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Author | Maerivoet, S.; Wanten, B.; De Meyer, R.; Van Hove, M.; Van Alphen, S.; Bogaerts, A. | ||||
Title | Effect of O2on Plasma-Based Dry Reforming of Methane: Revealing the Optimal Gas Composition via Experiments and Modeling of an Atmospheric Pressure Glow Discharge | Type | A1 Journal Article | ||
Year | 2024 | Publication | ACS Sustainable Chemistry & Engineering | Abbreviated Journal | ACS Sustainable Chem. Eng. |
Volume | 12 | Issue | 30 | Pages | 11419-11434 |
Keywords | A1 Journal Article; plasma-based conversion, thermal plasma, syngas production, CO2 conversion, CH4 conversio; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | Plasma technology is gaining increasing interest for the conversion of greenhouse gases, such as CO2 and CH4, into value-added chemicals using (renewable) electricity. In this paper, we study the effect of O2 addition to the combined conversion of CO2 and CH4 in an atmospheric pressure glow discharge plasma. This process is called “oxidative CO2 reforming of methane”, and we search for the optimal gas mixing ratio in terms of conversion, energy cost, product output and plasma stability. A mixing ratio of 42.5:42.5:15 CO2/CH4/O2 yields the best performance, with a CO2 and CH4 conversion of 50 and 74%, respectively, and an energy cost as low as 2 eV molecule−1 (corresponding to 7.9 kJ L−1 and 190 kJ mol−1), i.e., clearly below the target defined to be competitive with other technologies. The syngas components (CO and H2) are the most important products, with a syngas ratio, H2/CO, being 0.8. Plasma destabilization at high CH4 fractions due to solid carbon formation is the limiting factor for further improving this syngas ratio. The solid carbon material is found to be contaminated with steel particles originating from the electrode material, rendering it unappealing as a side product. Therefore, O2 addition helps to remove the carbon formation. Besides the experiments, we developed a 2D axisymmetric fluid dynamics model, which can successfully predict the experimental trends in conversion, product composition and temperatures, while providing unique insights in the formation of CxHy species. | ||||
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Language | Wos | https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=brocade2&SrcAuth=WosAPI&KeyUT=WOS:001280 | Publication Date | 2024-07-29 | |
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Series Volume | Series Issue | Edition | |||
ISSN | 2168-0485 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 8.4 | Times cited | Open Access | ||
Notes | Universiteit Antwerpen; Fonds Wetenschappelijk Onderzoek, 40007511 G0I1822N ; H2020 European Research Council, 810182 ; | Approved | Most recent IF: 8.4; 2024 IF: 5.951 | ||
Call Number | PLASMANT @ plasmant @c:irua:207488 | Serial | 9257 | ||
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Author | Vertongen, R.; De Felice, G.; van den Bogaard, H.; Gallucci, F.; Bogaerts, A.; Li, S. | ||||
Title | Sorption-Enhanced Dry Reforming of Methane in a DBD Plasma Reactor for Single-Stage Carbon Capture and Utilization | Type | A1 Journal Article | ||
Year | 2024 | Publication | ACS Sustainable Chemistry & Engineering | Abbreviated Journal | ACS Sustainable Chem. Eng. |
Volume | 12 | Issue | 29 | Pages | 10841-10853 |
Keywords | A1 Journal Article; plasma, dry reforming of methane, dielectric barrier discharge, sorbent, carbon capture and utilization, zeolite; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | Plasma−sorbent systems are a novel technology for single-stage carbon capture and utilization (CCU), where the plasma enables the desorption of CO2 from a sorbent and the simultaneous conversion to CO. In this study, we test the flexibility of a plasma−sorbent system in a single unit, specifically for sorption-enhanced dry reforming of methane (DRM). The experimental results indicate the selective adsorption of CO2 by the sorbent zeolite 5A in the first step, and CH4 addition during the plasma-based desorption of CO2 enables DRM to various value-added products in the second step, such as H2, CO, hydrocarbons, and the byproduct H2O. Furthermore, our work also demonstrates that zeolite has the potential to increase the conversion of CO2 and CH4, attributed to its capability to capture H2O. Aside from the notable carbon deposition, material analysis shows that the zeolite remains relatively stable under plasma exposure. | ||||
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Language | Wos | Publication Date | 2024-07-22 | ||
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ISSN | 2168-0485 | ISBN | Additional Links | ||
Impact Factor | 8.4 | Times cited | Open Access | ||
Notes | Fonds Wetenschappelijk Onderzoek, 110221N V404823N ; H2020 European Research Council, 810182 ; | Approved | Most recent IF: 8.4; 2024 IF: 5.951 | ||
Call Number | PLASMANT @ plasmant @ | Serial | 9264 | ||
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Author | Li, S.; Sun, J.; Gorbanev, Y.; van’t Veer, K.; Loenders, B.; Yi, Y.; Kenis, T.; Chen, Q.; Bogaerts, A. | ||||
Title | Plasma-Assisted Dry Reforming of CH4: How Small Amounts of O2Addition Can Drastically Enhance the Oxygenate Production─Experiments and Insights from Plasma Chemical Kinetics Modeling | Type | A1 Journal Article | ||
Year | 2023 | Publication | ACS Sustainable Chemistry & Engineering | Abbreviated Journal | ACS Sustainable Chem. Eng. |
Volume | 11 | Issue | 42 | Pages | 15373-15384 |
Keywords | A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | Plasma-based dry reforming of methane (DRM) into high-value-added oxygenates is an appealing approach to enable otherwise thermodynamically unfavorable chemical reactions at ambient pressure and near room temperature. However, it suffers from coke deposition due to the deep decomposition of CH4. In this work, we assess the DRM performance upon O2 addition, as well as varying temperature, CO2/CH4 ratio, discharge power, and gas residence time, for optimizing oxygenate production. By adding O2, the main products can be shifted from syngas (CO + H2) toward oxygenates. Chemical kinetics modeling shows that the improved oxygenate production is due to the increased concentration of oxygen-containing radicals, e.g., O, OH, and HO2, formed by electron impact dissociation [e + O2 → e + O + O/O(1D)] and subsequent reactions with H atoms. Our study reveals the crucial role of oxygen-coupling in DRM aimed at oxygenates, providing practical solutions to suppress carbon deposition and at the same time enhance the oxygenates production in plasma-assisted DRM. |
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Language | Wos | 001082603900001 | Publication Date | 2023-10-23 | |
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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 | Not_Open_Access | |
Notes | Fonds Wetenschappelijk Onderzoek, S001619N ; China Scholarship Council, 202006060029 ; National Natural Science Foundation of China, 21975018 ; H2020 European Research Council, 810182 ; | Approved | Most recent IF: 8.4; 2023 IF: 5.951 | ||
Call Number | PLASMANT @ plasmant @c:irua:201013 | Serial | 8966 | ||
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Author | Engelmann, Y.; van ’t Veer, K.; Gorbanev, Y.; Neyts, E.C.; Schneider, W.F.; Bogaerts, A. | ||||
Title | Plasma Catalysis for Ammonia Synthesis: A Microkinetic Modeling Study on the Contributions of Eley–Rideal Reactions | Type | A1 Journal Article;Plasma catalysis | ||
Year | 2021 | Publication | Acs Sustainable Chemistry & Engineering | Abbreviated Journal | Acs Sustain Chem Eng |
Volume | 9 | Issue | 39 | Pages | 13151-13163 |
Keywords | A1 Journal Article;Plasma catalysis; Eley−Rideal reactions; Volcano plots; Vibrational excitation; Radical reactions; Dielectric barrier discharge; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | Plasma catalysis is an emerging new technology for the electrification and downscaling of NH3 synthesis. Increasing attention is being paid to the optimization of plasma catalysis with respect to the plasma conditions, the catalyst material, and their mutual interaction. In this work we use microkinetic models to study how the total conversion process is impacted by the combination of different plasma conditions and transition metal catalysts. We study how plasma-generated radicals and vibrationally excited N2 (present in a dielectric barrier discharge plasma) interact with the catalyst and impact the NH3 turnover frequencies (TOFs). Both filamentary and uniform plasmas are studied, based on plasma chemistry models that provided plasma phase speciation and vibrational distribution functions. The Langmuir−Hinshelwood reaction rate coefficients (i.e., adsorption reactions and subsequent reactions among adsorbates) are determined using conventional scaling relations. An additional set of Eley−Rideal reactions (i.e., direct reactions of plasma radicals with adsorbates) was added and a sensitivity analysis on the assumed reaction rate coefficients was performed. We first show the impact of different vibrational distribution functions on the catalytic dissociation of N2 and subsequent production of NH3, and we gradually include more radical reactions, to illustrate the contribution of these species and their corresponding reaction pathways. Analysis over a large range of catalysts indicates that different transition metals (metals such as Rh, Ni, Pt, and Pd) optimize the NH3TOFs depending on the population of the vibrational levels of N2. At higher concentrations of plasma-generated radicals, the NH3 TOFs become less dependent on the catalyst material, due to radical adsorptions on the more noble catalysts and Eley−Rideal reactions on the less noble catalysts. | ||||
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Language | Wos | 000705367800004 | Publication Date | 2021-10-04 | |
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 | 5.951 | Times cited | Open Access | OpenAccess | |
Notes | Basic Energy Sciences, DE-SC0021107 ; Vlaamse regering, HBC.2019.0108 ; H2020 European Research Council, 810182 ; Methusalem project – University of Antwerp; Excellence of science FWO-FNRS, GoF9618n ; TOP-BOF – University of Antwerp; DOCPRO3 – University of Antwerp; We acknowledge the financial support from the DOC-PRO3, the TOP-BOF, and the Methusalem project of the University of Antwerp, as well as from the European Research Council (ERC) (grant agreement No, 810182−SCOPE ERC Synergy project), under the European Union’s Horizon 2020 research and innovation programme, the Flemish Government through the Moonshot cSBO project P2C (HBC.2019.0108), and the Excellence of Science FWO-FNRS project (FWO grant ID GoF9618n, EOS ID 30505023). 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), 13162 | Approved | Most recent IF: 5.951 | ||
Call Number | PLASMANT @ plasmant @c:irua:182482 | Serial | 6811 | ||
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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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Language | Wos | 000548456600013 | Publication Date | 2020-07-06 | |
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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 | ||
Call Number | 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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Language | Wos | 000526884000025 | Publication Date | 2020-04-20 | |
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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 | ||
Call Number | PLASMANT @ plasmant @c:irua:169228 | Serial | 6366 | ||
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Author | Gorbanev, Y.; Vervloessem, E.; Nikiforov, A.; Bogaerts, A. | ||||
Title | Nitrogen fixation with water vapor by nonequilibrium plasma : toward sustainable ammonia production | Type | A1 Journal article | ||
Year | 2020 | Publication | Acs Sustainable Chemistry & Engineering | Abbreviated Journal | Acs Sustain Chem Eng |
Volume | 8 | Issue | 7 | Pages | 2996-3004 |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Ammonia is a crucial nutrient used for plant growth and as a building block in the pharmaceutical and chemical industry, produced via nitrogen fixation of the ubiquitous atmospheric N2. Current industrial ammonia production relies heavily on fossil resources, but a lot of work is put into developing nonfossil-based pathways. Among these is the use of nonequilibrium plasma. In this work, we investigated water vapor as a H source for nitrogen fixation into NH3 by nonequilibrium plasma. The highest selectivity toward NH3 was observed with low amounts of added H2O vapor, but the highest production rate was reached at high H2O vapor contents. We also studied the role of H2O vapor and of the plasma-exposed liquid H2O in nitrogen fixation by using isotopically labeled water to distinguish between these two sources of H2O. We show that added H2O vapor, and not liquid H2O, is the main source of H for NH3 generation. The studied catalyst- and H2-free method offers excellent selectivity toward NH3 (up to 96%), with energy consumption (ca. 95–118 MJ/mol) in the range of many plasma-catalytic H2-utilizing processes. | ||||
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Language | Wos | 000516665500045 | Publication Date | 2020-02-03 | |
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ISSN | 2168-0485 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.4 | Times cited | 14 | Open Access | |
Notes | ; This research was supported by the Excellence of Science FWO-FNRS project (FWO grant ID GoF9618n, EOS ID 30505023), the Catalisti Moonshot project P2C, and the Methusalem project of the University of Antwerp. ; | Approved | Most recent IF: 8.4; 2020 IF: 5.951 | ||
Call Number | UA @ admin @ c:irua:167134 | Serial | 6568 | ||
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