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Author Vanraes, P.; Parayil Venugopalan, S.; Besemer, M.; Bogaerts, A.
Title Assessing neutral transport mechanisms in aspect ratio dependent etching by means of experiments and multiscale plasma modeling Type A1 Journal Article
Year 2023 Publication Plasma Sources Science and Technology Abbreviated Journal Plasma Sources Sci. Technol.
Volume 32 Issue 6 Pages 064004
Keywords A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Abstract Since the onset of pattern transfer technologies for chip manufacturing, various strategies have been developed to circumvent or overcome aspect ratio dependent etching (ARDE). These methods have, however, their own limitations in terms of etch non-idealities, throughput or costs. Moreover, they have mainly been optimized for individual in-device features and die-scale patterns, while occasionally ending up with poor patterning of metrology marks, affecting the alignment and overlay in lithography. Obtaining a better understanding of the underlying mechanisms of ARDE and how to mitigate them therefore remains a relevant challenge to date, for both marks and advanced nodes. In this work, we accordingly assessed the neutral transport mechanisms in ARDE by means of experiments and multiscale modeling for SiO<sub>2</sub>etching with CHF<sub>3</sub>/Ar and CF<sub>4</sub>/Ar plasmas. The experiments revealed a local maximum in the etch rate for an aspect ratio around unity, i.e. the simultaneous occurrence of regular and inverse reactive ion etching lag for a given etch condition. We were able to reproduce this ARDE trend in the simulations without taking into account charging effects and the polymer layer thickness, suggesting shadowing and diffuse reflection of neutrals as the primary underlying mechanisms. Subsequently, we explored four methods with the simulations to regulate ARDE, by varying the incident plasma species fluxes, the amount of polymer deposition, the ion energy and angular distribution and the initial hardmask sidewall angle, for which the latter was found to be promising in particular. Although our study focusses on feature dimensions characteristic to metrology marks and back-end-of-the-line integration, the obtained insights have a broader relevance, e.g. to the patterning of advanced nodes. Additionally, this work supports the insight that physisorption may be more important in plasma etching at room temperature than originally thought, in line with other recent studies, a topic on which we recommend further research.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001021250100001 Publication Date 2023-06-01
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0963-0252 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.8 Times cited Open Access Not_Open_Access
Notes P Vanraes acknowledges funding by ASML for the project ‘Computational simulation of plasma etching of trench structures’. P Vanraes and A Bogaerts want to express their gratitude to Mark J Kushner (University of Michigan) for the sharing of the HPEM and MCFPM codes, and for the interesting exchange of views. P Vanraes wishes to thank Violeta Georgieva and Stefan Tinck for the fruitful discussions on the HPEM code, Yu-Ru Zhang for an example of the CCP reactor code and Karel Venken for his technical help with the server maintenance and use. S P Venugopalan and M Besemer wish to thank Luigi Scaccabarozzi, Sander Wuister, Coen Verschuren, Michael Kubis, Kuan-Ming Chen, Ruben Maas, Huaichen Zhang and Julien Mailfert (ASML) for the insightful discussions. Approved Most recent IF: 3.8; 2023 IF: 3.302
Call Number PLASMANT @ plasmant @c:irua:197760 Serial (down) 8811
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Author Sa, J.; Hu, N.; Heyvaert, W.; Van Gordon, K.; Li, H.; Wang, L.; Bals, S.; Liz-Marzán, L.M.; Ni, W.
Title Spontaneous Chirality Evolved at the Au–Ag Interface in Plasmonic Nanorods Type A1 Journal article
Year 2023 Publication Chemistry of materials Abbreviated Journal Chem. Mater.
Volume Issue Pages
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Chiral ligands are considered a required ingredient during the synthesis of dissymmetric plasmonic metal nanocrystals. The mechanism behind the generation of chiral structures involves the formation of high Miller index chiral facets, induced by the adsorption of such chiral ligands. We found however that, chirality can also evolve spontaneously, without the involvement of any chiral ligands, during the co-deposition of Au and Ag on Au nanorods. When using a specific Au/Ag ratio, phase segregation of the two metals leads to an interface within the obtained AuAg shell, which can be exposed by removing the Ag component via oxidative etching. Although a close-to-racemic mixture of chiral Au nanorods with right and left handedness is found in solution, electron tomography analysis evidences left- and righthanded helicities, both at the Au-Ag interface and at the exposed surface of Au NRs after Ag etching. The helicity profile of the NRs indicates dominating inclination angles in a range from 30° to 60°. Single-particle optical characterization also reveals random handedness in the plasmonic response of individual nanorods. We hypothesize that, the origin of chirality is related with symmetry breaking during the co-deposition of Au and Ag, through an initial perturbation in a small region on the Au-Ag interface that eventually leads to chiral segregation throughout the nanocrystal.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001052093300001 Publication Date 2023-08-21
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756 ISBN Additional Links UA library record; WoS full record
Impact Factor 8.6 Times cited Open Access OpenAccess
Notes The authors acknowledge the financial support from the National Natural Science Foundation of China (grant 22074102). LMLM acknowledges funding from 26 MCIN/AEI/10.13039/501100011033 and “ESF Investing in your future” (Grant PID2020- 117779RB-I00). This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 823717 – ESTEEM3.; Ministerio de Ciencia e Innovaci?n, PID2020-117779RB-I00 ; H2020 Research Infrastructures, 823717 ; European Social Fund, PID2020-117779RB-I00 ; National Natural Science Foundation of China, 22074102 ; Approved Most recent IF: 8.6; 2023 IF: 9.466
Call Number EMAT @ emat @c:irua:198151 Serial (down) 8810
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Author Paulus, A.; Hendrickx, M.; Mayda, S.; Batuk, M.; Reekmans, G.; von Holst, M.; Elen, K.; Abakumov, A.M.; Adriaensens, P.; Lamoen, D.; Partoens, B.; Hadermann, J.; Van Bael, M.K.; Hardy, A.
Title Understanding the Activation of Anionic Redox Chemistry in Ti4+-Substituted Li2MnO3as a Cathode Material for Li-Ion Batteries Type A1 Journal article
Year 2023 Publication ACS applied energy materials Abbreviated Journal ACS Appl. Energy Mater.
Volume 6 Issue 13 Pages 6956-6971
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT)
Abstract Layered Li-rich oxides, demonstrating both cationic and anionic redox chemistry being used as positive electrodes for Li-ion batteries,have raised interest due to their high specific discharge capacities exceeding 250 mAh/g. However, irreversible structural transformations triggered by anionic redox chemistry result in pronounced voltagefade (i.e., lowering the specific energy by a gradual decay of discharge potential) upon extended galvanostatic cycling. Activating or suppressing oxygen anionic redox through structural stabilization induced by redox-inactivecation substitution is a well-known strategy. However, less emphasishas been put on the correlation between substitution degree and theactivation/suppression of the anionic redox. In this work, Ti4+-substituted Li2MnO3 was synthesizedvia a facile solution-gel method. Ti4+ is selected as adopant as it contains no partially filled d-orbitals. Our study revealedthat the layered “honeycomb-ordered” C2/m structure is preserved when increasing the Ticontent to x = 0.2 in the Li2Mn1-x Ti (x) O-3 solidsolution, as shown by electron diffraction and aberration-correctedscanning transmission electron microscopy. Galvanostatic cycling hintsat a delayed oxygen release, due to an improved reversibility of theanionic redox, during the first 10 charge-discharge cyclesfor the x = 0.2 composition compared to the parentmaterial (x = 0), followed by pronounced oxygen redoxactivity afterward. The latter originates from a low activation energybarrier toward O-O dimer formation and Mn migration in Li2Mn0.8Ti0.2O3, as deducedfrom first-principles molecular dynamics (MD) simulations for the“charged” state. Upon lowering the Ti substitution to x = 0.05, the structural stability was drastically improvedbased on our MD analysis, stressing the importance of carefully optimizingthe substitution degree to achieve the best electrochemical performance.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001018266700001 Publication Date 2023-07-10
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2574-0962 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.4 Times cited Open Access Not_Open_Access: Available from 24.12.2023
Notes Universiteit Hasselt, AUHL/15/2 – GOH3816N ; Russian Science Foundation, 20-43-01012 ; Fonds Wetenschappelijk Onderzoek, AUHL/15/2 – GOH3816N G040116N ; 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 Vlaanderen and the Flemish Government-department EWI. Approved Most recent IF: 6.4; 2023 IF: NA
Call Number EMAT @ emat @c:irua:198160 Serial (down) 8809
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Author Arteaga Cardona, F.; Jain, N.; Popescu, R.; Busko, D.; Madirov, E.; Arús, B.A.; Gerthsen, D.; De Backer, A.; Bals, S.; Bruns, O.T.; Chmyrov, A.; Van Aert, S.; Richards, B.S.; Hudry, D.
Title Preventing cation intermixing enables 50% quantum yield in sub-15 nm short-wave infrared-emitting rare-earth based core-shell nanocrystals Type A1 Journal article
Year 2023 Publication Nature communications Abbreviated Journal Nat Commun
Volume 14 Issue 1 Pages 4462
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Short-wave infrared (SWIR) fluorescence could become the new gold standard in optical imaging for biomedical applications due to important advantages such as lack of autofluorescence, weak photon absorption by blood and tissues, and reduced photon scattering coefficient. Therefore, contrary to the visible and NIR regions, tissues become translucent in the SWIR region. Nevertheless, the lack of bright and biocompatible probes is a key challenge that must be overcome to unlock the full potential of SWIR fluorescence. Although rare-earth-based core-shell nanocrystals appeared as promising SWIR probes, they suffer from limited photoluminescence quantum yield (PLQY). The lack of control over the atomic scale organization of such complex materials is one of the main barriers limiting their optical performance. Here, the growth of either homogeneous (α-NaYF<sub>4</sub>) or heterogeneous (CaF<sub>2</sub>) shell domains on optically-active α-NaYF<sub>4</sub>:Yb:Er (with and without Ce<sup>3+</sup>co-doping) core nanocrystals is reported. The atomic scale organization can be controlled by preventing cation intermixing only in heterogeneous core-shell nanocrystals with a dramatic impact on the PLQY. The latter reached 50% at 60 mW/cm<sup>2</sup>; one of the highest reported PLQY values for sub-15 nm nanocrystals. The most efficient nanocrystals were utilized for in vivo imaging above 1450 nm.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001037058500022 Publication Date 2023-07-25
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2041-1723 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 16.6 Times cited 1 Open Access OpenAccess
Notes D.H. would like to thank Dominique Ectors (Bruker AXS GmbH, Karlsruhe, Germany) for assistance and discussion on the PXRD data and TOPAS evaluations. The authors would like to acknowledge the financial support provided by the Helmholtz Association via: i) the Professorial Recruitment Initiative Funding (B.S.R.); ii) the Research Field Energy – Program Materials and Technologies for the Energy Transition – Topic 1 Photovoltaics (F.A.C., D.B., E.M., B.S.R., D.H.). This project received funding from the European Union’s Horizon 2020 innovation programme under grant agreement 823717. This work was supported by the European Research Council (grant 770887-PICOMETRICS to S.V.A. and Grant 815128-REALNANO to S.B.). The authors acknowledge financial support from the ResearchFoundation Flanders (FWO, Belgium) through project fundings (G.0346.21 N to S.V.A. and S.B.) and a postdoctoral grant (A.D.B.). The authors (B.A.A., O.T.B. and A.C.) acknowledge funding from the Helmholtz Zentrum München, the DFG-Emmy Noether program (BR 5355/2-1) and from the CZI Deep Tissue Imaging (DTI-0000000248). The authors (O.T.B. and D.H.) would like to thank the Helmholtz Imaging (ZT-I-PF-4-038-BENIGN). Approved Most recent IF: 16.6; 2023 IF: 12.124
Call Number EMAT @ emat @c:irua:198158 Serial (down) 8808
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Author Kelly, S.; Mercer, E.; De Meyer, R.; Ciocarlan, R.-G.; Bals, S.; Bogaerts, A.
Title Microwave plasma-based dry reforming of methane: Reaction performance and carbon formation Type A1 Journal article
Year 2023 Publication Journal of CO2 utilization Abbreviated Journal Journal of CO2 Utilization
Volume 75 Issue Pages 102564
Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Abstract e investigate atmospheric pressure microwave (MW) plasma (2.45 GHz) conversion in CO2 and CH4 mixtures (i.e., dry reforming of methane, DRM) focusing on reaction performance and carbon formation. Promising energy costs of ~2.8–3.0 eV/molecule or ~11.1–11.9 kJ/L are amongst the best performance to date considering the current state-of-the-art for plasma-based DRM for all types of plasma. The conversion is in the range of ~46–49% and ~55–67% for CO2 and CH4, respectively, producing primarily syngas (i.e., H2 and CO) with H2/CO ratios of ~0.6–1 at CH4 fractions ranging from 30% to 45%. Water is the largest byproduct with levels ranging ~7–14% in the exhaust. Carbon particles visibly impact the plasma at higher CH4 fractions (> 30%), where they become heated and incandescent. Particle luminosity increases with increasing CH4 fractions, with the plasma becoming unstable near a 1:1 mixture (i.e., > 45% CH4). Electron microscopy of the carbon material reveals an agglomerated morphology of pure carbon nanoparticles. The mean particle size is determined as ~20 nm, free of any metal contamination, consistent with the electrode-less MW design.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001065310000001 Publication Date 2023-08-10
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2212-9820 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 7.7 Times cited 6 Open Access OpenAccess
Notes We acknowledge financial support by a European Space Agency (ESA) Open Science Innovation Platform study (contract no. 4000137001/21/NL/GLC/ov), the European 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), the Excellence of Science FWOFNRS PLASyntH2 project (FWO grant no. G0I1822N and EOS no. 4000751) and the Methusalem project of the University of Antwerp Approved Most recent IF: 7.7; 2023 IF: 4.292
Call Number PLASMANT @ plasmant @c:irua:198155 Serial (down) 8807
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Author Loenders, B.; Michiels, R.; Bogaerts, A.
Title Is a catalyst always beneficial in plasma catalysis? Insights from the many physical and chemical interactions Type A1 Journal Article
Year 2023 Publication Journal of Energy Chemistry Abbreviated Journal Journal of Energy Chemistry
Volume 85 Issue Pages 501-533
Keywords A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Abstract Plasma-catalytic dry reforming of CH4 (DRM) is promising to convert the greenhouse gasses CH4 and CO2 into value-added chemicals, thus simultaneously providing an alternative to fossil resources as feedstock for the chemical industry. However, while many experiments have been dedicated to plasma-catalytic DRM, there is no consensus yet in literature on the optimal choice of catalyst for targeted products, because the underlying mechanisms are far from understood. Indeed, plasma catalysis is very complex, as it encompasses various chemical and physical interactions between plasma and catalyst, which depend on many parameters. This complexity hampers the comparison of experimental results from different studies, which, in our opinion, is an important bottleneck in the further development of this promising research field. Hence, in this perspective paper, we describe the important physical and chemical effects that should be accounted for when designing plasma-catalytic experiments in general, highlighting the need for standardized experimental setups, as well as careful documentation of packing properties and reaction conditions, to further advance this research field. On the other hand, many parameters also create many windows of opportunity for further optimizing plasma-catalytic systems. Finally, various experiments also reveal the lack of improvement in plasma catalysis compared to plasma-only, specifically for DRM, but the underlying mechanisms are unclear. Therefore, we present our newly developed coupled plasma-surface kinetics model for DRM, to provide more insight in the underlying reasons. Our model illustrates that transition metal catalysts can adversely affect plasmacatalytic DRM, if radicals dominate the plasma-catalyst interactions. Thus, we demonstrate that a good understanding of the plasma-catalyst interactions is crucial to avoiding conditions at which these interactions negatively affect the results, and we provide some recommendations for improvement. For instance, we believe that plasma-catalytic DRM may benefit more from higher reaction temperatures, at which vibrational excitation can enhance the surface reactions.
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Publisher Place of Publication Editor
Language Wos Publication Date 2023-06-30
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2095-4956 ISBN Additional Links UA library record
Impact Factor 13.1 Times cited Open Access Not_Open_Access
Notes This research was supported by the FWO-SBO project PlasMa- CatDESIGN (FWO grant ID S001619N), the FWO fellowship of R. Michiels (FWO grant ID 1114921N), 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 computational resources and services used in this work were provided by the HPC core facility CalcUA of the Universiteit Antwerpen, and VSC (Flemish Supercomputer Center), funded by the Research Foundation – Flanders (FWO) and the Flemish Government. Approved Most recent IF: 13.1; 2023 IF: 2.594
Call Number PLASMANT @ plasmant @c:irua:198159 Serial (down) 8806
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Author Vijayakumar, J.; Savchenko, T.M.; Bracher, D.M.; Lumbeeck, G.; Béché, A.; Verbeeck, J.; Vajda, Š.; Nolting, F.; Vaz, Ca.f.; Kleibert, A.
Title Absence of a pressure gap and atomistic mechanism of the oxidation of pure Co nanoparticles Type A1 Journal article
Year 2023 Publication Nature communications Abbreviated Journal Nat Commun
Volume 14 Issue 1 Pages 174
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Understanding chemical reactivity and magnetism of 3<italic>d</italic>transition metal nanoparticles is of fundamental interest for applications in fields ranging from spintronics to catalysis. Here, we present an atomistic picture of the early stage of the oxidation mechanism and its impact on the magnetism of Co nanoparticles. Our experiments reveal a two-step process characterized by (i) the initial formation of small CoO crystallites across the nanoparticle surface, until their coalescence leads to structural completion of the oxide shell passivating the metallic core; (ii) progressive conversion of the CoO shell to Co<sub>3</sub>O<sub>4</sub>and void formation due to the nanoscale Kirkendall effect. The Co nanoparticles remain highly reactive toward oxygen during phase (i), demonstrating the absence of a pressure gap whereby a low reactivity at low pressures is postulated. Our results provide an important benchmark for the development of theoretical models for the chemical reactivity in catalysis and magnetism during metal oxidation at the nanoscale.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000955726400021 Publication Date 2023-01-12
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2041-1723 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 16.6 Times cited 1 Open Access OpenAccess
Notes Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung, 200021160186 2002153540 ; EC | Horizon 2020 Framework Programme, 810310 823717 ; University of Basel | Swiss Nanoscience Institute, P1502 ; This work is funded by Swiss National Foundation (SNF) (Grants. No 200021160186 and 2002153540) and the Swiss Nanoscience Institut (SNI) (Grant No. SNI P1502). S.V. acknowledges support from the European Union’s Horizon 2020 research and innovation programme under grant agreement no. 810310, which corresponds to the J. Heyrovsky Chair project (“ERA Chair at J. Heyrovský Institute of Physical Chemistry AS CR – The institutional approach towards ERA”). The funders had no role in the preparation of the article. Part of this work was performed at the Surface/Interface: Microscopy (SIM) beamline of the Swiss Light Source (SLS), Paul Scherrer Institut, Villigen, Switzerland. We kindly acknowledge Anja Weber and Elisabeth Müller from PSI for their help in fabricating the sample markers. A.B. and J. Verbeeck received funding from the European Union’s Horizon 2020 Research Infrastructure – Integrating Activities for Advanced Communities under grant agreement No. 823717 – ESTEEM3 reported Approved Most recent IF: 16.6; 2023 IF: 12.124
Call Number EMAT @ emat @c:irua:196738 Serial (down) 8804
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Author Abduvokhidov, D.; Yusupov, M.; Shahzad, A.; Attri, P.; Shiratani, M.; Oliveira, M.C.; Razzokov, J.
Title Unraveling the Transport Properties of RONS across Nitro-Oxidized Membranes Type A1 Journal Article
Year 2023 Publication Biomolecules Abbreviated Journal Biomolecules
Volume 13 Issue 7 Pages 1043
Keywords A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Abstract The potential of cold atmospheric plasma (CAP) in biomedical applications has received significant interest, due to its ability to generate reactive oxygen and nitrogen species (RONS). Upon exposure to living cells, CAP triggers alterations in various cellular components, such as the cell membrane. However, the permeation of RONS across nitrated and oxidized membranes remains understudied. To address this gap, we conducted molecular dynamics simulations, to investigate the permeation capabilities of RONS across modified cell membranes. This computational study investigated the translocation processes of less hydrophilic and hydrophilic RONS across the phospholipid bilayer (PLB), with various degrees of oxidation and nitration, and elucidated the impact of RONS on PLB permeability. The simulation results showed that less hydrophilic species, i.e., NO, NO2, N2O4, and O3, have a higher penetration ability through nitro-oxidized PLB compared to hydrophilic RONS, i.e., HNO3, s-cis-HONO, s-trans-HONO, H2O2, HO2, and OH. In particular, nitro-oxidation of PLB, induced by, e.g., cold atmospheric plasma, has minimal impact on the penetration of free energy barriers of less hydrophilic species, while it lowers these barriers for hydrophilic RONS, thereby enhancing their translocation across nitro-oxidized PLB. This research contributes to a better understanding of the translocation abilities of RONS in the field of plasma biomedical applications and highlights the need for further analysis of their role in intracellular signaling pathways.
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Publisher Place of Publication Editor
Language Wos 001035160000001 Publication Date 2023-06-27
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2218-273X ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor Times cited Open Access Not_Open_Access
Notes This research was funded by the Innovative Development Agency of the Republic of Uzbekistan, grant number FZ-2020092817. Approved Most recent IF: NA
Call Number PLASMANT @ plasmant @c:irua:198154 Serial (down) 8803
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Author Adhami Sayad Mahaleh, M.; Narimisa, M.; Nikiforov, A.; Gromov, M.; Gorbanev, Y.; Bitar, R.; Morent, R.; De Geyter, N.
Title Nitrogen Oxidation in a Multi-Pin Plasma System in the Presence and Absence of a Plasma/Liquid Interface Type A1 Journal Article
Year 2023 Publication Applied Sciences Abbreviated Journal Applied Sciences
Volume 13 Issue 13 Pages 7619
Keywords A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Abstract The recent energy crisis revealed that there is a strong need to replace hydrocarbon-fueled industrial nitrogen fixation processes by alternative, more sustainable methods. In light of this, plasma-based nitrogen fixation remains one of the most promising options, considering both theoretical and experimental aspects. Lately, plasma interacting with water has received considerable attention in nitrogen fixation applications as it can trigger a unique gas- and liquid-phase chemistry. Within this context, a critical exploration of plasma-assisted nitrogen fixation with or without water presence is of great interest with an emphasis on energy costs, particularly in plasma reactors which have potential for large-scale industrial application. In this work, the presence of water in a multi-pin plasma system on nitrogen oxidation is experimentally investigated by comparing two pulsed negative DC voltage plasmas in metal–metal and metal–liquid electrode configurations. The plasma setups are designed to create similar plasma properties, including plasma power and discharge regime in both configurations. The system energy cost is calculated, considering nitrogen-containing species generated in gas and liquid phases as measured by a gas analyzer, nitrate sensor, and a colorimetry method. The energy cost profile as a function of specific energy input showed a strong dependency on the plasma operational frequency and the gas flow rate, as a result of different plasma operation regimes and initiated reverse processes. More importantly, the presence of the plasma/liquid interface increased the energy cost up to 14 ± 8%. Overall, the results showed that the presence of water in the reaction zone has a negative impact on the nitrogen fixation process.
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Publisher Place of Publication Editor
Language Wos 001031217300001 Publication Date 2023-06-28
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2076-3417 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 2.7 Times cited Open Access Not_Open_Access
Notes NITROPLASM FWO-FNRS Excellence of Science, 30505023 ; European Union-NextGenerationEU, G0G2322N ; Approved Most recent IF: 2.7; 2023 IF: 1.679
Call Number PLASMANT @ plasmant @c:irua:198153 Serial (down) 8802
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Author Muravev, V.; Parastaev, A.; van den Bosch, Y.; Ligt, B.; Claes, N.; Bals, S.; Kosinov, N.; Hensen, E.J.M.
Title Size of cerium dioxide support nanocrystals dictates reactivity of highly dispersed palladium catalysts Type A1 Journal article
Year 2023 Publication Science Abbreviated Journal
Volume 380 Issue 6650 Pages 1174-1179
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract The catalytic performance of heterogeneous catalysts can be tuned by modulation of the size and structure of supported transition metals, which are typically regarded as the active sites. In single-atom metal catalysts, the support itself can strongly affect the catalytic properties. Here, we demonstrate that the size of cerium dioxide (CeO2) support governs the reactivity of atomically dispersed palladium (Pd) in carbon monoxide (CO) oxidation. Catalysts with small CeO2 nanocrystals (~4 nanometers) exhibit unusually high activity in a CO-rich reaction feed, whereas catalysts with medium-size CeO2 (~8 nanometers) are preferred for lean conditions. Detailed spectroscopic investigations reveal support size–dependent redox properties of the Pd-CeO2 interface.
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Publisher Place of Publication Editor
Language Wos 001010846100008 Publication Date 2023-06-16
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0036-8075 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 56.9 Times cited 22 Open Access OpenAccess
Notes We thank the staff of the MAX IV Laboratory for time on beamline SPECIES under proposals 20200412 and 20190983; E. Kokkonen and A. Klyushin for assistance with NAP-XPS and RPES experiments conducted at SPECIES; staff of the MAX IV Laboratory for time on beamline BALDER under proposal 20200378; K. Klementiev for assistance with XAS measurements; J. Drnec at the ESRF for providing assistance in using beamline ID31; and V. Perez-Dieste and I. Villar Garcia at the CIRCE beamline at ALBA Synchrotron for help with acquiring preliminary RPES data obtained under proposal 2020024219. The synchrotron-based XRD measurements were performed on beamline ID31 at the European Synchrotron Radiation Facility (ESRF), Grenoble, France. Funding: This work was supported by the Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), a NWO Gravitation program funded by the Ministry of Education, Culture and Science of the Government of the Netherlands (V.M. and E.J.M.H.); the European Research Council (ERC consolidator grant 815128 REALNANO to S.B. and N.C.); and the European Union’s Horizon 2020 Research and Innovation Program (grant 823717–ESTEEM to S.B. and N.C). Research conducted at MAX IV, a Swedish national user facility, is supported by the Swedish Research council under contract 2018-07152, the Swedish Governmental Agency for Innovation Systems under contract 2018-04969, and Formas under contract 2019-02496 (VM). Approved Most recent IF: 56.9; 2023 IF: 37.205
Call Number EMAT @ emat @c:irua:197199 Serial (down) 8801
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Author Carrasco, S.; Orcajo, G.; Martínez, F.; Imaz, I.; Kavak, S.; Arenas-Esteban, D.; Maspoch, D.; Bals, S.; Calleja, G.; Horcajada, P.
Title Hf/porphyrin-based metal-organic framework PCN-224 for CO2 cycloaddition with epoxides Type A1 Journal article
Year 2023 Publication Materials Today Advances Abbreviated Journal
Volume 19 Issue Pages 100390
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Herein, we describe for the first time the synthesis of the highly porous Hf-tetracarboxylate porphyrin-based metal-organic framework (MOF) (Hf)PCN-224(M) (M = H2, Co2+). (Hf)PCN-224(H2) was easily and efficiently prepared following a simple microwave-assisted procedure with good yields (56–67%; space-time yields: 1100–1270 kg m−3·day−1), high crystallinity and phase purity by using trifluoromethanesulfonic acid and benzoic acid as modulators in less than 30 min. By simply introducing a preliminary step (10 min), 5,10,15,20-(tetra-4-carboxyphenyl)porphyrin linker (TCPP) was quantitatively metalated with Co2+ without additional purification and/or time consuming protection/deprotection steps to further obtain (Hf)PCN-224(Co). (Hf)PCN-224(Co) was then tested as catalyst in CO2 cycloaddition reaction with different epoxides to yield cyclic carbonates, showing the best catalytic performance described to date compared to other PCNs, under mild conditions (1 bar CO2, room temperature, 18–24 h). Twelve epoxides were tested, obtaining from moderate to excellent conversions (35–96%). Moreover, this reaction was gram scaled-up (x50) without significant loss of yield to cyclic carbonates. (Hf)PCN-224(Co) maintained its integrity and crystallinity even after 8 consecutive runs, and poisoning was efficiently reverted by a simple thermal treatment (175 °C, 6 h), fully recovering the initial catalytic activity.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001025764000001 Publication Date 2023-06-19
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2590-0498 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 10 Times cited 1 Open Access OpenAccess
Notes S.C. acknowledges the European Union's Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie (MSCA-COFUND) grant agreement No 754382 (GOT Energy Talent). S.C. and P.H. acknowledge “Comunidad de Madrid” and European Regional Development Fund-FEDER 2014-2020-OE REACT-UE 1 for their financial support to VIRMOF-CM project associated to R&D projects in response to COVID-19. The authors acknowledge H2020-MSCA-ITN-2019 HeatNMof (ref. 860942), the M-ERA-NET C-MOF-cell (grant PCI2020-111998 funded by MCIN/AEI /10.13039/501100011033 and European Union NextGenerationEU/PRTR) project, and Retos Investigación MOFSEIDON (grant PID2019-104228RB-I00 funded by MCIN/AEI/10.13039/501100011033) project. This work has been also supported by the Regional Government of Madrid (Project ACES2030-CM, S2018/EMT-4319) and the Universidad Rey Juan Carlos IMPULSO Project (grant MATER M − 3000). S.K acknowledges the Flemish Fund for Scientific Research (FWO Vlaanderen) through a PhD research grant (1181122 N). Approved Most recent IF: 10; 2023 IF: NA
Call Number EMAT @ emat @c:irua:197198 Serial (down) 8800
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Author Vertongen, R.; Bogaerts, A.
Title How important is reactor design for CO2 conversion in warm plasmas? Type A1 Journal Article
Year 2023 Publication Journal of CO2 Utilization Abbreviated Journal
Volume 72 Issue Pages 102510
Keywords A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Abstract In this work, we evaluated several new electrode configurations for CO2 conversion in a gliding arc plasmatron

(GAP) reactor. Although the reactor design influences the performance, the best results give only slightly higher

CO2 conversion than the basic GAP reactor design, which indicates that this reactor may have reached its performance

limits. Moreover, we compared our results to those of four completely different plasma reactors, also

operating at atmospheric pressure and with contact between the plasma and the electrodes. Surprisingly, the

performance of all these warm plasmas is very similar (CO2 conversion around 10 % for an energy efficiency

around 30 %). In view of these apparent performance limits regarding the reactor design, we believe further

improvements should focus on other aspects, such as the post-plasma-region where the implementation of

nozzles or a carbon bed are promising. We summarize the performance of our GAP reactor by comparing the

energy efficiency and CO2 conversion for all different plasma reactors reported in literature. We can conclude

that the GAP is not the best plasma reactor, but its operation at atmospheric pressure makes it appealing for

industrial application. We believe that future efforts should focus on process design, techno-economic assessments

and large-scale demonstrations: these will be crucial to assess the real industrial potential of this warm

plasma technology
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001024970900001 Publication Date 2023-06-16
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2212-9820 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 7.7 Times cited Open Access Not_Open_Access
Notes We acknowledge financial support from the Fund for Scientific Research (FWO) Flanders (Grant ID 110221N) and the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreements No 810182 – SCOPE ERC Synergy project and No. 101081162 — “PREPARE” ERC Proof of Concept project). We also thank I. Tsonev, P. Heirman, F. Girard-Sahun and G. Trenchev for the interesting discussions and practical help with the experiments, as well as J. Creel for his ideas on the inserted anode designs. Approved Most recent IF: 7.7; 2023 IF: 4.292
Call Number PLASMANT @ plasmant @c:irua:197044 Serial (down) 8799
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Author Wang, J.; Zhang, K.; Mertens, M.; Bogaerts, A.; Meynen, V.
Title Plasma-based dry reforming of methane in a dielectric barrier discharge reactor: Importance of uniform (sub)micron packings/catalysts to enhance the performance Type A1 Journal Article
Year 2023 Publication APPLIED CATALYSIS B-ENVIRONMENTAL Abbreviated Journal
Volume 337 Issue Pages 122977
Keywords A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Abstract This study presents new insights on the effect of (sub)micrometer particle sized materials in plasma-based CO2-

CH4 reforming by investigating the performance of SiO2 spheres (with/without supported metal) of varying

particle sizes. (Sub)micron particles synthesized through the St¨ober method were used instead of (sub)millimeter

particles employed in previous studies. Increasing particle size (from 120 nm to 2390 nm) was found to first

increase and then decrease conversion and energy yield, with optimal performance achieved using 740 nm 5 wt%

Ni loaded SiO2, which improved CO2 and CH4 conversion, and energy yield to 44%, 55%, and 0.271 mmol/kJ,

respectively, compared to 20%, 27%, and 0.116 mmol/kJ in an empty reactor at the same flow rate. This is the

first to achieve significant performance improvement in a fully packed reactor, highlighting the importance of

selecting a suitable particle size. The findings can offer guidance towards rational design of catalysts for plasmabased

reactions.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001056527600001 Publication Date 2023-06-09
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0926-3373 ISBN Additional Links UA library record; WoS full record
Impact Factor 22.1 Times cited Open Access Not_Open_Access
Notes This work is supported by the China Scholarship Council (No. 201806060123); and the VLAIO Catalisti transition project CO2PERATE (HBC.2017.0692). 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). Approved Most recent IF: 22.1; 2023 IF: 9.446
Call Number PLASMANT @ plasmant @c:irua:196955 Serial (down) 8798
Permanent link to this record
 

 
Author Wang, J.; Zhang, K.; Mertens, M.; Bogaerts, A.; Meynen, V.
Title Plasma-based dry reforming of methane in a dielectric barrier discharge reactor: Importance of uniform (sub)micron packings/catalysts to enhance the performance Type A1 Journal Article
Year 2023 Publication APPLIED CATALYSIS B-ENVIRONMENTAL Abbreviated Journal
Volume 337 Issue Pages 122977
Keywords A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Abstract This study presents new insights on the effect of (sub)micrometer particle sized materials in plasma-based CO2-

CH4 reforming by investigating the performance of SiO2 spheres (with/without supported metal) of varying

particle sizes. (Sub)micron particles synthesized through the St¨ober method were used instead of (sub)millimeter

particles employed in previous studies. Increasing particle size (from 120 nm to 2390 nm) was found to first

increase and then decrease conversion and energy yield, with optimal performance achieved using 740 nm 5 wt%

Ni loaded SiO2, which improved CO2 and CH4 conversion, and energy yield to 44%, 55%, and 0.271 mmol/kJ,

respectively, compared to 20%, 27%, and 0.116 mmol/kJ in an empty reactor at the same flow rate. This is the

first to achieve significant performance improvement in a fully packed reactor, highlighting the importance of

selecting a suitable particle size. The findings can offer guidance towards rational design of catalysts for plasmabased

reactions.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001056527600001 Publication Date 2023-06-09
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0926-3373 ISBN Additional Links UA library record; WoS full record
Impact Factor 22.1 Times cited Open Access Not_Open_Access
Notes This work is supported by the China Scholarship Council (No. 201806060123); and the VLAIO Catalisti transition project CO2PERATE (HBC.2017.0692). 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). Approved Most recent IF: 22.1; 2023 IF: 9.446
Call Number PLASMANT @ plasmant @c:irua:196955 Serial (down) 8797
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Author Saniz, R.; Baldinozzi, G.; Arts, I.; Lamoen, D.; Leinders, G.; Verwerft, M.
Title Charge order, frustration relief, and spin-orbit coupling in U3O8 Type A1 Journal article
Year 2023 Publication Physical review materials Abbreviated Journal
Volume 7 Issue 5 Pages 054410
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Research efforts on the description of the low-temperature magnetic order and electronic properties of U3O8 have been inconclusive so far. Reinterpreting neutron scattering results, we use group representation theory to show that the ground state presents collinear out-of-plane magnetic moments, with antiferromagnetic coupling both in-layer and between layers. Charge order relieves the initial geometric frustration, generating a slightly distorted honeycomb sublattice with Néel-type order. The precise knowledge of the characteristics of this magnetic ground state is then used to explain the fine features of the band gap. In this system, spin-orbit coupling (SOC) is of critical importance, as it strongly affects the electronic structure, narrowing the gap by ∼38%, compared to calculations neglecting SOC. The predicted electronic structure actually explains the salient features of recent optical absorption measurements, further demonstrating the excellent agreement between the calculated ground state properties and experiment.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001041429800007 Publication Date 2023-05-31
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2475-9953 ISBN Additional Links UA library record; WoS full record
Impact Factor 3.4 Times cited Open Access OpenAccess
Notes Financial support for this research was partly provided by the Energy Transition Fund of the Belgian FPS Economy (Project SF-CORMOD Spent Fuel CORrosion MODeling).Fonds Wetenschappelijk Onderzoek; Vlaams Supercomputer Centrum; Universiteit Antwerpen; Vlaamse regering; Approved Most recent IF: 3.4; 2023 IF: NA
Call Number EMAT @ emat @c:irua:197043 Serial (down) 8796
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Author Vlasov, E.; Skorikov, A.; Sánchez-Iglesias, A.; Liz-Marzán, L.M.; Verbeeck, J.; Bals, S.
Title Secondary electron induced current in scanning transmission electron microscopy: an alternative way to visualize the morphology of nanoparticles Type A1 Journal article
Year 2023 Publication ACS materials letters Abbreviated Journal ACS Materials Lett.
Volume Issue Pages 1916-1921
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Electron tomography (ET) is a powerful tool to determine the three-dimensional (3D) structure of nanomaterials in a transmission electron microscope. However, the acquisition of a conventional tilt series for ET is a time-consuming process and can therefore not provide 3D structural information in a time-efficient manner. Here, we propose surface-sensitive secondary electron (SE) imaging as an alternative to ET for the investigation of the morphology of nanomaterials. We use the SE electron beam induced current (SEEBIC) technique that maps the electrical current arising from holes generated by the emission of SEs from the sample. SEEBIC imaging can provide valuable information on the sample morphology with high spatial resolution and significantly shorter throughput times compared with ET. In addition, we discuss the contrast formation mechanisms that aid in the interpretation of SEEBIC data.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001006191600001 Publication Date 2023-06-12
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2639-4979 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor Times cited 1 Open Access OpenAccess
Notes The funding for this project was provided by European Research Council (ERC Consolidator Grant 815128, REALNANO). J.V. acknowledges the eBEAM project, which is supported by the European Union’s Horizon 2020 research and innovation program under grant agreement no. 101017720 (FET-Proactive EBEAM). L.M.L.-M. acknowledges funding from MCIN/AEI/10.13039/501100011033 (grant # PID2020-117779RB-I00). Approved Most recent IF: NA
Call Number EMAT @ emat @c:irua:197004 Serial (down) 8795
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Author Tampieri, F.; Espona-Noguera, A.; Labay, C.; Ginebra, M.-P.; Yusupov, M.; Bogaerts, A.; Canal, C.
Title Does non-thermal plasma modify biopolymers in solution? A chemical and mechanistic study for alginate Type A1 Journal Article
Year 2023 Publication Biomaterials Science Abbreviated Journal
Volume Issue Pages
Keywords A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Abstract In the last decades, non-thermal plasma has been extensively investigated as a relevant tool for various biomedical applications, ranging from tissue decontamination to regeneration and from skin treatment to tumor therapies. This high versatility is due to the different kinds and amount of reactive oxygen and nitrogen species that can be generated during a plasma treatment and put in contact with the biological target. Some recent studies report that solutions of biopolymers with the ability to generate hydrogels, when treated with plasma, can enhance the generation of reactive species and influence their stability, resulting thus in the ideal media for indirect treatments of biological targets. The direct effects of the plasma treatment on the structure of biopolymers in water solution, as well as the chemical mechanisms responsible for the enhanced generation of RONS, are not yet fully understood. In this study, we aim at filling this gap by investigating, on the one hand, the nature and extent of the modifications induced by plasma treatment in alginate solutions, and, on the other hand, at using this information to explain the mechanisms responsible for the enhanced generation of reactive species as a consequence of the treatment. The approach we use is twofold: (i) investigating the effects of plasma treatment on alginate solutions, by size exclusion chromatography, rheology and scanning electron microscopy and (ii) study of a molecular model (glucuronate) sharing its chemical structure, by chromatography coupled with mass spectrometry and by molecular dynamics simulations. Our results point out the active role of the biopolymer chemistry during direct plasma treatment. Short-lived reactive species, such as OH radicals and O atoms, can modify the polymer structure, affecting its functional groups and causing partial fragmentation. Some of these chemical modifications, like the generation of organic peroxide, are likely responsible for the secondary generation of long-lived reactive species such as hydrogen peroxide and nitrite ions. This is relevant in view of using biocompatible hydrogels as vehicles for storage and delivery reactive species for targeted therapies.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000973699000001 Publication Date 2023-04-11
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2047-4830 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.6 Times cited Open Access Not_Open_Access
Notes Agència de Gestió d’Ajuts Universitaris i de Recerca, SGR2022-1368 ; H2020 European Research Council, 714793 ; European Cooperation in Science and Technology, CA19110 CA20114 ; Secretaría de Estado de Investigación, Desarrollo e Innovación, PID2019-103892RB-I00/AEI/10.13039/501100011033 ; We thank Gonzalo Rodríguez Cañada and Xavier Solé-Martí (Universitat Politècnica de Catalunya) for help in collecting some of the experimental data and for the useful discussions. This work has been primarily funded by the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (grant agreement no. 714793). The authors acknowledge MINECO for PID2019103892RB-I00/AEI/10.13039/501100011033 project (CC). The authors belong to SGR2022-1368 (FT, AEN, CL, MPG, CC) and acknowledge Generalitat de Catalunya for the ICREA Academia Award for Excellence in Research of CC. We thank also COST Actions CA20114 (Therapeutical Applications of Cold Plasmas) and CA19110 (Plasma Applications for Smart and Sustainable Agriculture) for the stimulating environment provided. Approved Most recent IF: 6.6; 2023 IF: 4.21
Call Number PLASMANT @ plasmant @c:irua:196773 Serial (down) 8794
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Author Kavak, S.; Kadu, A.A.; Claes, N.; Sánchez-Iglesias, A.; Liz-Marzán, L.M.; Batenburg, K.J.; Bals, S.
Title Quantitative 3D Investigation of Nanoparticle Assemblies by Volumetric Segmentation of Electron Tomography Data Sets Type A1 Journal article
Year 2023 Publication The journal of physical chemistry: C : nanomaterials and interfaces Abbreviated Journal
Volume 127 Issue 20 Pages 9725-9734
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Morphological characterization of nanoparticle assemblies and hybrid nanomaterials is critical in determining their structure-property relationships as well as in the development of structures with desired properties. Electron tomography has become a widely utilized technique for the three-dimensional characterization of nanoparticle assemblies. However, the extraction of quantitative morphological parameters from the reconstructed volume can be a complex and labor-intensive task. In this study, we aim to overcome this challenge by automating the volumetric segmentation process applied to three-dimensional reconstructions of nanoparticle assemblies. The key to enabling automated characterization is to assess the performance of different volumetric segmentation methods in accurately extracting predefined quantitative descriptors for morphological characterization. In our methodology, we compare the quantitative descriptors obtained through manual segmentation with those obtained through automated segmentation methods, to evaluate their accuracy and effectiveness. To show generality, our study focuses on the characterization of assemblies of CdSe/CdS quantum dots, gold nanospheres and CdSe/CdS encapsulated in polymeric micelles, and silica-coated gold nanorods decorated with both CdSe/CdS or PbS quantum dots. We use two unsupervised segmentation algorithms: the watershed transform and the spherical Hough transform. Our results demonstrate that the choice of automated segmentation method is crucial for accurately extracting the predefined quantitative descriptors. Specifically, the spherical Hough transform exhibits superior performance in accurately extracting quantitative descriptors, such as particle size and interparticle distance, thereby allowing for an objective, efficient, and reliable volumetric segmentation of complex nanoparticle assemblies.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000991752700001 Publication Date 2023-05-25
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1932-7447 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.7 Times cited 2 Open Access OpenAccess
Notes Fonds Wetenschappelijk Onderzoek, 1181122N ; Horizon 2020 Framework Programme, 861950 ; H2020 European Research Council, 815128 ; Approved Most recent IF: 3.7; 2023 IF: 4.536
Call Number EMAT @ emat @c:irua:196971 Serial (down) 8793
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Author Zheng, J.; Zhang, H.; Lv, J.; Zhang, M.; Wan, J.; Gerrits, N.; Wu, A.; Lan, B.; Wang, W.; Wang, S.; Tu, X.; Bogaerts, A.; Li, X.
Title Enhanced NH3Synthesis from Air in a Plasma Tandem-Electrocatalysis System Using Plasma-Engraved N-Doped Defective MoS2 Type A1 Journal Article
Year 2023 Publication JACS Au Abbreviated Journal JACS Au
Volume 3 Issue 5 Pages 1328-1336
Keywords A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Abstract We have developed a sustainable method to produce NH3 directly from air using a plasma tandem-electrocatalysis system that operates via the N2−NOx−NH3 pathway. To efficiently reduce NO2− to NH3, we propose a novel electrocatalyst consisting of defective N-doped molybdenum sulfide nanosheets on vertical graphene arrays (N-MoS2/VGs). We used a plasma engraving process to form the metallic 1T phase, N doping, and S vacancies in the electrocatalyst simultaneously. Our system exhibited a remarkable NH3 production rate of 7.3 mg h−1 cm−2 at −0.53 V vs RHE, which is almost 100 times higher than the state-of-the-art electrochemical nitrogen reduction reaction and more than double that of other hybrid systems. Moreover, a low energy consumption of only 2.4 MJ molNH3−1 was achieved in this study. Density functional theory calculations revealed that S vacancies and doped N atoms play a dominant role in the selective reduction of NO2− to NH3. This study opens up new avenues for efficient NH3 production using cascade systems.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000981779300001 Publication Date 2023-05-22
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2691-3704 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor Times cited Open Access Not_Open_Access
Notes ACKNOWLEDGMENTS This work was supported by the National Natural Science Foundation of China (51976191, 5227060056, 52276214) and the National Key Technologies R&D Program of China (2018YFE0117300). N.G. was financially supported through an NWO Rubicon Grant (019.202EN.012). X.T. acknowl- edges the support of the Engineering and Physical Sciences Research Council (EP/X002713/1). Approved Most recent IF: NA
Call Number PLASMANT @ plasmant @c:irua:196761 Serial (down) 8792
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Author Mary Joy, R.; Pobedinskas, P.; Bourgeois, E.; Chakraborty, T.; Görlitz, J.; Herrmann, D.; Noël, C.; Heupel, J.; Jannis, D.; Gauquelin, N.; D'Haen, J.; Verbeeck, J.; Popov, C.; Houssiau, L.; Becher, C.; Nesládek, M.; Haenen, K.
Title Germanium vacancy centre formation in CVD nanocrystalline diamond using a solid dopant source Type A3 Journal article
Year 2023 Publication Science talks Abbreviated Journal Science Talks
Volume 5 Issue Pages 100157
Keywords A3 Journal article; Electron microscopy for materials research (EMAT)
Abstract
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos Publication Date 2023-02-09
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2772-5693 ISBN Additional Links UA library record
Impact Factor Times cited Open Access OpenAccess
Notes Approved Most recent IF: NA
Call Number EMAT @ emat @c:irua:196969 Serial (down) 8791
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Author Samal, D.; Gauquelin, N.; Takamura, Y.; Lobato, I.; Arenholz, E.; Van Aert, S.; Huijben, M.; Zhong, Z.; Verbeeck, J.; Van Tendeloo, G.; Koster, G.
Title Unusual structural rearrangement and superconductivity in infinite layer cuprate superlattices Type A1 Journal article
Year 2023 Publication Physical review materials Abbreviated Journal
Volume 7 Issue 5 Pages 054803
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001041792100007 Publication Date 2023-05-30
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2475-9953 ISBN Additional Links UA library record; WoS full record
Impact Factor 3.4 Times cited Open Access OpenAccess
Notes Air Force Office of Scientific Research; European Office of Aerospace Research and Development, FA8655-10-1-3077 ; Office of Science, DE-AC02-05CH11231 ; National Science Foundation, DMR-1745450 ; Seventh Framework Programme, 278510 ; Bijzonder Onderzoeksfonds UGent; Approved Most recent IF: 3.4; 2023 IF: NA
Call Number EMAT @ emat @c:irua:196973 Serial (down) 8790
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Author Gauquelin, N.; Forte, F.; Jannis, D.; Fittipaldi, R.; Autieri, C.; Cuono, G.; Granata, V.; Lettieri, M.; Noce, C.; Miletto-Granozio, F.; Vecchione, A.; Verbeeck, J.; Cuoco, M.
Title Pattern Formation by Electric-Field Quench in a Mott Crystal Type A1 Journal article
Year 2023 Publication Nano letters Abbreviated Journal
Volume Issue Pages
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract The control of Mott phase is intertwined with the spatial reorganization of the electronic states. Out-of-equilibrium driving forces typically lead to electronic patterns that are absent at equilibrium, whose nature is however often elusive. Here, we unveil a nanoscale pattern formation in the Ca2 RuO4 Mott insulator. We demonstrate how an applied electric field spatially reconstructs the insulating phase that, uniquely after switching off the electric field, exhibits nanoscale stripe domains. The stripe pattern has regions with inequivalent octahedral distortions that we directly observe through high-resolution scanning transmission electron

microscopy. The nanotexture depends on the orientation of the electric field, it is non-volatile and rewritable. We theoretically simulate the charge and orbital reconstruction induced by a quench dynamics of the applied electric field providing clear-cut mechanisms for the stripe phase formation. Our results open the path for the design of non-volatile electronics based on voltage-controlled nanometric phases.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001012061600001 Publication Date 2023-05-18
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1530-6984 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 10.8 Times cited 2 Open Access OpenAccess
Notes This project has received funding from the European Union’s Horizon 2020 research and innova- tion programme under grant agreement No 823717 – ESTEEM3. The Merlin camera used in the experiment received funding from the FWO-Hercules fund G0H4316N ’Direct electron detector 15for soft matter TEM’. C. A. and G. C. are supported by the Foundation for Polish Science through the International Research Agendas program co-financed by the European Union within the Smart Growth Operational Programme. C. A. and G. C. acknowledge the access to the computing facil- ities of the Interdisciplinary Center of Modeling at the University of Warsaw, Grant No. GB84-0, GB84-1 and GB84-7 and GB84-7 and Poznan Supercomputing and Networking Center Grant No. 609.. C. A. and G. C. acknowledge the CINECA award under the ISCRA initiative IsC85 “TOP- MOST” Grant, for the availability of high-performance computing resources and support. We acknoweldge A. Guarino and C. Elia for providing support about the electrical characterization of the sample. M.C., R.F., and A.V. acknowledge support from the EU’s Horizon 2020213 research and innovation program under Grant Agreement No. 964398 (SUPERGATE). Approved Most recent IF: 10.8; 2023 IF: 12.712
Call Number EMAT @ emat @c:irua:196970 Serial (down) 8789
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Author Tsonev, I.; Boothroyd, J.; Kolev, S.; Bogaerts, A.
Title Simulation of glow and arc discharges in nitrogen: effects of the cathode emission mechanisms Type A1 Journal Article
Year 2023 Publication PLASMA SOURCES SCIENCE & TECHNOLOGY Abbreviated Journal
Volume 32 Issue 5 Pages 054002
Keywords A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Abstract Experimental evidence in the literature has shown that low-current direct current nitrogen discharges can exist in both glow and arc regimes at atmospheric pressure. However, modelling investigations of the positive column that include the influence of the cathode phenomena are scarce. In this work we developed a 2D axisymmetric model of a plasma discharge in flowing nitrogen gas, studying the influence of the two cathode emission mechanisms—thermionic field emission and secondary electron emission—on the cathode region and the positive column. We show for an inlet gas flow velocity of 1 m s<sup>−1</sup>in the current range of 80–160 mA, that the electron emission mechanism from the cathode greatly affects the size and temperature of the cathode region, but does not significantly influence the discharge column at atmospheric pressure. We also demonstrate that in the discharge column the electron density balance is local and the electron production and destruction is dominated by volume processes. With increasing flow velocity, the discharge contraction is enhanced due to the increased convective heat loss. The cross sectional area of the conductive region is strongly dependent on the gas velocity and heat conductivity of the gas.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000987841800001 Publication Date 2023-05-01
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0963-0252 ISBN Additional Links UA library record; WoS full record
Impact Factor 3.8 Times cited Open Access Not_Open_Access
Notes This research is financially supported by the European Union’s Horizon 2020 research and innovation programme under Grant Agreement No. 965546. Approved Most recent IF: 3.8; 2023 IF: 3.302
Call Number PLASMANT @ plasmant @c:irua:196972 Serial (down) 8788
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Author Van Alsenoy, W.; Bernard, P.; Van Grieken, R.
Title Zware metalen in Noordzee- en Schelde-sedimenten Type A3 Journal article
Year 1990 Publication Wtare Abbreviated Journal
Volume 5 Issue Pages 113-121
Keywords A3 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Abstract
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos Publication Date
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN ISBN Additional Links UA library record
Impact Factor Times cited Open Access
Notes Approved no
Call Number UA @ admin @ c:irua:116829 Serial (down) 8787
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Author Tsuji, K.; Injuk, J.; Van Grieken, R.
Title X-ray spectrometry: recent technological advances Type ME1 Book as editor or co-editor
Year 2004 Publication Abbreviated Journal
Volume Issue Pages 616 p.
Keywords ME1 Book as editor or co-editor; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Abstract
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos Publication Date
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN ISBN 0-471-48640-x Additional Links UA library record
Impact Factor Times cited Open Access
Notes Approved no
Call Number UA @ admin @ c:irua:43876 Serial (down) 8786
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Author Van Grieken, R.; Worobiec, A.
Title X-ray spectrometry for preventive conservation of cultural heritage Type A1 Journal article
Year 2011 Publication Pramåna: a journal of physics Abbreviated Journal
Volume 72 Issue 2 Pages 191-200
Keywords A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Laboratory Experimental Medicine and Pediatrics (LEMP)
Abstract Analytical chemistry does play a key role in the chemical characterization of the environment and it appears that X-ray spectrometry, in its many forms, is one of the most relevant analytical techniques in preventive conservation, as it is in cultural heritage research in general. X-ray spectrometry has indeed been the method of choice for the characterization of the inorganic composition of atmospheric aerosols, for a long time. We have, over the last decade, intensively used various forms of X-ray spectrometry, viz., mostly energy-dispersive X-ray fluorescence, e.g. with polarized high-energy beam excitation, and automated electron probe X-ray microanalysis, together with other techniques, to identify particle types and their sources in indoor environments, including museums, while gaseous indoor pollutants were assessed using passive diffusion samplers. In each case, both bulk aerosols and individual aerosol particles were studied. For microanalysis of single particles, we have investigated a dozen techniques, but for wide, real-life applications, automated electron probe X-ray microanalysis is the most rewarding. We have first studied atmospheric aerosols in and around the Correr Museum in Venice, many other museums in Austria, Japan and England, and in the caves with prehistoric rock paintings in Altamira, Spain. Very recently, measurements were done in the Metropolitan Museum of Art in New York and theWawel Castle in Cracow, in Italian and Polish mountain churches, in a number of museums in Belgium and the Netherlands, and in cathedrals with medieval stained glass windows. In the Correr museum, it appeared that the particles most threatening for the Bellini paintings were released by the deteriorating plaster renderings, and this could be avoided by simply improving the rendering on the museum walls. In the Wawel Castle, outdoor pollution particles, like fine soot from diesel traffic, entering via leaks in the windows and doors, and also street-deicing salts and coal burning pollution particles, brought in by visitors, mostly in winter, were found to be most worrisome. Urgent questions that are not solved at this moment pertain to the deposition processes from the atmosphere to the cultural heritage items, the critical surface interactions that take place on these items, and the establishment of suitable particle concentration standards.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000288861000002 Publication Date 2011-05-20
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0304-4289; 0973-7111 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor Times cited Open Access
Notes Approved no
Call Number UA @ admin @ c:irua:87025 Serial (down) 8785
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Author Van Grieken, R.; Makarovska, Y.; van Meel, K.; Worobiec, A.
Title X-ray spectrometry for analysis of atmospheric particulate matter: detection limits versus legal levels Type H3 Book chapter
Year 2007 Publication Abbreviated Journal
Volume Issue Pages 153-161 T2 - Topics in X-ray spectrometry / Vázque
Keywords H3 Book chapter; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Laboratory Experimental Medicine and Pediatrics (LEMP)
Abstract
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos Publication Date
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN ISBN Additional Links UA library record
Impact Factor Times cited Open Access
Notes Approved no
Call Number UA @ admin @ c:irua:64402 Serial (down) 8784
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Author Van Grieken, R.; Delalieux, F.
Title X-ray spectrometry for air pollution and cultural heritage research Type P3 Proceeding
Year 2004 Publication Abbreviated Journal
Volume Issue Pages
Keywords P3 Proceeding; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Abstract
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos Publication Date
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN ISBN Additional Links UA library record
Impact Factor Times cited Open Access
Notes Approved no
Call Number UA @ admin @ c:irua:51259 Serial (down) 8783
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Author Markowicz, A.A.; Van Grieken, R.E.
Title X-ray spectrometry Type A1 Journal article
Year 1984 Publication Reviews in analytical chemistry Abbreviated Journal
Volume 56 Issue Pages 241r-250r
Keywords A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Abstract
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos Publication Date
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0048-752x ISBN Additional Links UA library record
Impact Factor Times cited Open Access
Notes Approved no
Call Number UA @ admin @ c:irua:116709 Serial (down) 8782
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Author Markowicz, A.A.; Van Grieken, R.E.
Title X-ray spectrometry Type A1 Journal article
Year 1986 Publication Analytical chemistry Abbreviated Journal
Volume 58 Issue 5 Pages 279r-294r
Keywords A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Abstract
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos Publication Date 2005-03-08
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0003-2700; 5206-882x ISBN Additional Links UA library record
Impact Factor Times cited Open Access
Notes Approved no
Call Number UA @ admin @ c:irua:116523 Serial (down) 8781
Permanent link to this record