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Author Schram, J.; Parrilla, M.; Sleegers, N.; Samyn, N.; Bijvoets, S.M.; Heerschop, M.W.J.; van Nuijs, A.L.N.; De Wael, K.
Title Identifying Electrochemical Fingerprints of Ketamine with Voltammetry and Liquid Chromatography–Mass Spectrometry for Its Detection in Seized Samples Type A1 Journal article
Year 2020 Publication Analytical Chemistry Abbreviated Journal Anal Chem
Volume 92 Issue 19 Pages 13485-13492
Keywords A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Toxicological Centre
Abstract Herein, a straightforward electrochemical approach for the determination of ketamine in street samples and seizures is presented by employing screen-printed electrodes (SPE). Square wave voltammetry (SWV) is used to study the electrochemical behavior of the illicit drug, thus profiling the different oxidation states of the substance at different pHs. Besides, the oxidation pathway of ketamine on SPE is investigated for the first time with liquid chromatography–high-resolution mass spectrometry. Under the optimized conditions, the calibration curve of ketamine at buffer solution (pH 12) exhibits a sensitivity of 8.2 μA μM–1, a linear relationship between 50 and 2500 μM with excellent reproducibility (RSD = 2.2%, at 500 μM, n = 7), and a limit of detection (LOD) of 11.7 μM. Subsequently, binary mixtures of ketamine with adulterants and illicit drugs are analyzed with SWV to investigate the electrochemical fingerprint. Moreover, the profile overlapping between different substances is addressed by the introduction of an electrode pretreatment and the integration of a tailor-made script for data treatment. Finally, the approach is tested on street samples from forensic seizures. Overall, this system allows for the on-site identification of ketamine by law enforcement agents in an easy-to-use and rapid manner on cargos and seizures, thereby disrupting the distribution channel and avoiding the illicit drug reaching the end-user.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000580426800091 Publication Date 2020-10-06
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0003-2700 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 7.4 Times cited Open Access
Notes (up) Universiteit Antwerpen; H2020 Societal Challenges, 833787 ; Fonds Wetenschappelijk Onderzoek, 1S3765817N 1SB8120N ; Approved Most recent IF: 7.4; 2020 IF: 6.32
Call Number AXES @ axes @c:irua:170523 Serial 6435
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Author Biondo, O.; van Deursen, C.F.A.M.; Hughes, A.; van de Steeg, A.; Bongers, W.; van de Sanden, M.C.M.; van Rooij, G.; Bogaerts, A.
Title Avoiding solid carbon deposition in plasma-based dry reforming of methane Type A1 Journal Article
Year 2023 Publication Green Chemistry Abbreviated Journal Green Chem.
Volume 25 Issue 24 Pages 10485-10497
Keywords A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Abstract Solid carbon deposition is a persistent challenge in dry reforming of methane (DRM), affecting both classical and plasma-based processes. In this work, we use a microwave plasma in reverse vortex flow configuration to overcome this issue in CO<sub>2</sub>/CH<sub>4</sub>plasmas. Indeed, this configuration efficiently mitigates carbon deposition, enabling operation even with pure CH<sub>4</sub>feed gas, in contrast to other configurations. At the same time, high reactor performance is achieved, with CO<sub>2</sub>and CH<sub>4</sub>conversions reaching 33% and 44% respectively, at an energy cost of 14 kJ L<sup>−1</sup>for a CO<sub>2</sub> : CH<sub>4</sub>ratio of 1 : 1. Laser scattering and optical emission imaging demonstrate that the shorter residence time in reverse vortex flow lowers the gas temperature in the discharge, facilitating a shift from full to partial CH<sub>4</sub>pyrolysis. This underscores the pivotal role of flow configuration in directing process selectivity, a crucial factor in complex chemistries like CO<sub>2</sub>/CH<sub>4</sub>mixtures and very important for industrial applications.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001110100100001 Publication Date 2023-11-24
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1463-9262 ISBN Additional Links UA library record; WoS full record
Impact Factor 9.8 Times cited Open Access
Notes (up) Universiteit Antwerpen; Nederlandse Organisatie voor Wetenschappelijk Onderzoek; HORIZON EUROPE Marie Sklodowska-Curie Actions, 813393 ; Approved Most recent IF: 9.8; 2023 IF: 9.125
Call Number PLASMANT @ plasmant @c:irua:202138 Serial 8978
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Author Heijkers, S.; Aghaei, M.; Bogaerts, A.
Title Plasma-Based CH4Conversion into Higher Hydrocarbons and H2: Modeling to Reveal the Reaction Mechanisms of Different Plasma Sources Type A1 Journal article
Year 2020 Publication Journal Of Physical Chemistry C Abbreviated Journal J Phys Chem C
Volume 124 Issue 13 Pages 7016-7030
Keywords A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract Plasma is gaining interest for CH4 conversion into higher hydrocarbons and H2. However, the performance in terms of conversion and selectivity toward different hydrocarbons is different for different plasma types, and the underlying mechanisms are not yet fully understood. Therefore, we study here these mechanisms in different plasma sources, by means of a chemical kinetics model. The model is first validated by comparing the calculated conversions and hydrocarbon/H2 selectivities with experimental results in these different plasma types and over a wide range of specific energy input (SEI) values. Our model predicts that vibrational−translational nonequilibrium is negligible in all CH4 plasmas investigated, and instead, thermal conversion is important. Higher gas temperatures also lead to a more selective production of unsaturated hydrocarbons (mainly C2H2) due to neutral dissociation of CH4 and subsequent dehydrogenation processes, while three-body recombination reactions into saturated hydrocarbons (mainly C2H6, but also higher hydrocarbons) are dominant in low temperature plasmas.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000526328500007 Publication Date 2020-04-02
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1932-7447 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.7 Times cited Open Access OpenAccess
Notes (up) Universiteit Antwerpen; Vlaamse regering; Fonds Wetenschappelijk Onderzoek, G.0383.16N ; H2020 European Research Council, 810182 ; We acknowledge financial support from the Fund for Scientific Research, Flanders (FWO; Grant No. G.0383.16N), the Methusalem Grant, and the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (Grant Agreement No. 810182 − SCOPE ERC Synergy project). This work was carried out in part using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen, a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the University of Antwerp. Approved Most recent IF: 3.7; 2020 IF: 4.536
Call Number PLASMANT @ plasmant @c:irua:168096 Serial 6358
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Author Leemans, J.; Singh, S.; Li, C.; Ten Brinck, S.; Bals, S.; Infante, I.; Moreels, I.; Hens, Z.
Title Near-Edge Ligand Stripping and Robust Radiative Exciton Recombination in CdSe/CdS Core/Crown Nanoplatelets Type A1 Journal article
Year 2020 Publication Journal Of Physical Chemistry Letters Abbreviated Journal J Phys Chem Lett
Volume 11 Issue 9 Pages 3339-3344
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract We address the relation between surface chemistry and optoelectronic properties in semiconductor nanocrystals using core/crown CdSe/CdS nanoplatelets passivated by cadmium oleate (Cd(Ol)2) as model systems. We show that addition of butylamine to a nanoplatelet (NPL) dispersion maximally displaces ∼40% of the original Cd(Ol)2 capping. On the basis of density functional theory simulations, we argue that this behavior reflects the preferential displacement of Cd(Ol)2 from (near)-edge surface sites. Opposite from CdSe core NPLs, core/crown NPL dispersions can retain 45% of their initial photoluminescence efficiency after ligand displacement, while radiative exciton recombination keeps dominating the luminescent decay. Using electron microscopy observations, we assign this robust photoluminescence to NPLs with a complete CdS crown, which prevents charge carrier trapping in the near-edge surface sites created by ligand displacement. We conclude that Z-type ligands such as cadmium carboxylates can provide full electronic passivation of (100) facets yet are prone to displacement from (near)-edge surface sites.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000535177500024 Publication Date 2020-05-07
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1948-7185 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 5.7 Times cited 24 Open Access OpenAccess
Notes (up) Universiteit Gent, GOA 01G01019 ; Fonds Wetenschappelijk Onderzoek, 17006602 FWO17/PDO/184 ; H2020 European Research Council, 714876 Phocona 815128 Realnano ; SIM-Flanders, SBO-QDOCCO ; Z.H. and S.B. acknowledge support by SIM-Flanders (SBO-QDOCCO). Z.H. acknowledges support by FWO-Vlaanderen (research project 17006602). Z.H. and I.M. acknowledge support by Ghent University (GOA n◦ 01G01019). J.L. acknowledges FWO-vlaanderen for a fellowship (SB PhD fellow at FWO). Sh.S acknowledges FWO postdoctoral funding (FWO17/PDO/184). This project has further received funding from the European Research Counsil under the European Union’s Horizon 2020 research and innovation programme (ERC Consolidator grant no. 815128 REALNANO and starting grant no. 714876 PHOCONA).; sygma Approved Most recent IF: 5.7; 2020 IF: 9.353
Call Number EMAT @ emat @c:irua:173994 Serial 6657
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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.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000772893400001 Publication Date 2022-03-25
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
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 (up) 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 der Stam, W.; Geuchies, J.J.; Altantzis, T.; van den Bos, K.H.W.; Meeldijk, J.D.; Van Aert, S.; Bals, S.; Vanmaekelbergh, D.; de Mello Donega, C.
Title Highly Emissive Divalent-Ion-Doped Colloidal CsPb1–xMxBr3Perovskite Nanocrystals through Cation Exchange Type A1 Journal article
Year 2017 Publication Journal of the American Chemical Society Abbreviated Journal J Am Chem Soc
Volume 139 Issue 139 Pages 4087-4097
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Colloidal CsPbX3 (X = Br, Cl, and I) perovskite nanocrystals (NCs) have emerged as promising phosphors and solar cell materials due to their remarkable optoelectronic properties. These properties can be tailored by not only controlling the size and shape of the NCs but also postsynthetic composition tuning through topotactic

anion exchange. In contrast, property control by cation exchange is still underdeveloped for colloidal CsPbX3 NCs. Here, we present a method that allows partial cation exchange in colloidal CsPbBr3 NCs, whereby Pb2+ is exchanged for several isovalent cations, resulting in doped CsPb1−xMxBr3 NCs (M= Sn2+, Cd2+, and Zn2+; 0 < x ≤ 0.1), with preservation of the original NC shape. The size of the parent NCs is also preserved in the product NCs, apart from a small (few

%) contraction of the unit cells upon incorporation of the guest cations. The partial Pb2+ for M2+ exchange leads to a blue-shift of the optical spectra, while maintaining the high photoluminescence quantum yields (>50%), sharp absorption features, and narrow emission of the parent CsPbBr3 NCs. The blue-shift in the optical spectra is attributed to the lattice contraction that accompanies the Pb2+ for M2+ cation exchange and is observed to scale linearly with the lattice contraction. This work opens up new possibilities to engineer the properties of halide perovskite NCs, which to date are demonstrated to be the only known

system where cation and anion exchange reactions can be sequentially combined while preserving the original NC shape, resulting in compositionally diverse perovskite NCs.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000397477700027 Publication Date 2017-03-10
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0002-7863 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.858 Times cited 535 Open Access OpenAccess
Notes (up) W.v.d.S. and C.d.M.D. acknowledge financial support from the division of Chemical Sciences (CW) of The Netherlands Organization for Scientific Research (NWO) under grant number ECHO.712.012.001. J.J.G. and D.V. acknowledge financial support from the Debye Graduate program. S.B. acknowledges financial support from the European Research Council (ERC Starting Grant # 335078-COLOURATOMS). K.H.W.v.d.B., S.B., S.V.A. and T.A. acknowledge financial support from the Research Foundation Flanders (FWO, Belgium) through project fundings (G.0374.13N, G.0368.15N, G.0369.15N), a Ph.D. grant to K.H.W.v.d.B, and a postdoctoral research grant to T.A. (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); ECAS_Sara Approved Most recent IF: 13.858
Call Number EMAT @ emat @ c:irua:141754UA @ admin @ c:irua:141754 Serial 4482
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Author van der Stam, W.; Gradmann, S.; Altantzis, T.; Ke, X.; Baldus, M.; Bals, S.; de Mello Donega, C.
Title Shape Control of Colloidal Cu2-x S Polyhedral Nanocrystals by Tuning the Nucleation Rates Type A1 Journal article
Year 2016 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 28 Issue 28 Pages 6705-6715
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Synthesis protocols for colloidal nanocrystals (NCs) with narrow size and shape distributions are of particular interest for the successful implementation of these nanocrystals into devices. Moreover, the preparation of NCs with well-defined crystal phases is of key importance. In this work, we show that Sn(IV)-thiolate complexes formed in situ strongly influence the nucleation and growth rates of colloidal Cu2-x S polyhedral NCs, thereby dictating their final size, shape, and crystal structure. This allowed us to successfully synthesize hexagonal bifrustums and hexagonal bipyramid NCs with low-chalcocite crystal structure, and hexagonal nanoplatelets with various thicknesses and aspect ratios with the djurleite crystal structure, by solely varying the concentration of Sn(IV)-additives (namely, SnBr4) in the reaction medium. Solution and solid-state 119Sn NMR measurements show that SnBr4 is converted in situ to Sn(IV)-thiolate complexes, which increase the Cu2-x S nucleation barrier without affecting the precursor conversion rates. This influences both the nucleation and growth rates in a concentration-dependent fashion and leads to a better separation between nucleation and growth. Our approach of tuning the nucleation and growth rates with in situ-generated Sn-thiolate complexes might have a more general impact due to the availability of various metal-thiolate complexes, possibly resulting in polyhedral NCs of a wide variety of metal-sulfide compositions.
Address Condensed Matter and Interfaces, Debye Institute for Nanomaterials Science, Utrecht University , P.O. Box 80000, 3508 TA Utrecht, The Netherlands
Corporate Author Thesis
Publisher Place of Publication Editor
Language English Wos 000384399000037 Publication Date 2016-09-02
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 9.466 Times cited 27 Open Access OpenAccess
Notes (up) W.v.d.S. and C.d.M.D. acknowledge financial support from the division of Chemical Sciences (CW) of The Netherlands Organization for Scientific Research (NWO) under grant number ECHO.712.012.001. M.B. also gratefully acknowledges NWO for funding the NMR infrastructure (Middle Groot program, grant number 700.58.102). S.B. acknowledges financial support from the European Research Council (ERC Starting Grant # 335078-COLOURATOMS).; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); Approved Most recent IF: 9.466
Call Number EMAT @ emat @ c:irua:135928 Serial 4285
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Author Bae, J.; Cichocka, M.O.; Zhang, Y.; Bacsik, Z.; Bals, S.; Zou, X.; Willhammar, T.; Hong, S.B.
Title Phase transformation behavior of a two-dimensional zeolite Type A1 Journal article
Year 2019 Publication Angewandte Chemie: international edition in English Abbreviated Journal
Volume 58 Issue 30 Pages 10230-10235
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Understanding the molecular-level mechanisms of phase transformation in solids is of fundamental interest for functional materials such as zeolites. Two-dimensional (2D) zeolites, when used as shape-selective catalysts, can offer improved access to the catalytically active sites and a shortened diffusion length in comparison with their 3D analogues. However, few materials are known to maintain both their intralayer microporosity and structure during calcination for organic structure-directing agent (SDA) removal. Herein we report that PST-9, a new 2D zeolite which has been synthesized via the multiple inorganic cation approach and fulfills the requirements for true layered zeolites, can be transformed into the small-pore zeolite EU-12 under its crystallization conditions through the single-layer folding process, but not through the traditional dissolution/recrystallization route. We also show that zeolite crystal growth pathway can differ according to the type of organic SDAs employed.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000476452700030 Publication Date 2019-05-22
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1433-7851; 0570-0833 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor Times cited 2 Open Access OpenAccess
Notes (up) We acknowledge financial support from National Creative Research Initiative Program (2012R1A3A-2048833) through the National Research Foundation of Korea, the National Research Council of Science & Technology (CRC-14-1-KRICT) grant by the Korea government (MSIP), the Swedish Research Council (2017-04321), and the Knut and Alice Wallenberg Foundation (KAW) through the project grant 3DEM-NATUR (2012.0112). T.W. acknowledges an international postdoc grant from the Swedish Research Council (2014-06948). Approved no
Call Number UA @ admin @ c:irua:181233 Serial 6878
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Author Uytdenhouwen, Y.; Van Alphen, S.; Michielsen, I.; Meynen, V.; Cool, P.; Bogaerts, A.
Title A packed-bed DBD micro plasma reactor for CO 2 dissociation: Does size matter? Type A1 Journal article
Year 2018 Publication Chemical engineering journal Abbreviated Journal Chem Eng J
Volume 348 Issue Pages 557-568
Keywords A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract DBD plasma reactors are of great interest for environmental and energy applications, such as CO2 conversion, but they suffer from limited conversion and especially energy efficiency. The introduction of packing materials has been a popular subject of investigation in order to increase the reactor performance. Reducing the discharge gap of the reactor below one millimetre can enhance the plasma performance as well. In this work, we combine both effects and use a packed-bed DBD micro plasma reactor to investigate the influence of gap size reduction, in combination with a packing material, on the conversion and efficiency of CO2 dissociation. Packing materials used in this work were SiO2, ZrO2, and Al2O3 spheres as well as glass wool. The results are compared to a regular size reactor as a benchmark. Reducing the discharge gap can greatly increase the CO2 conversion, although at a lower energy efficiency. Adding a packing material further increases the conversion when keeping a constant residence time, but is greatly dependent on the material composition, gap and sphere size used. Maximum conversions of 50–55% are obtained for very long residence times (30 s and higher) in an empty reactor or with certain packing material combinations, suggesting a balance in CO2 dissociation and recombination reactions. The maximum energy efficiency achieved is 4.3%, but this is for the regular sized reactor at a short residence time (7.5 s). Electrical characterization is performed to reveal some trends in the electrical behaviour of the plasma upon reduction of the discharge gap and addition of a packing material.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000434467000055 Publication Date 2018-05-03
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 6.216 Times cited 22 Open Access Not_Open_Access: Available from 03.05.2020
Notes (up) We acknowledge financial support from the European Fund for Regional Development through the cross-border collaborative Interreg V program Flanders-the Netherlands (project EnOp), the Fund for Scientific Research (FWO; Grant Number: G.0254.14N) and an IOF-SBO (SynCO2Chem) project from the University of Antwerp. Approved Most recent IF: 6.216
Call Number PLASMANT @ plasmant @c:irua:151238 Serial 4956
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Author Wanten, B.; Vertongen, R.; De Meyer, R.; Bogaerts, A.
Title Plasma-based CO2 conversion: How to correctly analyze the performance? Type A1 journal article
Year 2023 Publication Journal of Energy Chemistry Abbreviated Journal Journal of Energy Chemistry
Volume 86 Issue Pages 180-196
Keywords A1 journal article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Abstract
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001070885000001 Publication Date 2023-07-22
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2095-4956 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.1 Times cited Open Access Not_Open_Access
Notes (up) We acknowledge financial support from the Fund for Scientific Research (FWO) Flanders (Grant ID 110221N), the European Research Council (ERC) under the European Union’s Horizon 2020 Research and Innovation Program (grant agreement No 810182 – SCOPE ERC Synergy project), and the Methusalem funding of the University of Antwerp. We acknowledge the icons from the graphical abstract made by dDara, geotatah, Spashicons and Freepik on www.flaticon.com. We also thank Stein Maerivoet, Joachim Slaets, Elizabeth Mercer, Colín Ó’Modráin, Joran Van Turnhout, Pepijn Heirman, dr. Yury Gorbanev, dr. Fanny Girard-Sahun and dr. Sean Kelly for the interesting discussions and feedback. Approved Most recent IF: 13.1; 2023 IF: 2.594
Call Number PLASMANT @ plasmant @c:irua:198709 Serial 8816
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Author Wang, W.; Kim, H.-H.; Van Laer, K.; Bogaerts, A.
Title Streamer propagation in a packed bed plasma reactor for plasma catalysis applications Type A1 Journal article
Year 2018 Publication Chemical engineering journal Abbreviated Journal Chem Eng J
Volume 334 Issue Pages 2467-2479
Keywords A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract A packed bed dielectric barrier discharge (DBD) is widely used for plasma catalysis applications, but the exact plasma characteristics in between the packing beads are far from understood. Therefore, we study here these plasma characteristics by means of fluid modelling and experimental observations using ICCD imaging, for packing materials with different dielectric constants. Our study reveals that a packed bed DBD reactor in dry air at atmospheric pressure may show three types of discharges, i.e. positive restrikes, filamentary microdischarges, which can also be localized between two packing beads, and surface discharges (so-called surface ionization

waves). Restrikes between the dielectric surfaces result in the formation of filamentary microdischarges, while surface charging creates electric field components parallel to the dielectric surfaces, leading to the formation of surface discharges. A transition in discharge mode occurs from surface discharges to local filamentary discharges between the packing beads when the dielectric constant of the packing rises from 5 to 1000. This may have implications for the efficiency of plasma catalytic gas treatment, because the catalyst activation may be limited by constraining the discharge to the contact points of the beads. The production of reactive species occurs most in the positive restrikes, the surface discharges and the local microdischarges in between the beads, and is less significant in the longer filamentary microdischarges. The faster streamer propagation and discharge development with higher dielectric constant of the packing beads leads to a faster production of reactive species. This study is of great interest for plasma catalysis, where packing beads with different dielectric constants are often used as supports for the catalytic materials. It allows us to better understand how different packing materials can influence the performance of packed bed plasma reactors for environmental applications.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000418533400246 Publication Date 2017-11-23
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1385-8947 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.216 Times cited 36 Open Access Not_Open_Access: Available from 10.01.2020
Notes (up) We acknowledge financial support from the Fund for Scientific Research Flanders (FWO) (grant nos G.0217.14 N, G.0254.14 N and G.0383.16 N), the TOP-BOF project of the University of Antwerp, the European Marie Skłodowska-Curie Individual Fellowship “GlidArc” within Horizon2020 (Grant No. 657304) and the Institute for the Promotion of Innovation by Science and Technology in Flanders (IWT Flanders). This research was carried out in the framework of the network on Physical Chemistry of Plasma-Surface Interactions – Interuniversity Attraction Poles, phase VII (http://psi-iap7.ulb.ac.be/), and supported by the Belgian Science Policy Office (BELSPO). The calculations were carried out 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: 6.216
Call Number PLASMANT @ plasmant @c:irua:147864 Serial 4800
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Author Bercx, M.; Sarmadian, N.; Saniz, R.; Partoens, B.; Lamoen, D.
Title First-principles analysis of the spectroscopic limited maximum efficiency of photovoltaic absorber layers for CuAu-like chalcogenides and silicon Type A1 Journal article
Year 2016 Publication Physical chemistry, chemical physics Abbreviated Journal Phys Chem Chem Phys
Volume 18 Issue 18 Pages 20542-20549
Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT)
Abstract Chalcopyrite semiconductors are of considerable interest for application as absorber layers in thin-film photovoltaic cells. When growing films of these compounds, however, they are often found to contain CuAu-like domains, a metastable phase of chalcopyrite. It has been reported that for CuInS2, the presence of the CuAu-like phase improves the short circuit current of the chalcopyrite-based photovoltaic cell. We investigate the thermodynamic stability of both phases for a selected list of I-III-VI2 materials using a first-principles density functional theory approach. For the CuIn-VI2 compounds, the difference in formation energy between the chalcopyrite and CuAu-like phase is found to be close to 2 meV per atom, indicating a high likelihood of the presence of CuAu-like domains. Next, we calculate the spectroscopic limited maximum efficiency (SLME) of the CuAu-like phase and compare the results with those of the corresponding chalcopyrite phase. We identify several candidates with a high efficiency, such as CuAu-like CuInS2, for which we obtain an SLME of 29% at a thickness of 500 nm. We observe that the SLME can have values above the Shockley-Queisser (SQ) limit, and show that this can occur because the SQ limit assumes the absorptivity to be a step function, thus overestimating the radiative recombination in the detailed balance approach. This means that it is possible to find higher theoretical efficiencies within this framework simply by calculating the J-V characteristic with an absorption spectrum. Finally, we expand our SLME analysis to indirect band gap absorbers by studying silicon, and find that the SLME quickly overestimates the reverse saturation current of indirect band gap materials, drastically lowering their calculated efficiency.
Address EMAT & CMT groups, Department of Physics, University of Antwerp, Campus Groenenborger, Groenenborgerlaan 171, 2020 Antwerp, Belgium. marnik.bercx@uantwerpen.be
Corporate Author Thesis
Publisher Place of Publication Editor
Language English Wos 000381428600058 Publication Date 2016-07-08
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1463-9076 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.123 Times cited 34 Open Access
Notes (up) We acknowledge financial support of FWO-Vlaanderen through projects G.0150.13N and G.0216.14N and ERA-NET RUS Plus/FWO, Grant G0D6515N. The computational resources and services used in this work were provided by the VSC (Flemish Supercomputer Center) and the HPC infrastructure of the University of Antwerp (CalcUA), both funded by the FWO FWOVlaanderen. Approved Most recent IF: 4.123
Call Number c:irua:135091 Serial 4112
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Author Cassidy, S.J.; Batuk, M.; Batuk, D.; Hadermann, J.; Woodruff, D.N.; Thompson, A.L.; Clarke, S.J.
Title Complex Microstructure and Magnetism in Polymorphic CaFeSeO Type A1 Journal article
Year 2016 Publication Inorganic chemistry Abbreviated Journal Inorg Chem
Volume 55 Issue 55 Pages 10714-10726
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The structural complexity of the antiferromagnetic oxide selenide CaFeSeO is described. The compound contains puckered FeSeO layers composed of FeSe2O2 tetrahedra sharing all their vertexes. Two polymorphs coexist that can be derived from an archetype BaZnSO structure by cooperative tilting of the FeSe2O2 tetrahedra. The polymorphs differ in the relative arrangement of the puckered layers of vertex-linked FeSe2O2 tetrahedra. In a noncentrosymmetric Cmc21 polymorph (a = 3.89684(2) A, b = 13.22054(8) A, c = 5.93625(2) A) the layers are related by the C-centering translation, while in a centrosymmetric Pmcn polymorph, with a similar cell metric (a = 3.89557(6) A, b = 13.2237(6) A, c = 5.9363(3) A), the layers are related by inversion. The compound shows long-range antiferromagnetic order below a Neel temperature of 159(1) K with both polymorphs showing antiferromagnetic coupling via Fe-O-Fe linkages and ferromagnetic coupling via Fe-Se-Fe linkages within the FeSeO layers. The magnetic susceptibility also shows evidence for weak ferromagnetism which is modeled in the refinements of the magnetic structure as arising from an uncompensated spin canting in the noncentrosymmetric polymorph. There is also a spin glass component to the magnetism which likely arises from the disordered regions of the structure evident in the transmission electron microscopy.
Address Department of Chemistry, Inorganic Chemistry Laboratory, University of Oxford , South Parks Road, Oxford OX1 3QR, United Kingdom
Corporate Author Thesis
Publisher Place of Publication Editor
Language English Wos 000385785700085 Publication Date 2016-10-05
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0020-1669 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.857 Times cited 6 Open Access
Notes (up) We acknowledge the financial support of the EPSRC (Grants EP/I017844/1 and EP/M020517/1), the Leverhulme Trust (RPG-2014-221), and the Diamond Light Source (studentship support for S. J. Cassidy). We thank the ESTEEM2 network for enabling the electron microscopy investigations and the ISIS facility and the Diamond Light Source Ltd. for the award of beam time. We thank Dr. P. Manuel for assistance on WISH, Dr. R. I. Smith for assistance on GEM and POLARIS, and Dr. C. Murray and Dr. A. Baker for assistance on I11. Approved Most recent IF: 4.857
Call Number EMAT @ emat @ c:irua:136823 Serial 4312
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Author Xu, W.; Van Alphen, S.; Galvita, V.V.; Meynen, V.; Bogaerts, A.
Title Effect of Gas Composition on Temperature and CO2Conversion in a Gliding Arc Plasmatron reactor: Insights for Post‐Plasma Catalysis from Experiments and Computation Type A1 Journal Article
Year 2024 Publication ChemSusChem Abbreviated Journal ChemSusChem
Volume Issue Pages
Keywords A1 Journal Article; CO2 conversion · Plasma · Gliding arc plasmatron · Temperature profiles · Computational modelling; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Abstract Plasma‐based CO<sub>2</sub>conversion has attracted increasing interest. However, to understand the impact of plasma operation on post‐plasma processes, we studied the effect of adding N<sub>2</sub>, N<sub>2</sub>/CH<sub>4</sub>and N<sub>2</sub>/CH<sub>4</sub>/H<sub>2</sub>O to a CO<sub>2</sub>gliding arc plasmatron (GAP) to obtain valuable insights into their impact on exhaust stream composition and temperature, which will serve as feed gas and heat for post‐plasma catalysis (PPC). Adding N<sub>2</sub>improves the CO<sub>2</sub>conversion from 4 % to 13 %, and CH<sub>4</sub>addition further promotes it to 44 %, and even to 61 % at lower gas flow rate (6 L/min), allowing a higher yield of CO and hydrogen for PPC. The addition of H<sub>2</sub>O, however, reduces the CO<sub>2</sub>conversion from 55 % to 22 %, but it also lowers the energy cost, from 5.8 to 3 kJ/L. Regarding the temperature at 4.9 cm post‐plasma, N<sub>2</sub>addition increases the temperature, while the CO<sub>2</sub>/CH<sub>4</sub>ratio has no significant effect on temperature. We also calculated the temperature distribution with computational fluid dynamics simulations. The obtained temperature profiles (both experimental and calculated) show a decreasing trend with distance to the exhaust and provide insights in where to position a PPC bed.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001200297300001 Publication Date 2024-04-11
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1864-5631 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.4 Times cited Open Access
Notes (up) We acknowledge the VLAIO Catalisti Moonshot project D2M and the VLAIO Catalisti transition project CO2PERATE (HBC.2017.0692) for financial support. We acknowledge Gilles Van Loon for his help to make the quartz and steel devices for the reactor. Vladimir V. Galvita also acknowledges a personal grant from the Research Fund of Ghent University (BOF; 01N16319). Approved Most recent IF: 8.4; 2024 IF: 7.226
Call Number PLASMANT @ plasmant @c:irua:205101 Serial 9128
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Author Bogaerts, A.; Yusupov, M.; Razzokov, J.; Van der Paal, J.
Title Plasma for cancer treatment: How can RONS penetrate through the cell membrane? Answers from computer modeling Type A1 Journal article
Year 2019 Publication Frontiers of Chemical Science and Engineering Abbreviated Journal Front Chem Sci Eng
Volume Issue Pages
Keywords A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract Plasma is gaining increasing interest for cancer

treatment, but the underlying mechanisms are not yet fully

understood. Using computer simulations at the molecular

level, we try to gain better insight in how plasma-generated

reactive oxygen and nitrogen species (RONS) can

penetrate through the cell membrane. Specifically, we

compare the permeability of various (hydrophilic and

hydrophobic) RONS across both oxidized and nonoxidized cell membranes. We also study pore formation,

and how it is hampered by higher concentrations of

cholesterol in the cell membrane, and we illustrate the

much higher permeability of H2O2 through aquaporin

channels. Both mechanisms may explain the selective

cytotoxic effect of plasma towards cancer cells. Finally, we

also discuss the synergistic effect of plasma-induced

oxidation and electric fields towards pore formation.

Keywords plasma medicine, cancer treatment, computer

modelling, cell membrane, reactive oxygen and nitrogen

species
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000468848400004 Publication Date 2019-03-22
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2095-0179 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 1.712 Times cited 5 Open Access Not_Open_Access: Available from 23.05.2020
Notes (up) We acknowledge financial support from the Research Foundation–Flanders (FWO; Grant Nos. 1200216N and 11U5416N). The computational work was carried out using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UA), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the UA. We are also very thankful to R. Cordeiro for the very interesting discussions. Approved Most recent IF: 1.712
Call Number PLASMANT @ plasmant @UA @ admin @ c:irua:159977 Serial 5172
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Author Batuk, D.; Tsirlin, A.A.; Filimonov, D.S.; Zakharov, K.V.; Volkova, O.S.; Vasiliev, A.; Hadermann, J.; Abakumov, A.M.
Title Bi(3n+1)Ti7Fe(3n-3)O(9n+11) Homologous Series: Slicing Perovskite Structure with Planar Interfaces Containing Anatase-like Chains Type A1 Journal article
Year 2016 Publication Inorganic chemistry Abbreviated Journal Inorg Chem
Volume 55 Issue 55 Pages 1245-1257
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The n = 3-6 members of a new perovskite-based homologous series Bi(3n+1)Ti7Fe(3n-3)O(9n+11) are reported. The crystal structure of the n = 3 Bi10Ti7Fe6O38 member is refined using a combination of X-ray and neutron powder diffraction data (a = 11.8511(2) A, b = 3.85076(4) A, c = 33.0722(6) A, S.G. Immm), unveiling the partially ordered distribution of Ti(4+) and Fe(3+) cations and indicating the presence of static random displacements of the Bi and O atoms. All Bi(3n+1)Ti7Fe(3n-3)O(9n+11) structures are composed of perovskite blocks separated by translational interfaces parallel to the (001)p perovskite planes. The thickness of the perovskite blocks increases with n, while the atomic arrangement at the interfaces remains the same. The interfaces comprise chains of double edge-sharing (Fe,Ti)O6 octahedra connected to the octahedra of the perovskite blocks by sharing edges and corners. This configuration shifts the adjacent perovskite blocks relative to each other over a vector (1/2)[110]p and creates S-shaped tunnels along the [010] direction. The tunnels accommodate double columns of the Bi(3+) cations, which stabilize the interfaces owing to the stereochemical activity of their lone electron pairs. The Bi(3n+1)Ti7Fe(3n-3)O(9n+11) structures can be formally considered either as intergrowths of perovskite modules and polysynthetically twinned modules of the Bi2Ti4O11 structure or as intergrowths of the 2D perovskite and 1D anatase fragments. Transmission electron microscopy (TEM) on Bi10Ti7Fe6O38 reveals that static atomic displacements of Bi and O inside the perovskite blocks are not completely random; they are cooperative, yet only short-range ordered. According to TEM, the interfaces can be laterally shifted with respect to each other over +/-1/3a, introducing an additional degree of disorder. Bi10Ti7Fe6O38 is paramagnetic in the 1.5-1000 K temperature range due to dilution of the magnetic Fe(3+) cations with nonmagnetic Ti(4+). The n = 3, 4 compounds demonstrate a high dielectric constant of 70-165 at room temperature.
Address Center for Electrochemical Energy Storage, Skolkovo Institute of Science and Technology , Nobelya str. 3, 143026 Moscow, Russia
Corporate Author Thesis
Publisher Place of Publication Editor
Language English Wos 000369356800031 Publication Date 2016-01-09
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0020-1669 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.857 Times cited 3 Open Access
Notes (up) We are grateful to the Laboratory for Neutron Scattering and Imaging of Paul Scherrer Institut (LNS PSI, Villigen, Switzerland) for granting beam time at the HRPT diffrac- tometer and to Dr. Denis Sheptyakov for the technical support during the experiment. We are also grateful to Valery Verchenko for his help with magnetization measurements. The work has been supported by the Russian Science Foundation (grant 14-13-00680). A.A.T. was partly supported by the Federal Ministry for Education and Science through a Sofja Kovalevskaya Award of Alexander von Humboldt Foundation. Approved Most recent IF: 4.857
Call Number c:irua:132247 Serial 4073
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Author Gorbanev, Y.; Verlackt, C.C.W.; Tinck, S.; Tuenter, E.; Foubert, K.; Cos, P.; Bogaerts, A.
Title Combining experimental and modelling approaches to study the sources of reactive species induced in water by the COST RF plasma jet Type A1 Journal article
Year 2018 Publication Physical chemistry, chemical physics Abbreviated Journal Phys Chem Chem Phys
Volume 20 Issue 4 Pages 2797-2808
Keywords A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract The vast biomedical potential of cold atmospheric pressure plasmas (CAPs) is governed by the formation of reactive species. These biologically active species are formed upon the interaction of CAPs with the surroundings. In biological milieu, water plays an essential role. The development of biomedical CAPs thus requires understanding of the sources of the reactive species in aqueous media exposed to the plasma. This is especially important in case of the COST RF plasma jet, which is developed as a reference microplasma system. In this work, we investigated the formation of the OH radicals, H atoms and H2O2 in aqueous solutions exposed to the COST plasma jet. This was done by combining experimental and modelling approaches. The liquid phase species were analysed using UV-Vis spectroscopy and spin trapping with hydrogen isotopes and electron paramagnetic resonance (EPR) spectroscopy. The discrimination between the species formed from the liquid phase and the gas phase molecules was performed by EPR and 1H-NMR analyses of the liquid samples. The concentrations of the reactive species in the gas phase plasma were obtained using a zero-dimensional (0D) chemical kinetics computational model. A three-dimensional (3D) fluid dynamics model was developed to provide information on the induced humidity in the plasma effluent. The comparison of the experimentally obtained trends for the formation of the species as a function of the feed gas and effluent humidity with the modelling results suggest that all reactive species detected in our system are mostly formed in the gas phase plasma inside the COST jet, with minor amounts arising from the plasma effluent humidity.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000423505500066 Publication Date 2018-01-05
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1463-9076 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.123 Times cited 23 Open Access OpenAccess
Notes (up) We are grateful to Volker Schulz-von der Gathen (Experimental Physics II: Application Oriented Plasma Physics, Ruhr-Universita¨t Bochum, Germany) for providing the COST RF plasma jet. We thank our colleagues at the University of Antwerp: Gilles Van Loon (Mechanical Workshop), Karen Leyssens (Research group PLASMANT), and Sylvia Dewilde (Department of Biomedical Sciences) for their help with the equipment. This work was funded by the European Marie Sklodowska-Curie Individual Fellowship ‘LTPAM’ within Horizon2020 (grant no. 657304). Stefan Tinck thanks the Fund for Scientific Research – Flanders (FWO) for supporting his work (grant no. 0880.212.840). Approved Most recent IF: 4.123
Call Number PLASMANT @ plasmant @c:irua:148365 Serial 4808
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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).
Address
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 (up) 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 Matsubara, M.; Saniz, R.; Partoens, B.; Lamoen, D.
Title Doping anatase TiO2with group V-b and VI-b transition metal atoms: a hybrid functional first-principles study Type A1 Journal article
Year 2017 Publication Physical chemistry, chemical physics Abbreviated Journal Phys Chem Chem Phys
Volume 19 Issue 19 Pages 1945-1952
Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT)
Abstract We investigate the role of transition metal atoms of group V-b (V, Nb, Ta) and VI-b (Cr, Mo, W) as n- or p-type dopants in anatase TiO$2$ using thermodynamic

principles and density functional theory with the Heyd-Scuseria-Ernzerhof HSE06 hybrid functional. The HSE06 functional provides a realistic value for the band gap, which ensures a correct classification of dopants as shallow or deep donors or acceptors. Defect formation energies and thermodynamic transition levels are calculated taking into account the constraints imposed by the stability of TiO$
2$ and the solubility limit of the impurities.

Nb, Ta, W and Mo are identified as shallow donors. Although W provides two electrons, Nb and Ta show a considerable lower formation energy, in particular under O-poor conditions. Mo donates in principle one electron, but under specific conditions can turn into a double donor. V impurities are deep donors and Cr

shows up as an amphoteric defect, thereby acting as an electron trapping center in n-type TiO$_2$ especially under O-rich conditions. A comparison with the available experimental data yields excellent agreement.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000394426400027 Publication Date 2016-12-12
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1463-9076 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.123 Times cited 19 Open Access OpenAccess
Notes (up) We gratefully acknowledge financial support from the IWTVlaanderenthrough projects G.0191.08 and G.0150.13, and the BOF-NOI of the University of Antwerp. This work was carried out using the HPC infrastructure of the University of Antwerp (CalcUA), a division of the Flemish Supercomputer Center VSC, which is funded by the Hercules foundation. M. M. acknowledges financial support from the GOA project ‘‘XANES meets ELNES’’ of the University of Antwerp. Approved Most recent IF: 4.123
Call Number EMAT @ emat @ c:irua:140835 Serial 4421
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Author Shetty, S.; Sinha, S.K.; Ahmad, R.; Singh, A.K.; Van Tendeloo, G.; Ravishankar, N.
Title Existence of Ti2+States on the Surface of Heavily Reduced SrTiO3Nanocubes Type A1 Journal article
Year 2017 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume Issue Pages acs.chemmater.7b04113
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Using advanced electron microscopy, we demonstrate the presence of Ti2+ on the 001 surfaces of heavily reduced strontium titanate nanocubes. While high-angle annular dark field images show a clear difference between the surfaces of the unreduced and reduced samples, electron energy loss spectroscopy detects the presence of Ti2+ on the surface of the reduced cubes. Conventional reduction only leads to the formation of Ti3+ and involves the use of high temperatures. In our case, reduction is achieved at relatively lower temperatures in the solid state using sodium borohydride as the reducing agent. Our findings provide insights into the optical properties of the samples and provide a convenient method to produce highly reduced surfaces that could demonstrate a range of exotic physical phenomena
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000418206600005 Publication Date 2017-11-17
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 9.466 Times cited 8 Open Access OpenAccess
Notes (up) We thank Advanced Facility for Microscopy and Microanalysis (AFMM), IISc, Bangalore for providing the TEM facility. We also thank MNCF, CeNSE, IISc for providing the XPS and FT-IR facilities. We acknowledge the help from Prof. Anshu Pandey for providing the PL facility and Mr. Ashutosh Gupta for the help with measurements. SS and NR thank DST for providing the financial support. RA and AKS acknowledge Super Computing Education and Research Center (SERC) and Materials Research Center (MRC), at IISc for providing required computational facilities. RA acknowledges the financial support from INSPIRE fellowship, AORC.Science and Engineering Research Board; Federaal Wetenschapsbeleid; Department of Science and Technology, Ministry of Science and Technology; Approved Most recent IF: 9.466
Call Number UA @ lucian @c:irua:147191 Serial 4767
Permanent link to this record
 

 
Author Saniz, R.; Bekaert, J.; Partoens, B.; Lamoen, D.
Title Structural and electronic properties of defects at grain boundaries in CuInSe2 Type A1 Journal article
Year 2017 Publication Physical chemistry, chemical physics Abbreviated Journal Phys Chem Chem Phys
Volume 19 Issue 19 Pages 14770-14780
Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT)
Abstract We report on a first-principles study of the structural and electronic properties of a Sigma3 (112) grain boundary model in CuInSe2. The study focuses on a coherent, stoichiometry preserving, cation–Se terminated grain boundary, addressing the properties of the grain boundary as such, as well as the effect

of well known defects in CuInSe2. We show that in spite of its apparent simplicity, such a grain boundary exhibits a very rich phenomenology, providing an explanation for several of the experimentally observed properties of grain boundaries in CuInSe2 thin films. In particular, we show that the combined effect of Cu vacancies and cation antisites can result in the observed Cu depletion with no In enrichment at the grain boundaries. Furthermore, Cu vacancies are unlikely to produce a hole barrier at the grain boundaries, but Na may indeed have such an effect. We find that Na-on-Cu defects will tend to form abundantly at

the grain boundaries, and can provide a mechanism for the carrier depletion and/or type inversion experimentally reported.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000403327200059 Publication Date 2017-05-12
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1463-9076 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.123 Times cited 12 Open Access OpenAccess
Notes (up) We thank B. Schoeters for his assistance running the GBstudio software. We acknowledge the financial support of FWO-Vlaanderen through project G.0150.13. The computational resources and services used in this work were provided by the VSC (Flemish Supercomputer Center) and the HPC infrastructure of the University of Antwerp (CalcUA), both funded by FWO-Vlaanderen and the Flemish Government-department EWI. Approved Most recent IF: 4.123
Call Number EMAT @ emat @ c:irua:143869 Serial 4577
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Author Zhang, Y.; Qin, S.; Claes, N.; Schilling, W.; Sahoo, P.K.; Ching, H.Y.V.; Jaworski, A.; Lemière, F.; Slabon, A.; Van Doorslaer, S.; Bals, S.; Das, S.
Title Direct Solar Energy-Mediated Synthesis of Tertiary Benzylic Alcohols Using a Metal-Free Heterogeneous Photocatalyst Type A1 Journal article
Year 2022 Publication ACS Sustainable Chemistry and Engineering Abbreviated Journal Acs Sustain Chem Eng
Volume 10 Issue 1 Pages 530-540
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Organic synthesis (ORSY)
Abstract Direct hydroxylation via the functionalization of tertiary benzylic C(sp3)-H bond is of great significance for obtaining tertiary alcohols which find wide applications in pharmaceuticals as well as in fine chemical industries. However, current synthetic procedures use toxic reagents and therefore, the development of a sustainable strategy for the synthesis of tertiary benzyl alcohols is highly desirable. To solve this problem, herein, we report a metal-free

heterogeneous photocatalyst to synthesize the hydroxylated products using oxygen as the key reagent. Various benzylic substrates were employed into our mild reaction conditions to afford the desirable products in good to excellent yields. More importantly, gram-scale reaction was achieved via harvesting direct solar energy and exhibited high quantity of the product. The high stability of the catalyst was proved via recycling the catalyst and spectroscopic analyses. Finally, a possible mechanism was proposed based on the EPR and other experimental

evidence.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000736518000001 Publication Date 2022-01-10
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 24 Open Access OpenAccess
Notes (up) We thank BOF joint PhD grant (to Y. Z.), Francqui Foundation and FWO research grant (to S.D.), Chinese Scholarship Council (to Y.Z.). A.S. would like to thank the Swedish Energy Agency for financial support (project nr: 5050-1). The SEM microscope was partly funded by the Hercules Fund from the Flemish Government. Approved Most recent IF: 8.4
Call Number EMAT @ emat @c:irua:184744 Serial 6900
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Author Paria Sena, R.; Babaryk, A.A.; Khainakov, S.; Garcia-Granda, S.; Slobodyanik, N.S.; Van Tendeloo, G.; Abakumov, A.M.; Hadermann, J.
Title A pseudo-tetragonal tungsten bronze superstructure: a combined solution of the crystal structure of K6.4(Nb,Ta)36.3O94 with advanced transmission electron microscopy and neutron diffraction Type A1 Journal article
Year 2016 Publication Journal of the Chemical Society : Dalton transactions Abbreviated Journal Dalton T
Volume 45 Issue 45 Pages 973-979
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The crystal structure of the K6.4Nb28.2Ta8.1O94 pseudo-tetragonal tungsten bronze-type oxide was determined using a combination of X-ray powder diffraction, neutron diffraction and transmission electron microscopy techniques, including electron diffraction, high angle annular dark field scanning transmission electron microscopy (HAADF-STEM), annular bright field STEM (ABF-STEM) and energy-dispersive X-ray compositional mapping (STEM-EDX). The compound crystallizes in the space group Pbam with unit cell parameters a = 37.468(9) A, b = 12.493(3) A, c = 3.95333(15) A. The structure consists of corner sharing (Nb,Ta)O6 octahedra forming trigonal, tetragonal and pentagonal tunnels. All tetragonal tunnels are occupied by K(+) ions, while 1/3 of the pentagonal tunnels are preferentially occupied by Nb(5+)/Ta(5+) and 2/3 are occupied by K(+) in a regular pattern. A fractional substitution of K(+) in the pentagonal tunnels by Nb(5+)/Ta(5+) is suggested by the analysis of the HAADF-STEM images. In contrast to similar structures, such as K2Nb8O21, also parts of the trigonal tunnels are fractionally occupied by K(+) cations.
Address Electron Microscopy for Materials Research (EMAT), University of Antwerp, Groenenborgerlaan 171, B-2020, Antwerp, Belgium. joke.hadermann@uantwerpen.be babaryk@univ.kiev.ua
Corporate Author Thesis
Publisher Place of Publication Editor
Language English Wos 000367614700018 Publication Date 2015-11-23
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1477-9226 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.029 Times cited 6 Open Access
Notes (up) We thank Dr E. Suard and Dr O. Fabello for assistance in collecting the neutron diffraction data. R.P.S. acknowledges funding from the European Research Council under the 7th Framework Program (FP7), ERC Grant No. 246791-COUNTATOMS. The titan microscope was partly funded by the Hercules fund from the Flemish Government. The authors acknowledge financial support from the European Union under the Seventh Framework Program under a contract for an Integrated Infrastructure Initiative. Reference No. 312483-ESTEEM2. AAB acknowledges the JSPDS ICDD Grant-in-Aid program (12-02).; esteem2jra1; esteem2jra2 Approved Most recent IF: 4.029
Call Number c:irua:130408 c:irua:130408 Serial 3998
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Author Fuchs, J.; Aghaei, M.; Schachel, T.D.; Sperling, M.; Bogaerts, A.; Karst, U.
Title Impact of the Particle Diameter on Ion Cloud Formation from Gold Nanoparticles in ICPMS Type A1 Journal article
Year 2018 Publication Analytical chemistry Abbreviated Journal Anal Chem
Volume 90 Issue 17 Pages 10271-10278
Keywords A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract The unique capabilities of microsecond dwell time (DT) single-particle inductively coupled plasma mass spectrometry (spICPMS) were utilized to characterize the cloud of ions generated from the introduction of suspensions of gold nanoparticles (AuNPs) into the plasma. A set of narrowly distributed particles with diameters ranging from 15.4 to 100.1 nm was synthesized and characterized according to established protocols. Statistically significant numbers of the short transient spICPMS events were evaluated by using 50 μs DT for their summed intensity, maximum intensity, and duration, of which all three were found to depend on the particle diameter. The summed intensity increases from 10 to 1661 counts and the maximum intensity from 6 to 309 counts for AuNPs with diameters from 15.4 to 83.2 nm. The event duration rises from 322 to 1007 μs upon increasing AuNP diameter. These numbers represent a comprehensive set of key data points of the ion clouds generated in ICPMS from AuNPs. The extension of event duration is of high interest to appoint the maximum possible particle number concentration at which separation of consecutive events in spICPMS can still be achieved. Moreover, the combined evaluation of all above-mentioned ion cloud characteristics can explain the regularly observed prolonged single-particle events. The transport and ionization behavior of AuNPs in the ICP was also computationally modeled to gain insight into the size-dependent signal generation. The simulated data reveals that the plasma temperature, and therefore the point of ionization of the particles, is the same for all diameters. However, the maximum number density of Au+, as well as the extent of the ion cloud, depends on the particle diameter, in agreement with the experimental data, and it provides an adequate explanation for the observed ion cloud characteristics.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000444060600028 Publication Date 2018-09-04
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0003-2700 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.32 Times cited 5 Open Access OpenAccess
Notes (up) We thank Dr. Harald Rösner from the Institute of Materials Physics of the University of Münster for the TEM imaging. Approved Most recent IF: 6.32
Call Number PLASMANT @ plasmant @c:irua:153651 Serial 5057
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Author Chin, C.–M.; Battle, P.D.; Hunter, E.C.; Avdeev, M.; Hendrickx, M.; Hadermann, J.
Title Magnetic properties of La3Ni2Sb Ta Nb1––O9; from relaxor to spin glass Type A1 Journal article
Year 2019 Publication Journal of solid state chemistry (Print) Abbreviated Journal Journal of Solid State Chemistry
Volume 273 Issue Pages 175-185
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Neutron diffraction experiments conducted at 5 K in a magnetic field 0 < H/kOe < 50 have shown that the monoclinic perovskite La3Ni2TaO9 behaves as a relaxor ferromagnet. Compositions in the series La3Ni2SbxTayNb1–x–yO9 have been synthesized in polycrystalline form. Electron microscopy, X–ray diffraction and neutron diffraction have shown that the solid solutions are largely homogeneous and monophasic. Magnetometry and neutron diffraction have shown that the relaxor magnetisation persists in low fields when x + y = 1 but is rapidly diminished by the introduction of niobium. This change in magnetic behaviour is ascribed to the differences in the d–orbital energies of Sb5+, Nb5+ and Ta5+.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000466261100026 Publication Date 2019-03-02
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0022-4596 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor Times cited Open Access
Notes (up) We thank EPSRC for funding through grant EP/M0189541. CMC thanks the Croucher Foundation and the University of Oxford for the award of a graduate scholarship. Approved no
Call Number EMAT @ emat @c:irua:166445 Serial 6346
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Author Jin, L.; Batuk, M.; Kirschner, F.K.K.; Lang, F.; Blundell, S.J.; Hadermann, J.; Hayward, M.A.
Title Exsolution of SrO during the Topochemical Conversion of LaSr3CoRuO8to the Oxyhydride LaSr3CoRuO4H4 Type A1 Journal article
Year 2019 Publication Inorganic chemistry Abbreviated Journal Inorg Chem
Volume 58 Issue 21 Pages 14863-14870
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Reaction of the n = 1 Ruddlesden-Popper oxide LaSr3CoRuO8 with CaH2 yields the oxyhydride phase LaSr3CoRuO4H4 via topochemical anion-exchange. Close inspection of X-ray and neutron powder diffraction data in combination with HAADF-STEM images reveals that nanoparticles of SrO are exsolved from the system during the reaction, with the change in cation stoichiometry accommodated by the inclusion of n > 1 (Co/Ru)nOn+1H2n ‘perovskite’ layers into the Ruddlesden-Popper stacking sequence. This novel pseudo-topochemical process offers a new route for the formation of n > 1 Ruddlesden-Popper structured materials. Magnetization data are consistent with a LaSr3Co1+Ru2+O4H4 (Co1+, d8, S = 1; Ru2+, d6, S = 0) oxidation/spin state combination. Neutron diffraction and μ+SR data show no evidence for long-range magnetic order down to 2 K, suggesting the diamagnetic Ru2+ centers impede the Co-Co magnetic exchange interactions.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000494894400062 Publication Date 2019-11-04
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0020-1669 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.857 Times cited 1 Open Access
Notes (up) We thank P. Manuel for assistance collecting the neutron powder diffraction data. We thank The Leverhulme Trust grant award RPG-2014-366 “Topochemical reduction of 4d and 5d transition metal oxides” for supporting this work. Experiments at the Diamond Light Source were performed as part of the Block Allocation Group award “Oxford Solid State Chemistry BAG to probe composition-structure-property relationships in solids” (EE13284). Investigation by TEM was supported through the FWO grant G035619N. Approved Most recent IF: 4.857
Call Number EMAT @ emat @c:irua:164625 Serial 5434
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Author Xu, X.; Jones, M.A.; Cassidy, S.J.; Manuel, P.; Orlandi, F.; Batuk, M.; Hadermann, J.; Clarke, S.J.
Title Magnetic Ordering in the Layered Cr(II) Oxide Arsenides Sr2CrO2Cr2As2and Ba2CrO2Cr2As2 Type A1 Journal article
Year 2020 Publication Inorganic Chemistry Abbreviated Journal Inorg Chem
Volume 59 Issue 21 Pages 15898-15912
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Sr2CrO2Cr2As2 and Ba2CrO2Cr2As2 with Cr2+ ions in CrO2 sheets and in CrAs layers crystallize with the Sr2Mn3Sb2O2 structure (space group I4/mmm, Z = 2) and lattice parameters a = 4.00800(2) Å, c = 18.8214(1) Å (Sr2CrO2Cr2As2) and a = 4.05506(2) Å, c = 20.5637(1) Å (Ba2CrO2Cr2As2) at room temperature. Powder neutron diffraction reveals checkerboard-type antiferromagnetic ordering of the Cr2+ ions in the arsenide layers below TN1Sr, of 600(10) K (Sr2CrO2Cr2As2) and TN1Ba 465(5) K (Ba2CrO2Cr2As2) with the moments initially directed perpendicular to the layers in both compounds. Checkerboard-type antiferromagnetic ordering of the Cr2+ ions in the oxide layer below 230(5) K for Ba2CrO2Cr2As2 occurs with these moments also perpendicular to the layers, consistent with the orientation preferences of d4 moments in the two layers. In contrast, below 330(5) K in Sr2CrO2Cr2As2, the oxide layer Cr2+ moments are initially oriented in the CrO2 plane; but on further cooling, these moments rotate to become perpendicular to the CrO2 planes, while the moments in the arsenide layers rotate by 90° with the moments on the two sublattices remaining orthogonal throughout [behavior recently reported independently by Liu et al. [Liu et al. Phys. Rev. B 2018, 98, 134416]]. In Sr2CrO2Cr2As2, electron diffraction and high resolution powder X-ray diffraction data show no evidence for a structural distortion that would allow the two Cr2+ sublattices to couple, but high resolution neutron powder diffraction data suggest a small incommensurability between the magnetic structure and the crystal structure, which may account for the coupling of the two sublattices and the observed spin reorientation. The saturation values of the Cr2+ moments in the CrO2 layers (3.34(1) μB (for Sr2CrO2Cr2As2) and 3.30(1) μB (for Ba2CrO2Cr2As2)) are larger than those in the CrAs layers (2.68(1) μB for Sr2CrO2Cr2As2 and 2.298(8) μB for Ba2CrO2Cr2As2) reflecting greater covalency in the arsenide layers.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000588738100035 Publication Date 2020-11-02
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0020-1669 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.6 Times cited Open Access OpenAccess
Notes (up) We thank the UK EPSRC (EP/M020517/1 and EP/P018874/ 1) and the Leverhulme Trust (RPG-2014-221) for funding and the ISIS pulsed neutron and muon source (RB1610357 and RB1700075) and the Diamond Light Source Ltd. (EE13284 and EE18786) for the award of beam time. We thank Dr. A. Baker and Dr. C. Murray for support on I11. Approved Most recent IF: 4.6; 2020 IF: 4.857
Call Number EMAT @ emat @c:irua:176058 Serial 6704
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Author Oliveira, M.C.; Yusupov, M.; Bogaerts, A.; Cordeiro, R.M.
Title Distribution of lipid aldehydes in phase-separated membranes: A molecular dynamics study Type A1 Journal article
Year 2022 Publication Archives Of Biochemistry And Biophysics Abbreviated Journal Arch Biochem Biophys
Volume 717 Issue Pages 109136
Keywords A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract It is well established that lipid aldehydes (LAs) are able to increase the permeability of cell membranes and induce their rupture. However, it is not yet clear how LAs are distributed in phase-separated membranes (PSMs), which are responsible for the transport of selected molecules and intracellular signaling. Thus, we investigate here the distribution of LAs in a PSM by coarse-grained molecular dynamics simulations. Our results reveal that LAs derived from mono-unsaturated lipids tend to accumulate at the interface between the liquid-ordered/liquiddisordered domains, whereas those derived from poly-unsaturated lipids remain in the liquid-disordered domain. These results are important for understanding the effects caused by oxidized lipids in membrane structure, properties and organization.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000767632000001 Publication Date 2022-01-24
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0003-9861 ISBN Additional Links UA library record; WoS full record
Impact Factor 3.9 Times cited Open Access OpenAccess
Notes (up) We thank the University of Antwerp and the Coordination of Superior Level Staff Improvement (CAPES, Brazil) for the scholarship granted. The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UAntwerpen), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the UAntwerpen. Approved Most recent IF: 3.9
Call Number PLASMANT @ plasmant @c:irua:185874 Serial 6905
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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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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001058978000001 Publication Date 2023-01-05
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 (up) 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 %).
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000946293200001 Publication Date 2023-02-09
Series Editor Series Title Abbreviated Series Title
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 (up) 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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