances the turnover frequency (TOF) of catalytic CH4 dissociation and has good potential for improving the selectivities toward CH3OH, HCOOH, and C2 hydrocarbons. Nevertheless, when also considering plasma-generated radicals, we find that these species mainly govern the surface chemistry. Additionally, we find that plasma-generated radicals and stable intermediates enhance the TOFs of COx and oxygenates, increase the selectivity toward oxygenates, and make the formation of HCOOH more significant on Pt(111). We also briefly illustrate the potential impact of Eley−Rideal reactions that involve plasma-generated radicals. Finally, we reveal how various radicals affect the catalyst surface chemistry and we link this to the formation of different products. This allows us to make suggestions on how the plasma composition should be altered to improve the formation of desired products. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000619760700017 | Publication Date | 2021-02-11 | |
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ISSN | 1932-7447 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 4.536 | Times cited | Open Access | OpenAccess | |
Notes | Universiteit Antwerpen; Fonds Wetenschappelijk Onderzoek, S001619N ; H2020 European Research Council, 810182 ; We thank Tom Butterworth for the interesting discussions regarding the calculation of the vibrational populations of methane and for taking the time to share his thoughts and experiences on the matter. This research is supported by the FWO-SBO project PLASMACATDesign (grant number S001619N). We also acknowledge financial support from the TOP-BOF project of the University of Antwerp and from the European Research Council (ERC) under the European Union’s Horizon 2020 Research and Innovation Program (grant agreement no. 810182SCOPE ERC Synergy project). The calculations were carried out 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. | Approved | Most recent IF: 4.536 | ||
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PLASMANT @ plasmant @c:irua:175873 | Serial | 6672 | ||
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Author | Michiels, R.; Engelmann, Y.; Bogaerts, A. | ||||
Title | Plasma Catalysis for CO2Hydrogenation: Unlocking New Pathways toward CH3OH | Type | A1 Journal article | ||
Year | 2020 | Publication | Journal Of Physical Chemistry C | Abbreviated Journal | J Phys Chem C |
Volume | 124 | Issue | 47 | Pages | 25859-25872 |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Movement Antwerp (MOVANT) | ||||
Abstract | We developed a microkinetic model to reveal the effects of plasma-generated radicals, intermediates, and vibrationally excited species on the catalytic hydrogenation of CO2 to CH3OH on a Cu(111) surface. As a benchmark, we first present the mechanisms of thermal catalytic CH3OH formation. Our model predicts that the reverse water-gas shift reaction followed by CO hydrogenation, together with the formate path, mainly contribute to CH3OH formation in thermal catalysis. Adding plasma-generated radicals and intermediates results in a higher CH3OH turnover frequency (TOF) by six to seven orders of magnitude, showing the potential of plasma-catalytic CO2 hydrogenation into CH3OH, in accordance with the literature. In addition, CO2 vibrational excitation further increases the CH3OH TOF, but the effect is limited due to relatively low vibrational temperatures under typical plasma catalysis conditions. The predicted increase in CH3OH formation by plasma catalysis is mainly attributed to the increased importance of the formate path. In addition, the conversion of plasma-generated CO to HCO* and subsequent HCOO* or H2CO* formation contribute to CH3OH formation. Both pathways bypass the HCOO* formation from CO2, which is the main bottleneck in the process. Hence, our model points toward the important role of CO, but also O, OH, and H radicals, as they influence the reactions that consume CO2 and CO. In addition, our model reveals that the H pressure should not be smaller than ca. half of the O pressure in the plasma as this would cause O* poisoning, which would result in very small product TOFs. Thus, plasma conditions should be targeted with a high CO and H content as this is favorable for CH3OH formation, while the O content should be minimized. | ||||
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Language | Wos | 000595545800023 | Publication Date | 2020-11-25 | |
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 | Not_Open_Access: Available from 15.07.2021 | |
Notes | Universiteit Antwerpen; Fonds Wetenschappelijk Onderzoek, 1114921N ; H2020 European Research Council, 810182 ; We acknowledge the financial support from the Fund for Scientific Research (FWO-Vlaanderen; grant ID 1114921N) and from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement no. 810182 − SCOPE ERC Synergy project) as well as from the DOC-PRO3 and the TOPBOF projects of the University of Antwerp. | Approved | Most recent IF: 3.7; 2020 IF: 4.536 | ||
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PLASMANT @ plasmant @c:irua:173864 | Serial | 6443 | ||
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Author | Oliveira, M.C.; Yusupov, M.; Bogaerts, A.; Cordeiro, R.M. | ||||
Title | How do nitrated lipids affect the properties of phospholipid membranes? | Type | A1 Journal article | ||
Year | 2020 | Publication | Archives Of Biochemistry And Biophysics | Abbreviated Journal | Arch Biochem Biophys |
Volume | 695 | Issue | Pages | 108548 | |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Biological membranes are under constant attack of free radicals, which may lead to lipid nitro-oxidation, pro ducing a complex mixture of nitro-oxidized lipids that are responsible for structural and dynamic changes on the membrane. Despite the latter, nitro-oxidized lipids are also associated with several inflammatory and neuro degenerative diseases, the underlying mechanisms of which remain elusive. We perform atomistic molecular dynamics simulations using several isomers of nitro-oxidized lipids to study their effect on the structure and permeability of the membrane, as well as the interaction between the mixture of these products in the phospholipid membrane environment. Our results show that the stereo- and positional isomers have a stronger effect on the properties of the membrane composed of oxidized lipids compared to that containing nitrated lipids. Nevertheless, nitrated lipids lead to three-fold increase in water permeability compared to oxidized lipids. In addition, we show that in a membrane consisting of combined nitro-oxidized lipid products, the presence of oxidized lipids protects the membrane from transient pores. Is well stablished that plasma application and photodynamic therapy produces a number of oxidative species used to kill cancer cells, through membrane damage induced by nitro-oxidative stress. This study is important to elucidate the mechanisms and the molecular level properties involving the reactive species produced during that cancer therapies. | ||||
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Language | Wos | 000594173400010 | Publication Date | 0000-00-00 | |
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ISSN | 0003-9861 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 3.9 | Times cited | Open Access | ||
Notes | CAPES; Flanders Research Foundation, 1200219N ; We thank Universidade Federal do ABC for providing the computational resources needed for completion of this work and CAPES for scholarship granted. M.Y. acknowledges the Flanders Research Foundation (grant 1200219N) for financial support. | Approved | Most recent IF: 3.9; 2020 IF: 3.165 | ||
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PLASMANT @ plasmant @c:irua:173861 | Serial | 6440 | ||
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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 | |
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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 | ||
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PLASMANT @ plasmant @c:irua:173587 | Serial | 6428 | ||
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Author | Rouwenhorst, K.H.R.; Engelmann, Y.; van ‘t Veer, K.; Postma, R.S.; Bogaerts, A.; Lefferts, L. | ||||
Title | Plasma-driven catalysis: green ammonia synthesis with intermittent electricity | Type | A1 Journal article | ||
Year | 2020 | Publication | Green Chemistry | Abbreviated Journal | Green Chem |
Volume | 22 | Issue | 19 | Pages | 6258-6287 |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Movement Antwerp (MOVANT) | ||||
Abstract | Ammonia is one of the most produced chemicals, mainly synthesized from fossil fuels for fertilizer applications. Furthermore, ammonia may be one of the energy carriers of the future, when it is produced from renewable electricity. This has spurred research on alternative technologies for green ammonia production. Research on plasma-driven ammonia synthesis has recently gained traction in academic literature. In the current review, we summarize the literature on plasma-driven ammonia synthesis. We distinguish between mechanisms for ammonia synthesis in the presence of a plasma, with and without a catalyst, for different plasma conditions. Strategies for catalyst design are discussed, as well as the current understanding regarding the potential plasma-catalyst synergies as function of the plasma conditions and their implications on energy efficiency. Finally, we discuss the limitations in currently reported models and experiments, as an outlook for research opportunities for further unravelling the complexities of plasma-catalytic ammonia synthesis, in order to bridge the gap between the currently reported models and experimental results. | ||||
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Language | Wos | 000575015700002 | Publication Date | 2020-09-08 | |
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ISSN | 1463-9262 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 9.8 | Times cited | 4 | Open Access | |
Notes | ; ; | Approved | Most recent IF: 9.8; 2020 IF: 9.125 | ||
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PLASMANT @ plasmant @c:irua:172671 | Serial | 6430 | ||
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Author | Zhang, Q.-Z.; Wang, W.Z.; Thille, C.; Bogaerts, A. | ||||
Title | H2S Decomposition into H2 and S2 by Plasma Technology: Comparison of Gliding Arc and Microwave Plasma | Type | A1 Journal article | ||
Year | 2020 | Publication | Plasma Chemistry And Plasma Processing | Abbreviated Journal | Plasma Chem Plasma P |
Volume | 40 | Issue | 5 | Pages | 1163-1187 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | We studied hydrogen sulfide (H2S) decomposition into hydrogen (H2) and sulfur (S2) in a gliding arc plasmatron (GAP) and microwave (MW) plasma by a combination of 0D and 2D models. The conversion, energy efficiency, and plasma distribution are examined for different discharge conditions, and validated with available experiments from literature. Furthermore, a comparison is made between GAP and MW plasma. The GAP operates at atmospheric pressure, while the MW plasma experiments to which comparison is made were performed at reduced pressure. Indeed, the MW discharge region becomes very much contracted near atmospheric pressure, at the conditions under study, as revealed by our 2D model. The models predict that thermal reactions play the most important role in H2S decomposition in both plasma types. The GAP has a higher energy efficiency but lower conversion than the MW plasma at their typical conditions. When compared at the same conversion, the GAP exhibits a higher energy efficiency and lower energy cost than the MW plasma. | ||||
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Language | Wos | 000543012200001 | Publication Date | 2020-06-24 | |
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ISSN | 0272-4324 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 3.6 | Times cited | Open Access | ||
Notes | This work was supported by the Scientific Research Foundation from Dalian University of Technology, DUT19RC(3)045. We gratefully acknowledge T. Godfroid (Materia Nova) for sharing the experimental data about the MW plasma. 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: 3.6; 2020 IF: 2.355 | ||
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PLASMANT @ plasmant @c:irua:172490 | Serial | 6409 | ||
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Author | Uytdenhouwen, Y.; Bal, Km.; Neyts, Ec.; Meynen, V.; Cool, P.; Bogaerts, A. | ||||
Title | On the kinetics and equilibria of plasma-based dry reforming of methane | Type | A1 Journal article | ||
Year | 2021 | Publication | Chemical Engineering Journal | Abbreviated Journal | Chem Eng J |
Volume | 405 | Issue | Pages | 126630 | |
Keywords | A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Plasma reactors are interesting for gas-based chemical conversion but the fundamental relation between the plasma chemistry and selected conditions remains poorly understood. Apparent kinetic parameters for the loss and formation processes of individual components of gas conversion processes, can however be extracted by performing experiments in an extended residence time range (2–75 s) and fitting the gas composition to a firstorder kinetic model of the evolution towards partial chemical equilibrium (PCE). We specifically investigated the differences in kinetic characteristics and PCE state of the CO2 dissociation and CH4 reforming reactions in a dielectric barrier discharge reactor (DBD), how these are mutually affected when combining both gases in the dry reforming of methane (DRM) reaction, and how they change when a packing material (non-porous SiO2) is added to the reactor. We find that CO2 dissociation is characterized by a comparatively high reaction rate of 0.120 s−1 compared to CH4 reforming at 0.041 s−1; whereas CH4 reforming reaches higher equilibrium conversions, 82% compared to 53.6% for CO2 dissociation. Combining both feed gases makes the DRM reaction to proceed at a relatively high rate (0.088 s−1), and high conversion (75.4%) compared to CO2 dissociation, through accessing new chemical pathways between the products of CO2 and CH4. The addition of the packing material can also distinctly influence the conversion rate and position of the equilibrium, but its precise effect depends strongly on the gas composition. Comparing different CO2:CH4 ratios reveals the delicate balance of the combined chemistry. CO2 drives the loss reactions in DRM, whereas CH4 in the mixture suppresses back reactions. As a result, our methodology provides some of the insight necessary to systematically tune the conversion process. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000621197700003 | Publication Date | 2020-08-12 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1385-8947 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 6.216 | Times cited | Open Access | OpenAccess | |
Notes | The authors acknowledge financial support from the European Fund for Regional Development through the cross-border collaborative Interreg V program Flanders-the Netherlands (project EnOp), the Fund for Scientific Research (FWO; grant number: G.0254.14N), a TOP-BOF project and an IOF-SBO (SynCO2Chem) project from the University of Antwerp. | Approved | Most recent IF: 6.216 | ||
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PLASMANT @ plasmant @c:irua:172458 | Serial | 6411 | ||
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Author | Bal, K.M.; Fukuhara, S.; Shibuta, Y.; Neyts, E.C. | ||||
Title | Free energy barriers from biased molecular dynamics simulations | Type | A1 Journal article | ||
Year | 2020 | Publication | Journal Of Chemical Physics | Abbreviated Journal | J Chem Phys |
Volume | 153 | Issue | 11 | Pages | 114118 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Atomistic simulation methods for the quantification of free energies are in wide use. These methods operate by sampling the probability density of a system along a small set of suitable collective variables (CVs), which is, in turn, expressed in the form of a free energy surface (FES). This definition of the FES can capture the relative stability of metastable states but not that of the transition state because the barrier height is not invariant to the choice of CVs. Free energy barriers therefore cannot be consistently computed from the FES. Here, we present a simple approach to calculate the gauge correction necessary to eliminate this inconsistency. Using our procedure, the standard FES as well as its gauge-corrected counterpart can be obtained by reweighing the same simulated trajectory at little additional cost. We apply the method to a number of systems—a particle solvated in a Lennard-Jones fluid, a Diels–Alder reaction, and crystallization of liquid sodium—to demonstrate its ability to produce consistent free energy barriers that correctly capture the kinetics of chemical or physical transformations, and discuss the additional demands it puts on the chosen CVs. Because the FES can be converged at relatively short (sub-ns) time scales, a free energy-based description of reaction kinetics is a particularly attractive option to study chemical processes at more expensive quantum mechanical levels of theory. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000574665600004 | Publication Date | 2020-09-21 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0021-9606 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 4.4 | Times cited | Open Access | ||
Notes | Japan Society for the Promotion of Science, 19H02415 18J22727 ; Fonds Wetenschappelijk Onderzoek, 12ZI420N ; This work was supported, in part, by a Grant-in-Aid for Scientific Research (B) (Grant No. 19H02415) and Grant-in-Aid for a JSPS Research Fellow (Grant No. 18J22727) from the Japan Society for the Promotion of Science (JSPS), Japan. K.M.B. was funded as a junior postdoctoral fellow of the FWO (Research Foundation – Flanders), Grant No. 12ZI420N. S.F. was supported by JSPS through the Program for Leading Graduate Schools (MERIT). The 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 FWO and the Flemish Government. The authors are grateful to Pablo Piaggi for making the pair entropy CV code publicly available. | Approved | Most recent IF: 4.4; 2020 IF: 2.965 | ||
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PLASMANT @ plasmant @c:irua:172456 | Serial | 6420 | ||
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Author | Vermeiren, V.; Bogaerts, A. | ||||
Title | Plasma-Based CO2Conversion: To Quench or Not to Quench? | Type | A1 Journal article | ||
Year | 2020 | Publication | Journal Of Physical Chemistry C | Abbreviated Journal | J Phys Chem C |
Volume | 124 | Issue | 34 | Pages | 18401-18415 |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Plasma technology is gaining increasing interest for CO2 conversion. The gas temperature in (and after) the plasma reactor largely affects the performance. Therefore, we examine the effect of cooling/quenching, during and after the plasma, on the CO2 conversion and energy efficiency, for typical “warm” plasmas, by means of chemical kinetics modeling. For plasmas at low specific energy input (SEI ∼ 0.5 eV/molecule), it is best to quench at the plasma end, while for high-SEI plasmas (SEI ∼ 4 eV/molecule), quenching at maximum conversion is better. For low-SEI plasmas, quenching can even increase the conversion beyond the dissociation in the plasma, known as superideal quenching. To better understand the effects of quenching at different plasma conditions, we study the dissociation and recombination rates, as well as the vibrational distribution functions (VDFs) of CO2, CO, and O2. When a high vibrational−translational (VT) nonequilibrium exists at the moment of quenching, the dissociation and recombination reaction rates both increase. Depending on the conversion degree at the moment of quenching, this can lead to a net increase or decrease of CO2 conversion. In general, however, and certainly for equilibrium plasmas at high temperature, quenching after the plasma helps prevent recombination reactions and clearly enhances the final CO2 conversion. We also investigate the effect of different quenching cooling rates on the CO2 conversion and energy efficiency. Finally, we compare plasma-based conversion to purely thermal conversion. For warm plasmas with typical temperatures of 3000−4000 K, the conversion is roughly thermal. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000566481000003 | Publication Date | 2020-08-27 | |
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, G.0383.16N ; H2020 European Research Council, 810182 ; This research was supported by the FWO project (grant no. G.0383.16N) and the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (grant agreement no. 810182SCOPE 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: 3.7; 2020 IF: 4.536 | ||
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PLASMANT @ plasmant @c:irua:172052 | Serial | 6407 | ||
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Author | Andersen, Ja.; Christensen, Jm.; Østberg, M.; Bogaerts, A.; Jensen, Ad. | ||||
Title | Plasma-catalytic dry reforming of methane: Screening of catalytic materials in a coaxial packed-bed DBD reactor | Type | A1 Journal article | ||
Year | 2020 | Publication | Chemical Engineering Journal | Abbreviated Journal | Chem Eng J |
Volume | 397 | Issue | Pages | 125519 | |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | The combination of catalysis with non-thermal plasma is a promising alternative to thermal catalysis. A dielectric-barrier discharge reactor was used to study plasma-catalytic dry reforming of methane at ambient pressure and temperature and a fixed plasma power of 45 W. The effect of different catalytic packing materials was evaluated in terms of conversion, product selectivity, and energy efficiency. The conversion of CO2 (~22%) and CH4 (~33%) were found to be similar in plasma-only and when introducing packing materials in plasma. The main reason is the shorter residence time of the gas due to packing geometry, when compared at identical flow rates. H2, CO, C2-C4 hydrocarbons, and oxygenates were identified in the product gas. High selectivity towards H2 and CO were found for all catalysts and plasma-only, with a H2/CO molar ratio of ~0.9. The lowest syngas selectivity was obtained with Cu/Al2O3 (~66%), which instead, had the highest alcohol selectivity (~3.6%). | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000542296100011 | Publication Date | 2020-05-17 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1385-8947 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 15.1 | Times cited | Open Access | ||
Notes | Department of Chemical and Biochemical Engineering, Technical University of Denmark; We thank Haldor Topsoe A/S for providing all the catalytic materials used and the Department of Chemical and Biochemical Engineering, Technical University of Denmark, for funding this project. | Approved | Most recent IF: 15.1; 2020 IF: 6.216 | ||
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PLASMANT @ plasmant @c:irua:170613 | Serial | 6406 | ||
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Author | Uytdenhouwen, Y.; Hereijgers, J.; Breugelmans, T.; Cool, P.; Bogaerts, A. | ||||
Title | How gas flow design can influence the performance of a DBD plasma reactor for dry reforming of methane | Type | A1 Journal article | ||
Year | 2021 | Publication | Chemical Engineering Journal | Abbreviated Journal | Chem Eng J |
Volume | 405 | Issue | Pages | 126618 | |
Keywords | A1 Journal article; Engineering sciences. Technology; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Applied Electrochemistry & Catalysis (ELCAT) | ||||
Abstract | DBD plasma reactors are commonly used in a static ‘one inlet – one outlet’ design that goes against reactor design principles for multi-component reactions, such as dry reforming of methane (DRM). Therefore, in this paper we have developed a novel reactor design, and investigated how the shape and size of the reaction zone, as well as gradual gas addition, and the method of mixing CO2 and CH4 can influence the conversion and product com position of DRM. Even in the standard ‘one inlet – one outlet’ design, the direction of the gas flow (i.e. short or long path through the reactor, which defines the gas velocity at fixed residence time), as well as the dimensions of the reaction zone and the power delivery to the reactor, largely affect the performance. Using gradual gas addition and separate plasma activation zones for the individual gases give increased conversions within the same operational parameters, by optimising mixing ratios and kinetics. The choice of the main (pre-activated) gas and the direction of gas flow largely affect the conversion and energy cost, while the gas inlet position during separate addition only influences the product distribution. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000626511800005 | Publication Date | 2020-08-12 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1385-8947 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 6.216 | Times cited | Open Access | OpenAccess | |
Notes | Interreg; Flanders; FWO; University of Antwerp; The authors acknowledge financial support from the European Fund for Regional Development through the cross-border collaborative Interreg V program Flanders-the Netherlands (project EnOp), the Fund 13 for Scientific Research (FWO; grant number: G.0254.14N), and an IOFSBO (SynCO2Chem) project from the University of Antwerp. | Approved | Most recent IF: 6.216 | ||
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PLASMANT @ plasmant @c:irua:170609 | Serial | 6410 | ||
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Author | Vervloessem, E.; Aghaei, M.; Jardali, F.; Hafezkhiabani, N.; Bogaerts, A. | ||||
Title | Plasma-Based N2Fixation into NOx: Insights from Modeling toward Optimum Yields and Energy Costs in a Gliding Arc Plasmatron | Type | A1 Journal article | ||
Year | 2020 | Publication | Acs Sustainable Chemistry & Engineering | Abbreviated Journal | Acs Sustain Chem Eng |
Volume | 8 | Issue | 26 | Pages | 9711-9720 |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Plasma technology provides a sustainable, fossil-free method for N2 fixation, i.e., the conversion of inert atmospheric N2 into valuable substances, such as NOx or ammonia. In this work, we present a novel gliding arc plasmatron at atmospheric pressure for NOx production at different N2/O2 gas feed ratios, offering a promising NOx yield of 1.5% with an energy cost of 3.6 MJ/mol NOx produced. To explain the underlying mechanisms, we present a chemical kinetics model, validated by experiments, which provides insight into the NOx formation pathways and into the ambivalent role of the vibrational kinetics. This allows us to pinpoint the factors limiting the yield and energy cost, which can help to further improve the process. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000548456600013 | Publication Date | 2020-07-06 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2168-0485 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.4 | Times cited | Open Access | OpenAccess | |
Notes | Herculesstichting; Universiteit Antwerpen; Vlaamse regering; H2020 European Research Council, 810182 ; N2 Applied; Excellence of Science FWO – FNRS project, 30505023 GoF9618n ; | Approved | Most recent IF: 8.4; 2020 IF: 5.951 | ||
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PLASMANT @ plasmant @c:irua:170138 | Serial | 6392 | ||
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Author | Engelmann, Y.; Mehta, P.; Neyts, E.C.; Schneider, W.F.; Bogaerts, A. | ||||
Title | Predicted Influence of Plasma Activation on Nonoxidative Coupling of Methane on Transition Metal Catalysts | Type | A1 Journal article | ||
Year | 2020 | Publication | Acs Sustainable Chemistry & Engineering | Abbreviated Journal | Acs Sustain Chem Eng |
Volume | 8 | Issue | 15 | Pages | 6043-6054 |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Movement Antwerp (MOVANT) | ||||
Abstract | The combination of catalysis and nonthermal plasma holds promise for enabling difficult chemical conversions. The possible synergy between both depends strongly on the nature of the reactive plasma species and the catalyst material. In this paper, we show how vibrationally excited species and plasma-generated radicals interact with transition metal catalysts and how changing the catalyst material can improve the conversion rates and product selectivity. We developed a microkinetic model to investigate the impact of vibrational excitations and plasma-generated radicals on the nonoxidative coupling of methane over transition metal surfaces. We predict a significant increase in ethylene formation for vibrationally excited methane. Plasma-generated radicals have a stronger impact on the turnover frequencies with high selectivity toward ethylene on noble catalysts and mixed selectivity on non-noble catalysts. In general, we show how the optimal catalyst material depends on the desired products as well as the plasma conditions. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000526884000025 | Publication Date | 2020-04-20 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2168-0485 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.4 | Times cited | Open Access | ||
Notes | Herculesstichting; University of Notre Dame; Universiteit Antwerpen; Division of Engineering Education and Centers, EEC-1647722 ; We would like to thank Tom Butterworth for his work on methane vibrational distribution functions (VDF) and for sharing his thoughts and experiences on this matter, specifically regarding the VDF of the degenerate modes of methane. We ACS Sustainable Chemistry & Engineering pubs.acs.org/journal/ascecg Research Article https://dx.doi.org/10.1021/acssuschemeng.0c00906 ACS Sustainable Chem. Eng. 2020, 8, 6043−6054 6052 also acknowledge financial support from the DOC-PRO3 and the TOP-BOF projects of the University of Antwerp. This work was carried out 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. Support for W.F.S. was provided by the National Science Foundation under cooperative agreement no. EEC-1647722, an Engineering Research Center for the Innovative and Strategic Transformation of Alkane Resources (CISTAR). P.M. acknowledges support through the Eilers Graduate Fellowship of the University of Notre Dame. | Approved | Most recent IF: 8.4; 2020 IF: 5.951 | ||
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PLASMANT @ plasmant @c:irua:169228 | Serial | 6366 | ||
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Author | Jafarzadeh, A.; Bal, K.M.; Bogaerts, A.; Neyts, E.C. | ||||
Title | Activation of CO2on Copper Surfaces: The Synergy between Electric Field, Surface Morphology, and Excess Electrons | Type | A1 Journal article | ||
Year | 2020 | Publication | Journal Of Physical Chemistry C | Abbreviated Journal | J Phys Chem C |
Volume | 124 | Issue | 12 | Pages | 6747-6755 |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | In this work, we use density functional theory calculations to study the combined effect of external electric fields, surface morphology, and surface charge on CO2 activation over Cu(111), Cu(211), Cu(110), and Cu(001) surfaces. We observe that the binding energy of the CO2 molecule on Cu surfaces increases significantly upon increasing the applied electric field strength. In addition, rougher surfaces respond more effectively to the presence of the external electric field toward facilitating the formation of a carbonate-like CO2 structure and the transformation of the most stable adsorption mode from physisorption to chemisorption. The presence of surface charges further strengthens the electric field effect and consequently causes an improved bending of the CO2 molecule and C−O bond length elongation. On the other hand, a net charge in the absence of an externally applied electric field shows only a marginal effect on CO2 binding. The chemisorbed CO2 is more stable and further activated when the effects of an external electric field, rough surface, and surface charge are combined. These results can help to elucidate the underlying factors that control CO2 activation in heterogeneous and plasma catalysis, as well as in electrochemical processes. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000526396900030 | Publication Date | 2020-03-26 | |
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 | ||
Notes | Bijzonder Onderzoeksfonds, 32249 ; The financial support from the TOP research project of the Research Fund of the University of Antwerp (grant ID: 32249) is highly acknowledged by the authors. The computational resources used in this study were provided by the VSC (Flemish Supercomputer Center), funded by the FWO and the Flemish Governmentdepartment EWI. | Approved | Most recent IF: 3.7; 2020 IF: 4.536 | ||
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PLASMANT @ plasmant @c:irua:168606 | Serial | 6361 | ||
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Author | Bogaerts, A. | ||||
Title | Modeling plasmas in analytical chemistry—an example of cross-fertilization | Type | A1 Journal article | ||
Year | 2020 | Publication | Analytical And Bioanalytical Chemistry | Abbreviated Journal | Anal Bioanal Chem |
Volume | 412 | Issue | 24 | Pages | 6059-6083 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | This paper gives an overview of the modeling work developed in our group in the last 25 years for various plasmas used in analytical spectrochemistry, i.e., glow discharges (GDs), inductively coupled plasmas (ICPs), and laser ablation (LA) for sample introduction in the ICP and for laser-induced breakdown spectroscopy (LIBS). The modeling approaches are briefly presented, which are different for each case, and some characteristic results are illustrated. These plasmas are used not only in analytical chemistry but also in other applications, and the insights obtained in these other fields were quite helpful for us to develop models for the analytical plasmas. Likewise, there is now a huge interest in plasma–liquid interaction, atmospheric pressure glow discharges (APGDs), and dielectric barrier discharges (DBDs) for environmental, medical, and materials applications of plasmas. The insights obtained in these fields are also very relevant for ambient desorption/ionization sources and for liquid sampling, which are nowadays very popular in analytical chemistry, and they could be very helpful in developing models for these sources as well. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000522701700005 | Publication Date | 2020-03-31 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1618-2642 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 4.3 | Times cited | Open Access | ||
Notes | M. Aghaei, Z. Chen, D. Autrique, T. Martens, and P. Heirman are gratefully acknowledged for their valuable efforts in the model developments illustrated in this paper. | Approved | Most recent IF: 4.3; 2020 IF: 3.431 | ||
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PLASMANT @ plasmant @c:irua:168600 | Serial | 6412 | ||
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Author | Heijkers, S.; Aghaei, M.; Bogaerts, A. | ||||
Title | Plasma-Based CH4Conversion into Higher Hydrocarbons and H2: Modeling to Reveal the Reaction Mechanisms of Different Plasma Sources | Type | A1 Journal article | ||
Year | 2020 | Publication | Journal Of Physical Chemistry C | Abbreviated Journal | J Phys Chem C |
Volume | 124 | Issue | 13 | Pages | 7016-7030 |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Plasma is gaining interest for CH4 conversion into higher hydrocarbons and H2. However, the performance in terms of conversion and selectivity toward different hydrocarbons is different for different plasma types, and the underlying mechanisms are not yet fully understood. Therefore, we study here these mechanisms in different plasma sources, by means of a chemical kinetics model. The model is first validated by comparing the calculated conversions and hydrocarbon/H2 selectivities with experimental results in these different plasma types and over a wide range of specific energy input (SEI) values. Our model predicts that vibrational−translational nonequilibrium is negligible in all CH4 plasmas investigated, and instead, thermal conversion is important. Higher gas temperatures also lead to a more selective production of unsaturated hydrocarbons (mainly C2H2) due to neutral dissociation of CH4 and subsequent dehydrogenation processes, while three-body recombination reactions into saturated hydrocarbons (mainly C2H6, but also higher hydrocarbons) are dominant in low temperature plasmas. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000526328500007 | Publication Date | 2020-04-02 | |
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 | Universiteit Antwerpen; Vlaamse regering; Fonds Wetenschappelijk Onderzoek, G.0383.16N ; H2020 European Research Council, 810182 ; We acknowledge financial support from the Fund for Scientific Research, Flanders (FWO; Grant No. G.0383.16N), the Methusalem Grant, 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). This work was carried out 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. | Approved | Most recent IF: 3.7; 2020 IF: 4.536 | ||
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PLASMANT @ plasmant @c:irua:168096 | Serial | 6358 | ||
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Author | Slaets, J.; Aghaei, M.; Ceulemans, S.; Van Alphen, S.; Bogaerts, A. | ||||
Title | CO2and CH4conversion in “real” gas mixtures in a gliding arc plasmatron: how do N2and O2affect the performance? | Type | A1 Journal article | ||
Year | 2020 | Publication | Green Chemistry | Abbreviated Journal | Green Chem |
Volume | 22 | Issue | 4 | Pages | 1366-1377 |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | In this paper we study dry reforming of methane (DRM) in a gliding arc plasmatron (GAP) in the presence of N<sub>2</sub>and O<sub>2</sub>. N<sub>2</sub>is added to create a stable plasma at equal fractions of CO<sub>2</sub>and CH<sub>4</sub>, and because emissions from industrial plants typically contain N<sub>2</sub>, while O<sub>2</sub>is added to enhance the process. We test different gas mixing ratios to evaluate the conversion and energy cost. We obtain conversions between 31 and 52% for CO<sub>2</sub>and between 55 and 99% for CH<sub>4</sub>, with total energy costs between 3.4 and 5.0 eV per molecule, depending on the gas mixture. This is very competitive when benchmarked with the literature. In addition, we present a chemical kinetics model to obtain deeper insight in the underlying plasma chemistry. This allows determination of the major reaction pathways to convert CO<sub>2</sub>and CH<sub>4</sub>, in the presence of O<sub>2</sub>and N<sub>2</sub>, into CO and H<sub>2</sub>. We show that N<sub>2</sub>assists in the CO<sub>2</sub>conversion, but part of the applied energy is also wasted in N<sub>2</sub>excitation. Adding O<sub>2</sub>enhances the CH<sub>4</sub>conversion, and lowers the energy cost, while the CO<sub>2</sub>conversion remains constant, and only slightly drops at the highest O<sub>2</sub>fractions studied, when CH<sub>4</sub>is fully oxidized into CO<sub>2</sub>. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000518034000032 | Publication Date | 2020-01-30 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1463-9262 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 9.8 | Times cited | Open Access | OpenAccess | |
Notes | H2020 European Research Council, 810182 ; Fonds Wetenschappelijk Onderzoek, GoF9618n 12M7118N ; We acknowledge financial support from 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 Excellence of Science FWO-FNRS project (FWO grant ID GoF9618n, EOS ID 30505023), and the FWO postdoctoral fellowship of M. A. (Grant number 12M7118N). This work was carried out 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. | Approved | Most recent IF: 9.8; 2020 IF: 9.125 | ||
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PLASMANT @ plasmant @c:irua:167136 | Serial | 6339 | ||
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Author | Cordeiro, R.M.; Yusupov, M.; Razzokov, J.; Bogaerts, A. | ||||
Title | Parametrization and Molecular Dynamics Simulations of Nitrogen Oxyanions and Oxyacids for Applications in Atmospheric and Biomolecular Sciences | Type | A1 Journal article | ||
Year | 2020 | Publication | Journal Of Physical Chemistry B | Abbreviated Journal | J Phys Chem B |
Volume | 124 | Issue | 6 | Pages | 1082-1089 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Nitrogen oxyanions and oxyacids are important agents in atmospheric chemistry and medical biology. Although their chemical behavior in solution is relatively well understood, they may behave very differently at the water/air interface of atmospheric aerosols or at the membrane/water interface of cells. Here, we developed a fully classical model for molecular dynamics simulations of NO3−, NO2−, HNO3, and HNO2 in the framework of the GROMOS 53A6 and 54A7 force field versions. The model successfully accounted for the poorly structured solvation shell and ion pairing tendency of NO3−. Accurate pure-liquid properties and hydration free energies were obtained for the oxyacids. Simulations at the water/air interface showed a local enrichment of HNO3 and depletion of NO3−. The effect was discussed in light of earlier spectroscopic data and ab initio calculations, suggesting that HNO3 behaves as a weaker acid at the surface of water. Our model will hopefully allow for efficient and accurate simulations of nitrogen oxyanions and oxyacids in solution and at microheterogeneous interface environments. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000512222500015 | Publication Date | 2020-02-13 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1520-6106 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 3.3 | Times cited | Open Access | ||
Notes | We thank Universidade Federal do ABC for providing the computational resources needed for completion of this work. This study was financed in part by the Coordenaçaõ de Aperfeiçoamento de Pessoal de Nı ́vel Superior – Brasil (CAPES) – Finance Code 001. | Approved | Most recent IF: 3.3; 2020 IF: 3.177 | ||
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PLASMANT @ plasmant @c:irua:166488 | Serial | 6340 | ||
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Author | Bal, K.M.; Bogaerts, A.; Neyts, E.C. | ||||
Title | Ensemble-Based Molecular Simulation of Chemical Reactions under Vibrational Nonequilibrium | Type | A1 Journal article | ||
Year | 2020 | Publication | Journal Of Physical Chemistry Letters | Abbreviated Journal | J Phys Chem Lett |
Volume | 11 | Issue | 2 | Pages | 401-406 |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | We present an approach to incorporate the effect of vibrational nonequilibrium in molecular dynamics (MD) simulations. A perturbed canonical ensemble, in which selected modes are excited to higher temperature while all others remain equilibrated at low temperature, is simulated by applying a specifically tailored bias potential. Our method can be readily applied to any (classical or quantum mechanical) MD setup at virtually no additional computational cost and allows the study of reactions of vibrationally excited molecules in nonequilibrium environments such as plasmas. In combination with enhanced sampling methods, the vibrational efficacy and mode selectivity of vibrationally stimulated reactions can then be quantified in terms of chemically relevant observables, such as reaction rates and apparent free energy barriers. We first validate our method for the prototypical hydrogen exchange reaction and then show how it can capture the effect of vibrational excitation on a symmetric SN2 reaction and radical addition on CO2. | ||||
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Language | Wos | 000508473400008 | Publication Date | 2020-01-16 | |
Series Editor | Series Title | Abbreviated Series Title | |||
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ISSN | 1948-7185 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 5.7 | Times cited | Open Access | ||
Notes | Universiteit Antwerpen; Fonds Wetenschappelijk Onderzoek, 12ZI420N ; Departement Economie, Wetenschap en Innovatie van de Vlaamse Overheid; K.M.B. was funded as a junior postdoctoral fellow of the FWO (Research Foundation − Flanders), Grant 12ZI420N, and through a TOP-BOF research project of the University of Antwerp. The computational resources and services used in this work were provided by the VSC (Flemish Supercomputer Center), funded by the FWO and the Flemish Government− department EWI. | Approved | Most recent IF: 5.7; 2020 IF: 9.353 | ||
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PLASMANT @ plasmant @c:irua:165587 | Serial | 5442 | ||
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Author | Van Alphen, S.; Vermeiren, V.; Butterworth, T.; van den Bekerom, D.C.M.; van Rooij, G.J.; Bogaerts, A. | ||||
Title | Power Pulsing To Maximize Vibrational Excitation Efficiency in N2Microwave Plasma: A Combined Experimental and Computational Study | Type | A1 Journal article | ||
Year | 2020 | Publication | Journal Of Physical Chemistry C | Abbreviated Journal | J Phys Chem C |
Volume | 124 | Issue | 3 | Pages | 1765-1779 |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Plasma is gaining increasing interest for N2 fixation, being a flexible, electricity-driven alternative for the current conventional fossil fuel-based N2 fixation processes. As the vibrational-induced dissociation of N2 is found to be an energy-efficient pathway to acquire atomic N for the fixation processes, plasmas that are in vibrational nonequilibrium seem promising for this application. However, an important challenge in using nonequilibrium plasmas lies in preventing vibrational−translational (VT) relaxation processes, in which vibrational energy crucial for N2 dissociation is lost to gas heating. We present here both experimental and modeling results for the vibrational and gas temperature in a microsecond-pulsed microwave (MW) N2 plasma, showing how power pulsing can suppress this unfavorable VT relaxation and achieve a maximal vibrational nonequilibrium. By means of our kinetic model, we demonstrate that pulsed plasmas take advantage of the long time scale on which VT processes occur, yielding a very pronounced nonequilibrium over the whole N2 vibrational ladder. Additionally, the effect of pulse parameters like the pulse frequency and pulse width are investigated, demonstrating that the advantage of pulsing to inhibit VT relaxation diminishes for high pulse frequencies (around 7000 kHz) and long power pulses (above 400 μs). Nevertheless, all regimes studied here demonstrate a clear vibrational nonequilibrium while only requiring a limited power-on time, and thus, we may conclude that a pulsed plasma seems very interesting for energyefficient vibrational excitation. | ||||
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Language | Wos | 000509438600001 | Publication Date | 2020-01-23 | |
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 | ||
Notes | Fonds Wetenschappelijk Onderzoek, 30505023 GoF9618n ; 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. | Approved | Most recent IF: 3.7; 2020 IF: 4.536 | ||
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PLASMANT @ plasmant @c:irua:165586 | Serial | 5443 | ||
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Author | Oliveira, M.C.; Yusupov, M.; Bogaerts, A.; Cordeiro, R.M. | ||||
Title | Molecular dynamics simulations of mechanical stress on oxidized membranes | Type | A1 Journal article | ||
Year | 2019 | Publication | Biophysical chemistry | Abbreviated Journal | Biophys Chem |
Volume | 254 | Issue | Pages | 106266 | |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Biomembranes are under constant attack of free radicals that may lead to lipid oxidation in conditions of oxidative stress. The products generated during lipid oxidation are responsible for structural and dynamical changes which may jeopardize the membrane function. For instance, the local rearrangements of oxidized lipid molecules may induce membrane rupture. In this study, we investigated the effects of mechanical stress on oxidized phospholipid bilayers (PLBs). Model bilayers were stretched until pore formation (or poration) using nonequilibrium molecular dynamics simulations. We studied single-component homogeneous membranes composed of lipid oxidation products, as well as two-component heterogeneous membranes with coexisting native and oxidized domains. In homogeneous membranes, the oxidation products with —OH and —OOH groups reduced the areal strain required for pore formation, whereas the oxidation product with ]O group behaved similarly to the native membrane. In heterogeneous membranes composed of oxidized and non-oxidized domains, we tested the hypothesis according to which poration may be facilitated at the domain interface region. However, results were inconclusive due to their large statistical variance and sensitivity to simulation setup parameters. We pointed out important technical issues that need to be considered in future simulations of mechanically-induced poration of heterogeneous membranes. This research is of interest for photodynamic therapy and plasma medicine, because ruptured and intact plasma membranes are experimentally considered hallmarks of necrotic and apoptotic cell death. | ||||
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Language | Wos | 000502890900015 | Publication Date | 2019-09-13 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0301-4622 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 2.402 | Times cited | Open Access | ||
Notes | São Paulo Research Foundation, 2012/50680-5 ; National Counsel of Technological and Scientific Development, 459270/2014-1 ; We are thankful for the financial support received from the São Paulo Research Foundation (FAPESP) (grant no. 2012/50680-5) and from the National Counsel of Technological and Scientific Development (CNPq) (grant no. 459270/2014-1). MCO acknowledges UFABC for the Master's scholarship granted. | Approved | Most recent IF: 2.402 | ||
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PLASMANT @ plasmant @c:irua:163477 | Serial | 5374 | ||
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Author | Ghasemitarei, M.; Yusupov, M.; Razzokov, J.; Shokri, B.; Bogaerts, A. | ||||
Title | Effect of oxidative stress on cystine transportation by xC‾ antiporter | Type | A1 Journal article | ||
Year | 2019 | Publication | Archives of biochemistry and biophysics | Abbreviated Journal | Arch Biochem Biophys |
Volume | 674 | Issue | Pages | 108114 | |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | We performed computer simulations to investigate the effect of oxidation on the extracellular cystine (CYC) uptake by the xC− antiporter. The latter is important for killing of cancer cells. Specifically, applying molecular dynamics (MD) simulations we studied the transport of CYC across xCT, i.e., the light subunit of the xC− antiporter, in charge of bidirectional transport of CYC and glutamate. We considered the outward facing (OF) configuration of xCT, and to study the effect of oxidation, we modified the Cys327 residue, located in the vicinity of the extracellular milieu, to cysteic acid (CYO327). Our computational results showed that oxidation of Cys327 results in a free energy barrier for CYC translocation, thereby blocking the access of CYC to the substrate binding site of the OF system. The formation of the energy barrier was found to be due to the conformational changes in the channel. Analysis of the MD trajectories revealed that the reorganization of the side chains of the Tyr244 and CYO327 residues play a critical role in the OF channel blocking. Indeed, the calculated distance between Tyr244 and either Cys327 or CYO327 showed a narrowing of the channel after oxidation. The obtained free energy barrier for CYC translocation was found to be 33.9kJmol−1, indicating that oxidation of Cys327, by e.g., cold atmospheric plasma, is more effective in inhibiting the xC− antiporter than in the mutation of this amino acid to Ala (yielding a barrier of 32.4kJmol−1). The inhibition of the xC− antiporter may lead to Cys starvation in some cancer cells, eventually resulting in cancer cell death. | ||||
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Language | Wos | 000525439700011 | Publication Date | 2019-09-23 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0003-9861 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 3.165 | Times cited | Open Access | ||
Notes | Ministry of Science, Research and Technology of Iran; University of Antwerp; Research Foundation − Flanders, 1200219N ; Universiteit Antwerpen; Hercules Foundation; Flemish Government; UA; M. G. acknowledges funding from the Ministry of Science, Research and Technology of Iran and from the University of Antwerp in Belgium. M. Y. gratefully acknowledges financial support from the Research Foundation − Flanders (FWO), grant number 1200219N. 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. Finally, we thank A. S. Mashayekh Esfehan and A. Mohseni for their important comments on the manuscript. | Approved | Most recent IF: 3.165 | ||
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PLASMANT @ plasmant @c:irua:163474 | Serial | 5372 | ||
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Author | Vermeiren, V.; Bogaerts, A. | ||||
Title | Improving the Energy Efficiency of CO2Conversion in Nonequilibrium Plasmas through Pulsing | Type | A1 Journal article | ||
Year | 2019 | Publication | The journal of physical chemistry: C : nanomaterials and interfaces | Abbreviated Journal | J Phys Chem C |
Volume | 123 | Issue | 29 | Pages | 17650-17665 |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Nonequilibrium plasmas offer a pathway for energy-efficient CO2 conversion through vibrationally induced dissociation. However, the efficiency of this pathway is limited by a rise in gas temperature, which increases vibrational−translational (VT) relaxation and quenches the vibrational levels. Therefore, we investigate here the effect of plasma pulsing on the VT nonequilibrium and on the CO2 conversion by means of a zerodimensional chemical kinetics model, with self-consistent gas temperature calculation. Specifically, we show that higher energy efficiencies can be reached by correctly tuning the plasma pulse and interpulse times. The ideal plasma pulse time corresponds to the time needed to reach the highest vibrational temperature. In addition, the highest energy efficiencies are obtained with long interpulse times, that is, ≥0.1 s, in which the gas temperature can entirely drop to room temperature. Furthermore, additional cooling of the reactor walls can give higher energy efficiencies at shorter interpulse times of 1 ms. Finally, our model shows that plasma pulsing can significantly improve the energy efficiency at low reduced electric fields (50 and 100 Td, typical for microwave and gliding arc plasmas) and intermediate ionization degrees (5 × 10−7 and 10−6). | ||||
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Language | Wos | 000477785000003 | Publication Date | 2019-07-25 | |
Series Editor | Series Title | Abbreviated Series Title | |||
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ISSN | 1932-7447 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 4.536 | Times cited | 1 | Open Access | |
Notes | Fonds Wetenschappelijk Onderzoek, G.0383.16N ; This research was supported by the FWO project (grant G.0383.16N). The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UAntwerpen), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI), and the UAntwerpen. We also like to thank N. Britun (ChIPS) for the interesting discussions. | Approved | Most recent IF: 4.536 | ||
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PLASMANT @ plasmant @c:irua:161621 | Serial | 5289 | ||
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Author | Gorbanev, Y.; Privat-Maldonado, A.; Bogaerts, A. | ||||
Title | Analysis of Short-Lived Reactive Species in Plasma–Air–Water Systems: The Dos and the Do Nots | Type | A1 Journal Article | ||
Year | 2018 | Publication | Analytical Chemistry | Abbreviated Journal | Anal Chem |
Volume | 90 | Issue | 22 | Pages | 13151-13158 |
Keywords | A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | This Feature addresses the analysis of the reactive species generated by nonthermal atmospheric pressure plasmas, which are widely employed in industrial and biomedical research, as well as first clinical applications. We summarize the progress in detection of plasma-generated short-lived reactive oxygen and nitrogen species in aqueous solutions, discuss the potential and limitations of various analytical methods in plasma−liquid systems, and provide an outlook on the possible future research goals in development of short-lived reactive species analysis methods for a general nonspecialist audience. |
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Language | Wos | 000451246100002 | Publication Date | 2018-11-20 | |
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Series Volume | Series Issue | Edition | |||
ISSN | 0003-2700 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 6.32 | Times cited | 17 | Open Access | Not_Open_Access |
Notes | European Commission, 743151 ; This work was supported by the European Marie Sklodowska- Curie Individual Fellowship within Horizon2020 (“LTPAM”, Grant No. 743151). | Approved | Most recent IF: 6.32 | ||
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PLASMANT @ plasmant @c:irua:156301 | Serial | 5152 | ||
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Author | Vermeiren, V.; Bogaerts, A. | ||||
Title | Supersonic Microwave Plasma: Potential and Limitations for Energy-Efficient CO2Conversion | Type | A1 Journal Article | ||
Year | 2018 | Publication | Journal Of Physical Chemistry C | Abbreviated Journal | J Phys Chem C |
Volume | 122 | Issue | 45 | Pages | 25869-25881 |
Keywords | A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | Supersonic flows provide a high thermodynamic nonequilibrium, which is crucial for energy-efficient conversion of CO 2 in microwave plasmas and are therefore of great interest. However, the effect of the flow on the chemical reactions is poorly understood. In this work, we present a combined flow and plasma chemical kinetics model of a microwave CO 2 plasma in a Laval nozzle setup. The effects of the flow field on the different dissociation and recombination mechanisms, the vibrational distribution, and the vibrational transfer mechanism are discussed. In addition, the effect of experimental parameters, like position of power deposition, outlet pressure, and specific energy input, on the CO 2 conversion and energy efficiency is examined. The short residence time of the gas in the plasma region, the shockwave, and the maximum critical heat, and thus power, that can be added to the flow to avoid thermal choking are the main obstacles to reaching high energy efficiencies. |
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000451101400016 | Publication Date | 2018-11-15 | |
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 | 5 | Open Access | Not_Open_Access |
Notes | Fonds Wetenschappelijk Onderzoek, G.0383.16N ; | Approved | Most recent IF: 4.536 | ||
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PLASMANT @ plasmant @c:irua:155412 | Serial | 5070 | ||
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Author | Fuchs, J.; Aghaei, M.; Schachel, T.D.; Sperling, M.; Bogaerts, A.; Karst, U. | ||||
Title | Impact of the Particle Diameter on Ion Cloud Formation from Gold Nanoparticles in ICPMS | Type | A1 Journal article | ||
Year | 2018 | Publication | Analytical chemistry | Abbreviated Journal | Anal Chem |
Volume | 90 | Issue | 17 | Pages | 10271-10278 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | The unique capabilities of microsecond dwell time (DT) single-particle inductively coupled plasma mass spectrometry (spICPMS) were utilized to characterize the cloud of ions generated from the introduction of suspensions of gold nanoparticles (AuNPs) into the plasma. A set of narrowly distributed particles with diameters ranging from 15.4 to 100.1 nm was synthesized and characterized according to established protocols. Statistically significant numbers of the short transient spICPMS events were evaluated by using 50 μs DT for their summed intensity, maximum intensity, and duration, of which all three were found to depend on the particle diameter. The summed intensity increases from 10 to 1661 counts and the maximum intensity from 6 to 309 counts for AuNPs with diameters from 15.4 to 83.2 nm. The event duration rises from 322 to 1007 μs upon increasing AuNP diameter. These numbers represent a comprehensive set of key data points of the ion clouds generated in ICPMS from AuNPs. The extension of event duration is of high interest to appoint the maximum possible particle number concentration at which separation of consecutive events in spICPMS can still be achieved. Moreover, the combined evaluation of all above-mentioned ion cloud characteristics can explain the regularly observed prolonged single-particle events. The transport and ionization behavior of AuNPs in the ICP was also computationally modeled to gain insight into the size-dependent signal generation. The simulated data reveals that the plasma temperature, and therefore the point of ionization of the particles, is the same for all diameters. However, the maximum number density of Au+, as well as the extent of the ion cloud, depends on the particle diameter, in agreement with the experimental data, and it provides an adequate explanation for the observed ion cloud characteristics. | ||||
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Language | Wos | 000444060600028 | Publication Date | 2018-09-04 | |
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Series Volume | Series Issue | Edition | |||
ISSN | 0003-2700 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 6.32 | Times cited | 5 | Open Access | OpenAccess |
Notes | We thank Dr. Harald Rösner from the Institute of Materials Physics of the University of Münster for the TEM imaging. | Approved | Most recent IF: 6.32 | ||
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PLASMANT @ plasmant @c:irua:153651 | Serial | 5057 | ||
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