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Author Mosquera, J.; Wang, D.; Bals, S.; Liz-Marzan, L.M.
Title Surfactant layers on gold nanorods Type A1 Journal article
Year 2023 Publication Accounts of chemical research Abbreviated Journal
Volume 56 Issue 10 Pages 1204-1212
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Gold nanorods (Au NRs) are an exceptionally promising tool in nanotechnology due to three key factors: (i) their strong interaction with electromagnetic radiation, stemming from their plasmonic nature, (ii) the ease with which the resonance frequency of their longitudinal plasmon mode can be tuned from the visible to the near-infrared region of the electromagnetic spect r u m based on their aspect ratio, and (iii) their simple and cost-effective preparation through seed-mediated chemical growth. In this synthetic method, surfactants play a critical role in controlling the size, shape, and colloidal stabi l i t y of Au NRs. For example, surfactants can stabilize specific crystallographic facets during the formation of Au NRs, leading to t h e formation of NRs with specific morphologies. The process of surfactant adsorption onto the NR surface may result in various assemblies of surfactant molecules, such as spherical micelles, elongated micelles, or bilayers. Again, the assembly mode is critical toward determining the further availabi l i t y of the Au NR surface to the surrounding medium. Despite its importance and a great deal of research effort, the interaction between Au NPs and surfactants remains insufficiently understood, because the assembly process is influenced by numerous factors, including the chemical nature of the surfactant, the surface morphology of Au NPs, and solution parameters. Therefore, gaining a more comprehensive understanding of these interactions is essential to unlock the full potential of the seed-mediated growth method and the applications of plasmonic NPs. A plethora of characterization techniques have been applied to reach such an understanding , but many open questions remain. In this Account, we review the current knowledge on the interactions between surfactants and Au NRs. We briefly introduce the state-of-the-art methods for synthesizing Au NRs and highlight the crucial role of cationic surfactants during this process. The self-assembly and organization of surfactants on the Au NR surface is then discussed to better understand their role in seed-mediated growth. Subsequently, we provide examples and elucidate how chemical additives can be used to modulate micellar assemblies, in turn allowing for a finer control over the growth of Au NRs, including chiral NRs. Next, we review the main experimental characterization and computational modeling techniques that have been applied to shed light on the arrangement of surfactants on Au NRs and summarize the advantages and disadvantages for each technique. The Account ends with a “Conclusions and Outlook” section, outlining promising future research directions and developments that we consider are sti l l required, mostly related to the application of electron microscopy in liquid and in 3D. Finally, we remark on the potential of exploiting machine learning techniques to predict synthetic routes for NPs with predefined structures and properties.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000986447000001 Publication Date 2023-05-08
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0001-4842 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 18.3 Times cited 8 Open Access (up) OpenAccess
Notes The authors acknowledge financial support by the European Research Council (ERC CoG No. 815128 REALNANO to S.B.; ERC AdG No. 787510, 4DbioSERS to L.M.L.-M.) , from MCIN/AEI/10.13039/501100011033 and “ESF Investing in your future” (Grant PID2020-117779RB-I00 to L.M.L.-M. and Grants RYC2019-027842-I , PID2020-117885GA-I00 to J.M.) , and by Guangdong Provincial Key Laboratory of Optical Information Materials and Technology (No. 2017B030301007) , National Center for International Research on Green Optoelectronics (No. 2016B01018) , MOE Interna-tional Laboratory for Optical Information Technologies, and the 111 projects. Approved Most recent IF: 18.3; 2023 IF: 20.268
Call Number UA @ admin @ c:irua:196768 Serial 8940
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Author Moggia, G.; Hoekx, S.; Daems, N.; Bals, S.; Breugelmans, T.
Title Synthesis and characterization of a highly electroactive composite based on Au nanoparticles supported on nanoporous activated carbon for electrocatalysis Type A1 Journal article
Year 2023 Publication ChemElectroChem Abbreviated Journal
Volume Issue Pages 1-11
Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Abstract A facile, “one-pot”, chemical approach to synthesize gold-based nanoparticles finely dispersed on porous activated carbon (Norit) was demonstrated in this work. The pH of the synthesis bath played a critical role in determining the optimal gold-carbon interaction, which enabled a successful deposition of the gold nanoparticles onto the carbon matrix with a maximized metal utilization of 93 %. The obtained AuNP/C nanocomposite was characterized using SEM, HAADF-STEM electron tomography and electrochemical techniques. It was found that the Au nanoparticles, with diameters between 5 and 20 nm, were evenly distributed over the carbon matrix, both inside and outside the pores. Electrochemical characterization indicated that the composite had a very large electroactive surface area (EASA), as high as 282.4 m2 gAu-1. By exploiting its very high EASA, the catalyst was intended to boost the productivity of glucaric acid in the electrooxidation of its precursor, gluconic acid. However, cyclic voltammetry experiments revealed a very limited reactivity towards gluconic acid oxidation, due to the spacial hindrance of gluconic acid molecule which prevented diffusion inside the catalyst nanopores. On the other hand, the as-synthesized nanocomposite promises to be effective towards the ORR, and might thus find potential application as anode catalyst for fuel cells as well as for the scalability of all those electrochemical reactions involving small molecules with high diffusivity and catalysed by noble metals (i. e. CO2, CH4, N2, etc..). Electrocatalysis: Gold nanoparticles with diameter between 5 and 20 nm evenly distributed onto porous activated carbon (Norit) were obtained using a facile “one-pot” chemical synthesis technique with very high metal utilization. The AuNP/C nanocomposite was characterized using SEM, HAADF-STEM electron tomography and electrochemical techniques, revealing a very large electroactive surface area (EASA). The figure shows the HAADF-STEM image (a) and the respective EDX elemental distribution (b) for the AuNP/C composite with 9.3 % Au-loading developed in this work (Au is marked in red and C in green).image
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001060398900001 Publication Date 2023-09-08
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2196-0216 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4 Times cited 1 Open Access (up) OpenAccess
Notes The research described in this article has not been supported by the Climate, Infrastructure and Environment Executive Agency of the European Commission. The views expressed in this article have not been adopted or in any way approved by the European Commission and do not constitute a statement of the European Commission & apos;s views.r S. Hoekx was supported by Research Foundation Flanders (FWO 1S42623N). The authors would like to thank Prof. Dr. Christophe Vande Velde, University of Antwerp, for the XRD analysis. Approved Most recent IF: 4; 2023 IF: 4.136
Call Number UA @ admin @ c:irua:199210 Serial 8941
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Author Monico, L.; d'Acapito, F.; Cotte, M.; Janssens, K.; Romani, A.; Ricci, G.; Miliani, C.; Cartechini, L.
Title Total electron yield (TEY) detection mode Cr K-edge XANES spectroscopy as a direct method to probe the composition of the surface of darkened chrome yellow (PbCr1-xSxO4) and potassium chromate paints Type A1 Journal article
Year 2023 Publication Nuclear instruments and methods in physics research: B: beam interactions with materials and atoms Abbreviated Journal
Volume 539 Issue Pages 141-147
Keywords A1 Journal article; Engineering sciences. Technology; Antwerp X-ray Imaging and Spectroscopy (AXIS)
Abstract The darkening of chromate-pigments, including chrome yellows (PbCr1-xSxO4), is a surface phenomenon affecting late 19th-early 20th c. paintings, such as those by Van Gogh. Exploring analytical strategies that contribute to a deep understanding of darkening is therefore significant for the long-term conservation of unique masterpieces. Here, we examined the capabilities of Cr K-edge XANES spectroscopy collected at the same time in X-ray fluorescence yield (XFY) and total electron yield (TEY) detection modes to selectively study the surface composition of darkened oil paint mock-ups composed of chrome yellow (PbCr0.2S0.8O4) or potassium chromate. By discussing advantages and drawbacks in using XFY/TEY modes in relation to XFY & mu;-XANES analysis from sectioned samples, we aim at assessing if TEY-XANES spectroscopy: (i) is a selective surface method to determine the abundance of different Cr-species from paint fragments; (ii) can contribute to optimize the analytical strategy by limiting time consuming sample preparation procedures; (iii) can decrease the probability of radiation damage.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001041485400001 Publication Date 2023-04-10
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0168-583x ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 1.3 Times cited Open Access (up) OpenAccess
Notes Approved Most recent IF: 1.3; 2023 IF: 1.109
Call Number UA @ admin @ c:irua:198427 Serial 8944
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Author Ortega Saez, N.; Arno, R.; Marchetti, A.; Cauberghs, S.; Janssens, K.; Van der Snickt, G.; Al-Emam, E.
Title Towards a novel strategy for soot removal from water-soluble materials : the synergetic effect of hydrogels and cyclomethicone on gelatine emulsion-based photographs Type A1 Journal article
Year 2023 Publication Heritage science Abbreviated Journal
Volume 11 Issue 1 Pages 78-17
Keywords A1 Journal article; Engineering sciences. Technology; Art; Antwerp Cultural Heritage Sciences (ARCHES); Antwerp X-ray Imaging and Spectroscopy (AXIS)
Abstract Gels are a popular cleaning method for paper conservators and a lot of research has been done concerning gel cleaning of paper objects over the last 15 years. Despite the close interconnection between the conservation fields of paper and photographic material, research on using gels for cleaning photographs is very scarce. However, gels can provide an excellent cleaning method for photographic material. Cleaning silver gelatine prints with aqueous solvents is very complex due to the hydrophilic properties and fragility of the gelatine layer which makes mechanical cleaning difficult. The properties of gels ensure better control over the flow and evaporation of the solvent, facilitating the cleaning process. This study is the first insight into the viability of using gellan gum gel and polyvinyl acetate-borax (PVAc-borax) gel to clean contaminants from the surface of silver gelatine photographs. It is based on self-made samples that were artificially aged and contaminated with soot. Water, ethanol (EtOH), and Kodak Photo-flo were studied as solvents to remove the soot from the silver gelatine-based prints. These solvents were loaded into the aforementioned gels and applied to the samples in two different methods. These gel cleaning methods were subsequently compared with traditional cleaning methods. In addition, the usage of cyclomethicone D4 as a protective mask for the gelatine layer was studied. Measuring methods used to evaluate the cleaning were visual comparison, microscopic observation, and densitometry. ATR-FTIR measurements were also conducted to investigate potential side-effects of the cleaning methods on the prints, such as unwanted chemical transformations or the presence of gel residues after the treatments. Most of the gel cleaning methods within this study proved to be inadequate, with the exception of the gellan gum gel loaded with 30% EtOH. It was used as a granulated gel applied mechanically on a print saturated with cyclomethicone (octamethylcyclotetrasiloxane D4). Cyclomethicone proved to be a very effective protective barrier for the water-sensitive gelatine layer with minimal reduction in cleaning effectiveness.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000970139500001 Publication Date 2023-04-18
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2050-7445 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 2.5 Times cited Open Access (up) OpenAccess
Notes Approved Most recent IF: 2.5; 2023 IF: NA
Call Number UA @ admin @ c:irua:196445 Serial 8945
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Author Detamornrat, U.; Parrilla, M.; Domínguez-Robles, J.; Anjani, Q.K.; Larrañeta, E.; De Wael, K.; Donnelly, R.F.
Title Transdermal on-demand drug delivery based on an iontophoretic hollow microneedle array system Type A1 Journal article
Year 2023 Publication Lab on a chip Abbreviated Journal
Volume 23 Issue 9 Pages 2304-2315
Keywords A1 Journal article; Engineering sciences. Technology; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab)
Abstract Transdermal drug delivery has emerged as an alternative administration route for therapeutic drugs, overcoming current issues in oral and parenteral administration. However, this technology is hindered by the low permeability of the stratum corneum of the skin. In this work, we develop a synergic combination of two enhancing technologies to contribute to an improved and on-demand drug delivery through an iontophoretic system coupled with hollow microneedles (HMNs). For the first time, a polymeric HMN array coupled with integrated iontophoresis for the delivery of charged molecules and macromolecules (e.g. proteins) is devised. To prove the concept, methylene blue, fluorescein sodium, lidocaine hydrochloride, and bovine serum albumin-fluorescein isothiocyanate conjugate (BSA-FITC) were first tested in an in vitro setup using 1.5% agarose gel model. Subsequently, the ex vivo drug permeation study using a Franz diffusion cell was conducted, exhibiting a 61-fold, 43-fold, 54-fold, and 17-fold increment of the permeation of methylene blue, fluorescein sodium, lidocaine hydrochloride, and BSA-FITC, respectively, during the application of 1 mA cm(-2) current for 6 h. Moreover, the total amount of drug delivered (i.e. in the skin and receptor compartment) was analysed to untangle the different delivery profiles according to the types of molecule. Finally, the integration of the anode and cathode into an iontophoretic hollow microneedle array system (IHMAS) offers the full miniaturisation of the concept. Overall, the IHMAS device provides a versatile wearable technology for transdermal on-demand drug delivery that can improve the administration of personalised doses, and potentially enhance precision medicine.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000971513000001 Publication Date 2023-04-18
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1473-0197 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.1 Times cited Open Access (up) OpenAccess
Notes Approved Most recent IF: 6.1; 2023 IF: 6.045
Call Number UA @ admin @ c:irua:195781 Serial 8946
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Author Soenen, M.; Milošević, M.V.
Title Tunable magnon topology in monolayer CrI₃ under external stimuli Type A1 Journal article
Year 2023 Publication Physical review materials Abbreviated Journal
Volume 7 Issue 8 Pages 084402-84409
Keywords A1 Journal article; Condensed Matter Theory (CMT)
Abstract Two-dimensional (2D) honeycomb ferromagnets, such as monolayer chromium trihalides, are predicted to behave as topological magnon insulators, characterized by an insulating bulk and topologically protected edge states, giving rise to a thermal magnon Hall effect. Here we report the behavior of the topological magnons in monolayer CrI3 under external stimuli, including biaxial and uniaxial strain, electric gating, as well as in-plane and out-of-plane magnetic field, revealing that one can thereby tailor the magnetic states as well as the size and the topology of the magnonic bandgap. These findings broaden the perspective of using 2D magnetic materials to design topological magnonic devices.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001052941600003 Publication Date 2023-08-08
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 (up) OpenAccess
Notes Approved Most recent IF: 3.4; 2023 IF: NA
Call Number UA @ admin @ c:irua:199201 Serial 8947
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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 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 (up) 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 Teunissen, J.L.; Braeckevelt, T.; Skvortsova, I.; Guo, J.; Pradhan, B.; Debroye, E.; Roeffaers, M.B.J.; Hofkens, J.; Van Aert, S.; Bals, S.; Rogge, S.M.J.; Van Speybroeck, V.
Title Additivity of Atomic Strain Fields as a Tool to Strain-Engineering Phase-Stabilized CsPbI3Perovskites Type A1 Journal Article
Year 2023 Publication The Journal of Physical Chemistry C Abbreviated Journal J. Phys. Chem. C
Volume 127 Issue 48 Pages 23400-23411
Keywords A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;
Abstract CsPbI3 is a promising perovskite material for photovoltaic applications in its photoactive perovskite or black phase. However, the material degrades to a photovoltaically inactive or yellow phase at room temperature. Various mitigation strategies are currently being developed to increase the lifetime of the black phase, many of which rely on inducing strains in the material that hinder the black-to-yellow phase transition. Physical insight into how these strategies exactly induce strain as well as knowledge of the spatial extent over which these strains impact the material is crucial to optimize these approaches but is still lacking. Herein, we combine machine learning potential-based molecular dynamics simulations with our in silico strain engineering approach to accurately quantify strained large-scale atomic structures on a nanosecond time scale. To this end, we first model the strain fields introduced by atomic substitutions as they form the most elementary strain sources. We demonstrate that the magnitude of the induced strain fields decays exponentially with the distance from the strain source, following a decay rate that is largely independent of the specific substitution. Second, we show that the total strain field induced by multiple strain sources can be predicted to an excellent approximation by summing the strain fields of each individual source. Finally, through a case study, we illustrate how this additive character allows us to explain how complex strain fields, induced by spatially extended strain sources, can be predicted by adequately combining the strain fields caused by local strain sources. Hence, the strain additivity proposed here can be adopted to further our insight into the complex strain behavior in perovskites and to design strain from the atomic level onward to enhance their sought-after phase stability.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001116862000001 Publication Date 2023-12-07
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1932-7447 ISBN Additional Links UA library record; WoS full record
Impact Factor 3.7 Times cited Open Access (up) OpenAccess
Notes This work was supported by iBOF-21-085 PERsist (Special Research Fund of Ghent University, KU Leuven Research Fund, and the Research Fund of the University of Antwerp). S.M.J.R., T.B., and B.P. acknowledge financial support from the Research Foundation-Flanders (FWO) through two postdoctoral fellow- ships [grant nos. 12T3522N (S.M.J.R.) and 1275521N (B.P.)] and an SB-FWO fellowship [grant no. 1SC1319 (T.B.)]. E.D., M.B.J.R., and J.H. acknowledge financial support from the Research Foundation-Flanders (FWO, grant nos. G.0B39.15, G.0B49.15, G098319N, S002019N, S004322N, and ZW15_09- GOH6316). J.H. acknowledges support from the Flemish government through long-term structural funding Methusalem (CASAS2, Meth/15/04) and the MPI as an MPI fellow. S.V.A. and S.B. acknowledge financial support from the Research Foundation-Flanders (FWO, grant no. G0A7723N). S.M.J.R. and V.V.S. acknowledge funding from the Research Board of Ghent University (BOF). The computational resources and services used in this work were provided by the VSC (Flemish Supercomputer Center), funded by the Research Foundation- Flanders (FWO) and the Flemish Government�department EWI.; KU Leuven, iBOF-21-085 PERsist ; Universiteit Antwerpen, iBOF-21-085 PERsist ; Universiteit Gent, iBOF-21-085 PERsist ; Vlaamse regering, CASAS2, Meth/15/04 ; Fonds Wetenschappelijk Onderzoek, G.0B39.15 G098319N G.0B49.15 1SC1319 12T3522N ZW15 09-GOH6316 G0A7723N 1275521N S004322N S002019N ; Approved Most recent IF: 3.7; 2023 IF: 4.536
Call Number EMAT @ emat @c:irua:202124 Serial 8985
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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 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 (up) 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 Van Echelpoel, R.; Parrilla, M.; Sleegers, N.; Thiruvottriyur Shanmugam, S.; van Nuijs, A.L.N.; Slosse, A.; Van Durme, F.; De Wael, K.
Title Validated portable device for the qualitative and quantitative electrochemical detection of MDMA ready for on-site use Type A1 Journal article
Year 2023 Publication Microchemical journal Abbreviated Journal
Volume 190 Issue Pages 108693-10
Keywords A1 Journal article; Engineering sciences. Technology; Toxicological Centre; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab)
Abstract Identifying and quantifying 3,4-methyl​enedioxy​methamphetamine (MDMA) on-site in suspected illicit drug samples, whether it be at recreational settings or manufacturing sites, is a major challenge for law enforcement agencies (LEAs). Various analytical techniques exist to fulfil this goal, e.g. colourimetry and portable spectroscopic techniques, each having its specific limitations (e.g. low accuracy, fluorescence, no quantification) and strengths (e.g. fast, easy to use). In this work, for the first time, an electrochemical MDMA sensor is presented to become a detection tool that can realistically be used on-site. More specifically, the use of a single buffer solution and an unmodified screen-printed electrode, along with the integration of a data analysis algorithm and mobile application permits the straightforward on-site identification and quantification of MDMA in suspicious samples. Multiple studies investigating different parameters, including pH, concentration, reproducibility, temperature and binary mixture analyses, were executed. To fully understand all the occurring redox processes, liquid chromatography coupled with high-resolution mass spectrometry analysis of partially electrolyzed MDMA samples was performed unravelling oxidation of the methylenedioxy group. Validation of the methodology was executed on 15 MDMA street samples analysed by gas chromatography coupled with mass spectrometry and compared with the performance of a commercial portable Raman and Attenuated Total Reflection Fourier Transform Infrared Spectroscopy (ATR-FTIR) device. The novel methodology outperformed the spectroscopic techniques, correctly identifying all 15 street samples. Additionally, the electrochemical sensor predicted the purity of the tablets with a mean absolute error of 2.3%. Overall, this new, electrochemical detection strategy provides LEAs the rapid, low-cost, on-site detection and quantification of MDMA in suspicious samples, without requiring specialized training.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000977060400001 Publication Date 2023-03-31
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0026-265x; 0026-265x ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.8 Times cited Open Access (up) OpenAccess
Notes Approved Most recent IF: 4.8; 2023 IF: 3.034
Call Number UA @ admin @ c:irua:195415 Serial 8952
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Author Linard, F.J.A.; Moura, V.N.; Covaci, L.; Milošević, M.V.; Chaves, A.
Title Wave-packet scattering at a normal-superconductor interface in two-dimensional materials : a generalized theoretical approach Type A1 Journal article
Year 2023 Publication Physical review B Abbreviated Journal
Volume 107 Issue 16 Pages 165306-165309
Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT)
Abstract A wave-packet time evolution method, based on the split-operator technique, is developed to investigate the scattering of quasiparticles at a normal-superconductor interface of arbitrary profile and shape. As a practical application, we consider a system where low-energy electrons can be described as Dirac particles, which is the case for most two-dimensional materials, such as graphene and transition-metal dichalcogenides. However, the method is easily adapted for other cases such as electrons in few-layer black phosphorus or any Schrodinger quasiparticles within the effective mass approximation in semiconductors. We employ the method to revisit Andreev reflection in mono-, bi-, and trilayer graphene, where specular-and retro-reflection cases are observed for electrons scattered by a steplike superconducting region. The effect of opening a zero-gap channel across the superconducting region on the electron and hole scattering is also addressed, as an example of the versatility of the technique proposed here.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000974675700006 Publication Date 2023-04-14
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2469-9969; 2469-9950 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.7 Times cited Open Access (up) OpenAccess
Notes Approved Most recent IF: 3.7; 2023 IF: 3.836
Call Number UA @ admin @ c:irua:196709 Serial 8954
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Author Parrilla, M.; Detamornrat, U.; Domínguez-Robles, J.; Donnelly, R.F.; De Wael, K.
Title Wearable hollow microneedle sensing patches for the transdermal electrochemical monitoring of glucose Type A1 Journal article
Year 2022 Publication Talanta : the international journal of pure and applied analytical chemistry Abbreviated Journal
Volume 249 Issue Pages 123695-123699
Keywords A1 Journal article; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab)
Abstract According to the World Health Organization, about 422 million people worldwide have diabetes, with 1.5 million deaths directly attributed each year. Therefore, there is still a need to effectively monitor glucose in diabetic patients for proper management. Recently, wearable patches based on microneedle (MN) sensors provide minimally invasive analysis of glucose through the interstitial fluid (ISF) while exhibiting excellent correlation with blood glucose. Despite many advances in wearable electrochemical sensors, long-term stability and continuous monitoring remain unsolved challenges. Herein, we present a highly stable electrochemical biosensor based on a redox mediator bilayer consisting of Prussian blue and iron-nickel hexacyanoferrate to increase the long-term stability of the readout coupled with a hollow MN array as a sampling unit for ISF uptake. First, the enzymatic biosensor is developed by using affordable screen-printed electrodes (SPE) and optimized for long-term stability fitting the physiological range of glucose in ISF (i.e., 2.5–22.5 mM). In parallel, the MN array is assessed for minimally invasive piercing of the skin. Subsequently, the biosensor is integrated with the MN array leaving a microfluidic spacer that works as the electrochemical cell. Interestingly, a microfluidic channel connects the cell with an external syringe to actively and rapidly withdraw ISF toward the cell. Finally, the robust MN sensing patch is characterized during in vitro and ex vivo tests. Overall, affordable wearable MN-based patches for the continuous monitoring of glucose in ISF are providing an advent in wearable devices for rapid and life-threatening decision-making processes.
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Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000826441800002 Publication Date 2022-06-16
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0039-9140; 1873-3573 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor Times cited Open Access (up) OpenAccess
Notes Approved no
Call Number UA @ admin @ c:irua:188955 Serial 8955
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Author Parrilla, M.; Vanhooydonck, A.; Watts, R.; De Wael, K.
Title Wearable wristband-based electrochemical sensor for the detection of phenylalanine in biofluids Type A1 Journal article
Year 2022 Publication Biosensors and bioelectronics Abbreviated Journal
Volume 197 Issue Pages
Keywords A1 Journal article; Engineering sciences. Technology; Product development; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab)
Abstract Wearable electrochemical sensors are driven by the user-friendly capability of on-site detection of key biomarkers for health management. Despite the advances in biomolecule monitoring such as glucose, still, several unmet clinical challenges need to be addressed. For example, patients suffering from phenylketonuria (PKU) should be able to monitor their phenylalanine (PHE) level in a rapid, decentralized, and affordable manner to avoid high levels of PHE in the body which can lead to a profound and irreversible mental disability. Herein, we report a wearable wristband electrochemical sensor for the monitoring of PHE tackling the necessity of controlling PHE levels in PHE hydroxylase deficiency patients. The proposed electrochemical sensor is based on a screen-printed electrode (SPE) modified with a membrane consisting of Nafion, to avoid interferences in biofluids. The membrane also consists of sodium 1,2-naphthoquinone-4-sulphonate for the in situ derivatization of PHE into an electroactive product, allowing its electrochemical oxidation at the surface of the SPE in alkaline conditions. Importantly, the electrochemical sensor is integrated into a wristband configuration to enhance user interaction and engage the patient with PHE self-monitoring. Besides, a paper-based sampling strategy is designed to alkalinize the real sample without the need for sample pretreatment, and thus simplify the analytical process. Finally, the wearable device is tested for the determination of PHE in saliva and blood serum. The proposed wristband-based sensor is expected to impact the PKU self-monitoring, facilitating the daily lives of PKU patients toward optimal therapy and disease management.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000719366400003 Publication Date 2021-11-02
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0956-5663 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor Times cited Open Access (up) OpenAccess
Notes Approved no
Call Number UA @ admin @ c:irua:183086 Serial 8957
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Author Şentürk, DG.; Yu, CP.; De Backer, A.; Van Aert, S.
Title Atom counting from a combination of two ADF STEM images Type A1 Journal Article
Year 2024 Publication Ultramicroscopy Abbreviated Journal Ultramicroscopy
Volume 255 Issue Pages 113859
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract To understand the structure–property relationship of nanostructures, reliably quantifying parameters, such as the number of atoms along the projection direction, is important. Advanced statistical methodologies have made it possible to count the number of atoms for monotype crystalline nanoparticles from a single ADF STEM image. Recent developments enable one to simultaneously acquire multiple ADF STEM images. Here, we present an extended statistics-based method for atom counting from a combination of multiple statistically independent ADF STEM images reconstructed from non-overlapping annular detector collection regions which improves the accuracy and allows one to retrieve precise atom-counts, especially for images acquired with low electron doses and multiple element structures.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001089064200001 Publication Date 2023-09-23
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0304-3991 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 2.2 Times cited Open Access (up) OpenAccess
Notes This work was supported by the European Research Council (Grant 770887 PICOMETRICS to S. Van Aert). The authors acknowledge financial support from the Research Foundation Flanders (FWO, Belgium) through project fundings (G034621N, G0A7723N, and EOS 40007495) and a postdoctoral grant to A. De Backer. S. Van Aert acknowledges funding from the University of Antwerp Research fund (BOF). Approved Most recent IF: 2.2; 2024 IF: 2.843
Call Number EMAT @ emat @c:irua:201008 Serial 8964
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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
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 (up) 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 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
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.
Address
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 (up) 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 Bhatia, H.; Keshavarz, M.; Martin, C.; Van Gaal, L.; Zhang, Y.; de Coen, B.; Schrenker, N.J.; Valli, D.; Ottesen, M.; Bremholm, M.; Van de Vondel, J.; Bals, S.; Hofkens, J.; Debroye, E.
Title Achieving High Moisture Tolerance in Pseudohalide Perovskite Nanocrystals for Light-Emitting Diode Application Type A1 Journal Article
Year 2023 Publication ACS Applied Optical Materials Abbreviated Journal ACS Appl. Opt. Mater.
Volume 1 Issue 6 Pages 1184-1191
Keywords A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;
Abstract The addition of potassium thiocyanate (KSCN) to the FAPbBr3 structure and subsequent post-treatment of nanocrystals (NCs) lead to high quantum confinement, resulting in a photoluminescent quantum yield (PLQY) approaching unity and microsecond decay times. This synergistic approach demonstrated exceptional stability under humid conditions, retaining 70% of the PLQY for over a month, while the untreated NCs degrade within 24 h. Additionally, the devices incorporating the post-treated NCs displayed 1.5% external quantum efficiency (EQE), a 5-fold improvement over untreated devices. These results provide promising opportunities for the use of perovskites in moisture-stable optoelectronics.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos Publication Date 2023-06-23
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2771-9855 ISBN Additional Links UA library record
Impact Factor Times cited Open Access (up) OpenAccess
Notes Hercules Foundation, HER/11/14 ; European Commission; Ministerio de Ciencia e Innovaci?n, PID2021-128761OA-C22 ; European Regional Development Fund; Vlaamse regering, CASAS2 Meth/15/04 ; Fonds Wetenschappelijk Onderzoek, 1238622N 1514220N 1S45223N G.0B39.15 G.0B49.15 G098319N S002019N ZW15_09-GOH6316 ; Onderzoeksraad, KU Leuven, C14/19/079 db/21/006/bm iBOF-21-085 STG/21/010 ; Junta de Comunidades de Castilla-La Mancha, SBPLY/21/180501/000127 ; H2020 European Research Council, 642196 815128 ; Approved Most recent IF: NA
Call Number EMAT @ emat @c:irua:201011 Serial 8975
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Author Delfino, C.L.; Hao, Y.; Martin, C.; Minoia, A.; Gopi, E.; Mali, K.S.; Van der Auweraer, M.; Geerts, Y.H.; Van Aert, S.; Lazzaroni, R.; De Feyter, S.
Title Conformation-Dependent Monolayer and Bilayer Structures of an Alkylated TTF Derivative Revealed using STM and Molecular Modeling Type A1 Journal Article
Year 2023 Publication The Journal of Physical Chemistry C Abbreviated Journal J. Phys. Chem. C
Volume 127 Issue 47 Pages 23023-23033
Keywords A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;
Abstract In this study, the multi-layer self-assembled molecular network formation of an alkylated tetrathiafulvalene compound is studied at the liquid-solid interface between 1-phenyloctane and graphite. A combined theoretical/experimental approach associating force-field and quantum-chemical calculations with scanning tunnelling microscopy is used to determine the two-dimensional self-assembly beyond the monolayer, but also to further the understanding of the molecular adsorption conformation and its impact on the molecular packing within the assemblies at the monolayer and bilayer level.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001111637100001 Publication Date 2023-11-30
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1932-7447 ISBN Additional Links UA library record; WoS full record
Impact Factor 3.7 Times cited Open Access (up) OpenAccess
Notes Financial support from the Research Foundation-Flanders (FWO G081518N, G0A3220N) and KU Leuven–Internal Funds (C14/19/079) is acknowledged. This work was in part supported by FWO and F. R. S.-FNRS under the Excellence of Science EOS program (project 30489208 and 40007495). C.M. acknowledges the financial support: Grants PID2021-128761OA-C22 and CNS2022-136052 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). Research in Mons is also supported by the Belgian National Fund for Scientific Research (FRS-FNRS) within the Consortium des Équipements de Calcul Intensif – CÉCI, under Grant 2.5020.11, and by the Walloon Region (ZENOBE Tier-1 supercomputer, under grant 1117545). Approved Most recent IF: 3.7; 2023 IF: 4.536
Call Number EMAT @ emat @c:irua:201671 Serial 8974
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Author Grünewald, L.; Chezganov, D.; De Meyer, R.; Orekhov, A.; Van Aert, S.; Bogaerts, A.; Bals, S.; Verbeeck, J.
Title In Situ Plasma Studies Using a Direct Current Microplasma in a Scanning Electron Microscope Type A1 Journal Article
Year 2024 Publication Advanced Materials Technologies Abbreviated Journal Adv Materials Technologies
Volume Issue Pages
Keywords A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;
Abstract Microplasmas can be used for a wide range of technological applications and to improve the understanding of fundamental physics. Scanning electron microscopy, on the other hand, provides insights into the sample morphology and chemistry of materials from the mm‐ down to the nm‐scale. Combining both would provide direct insight into plasma‐sample interactions in real‐time and at high spatial resolution. Up till now, very few attempts in this direction have been made, and significant challenges remain. This work presents a stable direct current glow discharge microplasma setup built inside a scanning electron microscope. The experimental setup is capable of real‐time in situ imaging of the sample evolution during plasma operation and it demonstrates localized sputtering and sample oxidation. Further, the experimental parameters such as varying gas mixtures, electrode polarity, and field strength are explored and experimental<italic>V</italic>–<italic>I</italic>curves under various conditions are provided. These results demonstrate the capabilities of this setup in potential investigations of plasma physics, plasma‐surface interactions, and materials science and its practical applications. The presented setup shows the potential to have several technological applications, for example, to locally modify the sample surface (e.g., local oxidation and ion implantation for nanotechnology applications) on the µm‐scale.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001168639900001 Publication Date 2024-02-25
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2365-709X ISBN Additional Links UA library record; WoS full record
Impact Factor 6.8 Times cited Open Access (up) OpenAccess
Notes L.G., S.B., and J.V. acknowledge support from the iBOF-21-085 PERsist research fund. D.C., S.V.A., and J.V. acknowledge funding from a TOPBOF project of the University of Antwerp (FFB 170366). R.D.M., A.B., and J.V. acknowledge funding from the Methusalem project of the University of Antwerp (FFB 15001A, FFB 15001C). A.O. and J.V. acknowledge funding from the Research Foundation Flanders (FWO, Belgium) project SBO S000121N. Approved Most recent IF: 6.8; 2024 IF: NA
Call Number EMAT @ emat @c:irua:204363 Serial 8995
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Author Şentürk, D.G.; De Backer, A.; Van Aert, S.
Title Element specific atom counting for heterogeneous nanostructures: Combining multiple ADF STEM images for simultaneous thickness and composition determination Type A1 Journal Article
Year 2024 Publication Ultramicroscopy Abbreviated Journal Ultramicroscopy
Volume 259 Issue Pages 113941
Keywords A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;
Abstract In this paper, a methodology is presented to count the number of atoms in heterogeneous nanoparticles based on the combination of multiple annular dark field scanning transmission electron microscopy (ADF STEM) images. The different non-overlapping annular detector collection regions are selected based on the principles of optimal statistical experiment design for the atom-counting problem. To count the number of atoms, the total intensities of scattered electrons for each atomic column, the so-called scattering cross-sections, are simultaneously compared with simulated library values for the different detector regions by minimising the squared differences. The performance of the method is evaluated for simulated Ni@Pt and Au@Ag core-shell nanoparticles. Our approach turns out to be a dose efficient alternative for the investigation of beam-sensitive heterogeneous materials as compared to the combination of ADF STEM and energy dispersive X-ray spectroscopy.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos Publication Date 2024-02-19
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0304-3991 ISBN Additional Links UA library record
Impact Factor 2.2 Times cited Open Access (up) OpenAccess
Notes This work was supported by the European Research Council (Grant 770887 PICOMETRICS to S. Van Aert). The authors acknowledge financial support from the Research Foundation Flanders (FWO, Belgium) through project fundings (G.0346.21N, GOA7723N, and EOS 40007495) and a postdoctoral grant to A. De Backer. S. Van Aert acknowledges funding from the University of Antwerp Research fund (BOF). Approved Most recent IF: 2.2; 2024 IF: 2.843
Call Number EMAT @ emat @c:irua:204353 Serial 8996
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Author Jenkinson, K.; Spadaro, M.C.; Golovanova, V.; Andreu, T.; Morante, J.R.; Arbiol, J.; Bals, S.
Title Direct operando visualization of metal support interactions induced by hydrogen spillover during CO₂ hydrogenation Type A1 Journal article
Year 2023 Publication Advanced materials Abbreviated Journal
Volume 35 Issue 51 Pages 2306447-10
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract The understanding of catalyst active sites is a fundamental challenge for the future rational design of optimized and bespoke catalysts. For instance, the partial reduction of Ce4+ surface sites to Ce3+ and the formation of oxygen vacancies are critical for CO2 hydrogenation, CO oxidation, and the water gas shift reaction. Furthermore, metal nanoparticles, the reducible support, and metal support interactions are prone to evolve under reaction conditions; therefore a catalyst structure must be characterized under operando conditions to identify active states and deduce structure-activity relationships. In the present work, temperature-induced morphological and chemical changes in Ni nanoparticle-decorated mesoporous CeO2 by means of in situ quantitative multimode electron tomography and in situ heating electron energy loss spectroscopy, respectively, are investigated. Moreover, operando electron energy loss spectroscopy is employed using a windowed gas cell and reveals the role of Ni-induced hydrogen spillover on active Ce3+ site formation and enhancement of the overall catalytic performance.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001106139400001 Publication Date 2023-10-22
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0935-9648 ISBN Additional Links UA library record; WoS full record
Impact Factor 29.4 Times cited Open Access (up) OpenAccess
Notes Approved Most recent IF: 29.4; 2023 IF: 19.791
Call Number UA @ admin @ c:irua:201143 Serial 9022
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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 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 (up) 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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