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| Author | Vervloessem, E.; Gorbanev, Y.; Nikiforov, A.; De Geyter, N.; Bogaerts, A. | ||||
| Title | Sustainable NOxproduction from air in pulsed plasma: elucidating the chemistry behind the low energy consumption | Type | A1 Journal article | ||
| Year | 2022 | Publication | Green Chemistry | Abbreviated Journal | Green Chem |
| Volume | 24 | Issue | 2 | Pages | 916-929 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | N-Based fertilisers are paramount to support our still-growing world population. Current industrial N<sub>2</sub>fixation is heavily fossil fuel-dependent, therefore, a lot of work is put into the development of fossil-free pathways. Plasma technology offers a fossil-free and flexible method for N<sub>2</sub>fixation that is compatible with renewable energy sources. We present here a pulsed plasma jet for direct NO<sub><italic>x</italic></sub>production from air. The pulsed power allows for a record-low energy consumption (EC) of 0.42 MJ (mol N)<sup>−1</sup>. This is the lowest reported EC in plasma-based N<sub>2</sub>fixation at atmospheric pressure thus far. We compare our experimental data with plasma chemistry modelling, and obtain very good agreement. Hence, we can use our model to explain the underlying mechanisms responsible for this low EC. The pulsed power and the corresponding pulsed gas temperature are the reason for the very low EC: they provide a strong vibrational–translational non-equilibrium and promote the non-thermal Zeldovich mechanism. This insight is important for the development of the next generation of plasma sources for energy-efficient NO<sub><italic>x</italic></sub>production. | ||||
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| Language | Wos | 000739578400001 | Publication Date | 2021-12-22 | |
| 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 | Not_Open_Access | |
| Notes | H2020 European Research Council, grant agreement no. 810182 – SCOPE ERC Synergy project ; Herculesstichting; Fonds Wetenschappelijk Onderzoek, EOS ID 30505023 FWO grant ID GoF9618n ; Universiteit Antwerpen; This research was supported by the Excellence of Science FWO-FNRS project (NITROPLASM, FWO grant ID GoF9618n, EOS ID 30505023), the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement no. 810182 – SCOPE ERC Synergy project), and through long-term structural funding (Methusalem). 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 thank E. H. Choi and coworkers from the Plasma Bioscience Research Center (Korea) for providing the Soft Jet plasma source, as well as K. van’t Veer and C. Verheyen for the fruitful discussion on the electron loss fraction calculations. The graphical abstract was designed using resources from Flaticon.com. | Approved | Most recent IF: 9.8 | ||
| Call Number | PLASMANT @ plasmant @c:irua:185450 | Serial | 6906 | ||
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| Author | Borah, R.; Verbruggen, S.W. | ||||
| Title | Effect of size distribution, skewness and roughness on the optical properties of colloidal plasmonic nanoparticles | Type | A1 Journal article | ||
| Year | 2022 | Publication | Colloids and surfaces: A: physicochemical and engineering aspects | Abbreviated Journal | Colloid Surface A |
| Volume | 640 | Issue | Pages | 128521 | |
| Keywords | A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL) | ||||
| Abstract | It is a generally accepted idea that the particle size distribution strongly affects the optical spectra of colloidal plasmonic nanoparticles. It is often quoted as one of the main reasons while explaining the mismatch between the theoretical and experimental optical spectra of such nanoparticles. In this work, these aspects are critically analyzed by means of a bottom up statistical approach that considers variables such as mean, standard deviation and skewness of the nanoparticle size distribution independently from one another. By assuming normal and log-normal distributions of the particle size, the effect of the statistical parameters on the Mie analytical optical spectra of colloidal nanoparticles was studied. The effect of morphology was also studied numerically in order to understand to what extent it can play a role. It is our finding that the particle polydispersity, skewness and surface morphology in fact only weakly impact the optical spectra. While, the selection of suitable optical constants with regard to the crystallinity of the nanoparticles is a far more influential factor for correctly predicting both the plasmon band position and the plasmon bandwidth in theoretical simulations of the optical spectra. It is shown that the mean particle size can be correctly estimated directly from the plasmon band position, as it is the mean that determines the resonance wavelength. The standard deviation can on the other hand be estimated from the intensity distribution data obtained from dynamic light scattering experiments. The results reported herein clear the ambiguity around particle size distribution and optical response of colloidal plasmonic nanoparticles. | ||||
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| Publisher | Elservier | Place of Publication | Editor | ||
| Language | Wos | 000765946900002 | Publication Date | 2022-02-04 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 0927-7757 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 5.2 | Times cited | Open Access | OpenAccess | |
| Notes | Approved | Most recent IF: 5.2 | |||
| Call Number | DuEL @ duel @c:irua:185704 | Serial | 6908 | ||
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| Author | Mallick, S.; Zhang, W.; Batuk, M.; Gibbs, A.S.; Hadermann, J.; Halasyamani, P.S.; Hayward, M.A. | ||||
| Title | The crystal and defect structures of polar KBiNb2O7 | Type | A1 Journal article | ||
| Year | 2022 | Publication | Journal of the Chemical Society : Dalton transactions | Abbreviated Journal | Dalton T |
| Volume | 51 | Issue | 5 | Pages | 1866-1873 |
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
| Abstract | KBiNb2O7 was prepared from RbBiNb2O7 by a sequence of cation exchange reactions which first convert RbBiNb2O7 to LiBiNb2O7, before KBiNb2O7 is formed by a further K-for-Li cation exchange. A combination of neutron, synchrotron X-ray and electron diffraction data reveal that KBiNb2O7 adopts a polar, layered, perovskite structure (space group A11m) in which the BiNb2O7 layers are stacked in a (0, ½, z) arrangement, with the K+ cations located in half of the available 10-coordinate interlayer cation sites. The inversion symmetry of the phase is broken by a large displacement of the Bi3+ cations parallel to the y-axis. HAADF-STEM images reveal that KBiNb2O7 exhibits frequent stacking faults which convert the (0. ½, z) layer stacking to (½, 0, z) stacking and vice versa, essentially switching the x- and y-axes of the material. By fitting the complex diffraction peak shape of the SXRD data collected from KBiNb2O7 it is estimated that each layer has approximately an ~11% chance of being defective – a high level which is attributed to the lack of cooperative NbO6 tilting in the material, which limits the lattice strain associated with each fault. | ||||
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| Language | Wos | 000741540300001 | Publication Date | 2022-01-05 | |
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| ISSN | 1477-9226 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 4 | Times cited | Open Access | OpenAccess | |
| Notes | Experiments at the Diamond Light Source were performed as part of the Block Allocation Group award “Oxford/Warwick Solid State Chemistry BAG to probe composition-structure-property relationships in solids” (EE18786). Experiments at the ISIS pulsed neutron facility were supported by a beam time allocation from the STFC (RB 2000148). SM thanks Somerville College for an Oxford Ryniker Lloyd scholarship. PSH and WZ thank the National Science Foundation (DMR-2002319) for support. | Approved | Most recent IF: 4 | ||
| Call Number | EMAT @ emat @c:irua:185504 | Serial | 6951 | ||
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| Author | Salzmann, B.B.V.; Wit, J. de; Li, C.; Arenas-Esteban, D.; Bals, S.; Meijerink, A.; Vanmaekelbergh, D. | ||||
| Title | Two-Dimensional CdSe-PbSe Heterostructures and PbSe Nanoplatelets: Formation, Atomic Structure, and Optical Properties | Type | A1 Journal article | ||
| Year | 2022 | Publication | The journal of physical chemistry: C : nanomaterials and interfaces | Abbreviated Journal | J Phys Chem C |
| Volume | 126 | Issue | 3 | Pages | 1513-1522 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
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| Language | Wos | 000744909200001 | Publication Date | 2022-01-27 | |
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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 | 12 | Open Access | OpenAccess |
| Notes | H. Meeldijk is kindly acknowledged for helping with electron microscopy at Utrecht University. T. Prins is kindly acknowledged for useful discussions. B.B.V.S. and D.V. acknowledge the Dutch NWO for financial support via the TOP-ECHO Grant No. 715.016.002. D.V. acknowledges financial support from the European ERC Council, ERC Advanced Grant 692691 “First Step”. J.W. and A.M. acknowledge financial support from the project CHEMIE.PGT.2019.004 of TKI/ Topsector Chemie, which is partly financed by the Dutch NWO. S.B, C.L., and D.A.E. acknowledge financial support from the European ERC Council, ERC Consolidator Grant realnano No. 815128. This project has received funding from the European Union’s Horizon 2020 research and innovation program under Grant No. 731019 (EUSMI). sygmaSB | Approved | Most recent IF: 3.7 | ||
| Call Number | EMAT @ emat @c:irua:185454 | Serial | 6953 | ||
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| Author | Windels, S.; Diefenhardt, T.; Jain, N.; Marquez, C.; Bals, S.; Schlummer, M.; De Vos, D.E. | ||||
| Title | Catalytic upcycling of PVC waste-derived phthalate esters into safe, hydrogenated plasticizers | Type | A1 Journal article | ||
| Year | 2022 | Publication | Green chemistry : cutting-edge research for a greener sustainable future | Abbreviated Journal | Green Chem |
| Volume | 24 | Issue | 2 | Pages | 754-766 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Recycling of end-of-life polyvinyl chloride (PVC) calls for solutions to deal with the vast amounts of harmful phthalate plasticizers that have historically been incorporated in PVC. Here, we report on the upcycling of such waste-extracted phthalate esters into analogues of the much safer diisononyl 1,2-cyclohexanedicarboxylate plasticizer (DINCH), via a catalytic one-pot (trans)esterification-hydrogenation process. For most of the virgin phthalates, Ru/Al2O3 is a highly effective hydrogenation catalyst, yielding >99% ring-hydrogenated products under mild reaction conditions (0.1 mol% Ru, 80 degrees C, 50 bar H-2). However, applying this reaction to PVC-extracted phthalates proved problematic, (1) as benzyl phthalates are hydrogenolyzed to benzoic acids that inhibit the Ru-catalyst, and (2) because impurities in the plasticizer extract (PVC, sulfur) further retard the hydrogenation. These complications were solved by coupling the hydrogenation to an in situ (trans)esterification with a higher alcohol, and by pretreating the extract with an activated carbon adsorbent. In this way, a real phthalate extract obtained from post-consumer PVC waste was eventually completely (>99%) hydrogenated to phthalate-free, cycloaliphatic plasticizers. | ||||
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| Language | Wos | 000726865200001 | Publication Date | 2021-11-30 | |
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| Series Volume | Series Issue | Edition | |||
| ISSN | 1463-9262; 1463-9270 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 9.8 | Times cited | 8 | Open Access | Not_Open_Access |
| Notes | This project has received funding from the European Union’s Horizon 2020 Research and Innovation Programme under grant agreement no. 821366 (programma acronym: Circular Flooring). D. E. D. V. thanks FWO for project funding (SBO project S001819N Triple Cycle); N. J. and S. B. acknowledge the financial support from FWO and FNRS (EOS 30489208). Finally, the authors also thank S. Smolders for assistance with the TGA-MS experiments and D. Paredaens for his experimental contribution | Approved | Most recent IF: 9.8 | ||
| Call Number | UA @ admin @ c:irua:184746 | Serial | 6958 | ||
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| Author | Ghasemitarei, M.; Privat-Maldonado, A.; Yusupov, M.; Rahnama, S.; Bogaerts, A.; Ejtehadi, M.R. | ||||
| Title | Effect of Cysteine Oxidation in SARS-CoV-2 Receptor-Binding Domain on Its Interaction with Two Cell Receptors: Insights from Atomistic Simulations | Type | A1 Journal article | ||
| Year | 2022 | Publication | Journal Of Chemical Information And Modeling | Abbreviated Journal | J Chem Inf Model |
| Volume | 62 | Issue | 1 | Pages | 129-141 |
| Keywords | A1 Journal article; Pharmacology. Therapy; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Binding of the SARS-CoV-2 S-glycoprotein to cell receptors is vital for the entry of the virus into cells and subsequent infection. ACE2 is the main cell receptor for SARS-CoV-2, which can attach to the C-terminal receptor-binding domain (RBD) of the SARS-CoV-2 S-glycoprotein. The GRP78 receptor plays an anchoring role, which attaches to the RBD and increases the chance of other RBDs binding to ACE2. Although high levels of reactive oxygen and nitrogen species (RONS) are produced during viral infections, it is not clear how they affect the RBD structure and its binding to ACE2 and GRP78. In this research, we apply molecular dynamics simulations to study the effect of oxidation of the highly reactive cysteine (Cys) amino acids of the RBD on its binding to ACE2 and GRP78. The interaction energy of both ACE2 and GRP78 with the whole RBD, as well as with the RBD main regions, is compared in both the native and oxidized RBDs. Our results show that the interaction energy between the oxidized RBD and ACE2 is strengthened by 155 kJ/mol, increasing the binding of the RBD to ACE2 after oxidation. In addition, the interaction energy between the RBD and GRP78 is slightly increased by 8 kJ/mol after oxidation, but this difference is not significant. Overall, these findings highlight the role of RONS in the binding of the SARS-CoV-2 S-glycoprotein to host cell receptors and suggest an alternative mechanism by which RONS could modulate the entrance of viral particles into the cells. | ||||
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| Language | Wos | 000740019000001 | Publication Date | 2022-01-10 | |
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| Series Volume | Series Issue | Edition | |||
| ISSN | 1549-9596 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 5.6 | Times cited | Open Access | Not_Open_Access | |
| Notes | Fonds Wetenschappelijk Onderzoek, 1200219N ; Binding of the SARS-CoV-2 S-glycoprotein to cell receptors is vital for the entry of the virus into cells and subsequent infection. ACE2 is the main cell receptor for SARS-CoV-2, which can attach to the C-terminal receptor-binding domain (RBD) of the SARS-CoV-2 S-glycoprotein. The GRP78 receptor plays an anchoring role, which attaches to the RBD and increases the chance of other RBDs binding to ACE2. Although high levels of reactive oxygen and nitrogen species (RONS) are produced during viral infections, it is not clear how they affect the RBD structure and its binding to ACE2 and GRP78. In this research, we apply molecular dynamics simulations to study the effect of oxidation of the highly reactive cysteine (Cys) amino acids of the RBD on its binding to ACE2 and GRP78. The interaction energy of both ACE2 and GRP78 with the whole RBD, as well as with the RBD main regions, is compared in both the native and oxidized RBDs. Our results show that the interaction energy between the oxidized RBD and ACE2 is strengthened by 155 kJ/mol, increasing the binding of the RBD to ACE2 after oxidation. In addition, the interaction energy between the RBD and GRP78 is slightly increased by 8 kJ/mol after oxidation, but this difference is not significant. Overall, these findings highlight the role of RONS in the binding of the SARS-CoV-2 S-glycoprotein to host cell receptors and suggest an alternative mechanism by which RONS could modulate the entrance of viral particles into the cells. | Approved | Most recent IF: 5.6 | ||
| Call Number | PLASMANT @ plasmant @c:irua:185485 | Serial | 7050 | ||
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| Author | Girard-Sahun, F.; Biondo, O.; Trenchev, G.; van Rooij, G.; Bogaerts, A. | ||||
| Title | Carbon bed post-plasma to enhance the CO2 conversion and remove O2 from the product stream | Type | A1 Journal article | ||
| Year | 2022 | Publication | Chemical Engineering Journal | Abbreviated Journal | Chem Eng J |
| Volume | 442 | Issue | Pages | 136268 | |
| Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | CO2 conversion by plasma technology is gaining increasing interest. We present a carbon (charcoal) bed placed after a Gliding Arc Plasmatron (GAP) reactor, to enhance the CO2 conversion, promote O/O2 removal and in crease the CO fraction in the exhaust mixture. By means of an innovative (silo) system, the carbon is constantly supplied, to avoid carbon depletion upon reaction with O/O2. Using this carbon bed, the CO2 conversion is enhanced by almost a factor of two (from 7.6 to 12.6%), while the CO concentration even increases by a factor of three (from 7.2 to 21.9%), and O2 is completely removed from the exhaust mixture. Moreover, the energy ef ficiency of the conversion process drastically increases from 27.9 to 45.4%, and the energy cost significantly drops from 41.9 to 25.4 kJ.L− 1. We also present the temperature as a function of distance from the reactor outlet, as well as the CO2, CO and O2 concentrations and the temperature in the carbon bed as a function of time, which is important for understanding the underlying mechanisms. Indeed, these time-resolved measurements reveal that the initial enhancements in CO2 conversion and in CO concentration are not maintained in our current setup. Therefore, we present a model to study the gasification of carbon with different feed gases (i.e., O2, CO and CO2 separately), from which we can conclude that the oxygen coverage at the surface plays a key role in determining the product composition and the rate of carbon consumption. Indeed, our model insights indicate that the drop in CO2 conversion and in CO concentration after a few minutes is attributed to deactivation of the carbon bed, due to rapid formation of oxygen complexes at the surface. | ||||
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| Language | Wos | 000797716700002 | Publication Date | 0000-00-00 | |
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| ISSN | 1385-8947 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 15.1 | Times cited | Open Access | OpenAccess | |
| Notes | Horizon 2020 Marie Skłodowska-Curie Actions; European Research Council; This research was supported 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) and the European Union’s Horizon 2020 Research and Innovation programme under the Marie Sklodowska-Curie grant agreement No 813393 (PIONEER). The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit | Approved | Most recent IF: 15.1 | ||
| Call Number | PLASMANT @ plasmant @c:irua:188286 | Serial | 7052 | ||
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| Author | Girard-Sahun, F.; Biondo, O.; Trenchev, G.; van Rooij, G.; Bogaerts, A. | ||||
| Title | Carbon bed post-plasma to enhance the CO2 conversion and remove O2 from the product stream | Type | A1 Journal article | ||
| Year | 2022 | Publication | Chemical Engineering Journal | Abbreviated Journal | Chem Eng J |
| Volume | 442 | Issue | Pages | 136268 | |
| Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | CO2 conversion by plasma technology is gaining increasing interest. We present a carbon (charcoal) bed placed after a Gliding Arc Plasmatron (GAP) reactor, to enhance the CO2 conversion, promote O/O2 removal and in crease the CO fraction in the exhaust mixture. By means of an innovative (silo) system, the carbon is constantly supplied, to avoid carbon depletion upon reaction with O/O2. Using this carbon bed, the CO2 conversion is enhanced by almost a factor of two (from 7.6 to 12.6%), while the CO concentration even increases by a factor of three (from 7.2 to 21.9%), and O2 is completely removed from the exhaust mixture. Moreover, the energy ef ficiency of the conversion process drastically increases from 27.9 to 45.4%, and the energy cost significantly drops from 41.9 to 25.4 kJ.L− 1. We also present the temperature as a function of distance from the reactor outlet, as well as the CO2, CO and O2 concentrations and the temperature in the carbon bed as a function of time, which is important for understanding the underlying mechanisms. Indeed, these time-resolved measurements reveal that the initial enhancements in CO2 conversion and in CO concentration are not maintained in our current setup. Therefore, we present a model to study the gasification of carbon with different feed gases (i.e., O2, CO and CO2 separately), from which we can conclude that the oxygen coverage at the surface plays a key role in determining the product composition and the rate of carbon consumption. Indeed, our model insights indicate that the drop in CO2 conversion and in CO concentration after a few minutes is attributed to deactivation of the carbon bed, due to rapid formation of oxygen complexes at the surface. | ||||
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| Language | Wos | 000797716700002 | Publication Date | 0000-00-00 | |
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| ISSN | 1385-8947 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 15.1 | Times cited | Open Access | OpenAccess | |
| Notes | Horizon 2020 Marie Skłodowska-Curie Actions; European Research Council; This research was supported 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) and the European Union’s Horizon 2020 Research and Innovation programme under the Marie Sklodowska-Curie grant agreement No 813393 (PIONEER). 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 R. De Meyer, K. Leyssens and S. Defossé for performing the charcoal characterizations. | Approved | Most recent IF: 15.1 | ||
| Call Number | PLASMANT @ plasmant @c:irua:188286 | Serial | 7053 | ||
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| Author | Hollevoet, L.; Vervloessem, E.; Gorbanev, Y.; Nikiforov, A.; De Geyter, N.; Bogaerts, A.; Martens, J.A. | ||||
| Title | Energy‐Efficient Small‐Scale Ammonia Synthesis Process with Plasma‐enabled Nitrogen Oxidation and Catalytic Reduction of Adsorbed NOx | Type | A1 Journal article | ||
| Year | 2022 | Publication | Chemsuschem | Abbreviated Journal | Chemsuschem |
| Volume | Issue | Pages | |||
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Industrial ammonia production without CO2 emission and with low energy consumption is one of the technological grand challenges of this age. Current Haber-Bosch ammonia mass production processes work with a thermally activated iron catalyst needing high pressure. The need for large volumes of hydrogen gas and the continuous operation mode render electrification of Haber-Bosch plants difficult to achieve. Electrochemical solutions at low pressure and temperature are faced with the problematic inertness of the nitrogen molecule on electrodes. Direct reduction of N2 to ammonia is only possible with very reactive chemicals such as lithium metal, the regeneration of which is energy intensive. Here, the attractiveness of an oxidative route for N2 activation was presented. N2 conversion to NOx in a plasma reactor followed by reduction with H2 on a heterogeneous catalyst at low pressure could be an energy-efficient option for small-scale distributed ammonia production with renewable electricity and without intrinsic CO2 footprint. | ||||
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| Language | Wos | 000772893400001 | Publication Date | 2022-03-25 | |
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| ISSN | 1864-5631 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 8.4 | Times cited | Open Access | OpenAccess | |
| Notes | Vlaamse regering, HBC.2019.0108 ; Vlaamse regering; KU Leuven, C3/20/067 ; We gratefully acknowledge financial support by the Flemish Government through the Moonshot cSBO project P2C (HBC.2019.0108). J.A.M. and A.B. acknowledge the Flemish Government for long-term structural funding (Methusalem). J.A.M. © 2022 Wiley-VCH GmbH | Approved | Most recent IF: 8.4 | ||
| Call Number | PLASMANT @ plasmant @c:irua:187251 | Serial | 7054 | ||
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| Author | Van Alphen, S.; Ahmadi Eshtehardi, H.; O'Modhrain, C.; Bogaerts, J.; Van Poyer, H.; Creel, J.; Delplancke, M.-P.; Snyders, R.; Bogaerts, A. | ||||
| Title | Effusion nozzle for energy-efficient NOx production in a rotating gliding arc plasma reactor | Type | A1 Journal article | ||
| Year | 2022 | Publication | Chemical Engineering Journal | Abbreviated Journal | Chem Eng J |
| Volume | 443 | Issue | Pages | 136529 | |
| Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Plasma-based NOx production is of interest for sustainable N2 fixation, but more research is needed to improve its performance. One of the current limitations is recombination of NO back into N2 and O2 molecules immediately after the plasma reactor. Therefore, we developed a novel so-called “effusion nozzle”, to improve the performance of a rotating gliding arc plasma reactor for NOx production, but the same principle can also be applied to other plasma types. Experiments in a wide range of applied power, gas flow rates and N2/O2 ratios demonstrate an enhancement in NOx concentration by about 8%, and a reduction in energy cost by 22.5%. In absolute terms, we obtain NOx concentrations up to 5.9%, at an energy cost down to 2.1 MJ/mol, which are the best values reported to date in literature. In addition, we developed four complementary models to describe the gas flow, plasma temperature and plasma chemistry, aiming to reveal why the effusion nozzle yields better performance. Our simulations reveal that the effusion nozzle acts as very efficient heat sink, causing a fast drop in gas temperature when the gas molecules leave the plasma, hence limiting the recombination of NO back into N2 and O2. This yields an overall higher NOx concentration than without the effusion nozzle. This immediate quenching right at the end of the plasma makes our effusion nozzle superior to more conventional cooling options, like water cooling In addition, this higher NOx concentration can be obtained at a slightly lower power, because the effusion nozzle allows for the ignition and sustainment of the plasma at somewhat lower power. Hence, this also explains the lower energy cost. Overall, our experimental results and detailed modeling analysis will be useful to improve plasma-based NOx production in other plasma reactors as well. | ||||
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| Language | Wos | 000800010600003 | Publication Date | 0000-00-00 | |
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| ISSN | 1385-8947 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 15.1 | Times cited | Open Access | OpenAccess | |
| Notes | This research was supported by the Excellence of Science FWO-FNRS project (FWO grant ID GoF9618n, EOS ID 30505023), the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No 810182 – SCOPE ERC Synergy project), and through long-term structural funding (Methusalem). 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: 15.1 | ||
| Call Number | PLASMANT @ plasmant @c:irua:188283 | Serial | 7057 | ||
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| Author | Rogolino, A.; Claes, N.; Cizaurre, J.; Marauri, A.; Jumbo-Nogales, A.; Lawera, Z.; Kruse, J.; Sanroman-Iglesias, M.; Zarketa, I.; Calvo, U.; Jimenez-Izal, E.; Rakovich, Y.P.; Bals, S.; Matxain, J.M.; Grzelczak, M. | ||||
| Title | Metal-polymer heterojunction in colloidal-phase plasmonic catalysis | Type | A1 Journal article | ||
| Year | 2022 | Publication | The journal of physical chemistry letters | Abbreviated Journal | J Phys Chem Lett |
| Volume | 13 | Issue | 10 | Pages | 2264-2272 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Plasmonic catalysis in the colloidal phase requires robust surface ligands that prevent particles from aggregation in adverse chemical environments and allow carrier flow from reagents to nanoparticles. This work describes the use of a water-soluble conjugated polymer comprising a thiophene moiety as a surface ligand for gold nanoparticles to create a hybrid system that, under the action of visible light, drives the conversion of the biorelevant NAD+ to its highly energetic reduced form NADH. A combination of advanced microscopy techniques and numerical simulations revealed that the robust metal-polymer heterojunction, rich in sulfonate functional groups, directs the interaction of electron-donor molecules with the plasmonic photocatalyst. The tight binding of polymer to the gold surface precludes the need for conventional transition-metal surface cocatalysts, which were previously shown to be essential for photocatalytic NAD(+) reduction but are known to hinder the optical properties of plasmonic nanocrystals. Moreover, computational studies indicated that the coating polymer fosters a closer interaction between the sacrificial electron-donor triethanolamine and the nanoparticles, thus enhancing the reactivity. | ||||
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| Language | Wos | 000776518000001 | Publication Date | 0000-00-00 | |
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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 | 1 | Open Access | OpenAccess |
| Notes | This work was supported by grant PID2019-111772RB-I00 funded by MCIN/AEI/10.13039/501100011033 and grant IT 1254-19 funded by Basque Government. The authors acknowledge the financial support of the European Commission (EUSMI, Grant 731019). S.B. is grateful to the European Research Council (ERC-CoG-2019 815128). The authors acknowledge the contributions by Dr. Adrian Pedrazo Tardajos related to sample support and electron microscopy experiments.; realnano;sygmaSB | Approved | Most recent IF: 5.7 | ||
| Call Number | UA @ admin @ c:irua:188008 | Serial | 7062 | ||
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| Author | Li, W.; Tong, W.; Yadav, A.; Bladt, E.; Bals, S.; Funston, A.M.; Etheridge, J. | ||||
| Title | Shape control beyond the seeds in gold nanoparticles | Type | A1 Journal article | ||
| Year | 2021 | Publication | Chemistry Of Materials | Abbreviated Journal | Chem Mater |
| Volume | 33 | Issue | 23 | Pages | 9152-9164 |
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
| Abstract | In typical seed-mediated syntheses of metal nanocrystals, the shape of the nanocrystal is determined largely by the seed nucleation environment and subsequent growth environment (where “environment” refers to the chemical environment, including the surfactant and additives). In this approach, crystallinity is typically determined by the seeds, and surfaces are controlled by the environment(s). However, surface energies, and crystallinity, are both influenced by the choice of environment(s). This limits the permutations of crystallinity and surface facets that can be mixed and matched to generate new nanocrystal morphologies. Here, we control post-seed growth to deliberately incorporate twin planes during the growth stage to deliver new final morphologies, including twinned cubes and bipyramids from single-crystal seeds. The nature and number of twin planes, together with surfactant control of facet growth, define the final nanoparticle morphology. Moreover, by breaking symmetry, the twin planes introduce new facet orientations. This additional mechanism opens new routes for the synthesis of different morphologies and facet orientations. | ||||
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| Language | Wos | 000753956100012 | Publication Date | 0000-00-00 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 0897-4756; 1520-5002 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 9.466 | Times cited | 3 | Open Access | Not_Open_Access |
| Notes | This work was supported by the Australian Research Council (ARC) Grants DP160104679 and CE170100026 and used microscopes at the Monash Centre for Electron Microscopy funded by ARC Grants LE0454166, LE110100223, and LE140100104. W.L. thanks the support of the Australian Government Research Training Program (RTP) scholarship. W.T. thanks the Australian Department of Education and Monash University for the IPRS and APA scholarships. E.B. acknowledges financial support and a post-doctoral grant from the Research Foundation Flanders (FWO, Belgium). The authors thank Dr. Matthew Weyland and Dr. Tim Peterson for helpful discussions. A.Y. thanks the support from Post Graduation Publication Award (PPA) scholarship from Monash University. | Approved | Most recent IF: 9.466 | ||
| Call Number | UA @ admin @ c:irua:187229 | Serial | 7065 | ||
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| Author | Canossa, S.; Ferrari, E.; Sippel, P.; Fischer, J.K.H.; Pfattner, R.; Frison, R.; Masino, M.; Mas-Torrent, M.; Lunkenheimer, P.; Rovira, C.; Girlando, A. | ||||
| Title | Tetramethylbenzidine-TetrafluoroTCNQ (TMB-TCNQF(4)) : a narrow-gap semiconducting salt with room-temperature relaxor ferroelectric behavior | Type | A1 Journal article | ||
| Year | 2021 | Publication | Journal Of Physical Chemistry C | Abbreviated Journal | J Phys Chem C |
| Volume | 125 | Issue | 46 | Pages | 25816-25824 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
| Abstract | We present an extension and revision of the spectroscopic and structural data of the mixed-stack charge-transfer (CT) crystal 3,3 ',5,5 '-tetramethylbenzidine-tetrafluorotetracyano-quinodimethane (TMB-TCNQF4), associated with new electric and dielectric measurements. Refinement of synchrotron structural data at low temperature has led to revise the previously reported C2/m structure. The revised structure is P2(1)/m, with two dimerized stacks per unit cell, and is consistent with the low temperature vibrational data. However, polarized Raman data in the low-frequency region also indicate that by increasing temperature above 200 K, the structure presents an increasing degree of disorder, mainly along the stack axis. X-ray diffraction data at room temperature have confirmed that the correct structure is P2(1)/ m -no phase transitions -but did not allow substantiating the presence of disorder. On the other hand, dielectric measurements have evidenced a typical relaxor ferroelectric behavior already at room temperature, with a peak in the real part of dielectric constant epsilon'(T,v) around 200 K and 0.1 Hz. The relaxor behavior is explained in terms of the presence of spin solitons separating domains of opposite polarity that yield to ferroelectric nanodomains. TMB-TCNQF(4) is confirmed to be a narrow-gap band semiconductor (Ea similar to 0.3 eV) with a room-temperature conductivity of similar to 10(-4) Omega(-1) cm(-1). | ||||
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| Language | Wos | 000731170500008 | Publication Date | 0000-00-00 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 1932-7447; 1932-7455 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 4.536 | Times cited | Open Access | Not_Open_Access | |
| Notes | A.G. thanks Prof. Pascale Foury-Leylekian for very helpful discussions about the crystallographic issues. R.F. thanks Prof. Anthony Linden for his help in the X-ray diffraction data collection. J.K.H.F. and P.L. acknowledge funding from the Deutsche Forschungsgemeinschaft (DFG) via the Transregional Collaborative Research Center TRR80 (Augsburg, Munich). R.P. and M.M.-T. acknowledge support from the Marie Curie Cofund, Beatriu de Pinós Fellowships (Grant nos. AGAUR 2017 BP 00064). This work was also supported by the Spanish Ministry project GENESIS PID2019-111682RBI00, the “Severo Ochoa” Programme for Centers of Excellence in R&D (FUNFUTURE, CEX2019-000917-S), and the Generalitat de Catalunya (2017-SGR-918). The Elettra Synchrotron (CNR Trieste) is acknowledged for granting the beamtime at the single-crystal diffraction beamline XRD1 (Proposal ID 20185483). In Parma, the work has benefited from the equipment and support of the COMP-HUB Initiative, funded by the “Departments of Excellence” program of the | Approved | Most recent IF: 4.536 | ||
| Call Number | UA @ admin @ c:irua:184866 | Serial | 7066 | ||
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| Author | Wang, Y.; Chen, Y.; Harding, J.; He, H.; Bogaerts, A.; Tu, X. | ||||
| Title | Catalyst-free single-step plasma reforming of CH4 and CO2 to higher value oxygenates under ambient conditions | Type | A1 Journal article | ||
| Year | 2022 | Publication | Chemical Engineering Journal | Abbreviated Journal | Chem Eng J |
| Volume | 450 | Issue | Pages | 137860 | |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Direct conversion of CH4 and CO2 to liquid fuels and chemicals under mild conditions is appealing for biogas conversion and utilization but challenging due to the inert nature of both gases. Herein, we report a promising plasma process for the catalyst-free single-step conversion of CH4 and CO2 into higher value oxygenates (i.e., methanol, acetic acid, ethanol, and acetone) at ambient pressure and room temperature using a water-cooled dielectric barrier discharge (DBD) reactor, with methanol being the main liquid product. The distribution of liquid products could be tailored by tuning the discharge power, reaction temperature and residence time. Lower discharge powers (10–15 W) and reaction temperatures (5–20 ◦ C) were favourable for the production of liquid products, achieving the highest methanol selectivity of 43% at 5 ◦ C and 15 W. A higher discharge power and reaction temperature, on the other hand, produced more gaseous products, particularly H2 (up to 26% selectivity) and CO (up to 33% selectivity). In addition, varying these process parameters (discharge power, reaction temperature and residence time) resulted in a simultaneous change in key discharge properties, such as mean electron energy (Ee), electron density (ne) and specific energy input (SEI), all of which are essential determiners of plasma chemical reactions. According to the results of artificial neural network (ANN) models, the relative importance of these process parameters and key discharge indicators on reaction performance follows the order: discharge power > reaction temperature > residence time, and SEI > ne > Ee, respectively. This work provides new insights into the contributions and tuning mechanism of multiple parameters for optimizing the reaction performance (e.g., liquid production) in the plasma gas conversion process. | ||||
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| Language | Wos | 000830813300004 | Publication Date | 0000-00-00 | |
| 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 | OpenAccess | |
| Notes | This project received funding from the European Union’s Horizon 2020 research and innovation program under the Marie SklodowskaCurie grant agreement No. 813393. | Approved | Most recent IF: 15.1 | ||
| Call Number | PLASMANT @ plasmant @c:irua:189502 | Serial | 7100 | ||
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| Author | Batuk, M.; Vandemeulebroucke, D.; Ceretti, M.; Paulus, W.; Hadermann, J. | ||||
| Title | Topotactic redox cycling in SrFeO2.5+δ explored by 3D electron diffraction in different gas atmospheres | Type | A1 Journal article | ||
| Year | 2022 | Publication | Journal of materials chemistry A : materials for energy and sustainability | Abbreviated Journal | J Mater Chem A |
| Volume | Issue | Pages | |||
| Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
| Abstract | For oxygen conducting materials applied in solid oxide fuel cells and chemical-looping processes, the understanding of the oxygen diffusion mechanism and the materials’ crystal structure at different stages of the redox reactions is a key parameter to control their performance. In this paper we report the first ever in situ 3D ED experiment in a gas environment and with it uncover the structure evolution of SrFeO2.5 as notably different from that reported from in situ X-ray and in situ neutron powder diffraction studies in gas environments. Using in situ 3D ED on submicron sized single crystals obtained from a high quality monodomain SrFeO2.5 single crystal , we observe the transformation under O2 flow of SrFeO2.5 with an intra- and interlayer ordering of the left and right twisted (FeO4) tetrahedral chains (space group Pcmb) into consecutively SrFeO2.75 with space group Cmmm (at 350°C, 33% O2) and SrFeO3-δ with space group Pm3 ̅m (at 400°C, 100% O2). Upon reduction in H2 flow, the crystals return to the brownmillerite structure with intralayer order, but without regaining the interlayer order of the pristine crystals. Therefore, redox cycling of SrFeO2.5 crystals in O2 and H2 introduces stacking faults into the structure, resulting in an I2/m(0βγ)0s symmetry with variable β. | ||||
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| Language | Wos | 000891928400001 | Publication Date | 0000-00-00 | |
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| ISSN | 2050-7488 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 11.9 | Times cited | Open Access | OpenAccess | |
| Notes | Financial support is acknowledged from the FWO-Hercules fund I003218N ‘Infrastructure for imaging nanoscale processes in gas/vapor or liquid environments’, from the University of Antwerp through grant BOF TOP 38689. This work was supported by the European Commission Horizon 2020 NanED grant number 956099. Financial support from the French National Research Agency (ANR) through the project “Structural induced Electronic Complexity controlled by low temperature Topotactic Reaction” (SECTOR No. ANR-14-CE36- 0006-01) is gratefully acknowledged. | Approved | Most recent IF: 11.9 | ||
| Call Number | EMAT @ emat @c:irua:192325 | Serial | 7229 | ||
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| Author | Wang, J.; Zhang, K.; Kavak, S.; Bals, S.; Meynen, V. | ||||
| Title | Modifying the Stöber Process: Is the Organic Solvent Indispensable? | Type | A1 Journal Article | ||
| Year | 2022 | Publication | Chemistry-A European Journal | Abbreviated Journal | Chem-Eur J |
| Volume | Issue | Pages | |||
| Keywords | A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; | ||||
| Abstract | The Stöber method is one of the most important and fundamental processes for the synthesis of inorganic (nano)materials but has the drawback of using a large amount of organic solvent. Herein, ethanol was used as an example to explore if the organic solvent in a typical Stöber method can be omitted. It was found that ethanol increases the particle size of the obtained silica spheres and aids the formation of uniform silica particles rather than forming a gel. Nevertheless, the results indicated that an organic solvent in the initial synthesis mixture is not indispensable. An initially immiscible synthesis method was discovered, which can replace the organic solvent-based Stöber method to successfully synthesize silica particles with the same size ranges as the original Stöber process without addition of organic solvents. Moreover, this process can be of further value for the extension to synthesis processes of other materials based on the Stöber process. | ||||
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| Language | Wos | 000898283500001 | Publication Date | 2022-12-14 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 0947-6539 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 4.3 | Times cited | 3 | Open Access | OpenAccess |
| Notes | The authors are grateful to Alexander Vansant and Dr. Steven Mullens of VITO for their contributions to the DLS measurements in this paper. J.W acknowledges the State Scholarship funded by the China Scholarship Council (201806060123). K.Z acknowledges the EASiCHEM project funded by the Flemish Strategic Basic Research Program of the Catalisti cluster and Flanders Innovation & Entrepreneurship (HBC.2018.0484). S.K acknowledges the Flemish Fund for Scientific Research (FWO Flanders) through a PhD research grant (1181122N). | Approved | Most recent IF: 4.3 | ||
| Call Number | EMAT @ emat @c:irua:191646 | Serial | 7233 | ||
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| Author | Andersen, Ja.; Holm, Mc.; van 't Veer, K.; Christensen, Jm.; Østberg, M.; Bogaerts, A.; Jensen, Ad. | ||||
| Title | Plasma-catalytic ammonia synthesis in a dielectric barrier discharge reactor: A combined experimental study and kinetic modeling | Type | A1 Journal article | ||
| Year | 2023 | Publication | Chemical engineering journal | Abbreviated Journal | |
| Volume | 457 | Issue | Pages | 141294 | |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Plasma-catalytic ammonia synthesis in a dielectric barrier discharge reactor has emerged as a possible route for electrification of nitrogen fixation. In this study, we use a combination of experiments and a plasma kinetic model to investigate the ammonia synthesis from N2 and H2, both with and without a solid packing material in the plasma zone. The effect of plasma power, feed flow rate, N2:H2 feed ratio, gas residence time, temperature, and packing material (MgAl2O4 alone or impregnated with Co or Ru) on the ammonia synthesis rate were examined in the experiments. The kinetic model was employed to improve our understanding of the ammonia formation pathways and identify possible changes in these pathways when altering the N2:H2 feed ratio. A higher NH3 synthesis rate was achieved when increasing the feed flow rate, as well as when increasing the gas tem-perature from 100 to 200 ◦C when a packing material was present in the plasma. At the elevated temperature of 200 ◦C, an optimum in the NH3 synthesis rate was observed at an equimolar feed ratio (N2:H2 =1:1) for the plasma alone and MgAl2O4, while a N2-rich feed was favored for Ru/MgAl2O4 and Co/MgAl2O4. The optimum in the synthesis rate with the N2-rich feed, where high energy electrons are more likely to collide with N2, suggests that the rate-limiting step is the dissociation of N2 in the gas phase. This is supported by the kinetic model when packing material was used. However, for the plasma alone, the model found that the N2 dissociation is only rate limiting in H2-rich feeds, whereas the limited access to H in N2-rich feeds makes the hydrogenation of N species limiting. | ||||
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| Language | Wos | 001058978000001 | Publication Date | 2023-01-05 | |
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| 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 | OpenAccess | |
| Notes | We thank Topsoe A/S for providing the catalytic materials used in the study, the research group PLASMANT (University of Antwerp) for sharing their plasma kinetic model and allocating time on their cluster for the calculations, and the Department of Chemical and Biochemical Engineering (Technical University of Denmark) for funding the project. | Approved | Most recent IF: 15.1; 2023 IF: 6.216 | ||
| Call Number | PLASMANT @ plasmant @c:irua:195877 | Serial | 7234 | ||
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| Author | Andersen, Ja.; van 't Veer, K.; Christensen, Jm.; Østberg, M.; Bogaerts, A.; Jensen, Ad. | ||||
| Title | Ammonia decomposition in a dielectric barrier discharge plasma: Insights from experiments and kinetic modeling | Type | A1 Journal article | ||
| Year | 2023 | Publication | Chemical engineering science | Abbreviated Journal | |
| Volume | 271 | Issue | Pages | 118550 | |
| Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Utilizing ammonia as a storage medium for hydrogen is currently receiving increased attention. A possible method to retrieve the hydrogen is by plasma-catalytic decomposition. In this work, we combined an experimental study, using a dielectric barrier discharge plasma reactor, with a plasma kinetic model, to get insights into the decomposition mechanism. The experimental results revealed a similar effect on the ammonia conversion when changing the flow rate and power, where increasing the specific energy input (higher power or lower flow rate) gave an increased conversion. A conversion as high as 82 % was achieved at a specific energy input of 18 kJ/Nl. Furthermore, when changing the discharge volume from 31 to 10 cm3, a change in the plasma distribution factor from 0.2 to 0.1 was needed in the model to best describe the conversions of the experiments. This means that a smaller plasma volume caused a higher transfer of energy through micro-discharges (non-uniform plasma), which was found to promote the decomposition of ammonia. These results indicate that it is the collisions between NH3 and the high-energy electrons that initiate the decomposition. Moreover, the rate of ammonia destruction was found by the model to be in the order of 1022 molecules/(cm3 s) during the micro-discharges, which is 5 to 6 orders of magnitude higher than in the afterglows. A considerable re-formation of ammonia was found to take place in the afterglows, limiting the overall conversion. In addition, the model revealed that implementation of packing material in the plasma introduced high concentrations of surface-bound hydrogen atoms, which introduced an additional ammonia re-formation pathway through an Eley-Rideal reaction with gas phase NH2. Furthermore, a more uniform plasma is predicted in the presence of MgAl2O4, which leads to a lower average electron energy during micro-discharges and a lower conversion (37 %) at a comparable residence time for the plasma alone (51 %). | ||||
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| Language | Wos | 000946293200001 | Publication Date | 2023-02-09 | |
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| Series Volume | Series Issue | Edition | |||
| ISSN | 0009-2509 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 4.7 | Times cited | Open Access | OpenAccess | |
| Notes | We thank Topsoe A/S for providing the packing material used, the research group PLASMANT (UAntwerpen) for sharing their plasma kinetic model and allowing us to perform the calculations on their clusters, and the Department of Chemical and Biochemical Engineering, Technical University of Denmark, for funding this project. | Approved | Most recent IF: 4.7; 2023 IF: 2.895 | ||
| Call Number | PLASMANT @ plasmant @c:irua:195204 | Serial | 7237 | ||
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| Author | Tsonev, I.; O’Modhrain, C.; Bogaerts, A.; Gorbanev, Y. | ||||
| Title | Nitrogen Fixation by an Arc Plasma at Elevated Pressure to Increase the Energy Efficiency and Production Rate of NOx | Type | A1 Journal article | ||
| Year | 2023 | Publication | ACS Sustainable Chemistry and Engineering | Abbreviated Journal | |
| Volume | 11 | Issue | 5 | Pages | 1888-1897 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Plasma-based nitrogen fixation for fertilizer production is an attractive alternative to the fossil fuel-based industrial processes. However, many factors hinder its applicability, e.g., the commonly observed inverse correlation between energy consumption and production rates or the necessity to enhance the selectivity toward NO2, the desired product for a more facile formation of nitrate-based fertilizers. In this work, we investigated the use of a rotating gliding arc plasma for nitrogen fixation at elevated pressures (up to 3 barg), at different feed gas flow rates and composition. Our results demonstrate a dramatic increase in the amount of NOx produced as a function of increasing pressure, with a record-low EC of 1.8 MJ/(mol N) while yielding a high production rate of 69 g/h and a high selectivity (94%) of NO2. We ascribe this improvement to the enhanced thermal Zeldovich mechanism and an increased rate of NO oxidation compared to the back reaction of NO with atomic oxygen, due to the elevated pressure. | ||||
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| Language | Wos | 000924366700001 | Publication Date | 2023-02-06 | |
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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 | OpenAccess | |
| Notes | Fonds Wetenschappelijk Onderzoek, G0G2322N ; Horizon 2020 Framework Programme, 965546 ; | Approved | Most recent IF: 8.4; 2023 IF: 5.951 | ||
| Call Number | PLASMANT @ plasmant @c:irua:194281 | Serial | 7239 | ||
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| Author | Eshtehardi, H.A.; van 't Veer, K.; Delplancke, M.-P.; Reniers, F.; Bogaerts, A. | ||||
| Title | Postplasma Catalytic Model for NO Production: Revealing the Underlying Mechanisms to Improve the Process Efficiency | Type | A1 Journal article | ||
| Year | 2023 | Publication | ACS Sustainable Chemistry and Engineering | Abbreviated Journal | |
| Volume | 11 | Issue | 5 | Pages | 1720-1733 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Plasma catalysis is emerging for plasma-assisted gas conversion processes. However, the underlying mechanisms of plasma catalysis are poorly understood. In this work, we present a 1D heterogeneous catalysis model with axial dispersion (i.e., accounting for back-mixing and molecular diffusion of fluid elements in the process stream in the axial direction), for plasma-catalytic NO production from N2/O2 mixtures. We investigate the concentration and reaction rates of each species formed as a function of time and position across the catalyst, in order to determine the underlying mechanisms. To obtain insights into how the performance of the process can be further improved, we also study how changes in the postplasma gas flow composition entering the catalyst bed and in the operation conditions of the catalytic stage affect the performance of NO production. | ||||
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| Language | Wos | 000926412800001 | Publication Date | 2023-02-06 | |
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| ISSN | 2168-0485 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 8.4 | Times cited | Open Access | OpenAccess | |
| Notes | Fonds Wetenschappelijk Onderzoek, 30505023 GoF9618n ; Fonds De La Recherche Scientifique FNRS, 30505023 GoF9618n ; H2020 European Research Council, 810182 ; | Approved | Most recent IF: 8.4; 2023 IF: 5.951 | ||
| Call Number | PLASMANT @ plasmant @c:irua:195377 | Serial | 7241 | ||
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| Author | Kelly, S.; Verheyen, C.; Cowley, A.; Bogaerts, A. | ||||
| Title | Producing oxygen and fertilizer with the Martian atmosphere by using microwave plasma | Type | A1 Journal article | ||
| Year | 2022 | Publication | Chem | Abbreviated Journal | Chem |
| Volume | 8 | Issue | 10 | Pages | 2797-2816 |
| Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | We explorethepotentialofmicrowave(MW)-plasma-based in situ utilizationoftheMartianatmospherewithafocusonthenovelpos- sibilityoffixingN2 forfertilizerproduction. Conversioninasimulant plasma (i.e., 96% CO2, 2% N2, and 2% Ar),performedunderen- ergyconditionssimilartothoseoftheMarsOxygen In Situ Resource UtilizationExperiment(MOXIE),currentlyonboardNASA’sPerse- verancerover,demonstratesthatO/O2 formedthroughCO2 dissociation facilitatesthefixationoftheN2 fractionviaoxidationtoNOx. PromisingproductionratesforO2, CO,andNOx of 47.0,76.1,and 1.25g/h,respectively,arerecordedwithcorrespondingenergy costs of0.021,0.013,and0.79kWh/g,respectively.Notably,O2 productionratesare 30 timeshigherthanthosedemonstrated by MOXIE,whiletheNOx production raterepresentsan 7% fixa- tionoftheN2 fraction presentintheMartian atmosphere.MW- plasma-basedconversionthereforeshowsgreatpotentialasan in situ resourceutilization(ISRU)technologyonMarsinthatitsimulta- neouslyfixesN2 and producesO2. |
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000875346600005 | Publication Date | 2022-08-22 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 2451-9294 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 23.5 | Times cited | Open Access | OpenAccess | |
| Notes | the Euro- pean Marie Skłodowska-Curie Individual Fellowship ‘‘PENFIX’’ within Horizon 2020 (grant no. 838181), the European Research Council (ERC) under the European Union’s Horizon 2020 Research and Innovation Program (grant no. 810182; SCOPE ERC Synergy project), and the Excellence of Science FWO-FNRS project (FWO grant no. GoF9618n and EOS no. 30505023). C.V. was supported by a FWO aspirant PhD fellowship (grant no. 1184820N). The calculations were per- formed with the Turing HPC infrastructure at the CalcUA core facility of the Univer- siteit Antwerpen (Uantwerpen), a division of the Flemish Supercomputer Centre VSC, funded by the Hercules Foundation, the Flemish government (department EWI), and Uantwerpen. | Approved | Most recent IF: 23.5 | ||
| Call Number | PLASMANT @ plasmant @c:irua:192174 | Serial | 7243 | ||
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| Author | Morais, E.; Delikonstantis, E.; Scapinello, M.; Smith, G.; Stefanidis, G.D.; Bogaerts, A. | ||||
| Title | Methane coupling in nanosecond pulsed plasmas: Correlation between temperature and pressure and effects on product selectivity | Type | A1 Journal article | ||
| Year | 2023 | Publication | Chemical engineering journal | Abbreviated Journal | |
| Volume | 462 | Issue | Pages | 142227 | |
| Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | We present a zero-dimensional kinetic model to characterise specifically the gas-phase dynamics of methane conversion in a nanosecond pulsed discharge (NPD) plasma reactor. The model includes a systematic approach to capture the nanoscale power discharges and the rapid ensuing changes in electric field, gas and electron temperature, as well as species densities. The effects of gas temperature and reactor pressure on gas conversion and product selectivity are extensively investigated and validated against experimental work. We discuss the important reaction pathways and provide an analysis of the dynamics of the heating and cooling mechanisms. H radicals are found to be the most populous plasma species and they participate in hydrogenation and dehydrogenation reactions, which are the dominant recombination reactions leading to C2H4 and C2H2 as main products (depending on the pressure). |
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000983631500001 | Publication Date | 2023-03-02 | |
| 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 | OpenAccess | |
| Notes | We gratefully acknowledge financial support by the Flemish Government through the Moonshot cSBO project “Power-to-Olefins” (P2O; HBC.2020.2620). | Approved | Most recent IF: 15.1; 2023 IF: 6.216 | ||
| Call Number | PLASMANT @ plasmant @c:irua:195881 | Serial | 7246 | ||
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| Author | Daele, K.V.; Arenas‐Esteban, D.; Choukroun, D.; Hoekx, S.; Rossen, A.; Daems, N.; Pant, D.; Bals, S.; Breugelmans, T. | ||||
| Title | Enhanced Pomegranate‐Structured SnO2Electrocatalysts for the Electrochemical CO2Reduction to Formate | Type | A1 Journal article | ||
| Year | 2023 | Publication | ChemElectroChem | Abbreviated Journal | |
| Volume | Issue | Pages | |||
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) | ||||
| Abstract | Although most state-of-the-art Sn-based electrocatalysts yield promising results in terms of selectivity and catalyst activity, their stability remains insufficient to date. Here, we demonstrate the successful application of the recently developed pomegranate-structured SnO2 (Pom. SnO2) and SnO2@C (Pom. SnO2@C) nanocomposite electrocatalysts for the efficient electrochemical conversion of CO2 to formate. With an initial selectivity of 83 and 86% towards formate and an operating potential of -0.72 V and -0.64 V vs. RHE, respectively, these pomegranate SnO2 electrocatalysts are able to compete with most of the current state-of-the-art Sn-based electrocatalysts in terms of activity and selectivity. Given the importance of electrocatalyst stability, long-term experiments (24 h) were performed and a temporary loss in selectivity for the Pom. SnO2@C electrocatalyst was largely restored to its initial selectivity upon drying and exposure to air. Of all the used (24 h) electrocatalysts, the pomegranate SnO2@C had the highest selectivity over a time period of one hour, reaching an average recovered FE of 85%, while the commercial SnO2 and bare pomegranate SnO2 electrocatalysts reached an average of 79 and 80% FE towards formate, respectively. Furthermore, the pomegranate structure of Pom. SnO2@C was largely preserved due to the presence of the heterogeneous carbon shell, which acts as a protective layer, physically inhibiting particle segregation/pulverisation and agglomeration. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000936694800001 | Publication Date | 2023-02-15 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 2196-0216 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 4 | Times cited | Open Access | OpenAccess | |
| Notes | European Regional Development Fund, E2C 2S03-019 ; | Approved | Most recent IF: 4; 2023 IF: 4.136 | ||
| Call Number | EMAT @ emat @c:irua:195228 | Serial | 7249 | ||
| Permanent link to this record | |||||
| Author | Van Alphen, S.; Hecimovic, A.; Kiefer, C.K.; Fantz, U.; Snyders, R.; Bogaerts, A. | ||||
| Title | Modelling post-plasma quenching nozzles for improving the performance of CO2 microwave plasmas | Type | A1 Journal article | ||
| Year | 2023 | Publication | Chemical engineering journal | Abbreviated Journal | |
| Volume | 462 | Issue | Pages | 142217 | |
| Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Given the ecological problems associated to the CO2 emissions of fossil fuels, plasma technology has gained interest for conversion of CO2 into value-added products. Microwave plasmas operating at atmospheric pressure have proven to be especially interesting, due to the high gas temperatures inside the reactor (i.e. up to 6000 K) allowing for efficient thermal dissociation of CO2 into CO and O2. However, the performance of these high temperature plasmas is limited by recombination of CO back into CO2 once the gas cools down in the afterglow. In this work, we computationally investigated several quenching nozzles, developed and experimentally tested by Hecimovic et al., [1] for their ability to quickly cool the gas after the plasma, thereby quenching the CO recombination reactions. Using a 3D computational fluid dynamics model and a quasi-1D chemical kinetics model, we reveal that a reactor without nozzle lacks gas mixing between hot gas in the center and cold gas near the reactor walls. Especially at low flow rates, where there is an inherent lack of convective cooling due to the low gas flow velocity, the temperature in the afterglow remains high (between 2000 and 3000 K) for a relatively long time (in the 0.1 s range). As shown by our quasi-1D chemical kinetics model, this results in a important loss of CO due to recombination reactions. Attaching a nozzle in the effluent of the reactor induces fast gas quenching right after the plasma. Indeed, it introduces (i) more convective cooling by forcing cool gas near the walls to mix with hot gas in the center of the reactor, as well as (ii) more conductive cooling through the water-cooled walls of the nozzle. Our model shows that gas quenching and the suppression of recombination reactions have more impact at low flow rates, where recombination is the most limiting factor in the conversion process. |
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000962382600001 | Publication Date | 2023-03-03 | |
| 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 | OpenAccess | |
| Notes | This research was supported by the Excellence of Science FWO-FNRS project (FWO grant ID GoF9618n, EOS ID 30505023), the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No 810182 – SCOPE ERC Synergy project), and through long-term structural funding (Methusalem). 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: 15.1; 2023 IF: 6.216 | ||
| Call Number | PLASMANT @ plasmant @c:irua:195889 | Serial | 7250 | ||
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| Author | Liu, R.; Hao, Y.; Wang, T.; Wang, L.; Bogaerts, A.; Guo, H.; Yi, Y. | ||||
| Title | Hybrid plasma-thermal system for methane conversion to ethylene and hydrogen | Type | A1 Journal article | ||
| Year | 2023 | Publication | Chemical engineering journal | Abbreviated Journal | |
| Volume | 463 | Issue | Pages | 142442 | |
| Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | By combining dielectric barrier discharge plasma and external heating, we exploit a two-stage hybrid plasmathermal system (HPTS), i.e., a plasma stage followed by a thermal stage, for direct non-oxidative coupling of CH4 to C2H4 and H2, yielding a CH4 conversion of ca. 17 %. In the two-stage HPTS, the plasma first converts CH4 into C2H6 and C3H8, which in the thermal stage leads to a high C2H4 selectivity of ca. 63 % by pyrolysis, with H2 selectivity of ca. 64 %. |
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| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000953890500001 | Publication Date | 2023-03-16 | |
| 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 | OpenAccess | |
| Notes | This work was supported by the National Natural Science Foundation of China [22272015, 21503032], the Fundamental Research Funds for the Central Universities of China [DUT21JC40]. | Approved | Most recent IF: 15.1; 2023 IF: 6.216 | ||
| Call Number | PLASMANT @ plasmant @c:irua:195888 | Serial | 7253 | ||
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| Author | Vervloessem, E.; Gromov, M.; De Geyter, N.; Bogaerts, A.; Gorbanev, Y.; Nikiforov, A. | ||||
| Title | NH3and HNOxFormation and Loss in Nitrogen Fixation from Air with Water Vapor by Nonequilibrium Plasma | Type | A1 Journal article | ||
| Year | 2023 | Publication | ACS Sustainable Chemistry and Engineering | Abbreviated Journal | |
| Volume | 11 | Issue | 10 | Pages | 4289-4298 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | The current global energy crisis indicated that increasing our insight into nonfossil fuel nitrogen fixation pathways for synthetic fertilizer production is more crucial than ever. Nonequilibrium plasma is a good candidate because it can use N2 or air as a N source and water directly as a H source, instead of H2 or fossil fuel (CH4). In this work, we investigate NH3 gas phase formation pathways from humid N2 and especially humid air up to 2.4 mol % H2O (100% relative humidity at 20 °C) by optical emission spectroscopy and Fouriertransform infrared spectroscopy. We demonstrate that the nitrogen fixation capacity is increased when water vapor is added, as this enables HNO2 and NH3 production in both N2 and air. However, we identified a significant loss mechanism for NH3 and HNO2 that occurs in systems where these species are synthesized simultaneously; i.e., downstream from the plasma, HNO2 reacts with NH3 to form NH4NO2, which rapidly decomposes into N2 and H2O. We also discuss approaches to prevent this loss mechanism, as it reduces the effective nitrogen fixation when not properly addressed and therefore should be considered in future works aimed at optimizing plasma-based N2 fixation. In-line removal of HNO2 or direct solvation in liquid are two proposed strategies to suppress this loss mechanism. Indeed, using liquid H2O is beneficial for accumulation of the N2 fixation products. Finally, in humid air, we also produce NH4NO3, from the reaction of HNO3 with NH3, which is of direct interest for fertilizer application. |
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| Language | Wos | 000953337700001 | Publication Date | 2023-03-13 | |
| 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 | This research is supported by the Excellence of Science FWOFNRS project (NITROPLASM, FWO grant ID GoF9618n, EOS ID 30505023), the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (grant No. 810182 − SCOPE ERC Synergy project), and the Fund for Scientific Research (FWO) Flanders Bioeconomy project (grant No. G0G2322N), funded by the European Union-NextGenerationEU. | Approved | Most recent IF: 8.4; 2023 IF: 5.951 | ||
| Call Number | PLASMANT @ plasmant @c:irua:195878 | Serial | 7254 | ||
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| Author | van der Sluijs, M.M.; Salzmann, B.B.V.; Arenas Esteban, D.; Li, C.; Jannis, D.; Brafine, L.C.; Laning, T.D.; Reinders, J.W.C.; Hijmans, N.S.A.; Moes, J.R.; Verbeeck, J.; Bals, S.; Vanmaekelbergh, D. | ||||
| Title | Study of the Mechanism and Increasing Crystallinity in the Self-Templated Growth of Ultrathin PbS Nanosheets | Type | A1 Journal article | ||
| Year | 2023 | Publication | Chemistry of materials | Abbreviated Journal | |
| Volume | Issue | Pages | |||
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Colloidal 2D semiconductor nanocrystals, the analogue of solid-state quantum wells, have attracted strong interest in material science and physics. Molar quantities of suspended quantum objects with spectrally pure absorption and emission can be synthesized. For the visible region, CdSe nanoplatelets with atomically precise thickness and tailorable emission have been (almost) perfected. For the near-infrared region, PbS nanosheets (NSs) hold strong promise, but the photoluminescence quantum yield is low and many questions on the crystallinity, atomic structure, intriguing rectangular shape, and formation mechanism remain to be answered. Here, we report on a detailed investigation of the PbS NSs prepared with a lead thiocyanate single source precursor. Atomically resolved HAADF-STEM imaging reveals the presence of defects and small cubic domains in the deformed orthorhombic PbS crystal lattice. Moreover, variations in thickness are observed in the NSs, but only in steps of 2 PbS monolayers. To study the reaction mechanism, a synthesis at a lower temperature allowed for the study of reaction intermediates. Specifically, we studied the evolution of pseudo-crystalline templates towards mature, crystalline PbS NSs. We propose a self-induced templating mechanism based on an oleylamine-lead-thiocyanate (OLAM-Pb-SCN) complex with two Pb-SCN units as a building block; the interactions between the long-chain ligands regulate the crystal structure and possibly the lateral dimensions. | ||||
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| Language | Wos | 000959572100001 | Publication Date | 2023-03-25 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 0897-4756 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 8.6 | Times cited | 2 | Open Access | OpenAccess |
| Notes | H2020 Research Infrastructures, 731019 ; H2020 European Research Council, 692691 815128 ; Nederlandse Organisatie voor Wetenschappelijk Onderzoek, 715.016.002 ; | Approved | Most recent IF: 8.6; 2023 IF: 9.466 | ||
| Call Number | EMAT @ emat @c:irua:195894 | Serial | 7255 | ||
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| Author | Eshtehardi, H.A.; Van ‘t Veer, K.; Delplancke, M.-P.; Reniers, F.; Bogaerts, A. | ||||
| Title | Postplasma Catalytic Model for NO Production: Revealing the Underlying Mechanisms to Improve the Process Efficiency | Type | A1 Journal article | ||
| Year | 2023 | Publication | ACS Sustainable Chemistry and Engineering | Abbreviated Journal | |
| Volume | 11 | Issue | 5 | Pages | 1720-1733 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Plasma catalysis is emerging for plasma-assisted gas conversion processes. However, the underlying mechanisms of plasma catalysis are poorly understood. In this work, we present a 1D heterogeneous catalysis model with axial dispersion (i.e., accounting for back-mixing and molecular diffusion of fluid elements in the process stream in the axial direction), for plasma-catalytic NO production from N2/O2 mixtures. We investigate the concentration and reaction rates of each species formed as a function of time and position across the catalyst, in order to determine the underlying mechanisms. To obtain insights into how the performance of the process can be further improved, we also study how changes in the postplasma gas flow composition entering the catalyst bed and in the operation conditions of the catalytic stage affect the performance of NO production. |
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| Language | Wos | 000926412800001 | Publication Date | 2023-02-06 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 2168-0485 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 8.4 | Times cited | Open Access | OpenAccess | |
| Notes | This research was supported by the Excellence of Science FWO-FNRS project (FWO grant ID GoF9618n, EOS ID 30505023) 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). 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: 8.4; 2023 IF: 5.951 | ||
| Call Number | PLASMANT @ plasmant @c:irua:195377 | Serial | 7257 | ||
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| Author | Eshtehardi, H.A.; Van ‘t Veer, K.; Delplancke, M.-P.; Reniers, F.; Bogaerts, A. | ||||
| Title | Postplasma Catalytic Model for NO Production: Revealing the Underlying Mechanisms to Improve the Process Efficiency | Type | A1 Journal article | ||
| Year | 2023 | Publication | ACS Sustainable Chemistry and Engineering | Abbreviated Journal | |
| Volume | 11 | Issue | 5 | Pages | 1720-1733 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Plasma catalysis is emerging for plasma-assisted gas conversion processes. However, the underlying mechanisms of plasma catalysis are poorly understood. In this work, we present a 1D heterogeneous catalysis model with axial dispersion (i.e., accounting for back-mixing and molecular diffusion of fluid elements in the process stream in the axial direction), for plasma-catalytic NO production from N2/O2 mixtures. We investigate the concentration and reaction rates of each species formed as a function of time and position across the catalyst, in order to determine the underlying mechanisms. To obtain insights into how the performance of the process can be further improved, we also study how changes in the postplasma gas flow composition entering the catalyst bed and in the operation conditions of the catalytic stage affect the performance of NO production. |
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| Language | Wos | 000926412800001 | Publication Date | 2023-02-06 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 2168-0485 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 8.4 | Times cited | Open Access | OpenAccess | |
| Notes | Fonds Wetenschappelijk Onderzoek, 30505023 GoF9618n ; Fonds De La Recherche Scientifique – FNRS, 30505023 GoF9618n ; H2020 European Research Council, 810182 ; | Approved | Most recent IF: 8.4; 2023 IF: 5.951 | ||
| Call Number | PLASMANT @ plasmant @c:irua:195377 | Serial | 7258 | ||
| Permanent link to this record | |||||
| Author | Van Alphen, S.; Hecimovic, A.; Kiefer, C.K.; Fantz, U.; Snyders, R.; Bogaerts, A. | ||||
| Title | Modelling post-plasma quenching nozzles for improving the performance of CO2 microwave plasmas | Type | A1 Journal article | ||
| Year | 2023 | Publication | Chemical engineering journal | Abbreviated Journal | |
| Volume | 462 | Issue | Pages | 142217 | |
| Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Given the ecological problems associated to the CO2 emissions of fossil fuels, plasma technology has gained interest for conversion of CO2 into value-added products. Microwave plasmas operating at atmospheric pressure have proven to be especially interesting, due to the high gas temperatures inside the reactor (i.e. up to 6000 K) allowing for efficient thermal dissociation of CO2 into CO and O2. However, the performance of these high temperature plasmas is limited by recombination of CO back into CO2 once the gas cools down in the afterglow. In this work, we computationally investigated several quenching nozzles, developed and experimentally tested by Hecimovic et al., [1] for their ability to quickly cool the gas after the plasma, thereby quenching the CO recombination reactions. Using a 3D computational fluid dynamics model and a quasi-1D chemical kinetics model, we reveal that a reactor without nozzle lacks gas mixing between hot gas in the center and cold gas near the reactor walls. Especially at low flow rates, where there is an inherent lack of convective cooling due to the low gas flow velocity, the temperature in the afterglow remains high (between 2000 and 3000 K) for a relatively long time (in the 0.1 s range). As shown by our quasi-1D chemical kinetics model, this results in a important loss of CO due to recombination reactions. Attaching a nozzle in the effluent of the reactor induces fast gas quenching right after the plasma. Indeed, it introduces (i) more convective cooling by forcing cool gas near the walls to mix with hot gas in the center of the reactor, as well as (ii) more conductive cooling through the water-cooled walls of the nozzle. Our model shows that gas quenching and the suppression of recombination reactions have more impact at low flow rates, where recombination is the most limiting factor in the conversion process. |
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| Language | Wos | 000962382600001 | Publication Date | 2023-03-03 | |
| 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 | OpenAccess | |
| Notes | This research was supported by the Excellence of Science FWO-FNRS project (FWO grant ID GoF9618n, EOS ID 30505023), the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No 810182 – SCOPE ERC Synergy project), and through long-term structural funding (Methusalem). 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: 15.1; 2023 IF: 6.216 | ||
| Call Number | PLASMANT @ plasmant @c:irua:195889 | Serial | 7259 | ||
| Permanent link to this record | |||||