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Author Radujković, D.; Vicca, S.; van Rooyen, M.; Wilfahrt, P.; Brown, L.; Jentsch, A.; Reinhart, K.O.; Brown, C.; De Gruyter, J.; Jurasinski, G.; Askarizadeh, D.; Bartha, S.; Beck, R.; Blenkinsopp, T.; Cahill, J.; Campetella, G.; Canullo, R.; Chelli, S.; Enrico, L.; Fraser, L.; Hao, X.; Henry, H.A.L.; Hohn, M.; Jouri, M.H.; Koch, M.; Lawrence Lodge, R.; Li, F.Y.; Lord, J.M.; Milligan, P.; Minggagud, H.; Palmer, T.; Schröder, B.; Szabó, G.; Zhang, T.; Zimmermann, Z.; Verbruggen, E.
Title Consistent predictors of microbial community composition across spatial scales in grasslands reveal low context‐dependency Type A1 Journal article
Year 2023 Publication Molecular ecology Abbreviated Journal
Volume 32 Issue 24 Pages (up) 6924-6938
Keywords A1 Journal article; Plant and Ecosystems (PLECO) – Ecology in a time of change
Abstract Environmental circumstances shaping soil microbial communities have been studied extensively. However, due to disparate study designs, it has been difficult to resolve whether a globally consistent set of predictors exists, or context‐dependency prevails. Here, we used a network of 18 grassland sites (11 of those containing regional plant productivity gradients) to examine (i) if similar abiotic or biotic factors predict both large‐scale (across sites) and regional‐scale (within sites) patterns in bacterial and fungal community composition, and (ii) if microbial community composition differs consistently at two levels of regional plant productivity (low vs. high). Our results revealed that bacteria were associated with particular soil properties (such as base saturation) and both bacteria and fungi were associated with plant community composition across sites and within the majority of sites. Moreover, a discernible microbial community signal emerged, clearly distinguishing high and low‐productivity soils across different grasslands independent of their location in the world. Hence, regional productivity differences may be typified by characteristic soil microbial communities across the grassland biome. These results could encourage future research aiming to predict the general effects of global changes on soil microbial community composition in grasslands and to discriminate fertile from infertile systems using generally applicable microbial indicators.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001090315100001 Publication Date 2023-10-24
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0962-1083 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.9 Times cited Open Access
Notes Approved Most recent IF: 4.9; 2023 IF: 6.086
Call Number UA @ admin @ c:irua:200464 Serial 9194
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Author Huang, S.; Griffin, E.; Cai, J.; Xin, B.; Tong, J.; Fu, Y.; Kravets, V.; Peeters, F.M.; Lozada-Hidalgo, M.
Title Gate-controlled suppression of light-driven proton transport through graphene electrodes Type A1 Journal article
Year 2023 Publication Nature communications Abbreviated Journal
Volume 14 Issue 1 Pages (up) 6932-6937
Keywords A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Abstract Recent experiments demonstrated that proton transport through graphene electrodes can be accelerated by over an order of magnitude with low intensity illumination. Here we show that this photo-effect can be suppressed for a tuneable fraction of the infra-red spectrum by applying a voltage bias. Using photocurrent measurements and Raman spectroscopy, we show that such fraction can be selected by tuning the Fermi energy of electrons in graphene with a bias, a phenomenon controlled by Pauli blocking of photo-excited electrons. These findings demonstrate a dependence between graphene's electronic and proton transport properties and provide fundamental insights into molecularly thin electrode-electrolyte interfaces and their interaction with light. Recent experiments have shown that proton transport through graphene electrodes can be promoted by light, but the understanding of this phenomenon remains unclear. Here, the authors report the electrical tunability of this photo-effect, showing a connection between graphene electronic and proton transport properties.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001094448600003 Publication Date 2023-10-31
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2041-1723 ISBN Additional Links UA library record; WoS full record
Impact Factor 16.6 Times cited Open Access
Notes Approved Most recent IF: 16.6; 2023 IF: 12.124
Call Number UA @ admin @ c:irua:201185 Serial 9041
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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 (up) 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 8809
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Author de la Croix, T.; Claes, N.; Eyley, S.; Thielemans, W.; Bals, S.; De Vos, D.
Title Heterogeneous Pt-catalyzed transfer dehydrogenation of long-chain alkanes with ethylene Type A1 Journal Article
Year 2023 Publication Catalysis Science & Technology Abbreviated Journal Catal. Sci. Technol.
Volume Issue Pages (up)
Keywords A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;
Abstract The dehydrogenation of long-chain alkanes to olefins and alkylaromatics is a challenging endothermic reaction, typically requiring harsh conditions which can lead to low selectivity and coking. More favorable thermodynamics can be achieved by using a hydrogen acceptor, such as ethylene. In this work, the potential of heterogeneous platinum catalysts for the transfer dehydrogenation of long-chain alkanes is investigated, using ethylene as a convenient hydrogen acceptor. Pt/C and Pt–Sn/C catalysts were prepared<italic>via</italic>a simple polyol method and characterized with CO pulse chemisorption, HAADF-STEM, and EDX measurements. Conversion of ethylene was monitored<italic>via</italic>gas-phase FTIR, and distribution of liquid products was analyzed<italic>via</italic>GC-FID, GC-MS, and 1H-NMR. Compared to unpromoted Pt/C, Sn-promoted catalysts show lower initial reaction rates, but better resistance to catalyst deactivation, while increasing selectivity towards alkylaromatics. Both reaction products and ethylene were found to inhibit the reaction significantly. At 250 °C for 22 h, TON up to 28 and 86 mol per mol Pt were obtained for Pt/C and PtSn<sub>2</sub>/C, respectively, with olefin selectivities of 94% and 53%. The remaining products were mainly unbranched alkylaromatics. These findings show the potential of simple heterogeneous catalysts in alkane transfer dehydrogenation, for the preparation of valuable olefins and alkylaromatics, or as an essential step in various tandem reactions.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001104905100001 Publication Date 2023-11-09
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2044-4753 ISBN Additional Links UA library record; WoS full record
Impact Factor 5 Times cited Open Access OpenAccess
Notes T. de la Croix gratefully acknowledges the support of the Flanders Research Foundation (FWO) under project 11F6622N. D. De Vos is grateful to FWO for support of project G0D3721N, and to KU Leuven for the iBOF project 21/016/C3. S. Bals and N. Claes acknowledge funding from the European Research Council under the European Union’s Horizon 2020 research and innovation program (ERC Consolidator Grant No. 815128- REALNANO). W. Thielemans and S. Eyley thank KU Leuven (grant C14/18/061) and FWO (G0A1219N) for financial support. Approved Most recent IF: 5; 2023 IF: 5.773
Call Number EMAT @ emat @c:irua:201010 Serial 8968
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Author Mazzola, F.; Hassani, H.; Amoroso, D.; Chaluvadi, S.K.; Fujii, J.; Polewczyk, V.; Rajak, P.; Koegler, M.; Ciancio, R.; Partoens, B.; Rossi, G.; Vobornik, I.; Ghosez, P.; Orgiani, P.
Title Unveiling the electronic structure of pseudotetragonal WO₃ thin films Type A1 Journal article
Year 2023 Publication The journal of physical chemistry letters Abbreviated Journal
Volume 14 Issue 32 Pages (up) 7208-7214
Keywords A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Abstract WO3 isa 5d compound that undergoes severalstructuraltransitions in its bulk form. Its versatility is well-documented,with a wide range of applications, such as flexopiezoelectricity,electrochromism, gating-induced phase transitions, and its abilityto improve the performance of Li-based batteries. The synthesis ofWO(3) thin films holds promise in stabilizing electronicphases for practical applications. However, despite its potential,the electronic structure of this material remains experimentally unexplored.Furthermore, its thermal instability limits its use in certain technologicaldevices. Here, we employ tensile strain to stabilize WO3 thin films, which we call the pseudotetragonal phase, and investigateits electronic structure using a combination of photoelectron spectroscopyand density functional theory calculations. This study reveals theFermiology of the system, notably identifying significant energy splittingsbetween different orbital manifolds arising from atomic distortions.These splittings, along with the system's thermal stability,offer a potential avenue for controlling inter- and intraband scatteringfor electronic applications.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001044522400001 Publication Date 2023-08-08
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1948-7185 ISBN Additional Links UA library record; WoS full record
Impact Factor 5.7 Times cited Open Access OpenAccess
Notes Approved Most recent IF: 5.7; 2023 IF: 9.353
Call Number UA @ admin @ c:irua:198391 Serial 8951
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Author Yuan, Y.; Wu, F.-J.; Xiao, S.-T.; Wang, Y.-T.; Yin, Z.-W.; Van Tendeloo, G.; Chang, G.-G.; Tian, G.; Hu, Z.-Y.; Wu, S.-M.; Yang, X.-Y.
Title Hierarchical zeolites containing embedded Cd0.2Zn0.8S as a photocatalyst for hydrogen production from seawater Type A1 Journal article
Year 2023 Publication Chemical communications Abbreviated Journal
Volume 59 Issue 47 Pages (up) 7275-7278
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Uncovering an efficient and stable photocatalytic system for seawater splitting is a highly desirable but challenging goal. Herein, Cd0.2Zn0.8S@Silicalite-1 (CZS@S-1) composites, in which CZS is embedded in the hierarchical zeolite S-1, were prepared and show remarkably high activity, stability and salt resistance in seawater.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000994367000001 Publication Date 2023-05-19
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1359-7345; 1364-548x ISBN Additional Links UA library record; WoS full record
Impact Factor 4.9 Times cited Open Access OpenAccess
Notes Approved Most recent IF: 4.9; 2023 IF: 6.319
Call Number UA @ admin @ c:irua:197291 Serial 8878
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Author Bhatia, H.; Martin, C.; Keshavarz, M.; Dovgaliuk, I.; Schrenker, N.J.; Ottesen, M.; Qiu, W.; Fron, E.; Bremholm, M.; Van de Vondel, J.; Bals, S.; Roeffaers, M.B.J.; Hofkens, J.; Debroye, E.
Title Deciphering the role of water in promoting the optoelectronic performance of surface-engineered lead halide perovskite nanocrystals Type A1 Journal article
Year 2023 Publication ACS applied materials and interfaces Abbreviated Journal
Volume 15 Issue 5 Pages (up) 7294-7307
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Lead halide perovskites are promising candidates for applicability is limited by their structural instability toward moisture. Although a deliberate addition of water to the precursor solution has recently been shown to improve the crystallinity and optical properties of perovskites, the corresponding thin films still do not exhibit a near-unity quantum yield. Herein, we report that the direct addition of a minute amount of water to post-treated substantially enhances the stability while achieving a 95% photoluminescence quantum yield in a NC thin film. We unveil the mechanism of how moisture assists in the formation of an additional NH4Br component. Alongside, we demonstrate the crucial role of moisture in assisting localized etching of the perovskite crystal, facilitating the partial incorporation of NH4+, which is key for improved performance under ambient conditions. Finally, as a proof-of-concept, the application of post-treated and watertreated perovskites is tested in LEDs, with the latter exhibiting a superior performance, offering opportunities toward commercial application in moisture-stable optoelectronics.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000931729400001 Publication Date 2023-01-27
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1944-8244 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.5 Times cited 3 Open Access Not_Open_Access
Notes H.B. would like to express her sincere gratitude to Dr. Peter Erk (formerly BASF SE, Germany) for very insightful discussions. The authors acknowledge financial support from the Research Foundation-Flanders (FWO grant numbers S002019N, 1514220N, G.0B39.15, G.0B49.15, G098319N, and ZW15_09-GOH6316) , the KU Leuven Research Fund (C14/19/079, iBOF-21-085 PERSIST, and STG/21/010) , the Flemish government through long-term structural funding Methusalem (CASAS2, Meth/15/04) , the Hercules Founda-tion (HER/11/14) , and the ERC through the Marie Curie ITN iSwitch Ph.D. fellowship to H.B. (grant number 642196) . C.M. acknowledges the financial support from grants PID2021-128761OA-C22 funded by MCIN/AEI/10.13039/501100011033 by the ?European Union? and SBPLY/21/180501/000127 funded by JCCM and by the EU through Fondo Europeo de Desarollo Regional? (FEDER) . Martin Bremholm and Martin Ottesen acknowledge funding from the Danish Council for Independent Research, Natural Sciences, under the Sapere Aude program (grant no. 7027-00077B) and VILLUM FONDEN through the Centre of Excellence for Dirac Materials (grant no. 11744) . Affiliation with the Center for Integrated Materials Research (iMAT) at Aarhus University is gratefully acknowledged.-N.J.S. acknowledges financial support from the research foundation Flanders (FWO) through a postdoctoral fellowship (FWO grant no. 1238622N) . S.B. acknowledges financial support from the European Commission by the ERC Consolidator grant REALNANO (no. 815128) . Approved Most recent IF: 9.5; 2023 IF: 7.504
Call Number UA @ admin @ c:irua:195375 Serial 7293
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Author Perreault, P.; Boruntea, C.-R.; Dhawan Yadav, H.; Portela Soliño, I.; Kummamuru, N.B.
Title Combined methane pyrolysis and solid carbon gasification for electrified CO₂-free hydrogen and syngas production Type A1 Journal article
Year 2023 Publication Energies Abbreviated Journal
Volume 16 Issue 21 Pages (up) 7316-7320
Keywords A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Abstract The coupling of methane pyrolysis with the gasification of a solid carbon byproduct provides CO2-free hydrogen and hydrogen-rich syngas, eliminating the conundrum of carbon utilization. Firstly, the various types of carbon that are known to result during the pyrolysis process and their dependencies on the reaction conditions for catalytic and noncatalytic systems are summarized. The synchronization of the reactions’ kinetics is considered to be of paramount importance for efficient performance. This translates to the necessity of finding suitable reaction conditions, carbon reactivities, and catalysts that might enable control over competing reactions through the manipulation of the reaction rates. As a consequence, the reaction kinetics of methane pyrolysis is then emphasized, followed by the particularities of carbon deposition and the kinetics of carbon gasification. Given the urgency in finding suitable solutions for decarbonizing the energy sector and the limited information on the gasification of pyrolytic carbon, more research is needed and encouraged in this area. In order to provide CO2-free hydrogen production, the reaction heat should also be provided without CO2. Electrification is one of the solutions, provided that low-carbon sources are used to generate the electricity. Power-to-heat, i.e., where electricity is used for heating, represents the first step for the chemical industry.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001103312100001 Publication Date 2023-10-29
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1996-1073 ISBN Additional Links UA library record; WoS full record
Impact Factor Times cited Open Access OpenAccess
Notes Approved Most recent IF: NA
Call Number UA @ admin @ c:irua:200456 Serial 8842
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Author Ying, J.; Xiao, Y.; Chen, J.; Hu, Z.-Y.; Tian, G.; Van Tendeloo, G.; Zhang, Y.; Symes, M.D.D.; Janiak, C.; Yang, X.-Y.
Title Fractal design of hierarchical PtPd with enhanced exposed surface atoms for highly catalytic activity and stability Type A1 Journal article
Year 2023 Publication Nano letters Abbreviated Journal
Volume 23 Issue 16 Pages (up) 7371-7378
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Hierarchicalassembly of arc-like fractal nanostructures not onlyhas its unique self-similarity feature for stability enhancement butalso possesses the structural advantages of highly exposed surface-activesites for activity enhancement, remaining a great challenge for high-performancemetallic nanocatalyst design. Herein, we report a facile strategyto synthesize a novel arc-like hierarchical fractal structure of PtPdbimetallic nanoparticles (h-PtPd) by using pyridinium-type ionic liquidsas the structure-directing agent. Growth mechanisms of the arc-likenanostructured PtPd nanoparticles have been fully studied, and precisecontrol of the particle sizes and pore sizes has been achieved. Dueto the structural features, such as size control by self-similaritygrowth of subunits, structural stability by nanofusion of subunits,and increased numbers of exposed active atoms by the curved homoepitaxialgrowth, h-PtPd displays outstanding electrocatalytic activity towardoxygen reduction reaction and excellent stability during hydrothermaltreatment and catalytic process.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001042181100001 Publication Date 2023-08-03
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 Open Access Not_Open_Access
Notes Approved Most recent IF: 10.8; 2023 IF: 12.712
Call Number UA @ admin @ c:irua:198408 Serial 8870
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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 (up) 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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Corporate Author Thesis
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 8802
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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 (up)
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.
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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 8789
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Author Kocabas, T.; Keceli, M.; Vazquez-Mayagoitia, A.; Sevik, C.
Title Gaussian approximation potentials for accurate thermal properties of two-dimensional materials Type A1 Journal article
Year 2023 Publication Nanoscale Abbreviated Journal
Volume 15 Issue 19 Pages (up) 8772-8780
Keywords A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Abstract Two-dimensional materials (2DMs) continue to attract a lot of attention, particularly for their extreme flexibility and superior thermal properties. Molecular dynamics simulations are among the most powerful methods for computing these properties, but their reliability depends on the accuracy of interatomic interactions. While first principles approaches provide the most accurate description of interatomic forces, they are computationally expensive. In contrast, classical force fields are computationally efficient, but have limited accuracy in interatomic force description. Machine learning interatomic potentials, such as Gaussian Approximation Potentials, trained on density functional theory (DFT) calculations offer a compromise by providing both accurate estimation and computational efficiency. In this work, we present a systematic procedure to develop Gaussian approximation potentials for selected 2DMs, graphene, buckled silicene, and h-XN (X = B, Al, and Ga, as binary compounds) structures. We validate our approach through calculations that require various levels of accuracy in interatomic interactions. The calculated phonon dispersion curves and lattice thermal conductivity, obtained through harmonic and anharmonic force constants (including fourth order) are in excellent agreement with DFT results. HIPHIVE calculations, in which the generated GAP potentials were used to compute higher-order force constants instead of DFT, demonstrated the first-principles level accuracy of the potentials for interatomic force description. Molecular dynamics simulations based on phonon density of states calculations, which agree closely with DFT-based calculations, also show the success of the generated potentials in high-temperature simulations.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000976615200001 Publication Date 2023-04-19
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2040-3364; 2040-3372 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.7 Times cited Open Access Not_Open_Access
Notes Approved Most recent IF: 6.7; 2023 IF: 7.367
Call Number UA @ admin @ c:irua:196722 Serial 8873
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Author Sevik, C.; Bekaert, J.; Milošević, M.V.
Title Superconductivity in functionalized niobium-carbide MXenes Type A1 Journal article
Year 2023 Publication Nanoscale Abbreviated Journal
Volume 15 Issue 19 Pages (up) 8792-8799
Keywords A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Abstract We detail the effects of Cl and S functionalization on the superconducting properties of layered (bulk) and monolayer niobium carbide (Nb2C) MXene crystals, based on first-principles calculations combined with Eliashberg theory. For bulk layered Nb2CCl2, the calculated superconducting transition temperature (T-c) is in very good agreement with the recently measured value of 6 K. We show that T-c is enhanced to 10 K for monolayer Nb2CCl2, due to an increase in the density of states at the Fermi level, and the corresponding electron-phonon coupling. We further demonstrate feasible gate- and strain-induced enhancements of T-c for both bulk-layered and monolayer Nb2CCl2 crystals, resulting in T-c values of around 38 K. In the S-functionalized Nb2CCl2 crystals, our calculations reveal the importance of phonon softening in understanding their superconducting properties. Finally, we predict that Nb3C2S2 in bulk-layered and monolayer forms is also superconducting, with a T-c of around 28 K. Considering that Nb2C is not superconducting in pristine form, our findings promote functionalization as a pathway towards robust superconductivity in MXenes.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000976973900001 Publication Date 2023-04-11
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2040-3364; 2040-3372 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.7 Times cited Open Access OpenAccess
Notes Approved Most recent IF: 6.7; 2023 IF: 7.367
Call Number UA @ admin @ c:irua:196711 Serial 8938
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Author Broers, F.T.H.; Janssens, K.; Weker, J.N.; Webb, S.M.; Mehta, A.; Meirer, F.; Keune, K.
Title Two pathways for the degradation of orpiment pigment (As₂S₃) found in paintings Type A1 Journal article
Year 2023 Publication Journal of the American Chemical Society Abbreviated Journal
Volume 145 Issue 16 Pages (up) 8847-8859
Keywords A1 Journal article; Antwerp X-ray Imaging and Spectroscopy (AXIS)
Abstract Paintings are complex objects containing many different chemical compounds that can react over time. The degradation of arsenic sulfide pigments causes optical changes in paintings. The main degradation product was thought to be white arsenolite (As2O3), but previous research also showed the abundant presence of As(V) species. In this study, we investigate the influence of the presence of a medium on the degradation mechanism of orpiment (As2S3) using synchrotron radiation (SR)-based tomographic transmission X-ray microscopy, SR-based micro-X-ray fluorescence, and Xray absorption near edge structure spectroscopy. Upon direct illumination of dry orpiment powder using UV-visible light, only the formation of As2O3 was observed. When As2S3 was surrounded by a medium and illuminated, As2O3 was only observed in the area directly exposed to light, while As(V) degradation species were found elsewhere in the medium. Without accelerated artificial light aging, As(V)(aq) species are formed and migrate throughout the medium within weeks after preparation. In both scenarios, the As(V) species form via intermediate As(III)(aq) species and the presence of a medium is necessary. As(V)(aq) species can react with available cations to form insoluble metal arsenates, which induces stress within the paint layers (leading to, e.g., cracks and delamination) or can lead to a visual change of the image of the painting.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000974346900001 Publication Date 2023-04-14
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 15 Times cited Open Access OpenAccess
Notes Approved Most recent IF: 15; 2023 IF: 13.858
Call Number UA @ admin @ c:irua:196762 Serial 8948
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Author Broers, F.T.H.; Verslype, I.; Bossers, K.W.; Vanmeert, F.; Gonzalez, V.; Garrevoet, J.; van Loon, A.; va Duijn, E.; Krekeler, A.; De Keyser, N.; Steeman, I.; Noble, P.; Janssens, K.; Meirer, F.; Keune, K.
Title Correlated x-ray fluorescence and ptychographic nano-tomography on Rembrandt's The Night Watch reveals unknown lead “layer” Type A1 Journal article
Year 2023 Publication Science Advances Abbreviated Journal
Volume 9 Issue 50 Pages (up) eadj9394-13
Keywords A1 Journal article; Engineering sciences. Technology; Art; Antwerp X-ray Imaging and Spectroscopy (AXIS)
Abstract The Night Watch, one of the most famous masterpieces by Rembrandt, is the subject of a large research and conservation project. For the conservation treatment, it is of great importance to understand its current condition. Correlated nano-tomography using x-ray fluorescence and ptychography revealed a-so far unknown-lead-containing “layer”, which likely acts as a protective impregnation layer applied on the canvas before the quartz-clay ground was applied. This layer might explain the presence of lead soap protrusions in areas where no other lead components are present. In addition to the three-dimensional elemental mapping, ptychography visualizes and quantifies components not detectable by hard x-ray fluorescence such as the organic fraction and quartz. The first-time use of this combination of synchrotron-based techniques on a historic paint micro-sample shows it to be an important tool to better interpret the results of noninvasive imaging techniques operating on the macroscale.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001142514700010 Publication Date 2023-12-15
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2375-2548 ISBN Additional Links UA library record; WoS full record
Impact Factor 13.6 Times cited Open Access
Notes Approved Most recent IF: 13.6; 2023 IF: NA
Call Number UA @ admin @ c:irua:203849 Serial 9016
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Author Manzaneda-Gonzalez, V.; Jenkinson, K.; Pena-Rodriguez, O.; Borrell-Grueiro, O.; Trivino-Sanchez, S.; Banares, L.; Junquera, E.; Espinosa, A.; Gonzalez-Rubio, G.; Bals, S.; Guerrero-Martinez, A.
Title From multi- to single-hollow trimetallic nanocrystals by ultrafast heating Type A1 Journal article
Year 2023 Publication Chemistry of materials Abbreviated Journal
Volume 35 Issue 22 Pages (up) 9603-9612
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Metal nanocrystals (NCs) display unique physicochemical features that are highly dependent on nanoparticle dimensions, anisotropy, structure, and composition. The development of synthesis methodologies that allow us to tune such parameters finely emerges as crucial for the application of metal NCs in catalysis, optical materials, or biomedicine. Here, we describe a synthetic methodology to fabricate hollow multimetallic heterostructures using a combination of seed-mediated growth routes and femtosecond-pulsed laser irradiation. The envisaged methodology relies on the coreduction of Ag and Pd ions on gold nanorods (Au NRs) to form Au@PdAg core-shell nanostructures containing small cavities at the Au-PdAg interface. The excitation of Au@PdAg NRs with low fluence femtosecond pulses was employed to induce the coalescence and growth of large cavities, forming multihollow anisotropic Au@PdAg nanostructures. Moreover, single-hollow alloy AuPdAg could be achieved in high yield by increasing the irradiation energy. Advanced electron microscopy techniques, energy-dispersive X-ray spectroscopy (EDX) tomography, X-ray absorption near-edge structure (XANES) spectroscopy, and finite differences in the time domain (FDTD) simulations allowed us to characterize the morphology, structure, and elemental distribution of the irradiated NCs in detail. The ability of the reported synthesis route to fabricate multimetallic NCs with unprecedented hollow nanostructures offers attractive prospects for the fabrication of tailored high-entropy alloy nanoparticles.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001110623500001 Publication Date 2023-11-06
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756; 1520-5002 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.6 Times cited 2 Open Access OpenAccess
Notes Approved Most recent IF: 8.6; 2023 IF: 9.466
Call Number UA @ admin @ c:irua:202144 Serial 9040
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Author Xiang, F.; Gupta, A.; Chaves, A.; Krix, Z.E.; Watanabe, K.; Taniguchi, T.; Fuhrer, M.S.; Peeters, F.M.; Neilson, D.; Milošević, M.V.; Hamilton, A.R.
Title Intra-zero-energy Landau level crossings in bilayer graphene at high electric fields Type A1 Journal article
Year 2023 Publication Nano letters Abbreviated Journal
Volume 23 Issue 21 Pages (up) 9683-9689
Keywords A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Abstract The highly tunable band structure of the zero-energy Landau level (zLL) of bilayer graphene makes it an ideal platform for engineering novel quantum states. However, the zero-energy Landau level at high electric fields has remained largely unexplored. Here we present magnetotransport measurements of bilayer graphene in high transverse electric fields. We observe previously undetected Landau level crossings at filling factors nu = -2, 1, and 3 at high electric fields. These crossings provide constraints for theoretical models of the zero-energy Landau level and show that the orbital, valley, and spin character of the quantum Hall states at high electric fields is very different from low electric fields. At high E, new transitions between states at nu = -2 with different orbital and spin polarization can be controlled by the gate bias, while the transitions between nu = 0 -> 1 and nu = 2 -> 3 show anomalous behavior.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001102148900001 Publication Date 2023-10-26
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1530-6984 ISBN Additional Links UA library record; WoS full record
Impact Factor 10.8 Times cited 1 Open Access
Notes Approved Most recent IF: 10.8; 2023 IF: 12.712
Call Number UA @ admin @ c:irua:201200 Serial 9052
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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 (up) 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 8793
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Author Van Gordon, K.; Baúlde, S.; Mychinko, M.; Heyvaert, W.; Obelleiro-Liz, M.; Criado, A.; Bals, S.; Liz-Marzán, L.M.; Mosquera, J.
Title Tuning the Growth of Chiral Gold Nanoparticles Through Rational Design of a Chiral Molecular Inducer Type A1 Journal Article
Year 2023 Publication Nano Letters Abbreviated Journal Nano Lett.
Volume Issue Pages (up)
Keywords A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;
Abstract The bottom-up production of chiral gold nanomaterials holds great potential for the advancement of biosensing and nano-optics, among other applications. Reproducible preparations of colloidal nanomaterials with chiral morphology have been reported, using cosurfactants or chiral inducers such as thiolated amino acids. However, the underlying growth mechanisms for these nanomaterials remain insufficiently understood. We introduce herein a purposely devised chiral inducer, a cysteine modified with a hydrophobic chain, as a versatile chiral inducer. The amphiphilic and chiral features of this molecule provide control over the chiral morphology and the chiroptical signature of the obtained nanoparticles by simply varying the concentration of chiral inducer. These results are supported by circular dichroism and electromagnetic modeling as well as electron tomography to analyze structural evolution at the facet scale. Our observations suggest complex roles for the factors involved in chiral synthesis: the chemical nature of the chiral inducers and the influence of cosurfactants.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001092787000001 Publication Date 2023-10-25
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1530-6984 ISBN Additional Links UA library record; WoS full record
Impact Factor 10.8 Times cited Open Access OpenAccess
Notes J.M. Taboada and F. Obelleiro are thanked for support with electromagnetic simulations. The authors acknowledge financial support by the European Research Council (ERC CoG No. 815128 REALNANO to S. Bals; ERC AdG No. 787510, 4DbioSERS to L.M.L.-M.) and from MCIN/AEI/10.13039/501100011033 and “ESF Investing in your future” (Grant PID2020-117779RB-I00 to L.M.L.-M., Grant RYC2020-030183-I to A.C., and Grants RYC2019-027842-I, PID2020-117885GA-I00 to J.M.). Approved Most recent IF: 10.8; 2023 IF: 12.712
Call Number EMAT @ emat @c:irua:200590 Serial 8963
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Author Maes, R.R.; Potters, G.; Fransen, E.; Geuens, J.; Van Schaeren, R.; Lenaerts, S.
Title Can we find an optimal fatty acid composition of biodiesel in order to improve oxidation stability? Type A1 Journal article
Year 2023 Publication Sustainability Abbreviated Journal
Volume 15 Issue 13 Pages (up) 10310-10
Keywords A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL); Medical Genetics (MEDGEN)
Abstract Air quality currently poses a major risk for human health. Currently, diesel is widely used as fuel and is a significant source of nitrogen oxides (NOx) and particulate matter (PM), both hazardous to human health. A good alternative for mineral diesel is biodiesel, not only for the improvement of hazardous components in the exhaust gases but also because it can be produced in view of a circular economy. Biodiesel consists of a mix of different fatty acid methyl esters, which can react with oxygen. As a consequence, the oxidation stability of biodiesel has to be studied, because the oxidation of biodiesel could affect the performance of the engine due to the wear of injectors and fuel pumps. The oxidation stability could also affect the quality of the exhaust gases due to increases in NOx and PM. The basic question we try to answer in this communication is: 'Can we find an optimal fatty acid composition in order to have a maximal oxidation stability?' In this article, we try to find the optimal fatty acid composition according to the five most common fatty acid methyl esters present in biodiesel in order to reach a maximal oxidation stability. The measurements and statistical analysis show, however, that there is no useful regression model because there are statistically significant two- and three-way interactions among the different fatty acids.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001028597300001 Publication Date 2023-06-30
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2071-1050 ISBN Additional Links UA library record; WoS full record
Impact Factor 3.9 Times cited Open Access OpenAccess
Notes Approved Most recent IF: 3.9; 2023 IF: 1.789
Call Number UA @ admin @ c:irua:198241 Serial 8839
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Author Mayda, S.; Monico, L.; Krishnan, D.; De Meyer, S.; Cotte, M.; Garrevoet, J.; Falkenberg, G.; Sandu, I.C.A.; Partoens, B.; Lamoen, D.; Romani, A.; Miliani, C.; Verbeeck, J.; Janssens, K.
Title A combined experimental and computational approach to understanding CdS pigment oxidation in a renowned early 20th century painting Type A1 Journal article
Year 2023 Publication Chemistry of materials Abbreviated Journal
Volume 35 Issue 24 Pages (up) 10403-10415
Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT); Antwerp X-ray Imaging and Spectroscopy (AXIS)
Abstract Cadmium sulfide (CdS)-based yellow pigments have been used in a number of early 20th century artworks, including The Scream series painted by Edvard Munch. Some of these unique paintings are threatened by the discoloration of these CdS-based yellow oil paints because of the oxidation of the original sulfides to sulfates. The experimental data obtained here prove that moisture and cadmium chloride compounds play a key role in promoting such oxidation. To clarify how these two factors effectively prompt the process, we studied the band alignment between CdS, CdCl2, and Cd-(OH)Cl as well as the radicals center dot OH and H3O center dot by density functional theory (DFT) methods. Our results show that a stack of several layers of Cd-(OH)Cl creates a pocket of positive holes at the Cl-terminated surface and a pocket of electrons at the OH-terminated surface by leading in a difference in ionization energy at both surfaces. The resulting band alignment indicates that Cd-(OH)Cl can indeed play the role of an oxidative catalyst for CdS in a moist environment, thus providing an explanation for the experimental evidence.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001133000900001 Publication Date 2023-12-08
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756; 1520-5002 ISBN Additional Links UA library record; WoS full record
Impact Factor 8.6 Times cited Open Access
Notes The experimental research on the cadmium yellow powders/paint mock-ups and The Scream (ca. 1910) was financially supported by the European Union, research projects IPERION-CH (H2020-INFRAIA-2014-2015, GA no. 654028) and IPERION-HS (H2020-INFRAIA-2019-1, GA no. 871034) and the project AMIS within the program Dipartimenti di Eccellenza 2018-2022 (funded by MUR and the University of Perugia). For the beamtime grants received, the authors thank the ESRF-ID21 beamline (experiments HG64 and HG95), the DESY-P06 beamline, a member of the Helmholtz Association HGF (experiments I-20130221 EC and I-20160126 EC), and the project CALIPSOplus under the GA no. 730872 from the E.U. Framework Programme for Research and Innovation Horizon 2020. All of the staff of the MUNCH Museum (Conservation Department) is acknowledged for their collaboration. 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: 8.6; 2023 IF: 9.466
Call Number UA @ admin @ c:irua:202836 Serial 8999
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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 (up) 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 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 Gamon, J.; Bassat, J.-M.; Villesuzanne, A.; Duttine, M.; Batuk, M.; Vandemeulebroucke, D.; Hadermann, J.; Alassani, F.; Weill, F.; Durand, E.; Demourgues, A.
Title Impact of anionic ordering on the iron site distribution and valence states in oxyfluoride Sr2FeO3+xF1-x(x=0.08, 0.2) with a layered Perovskite network Type A1 Journal article
Year 2023 Publication Inorganic chemistry Abbreviated Journal
Volume 62 Issue 27 Pages (up) 10822-10832
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Sr2FeO3+x F1-x (x = 0.08, 0.2), an n = 1 Ruddlesden-Popperphase, was synthesized from the oxidationof Sr2FeO3F in air at high temperature followinga fluorine for oxygen substitution and Fe3+ to Fe4+ oxidation. A structural investigation of both compounds was performedusing complementary and high-resolution techniques (Synchrotron X-rayand electron diffraction, Mo''ssbauer spectroscopy, HR-STEM)coupled to DFT calculation. This study reveals that oxidation leadsto a high degree of apical anion disorder coupled to antiphase boundaries. Sr2FeO3F, an oxyfluoride compoundwith an n = 1 Ruddlesden-Popper structure,was identifiedas a potential interesting mixed ionic and electronic conductor (MIEC).The phase can be synthesized under a range of different pO(2) atmospheres, leading to various degrees of fluorinefor oxygen substitution and Fe4+ content. A structuralinvestigation and thorough comparison of both argon- and air-synthesizedcompounds were performed by combining high-resolution X-ray and electrondiffraction, high-resolution scanning transmission electron microscopy,Mo''ssbauer spectroscopy, and DFT calculations. While the argon-synthesizedphase shows a well-behaved O/F ordered structure, this study revealedthat oxidation leads to averaged large-scale anionic disorder on theapical site. In the more oxidized Sr2FeO3.2F0.8 oxyfluoride, containing 20% of Fe4+, two differentFe positions can be identified with a 32%/68% occupancy (P4/nmm space group). This originates due to the presenceof antiphase boundaries between ordered domains within the grains.Relations between site distortion and valence states as well as stabilityof apical anionic sites (O vs F) are discussed. This study paves theway for further studies on both ionic and electronic transport propertiesof Sr2FeO3.2F0.8 and its use in MIEC-baseddevices, such as solid oxide fuel cells.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001018974700001 Publication Date 2023-06-29
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0020-1669 ISBN Additional Links UA library record; WoS full record
Impact Factor 4.6 Times cited Open Access Not_Open_Access
Notes Approved Most recent IF: 4.6; 2023 IF: 4.857
Call Number UA @ admin @ c:irua:197789 Serial 8881
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Author Pandey, T.; Peeters, F.M.; Milošević, M.V.
Title High thermoelectric figure of merit in p-type Mg₃Si₂Te₆: role of multi-valley bands and high anharmonicity Type A1 Journal article
Year 2023 Publication Journal of materials chemistry C : materials for optical and electronic devices Abbreviated Journal
Volume 11 Issue 33 Pages (up) 11185-11194
Keywords A1 Journal article; Condensed Matter Theory (CMT)
Abstract Silicon-based materials are attractive for thermoelectric applications due to their thermal stability, chemical inertness, and natural abundance of silicon. Here, using a combination of first-principles and Boltzmann transport calculations we report the thermoelectric properties of the recently synthesized compound Mg3Si2Te6. Our analysis reveals that Mg3Si2Te6 is a direct bandgap semiconductor with a bandgap of 1.6 eV. The combination of heavy and light valence bands, along with a high valley degeneracy, results in a large power factor under p-type doping. We also find that Mg is weakly bonded both within and between the layers, leading to low phonon group velocities. The vibrations of the Mg atoms are localized and make a significant contribution to phonon-phonon scattering. This high anharmonicity, coupled with low phonon group velocity, results in a low lattice thermal conductivity of & kappa;(l) = 0.5 W m(-1) K-1 at room temperature, along the cross-plane direction. Combining excellent electronic transport properties and low & kappa;(l), p-type Mg3Si2Te6 achieves figure-of-merit (zT) values greater than 1 at temperatures above 600 K. Specifically, a zT of 2.0 is found at 900 K along the cross-plane direction. Our findings highlight the importance of structural complexity and chemical bonding in electronic and phonon transport, providing guiding insights for further design of Si-based thermoelectrics.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001041124900001 Publication Date 2023-07-26
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2050-7526; 2050-7534 ISBN Additional Links UA library record; WoS full record
Impact Factor 6.4 Times cited 1 Open Access Not_Open_Access
Notes Approved Most recent IF: 6.4; 2023 IF: 5.256
Call Number UA @ admin @ c:irua:198296 Serial 8821
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Author Annys, A.; Jannis, D.; Verbeeck, J.; Annys, A.; Jannis, D.; Verbeeck, J.
Title Deep learning for automated materials characterisation in core-loss electron energy loss spectroscopy Type A1 Journal article
Year 2023 Publication Scientific reports Abbreviated Journal
Volume 13 Issue 1 Pages (up) 13724
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Electron energy loss spectroscopy (EELS) is a well established technique in electron microscopy that yields information on the elemental content of a sample in a very direct manner. One of the persisting limitations of EELS is the requirement for manual identification of core-loss edges and their corresponding elements. This can be especially bothersome in spectrum imaging, where a large amount of spectra are recorded when spatially scanning over a sample area. This paper introduces a synthetic dataset with 736,000 labeled EELS spectra, computed from available generalized oscillator strength tables, that represents 107 K, L, M or N core-loss edges and 80 chemical elements. Generic lifetime broadened peaks are used to mimic the fine structure due to band structure effects present in experimental core-loss edges. The proposed dataset is used to train and evaluate a series of neural network architectures, being a multilayer perceptron, a convolutional neural network, a U-Net, a residual neural network, a vision transformer and a compact convolutional transformer. An ensemble of neural networks is used to further increase performance. The ensemble network is used to demonstrate fully automated elemental mapping in a spectrum image, both by directly mapping the predicted elemental content and by using the predicted content as input for a physical model-based mapping.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001052937600046 Publication Date 2023-08-22
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2045-2322 ISBN Additional Links UA library record; WoS full record
Impact Factor 4.6 Times cited Open Access OpenAccess
Notes A.A. would like to acknowledge the resources and services used in this work provided by the VSC (Flemish Supercomputer Center), funded by the Research Foundation – Flanders (FWO) and the Flemish Government. J.V. acknowledges the IMPRESS project. The IMPRESS project has received funding from the HORIZON EUROPE framework program for research and innovation under grant agreement n. 101094299. Approved Most recent IF: 4.6; 2023 IF: 4.259
Call Number UA @ admin @ c:irua:198647 Serial 8846
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Author Tiwari, S.; Van de Put, M.L.; Temst, K.; Vandenberghe, W.G.; Sorée, B.
Title Atomistic modeling of spin and electron dynamics in two-dimensional magnets switched by two-dimensional topological insulators Type A1 Journal article
Year 2023 Publication Physical review applied Abbreviated Journal
Volume 19 Issue 1 Pages (up) 014040-14049
Keywords A1 Journal article; Condensed Matter Theory (CMT)
Abstract To design fast memory devices, we need material combinations that can facilitate fast read and write operations. We present a heterostructure comprising a two-dimensional (2D) magnet and a 2D topological insulator (TI) as a viable option for designing fast memory devices. We theoretically model the spin-charge dynamics between 2D magnets and 2D TIs. Using the adiabatic approximation, we combine the nonequi-librium Green's function method for spin-dependent electron transport and a time-quantified Monte Carlo method for simulating magnetization dynamics. We show that it is possible to switch a magnetic domain of a ferromagnet using the spin torque from spin-polarized edge states of a 2D TI. We show further that the switching of 2D magnets by TIs is strongly dependent on the interface exchange (Jint), and an opti-mal interface exchange, is required for efficient switching. Finally, we compare experimentally grown Cr compounds and show that Cr compounds with higher anisotropy (such as CrI3) result in a lower switching speed but a more stable magnetic order.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000920227500002 Publication Date 2023-01-12
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2331-7019 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.6 Times cited Open Access Not_Open_Access
Notes Approved Most recent IF: 4.6; 2023 IF: 4.808
Call Number UA @ admin @ c:irua:194312 Serial 7283
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Author Zi, L.; Reynaert, S.; Nijs, I.; De Boeck, H.; Verbruggen, E.; Beemster, G.T.S.; Asard, H.; Abdelgawad, H.
Title Biochemical composition changes can be linked to the tolerance of four grassland species under more persistent precipitation regimes Type A1 Journal article
Year 2023 Publication Physiologia plantarum Abbreviated Journal
Volume 175 Issue 6 Pages (up) e14083-13
Keywords A1 Journal article; Integrated Molecular Plant Physiology Research (IMPRES); Plant and Ecosystems (PLECO) – Ecology in a time of change
Abstract Climate models suggest that the persistence of summer precipitation regimes (PRs) is on the rise, characterized by both longer dry and longer wet durations. These PR changes may alter plant biochemical composition and thereby their economic and ecological characteristics. However, impacts of PR persistence have primarily been studied at the community level, largely ignoring the biochemistry of individual species. Here, we analyzed biochemical components of four grassland species with varying sensitivity to PR persistence (Holcus lanatus, Phleum pratense, Lychnis flos-cuculi, Plantago lanceolata) along a range of increasingly persistent PRs (longer consecutive dry and wet periods) in a mesocosm experiment. The more persistent PRs decreased nonstructural sugars, whereas they increased lignin in all species, possibly reducing plant quality. The most sensitive species Lychnis seemed less capable of altering its biochemical composition in response to altered PRs, which may partly explain its higher sensitivity. The more tolerant species may have a more robust and dynamic biochemical network, which buffers the effects of changes in individual biochemical components on biomass. We conclude that the biochemical composition changes are important determinants for plant performance under increasingly persistent precipitation regimes.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001108556200001 Publication Date 2023-11-25
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0031-9317 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.4 Times cited Open Access
Notes Approved Most recent IF: 6.4; 2023 IF: 3.33
Call Number UA @ admin @ c:irua:202003 Serial 9190
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Author Li, S.; Sun, J.; Gorbanev, Y.; van’t Veer, K.; Loenders, B.; Yi, Y.; Kenis, T.; Chen, Q.; Bogaerts, A.
Title Plasma-Assisted Dry Reforming of CH4: How Small Amounts of O2Addition Can Drastically Enhance the Oxygenate Production─Experiments and Insights from Plasma Chemical Kinetics Modeling Type A1 Journal Article
Year 2023 Publication ACS Sustainable Chemistry & Engineering Abbreviated Journal ACS Sustainable Chem. Eng.
Volume 11 Issue 42 Pages (up) 15373-15384
Keywords A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Abstract Plasma-based dry reforming of methane (DRM) into

high-value-added oxygenates is an appealing approach to enable

otherwise thermodynamically unfavorable chemical reactions at

ambient pressure and near room temperature. However, it suffers

from coke deposition due to the deep decomposition of CH4. In this

work, we assess the DRM performance upon O2 addition, as well as

varying temperature, CO2/CH4 ratio, discharge power, and gas

residence time, for optimizing oxygenate production. By adding O2,

the main products can be shifted from syngas (CO + H2) toward

oxygenates. Chemical kinetics modeling shows that the improved

oxygenate production is due to the increased concentration of

oxygen-containing radicals, e.g., O, OH, and HO2, formed by electron

impact dissociation [e + O2 → e + O + O/O(1D)] and subsequent

reactions with H atoms. Our study reveals the crucial role of oxygen-coupling in DRM aimed at oxygenates, providing practical

solutions to suppress carbon deposition and at the same time enhance the oxygenates production in plasma-assisted DRM.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001082603900001 Publication Date 2023-10-23
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2168-0485 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.4 Times cited Open Access Not_Open_Access
Notes Fonds Wetenschappelijk Onderzoek, S001619N ; China Scholarship Council, 202006060029 ; National Natural Science Foundation of China, 21975018 ; H2020 European Research Council, 810182 ; Approved Most recent IF: 8.4; 2023 IF: 5.951
Call Number PLASMANT @ plasmant @c:irua:201013 Serial 8966
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Author Souza, J.C.B.; Vizarim, N.P.; Reichhardt, C.J.O.; Reichhardt, C.; Venegas, P.A.
Title Magnus induced diode effect for skyrmions in channels with periodic potentials Type A1 Journal article
Year 2023 Publication Journal of physics : condensed matter Abbreviated Journal
Volume 35 Issue 1 Pages (up) 015804-15810
Keywords A1 Journal article; Condensed Matter Theory (CMT)
Abstract Using a particle based model, we investigate the skyrmion dynamical behavior in a channel where the upper wall contains divots of one depth and the lower wall contains divots of a different depth. Under an applied driving force, skyrmions in the channels move with a finite skyrmion Hall angle that deflects them toward the upper wall for -x direction driving and the lower wall for +x direction driving. When the upper divots have zero height, the skyrmions are deflected against the flat upper wall for -x direction driving and the skyrmion velocity depends linearly on the drive. For +x direction driving, the skyrmions are pushed against the lower divots and become trapped, giving reduced velocities and a nonlinear velocity-force response. When there are shallow divots on the upper wall and deep divots on the lower wall, skyrmions get trapped for both driving directions; however, due to the divot depth difference, skyrmions move more easily under -x direction driving, and become strongly trapped for +x direction driving. The preferred -x direction motion produces what we call a Magnus diode effect since it vanishes in the limit of zero Magnus force, unlike the diode effects observed for asymmetric sawtooth potentials. We show that the transport curves can exhibit a series of jumps or dips, negative differential conductivity, and reentrant pinning due to collective trapping events. We also discuss how our results relate to recent continuum modeling on a similar skyrmion diode system.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000880827900001 Publication Date 2022-10-22
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0953-8984 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 2.7 Times cited Open Access OpenAccess
Notes Approved Most recent IF: 2.7; 2023 IF: 2.649
Call Number UA @ admin @ c:irua:192031 Serial 7320
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Author Zhang, Y.; van Schayck, J.P.; Pedrazo-Tardajos, A.; Claes, N.; Noteborn, W.E.M.; Lu, P.-H.; Duimel, H.; Dunin-Borkowski, R.E.; Bals, S.; Peters, P.J.; Ravelli, R.B.G.
Title Charging of vitreous samples in cryogenic electron microscopy mitigated by graphene Type A1 Journal article
Year 2023 Publication ACS nano Abbreviated Journal
Volume 17 Issue 16 Pages (up) 15836-15846
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Cryogenic electronmicroscopy can provide high-resolution reconstructionsof macromolecules embedded in a thin layer of ice from which atomicmodels can be built de novo. However, the interactionbetween the ionizing electron beam and the sample results in beam-inducedmotion and image distortion, which limit the attainable resolutions.Sample charging is one contributing factor of beam-induced motionsand image distortions, which is normally alleviated by including partof the supporting conducting film within the beam-exposed region.However, routine data collection schemes avoid strategies wherebythe beam is not in contact with the supporting film, whose rationaleis not fully understood. Here we characterize electrostatic chargingof vitreous samples, both in imaging and in diffraction mode. We mitigatesample charging by depositing a single layer of conductive grapheneon top of regular EM grids. We obtained high-resolution single-particleanalysis (SPA) reconstructions at 2 & ANGS; when the electron beamonly irradiates the middle of the hole on graphene-coated grids, usingdata collection schemes that previously failed to produce sub 3 & ANGS;reconstructions without the graphene layer. We also observe that theSPA data obtained with the graphene-coated grids exhibit a higher b factor and reduced particle movement compared to dataobtained without the graphene layer. This mitigation of charging couldhave broad implications for various EM techniques, including SPA andcryotomography, and for the study of radiation damage and the developmentof future sample carriers. Furthermore, it may facilitate the explorationof more dose-efficient, scanning transmission EM based SPA techniques.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001041649900001 Publication Date 2023-08-02
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record
Impact Factor 17.1 Times cited Open Access OpenAccess
Notes We thank H. Nguyen for editing the manuscript. We warmly thank the M4i Microscopy CORE Lab team of FHML Maastricht University (MU) for their support and collaboration and Eve Timlin and Ye Gao (MU) for providing protein samples. Members of the Amsterdam Scientific Instruments team are acknowledged for their Timepix detector support. This work benefited from access to The Netherlands Centre for Electron Nanoscopy (NeCEN) with assistance from Ludovic Renault and Meindert Lamers. The authors acknowledge financial support of the Netherlands Electron Microscopy Infrastructure (NEMI), project number 184.034.014 of the National Roadmap for Large-Scale Research Infrastructure of the Dutch Research Council (NWO), the PPP Allowance made available by Health-Holland, Top Sector Life Sciences & Health, to stimulate public-private partnerships, project 4DEM, number LSHM21029, and the LINK program from the Province of Limburg, The Netherlands, as well as financial support from the European Commission under the Horizon 2020 Programme by grant no. 815128 (REALNANO). Approved Most recent IF: 17.1; 2023 IF: 13.942
Call Number UA @ admin @ c:irua:198376 Serial 8840
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