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| Author | Kashiwar, A. | ||||
| Title | TEM investigations of deformation mechanisms in nanocrystalline metals and multilayered composites | Type | Doctoral thesis | ||
| Year | 2022 | Publication | Abbreviated Journal | ||
| Volume | Issue | Pages | xvi, 129 p. | ||
| Keywords | Doctoral thesis; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
| Abstract | In the last few decades, nanostructuring has driven significant attention towards the development of novel metallic materials with advanced mechanical properties. Nanocrystalline (nc) metals are a class of nanostructured materials with grain sizes smaller than about 100 nm. These exhibit outstanding mechanical strength and fatigue properties compared to their coarse-grained (cg) counterparts. These are promising candidates for application as structural or functional materials. Nc metals in the form of thin films are employed as hard coatings on bulk components, structural components, and conductive layers in various micro-/nanoscale devices. These structural components and devices are often subjected to cyclic stresses or fatigue loading. Under these cyclic stresses, nc metals tend to exhibit the Bauschinger effect (BE). The strength loss during the BE is of great importance concerning the strength-ductility trade-off in nc metals. Furthermore, contact surfaces of the engineering components in service often undergo relative motion and are subject to both friction and wear. These extreme loading conditions demand nc metals with tailored interfacial characteristics for improved tribological performance. Aiming at ensuring high reliability and mechanical robustness for optimum performance of these components, there has been a strong motivation for understanding the mechanical properties and governing deformation mechanisms in nc metallic materials. This thesis aimed at in-depth investigation of microstructures at micro-/nanoscales using state-of-the-art in situ and ex situ transmission electron microscopy (TEM) to develop a closer link between the deformation structure and underlying deformation mechanisms in some nc metallic materials. The thesis has primarily focused on the in situ TEM nanomechanics of the BE and rotational deformation of grains in nc palladium thin films. A sputtered thin film of nc Pd was deformed inside TEM by cyclic loading-unloading experiments and the evolving microstructure was studied in real-time under different TEM imaging modes. The stress-strain response of the film exhibited a characteristic non-linear unloading behavior confirming the BE in the film. The corresponding bright-field TEM imaging revealed evidence of partially reversible dislocation activity. Towards a quantitative understanding of the deformation structure in real-time, in situ nanomechanical testing was coupled with precession-assisted automated crystal orientation mapping in scanning TEM (ACOM-STEM). Global ACOM-STEM analysis offered crystal orientation of a large number of grains at different states of deformation and confirmed partially reversible rotations of nanosized grains fitting to the observed BE during loading and unloading. Analysis of intragranular rotations showed substantial changes in the sub-structure within most of these grains indicating a dominant role of dislocation-based processes in driving these rotations. Globally, an unusually random evolution of texture was seen that demonstrated the influence of deformation heterogeneity and grain interactions on the resulting texture characteristics in nc metals. In the quest of understanding the grain interactions, local investigations based on annular dark-field STEM imaging during loading-unloading showed reversible changes in the contrast of grains with sets of adjoining grains exhibiting a unique cooperative rotation. Local analysis of the density of geometrically necessary dislocations (GNDs) showed the formation of dislocation pile-up at grain boundaries due to the generation of back-stresses during unloading. Critical observations of the evolution of GND density offered greater insights into the mechanism of cooperative grain rotations and these rotations were related to grain structure and grain boundary characteristics. In addition to understanding the influence of grain structure and grain boundaries, the thesis has further investigated the role of heterointerfaces in sputtered Au-Cu and Cu-Cr nanocrystalline multilayered composites (NMCs) deformed under cyclic sliding contact. The microstructural evolution in the NMCs was investigated at different deformation states by classical TEM imaging, ACOM-STEM as well as energy-filtered TEM (EFTEM). Au-Cu NMC with an initial high density of twin boundaries deformed by stress-driven detwinning with a concurrent change in grain structure in both Au and Cu. The formation of a vortex structure was observed due to plastic flow instabilities at Au-Cu interfaces that led to codeformation and mechanical intermixing. Cu-Cr NMC showed a preferential grain growth in Cu layers whereas no noticeable change in the grain sizes was seen in Cr layers. The phase maps revealed sharp interfaces between Cu and Cr layers indicating no intermixing between the immiscible phases. EFTEM results exposed the cracking processes in Cr layers with a concurrent migration of Cu in the cracks. Overall, the thesis has attempted to analyze the competing deformation processes and relate these with the microstructural heterogeneity in terms of grain structure and GB and interfacial characteristics in nc metallic materials. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | Publication Date | |||
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | ISBN | Additional Links | UA library record | ||
| Impact Factor | Times cited | Open Access  |
OpenAccess | ||
| Notes | Approved | Most recent IF: NA | |||
| Call Number | UA @ admin @ c:irua:189013 | Serial | 7343 | ||
| Permanent link to this record | |||||
| Author | Parzyszek, S.; Tessarolo, J.; Pedrazo-Tardajos, A.; Ortuno, A.M.; Baginski, M.; Bals, S.; Clever, G.H.; Lewandowski, W. | ||||
| Title | Tunable circularly polarized luminescence via chirality induction and energy transfer from organic films to semiconductor nanocrystals | Type | A1 Journal article | ||
| Year | 2022 | Publication | ACS nano | Abbreviated Journal | Acs Nano |
| Volume | 16 | Issue | 11 | Pages | 18472-18482 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Circularly polarized luminescent (CPL) films with high dissymmetry factors hold great potential for optoelectronic applications. Herei n , we propose a strategy for achieving strongly dissymetric CPL in nanocomposite films based on chira l i t y induction and energy transfer to semiconductor nanocrystals. First, focusing on a purely organic system, aggregation-induced emission (AIE) and CPL activity of organic liquid crystals (LCs) forming helical nanofilaments was detected, featuring green emission with high dissymmetry factors g(lum) similar to 10(-2). The handedness of helical filaments, and thus the sign of CPL, was controlled via minute amounts of a small chiral organic dopant. Second, nanocomposite films were fabricated by incorporating InP/ZnS semi-conductor quantum dots (QDs) into the LC matri x , which induced the chiral assembly of QDs and endowed them with chiroptical properties. Due to the spectral matching of the components, energy transfer (ET) from LC to QDs was possible enabling a convenient way of tuning CPL wavelengths by varying the LC/QD ratio. As obtained, composite films exhibited absolute glum values up to similar to 10(-2) and thermally on/off switchable luminescence. Overall, we demonstrate the induction of chiroptical properties by the assembly of nonchiral building QDs on the chiral organic template and energy transfer from organic films to QDs, representing a simple and versatile approach to tune the CPL activity of organic materials. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000883943600001 | Publication Date | 2022-11-07 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 1936-0851 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 17.1 | Times cited | 10 | Open Access |
OpenAccess |
| Notes | W.L., S.P., and M.B. acknowledge support from the National Science Center Poland under the OPUS Grant UMO-2019/35/B/ST5/04488. J.T. and G.H.C. acknowledge the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany's Excellence Strategy, Grant EXC 2033-390677874-RESOLV. W.L. acknowledges financial support from the European Commission under the Horizon 2020 Programme by Grant E210400529. S.B. and A.P.-T. acknowledge financial support from the European Commission under the Horizon 2020 Programme by Grant 731019 (EUSMI) and ERC Consolidator Grant 815128 (REALNANO). We thank Elie Benchimol for his help with the CPL measurements. We thank Damian Pociecha for his help in the determination of phase sequences of organic compounds. | Approved | Most recent IF: 17.1 | ||
| Call Number | UA @ admin @ c:irua:192101 | Serial | 7345 | ||
| Permanent link to this record | |||||
| Author | Mulder, J.T.; Meijer, M.S.; van Blaaderen, J.J.; du Fosse, I.; Jenkinson, K.; Bals, S.; Manna, L.; Houtepen, A.J. | ||||
| Title | Understanding and preventing photoluminescence quenching to achieve unity photoluminescence quantum yield in Yb:YLF nanocrystals | Type | A1 Journal article | ||
| Year | 2023 | Publication | ACS applied materials and interfaces | Abbreviated Journal | |
| Volume | 15 | Issue | 2 | Pages | 3274-3286 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Ytterbium-doped LiYF4 (Yb:YLF) is a commonly used material for laser applications, as a photon upconversion medium, and for optical refrigeration. As nanocrystals (NCs), the material is also of interest for biological and physical applications. Unfortunately, as with most phosphors, with the reduction in size comes a large reduction of the photoluminescence quantum yield (PLQY), which is typically associated with an increase in surface-related PL quenching. Here, we report the synthesis of bipyramidal Yb:YLF NCs with a short axis of similar to 60 nm. We systematically study and remove all sources of PL quenching in these NCs. By chemically removing all traces of water from the reaction mixture, we obtain NCs that exhibit a near-unity PLQY for an Yb3+ concentration below 20%. At higher Yb3+ concentrations, efficient concentration quenching occurs. The surface PL quenching is mitigated by growing an undoped YLF shell around the NC core, resulting in near-unity PLQY values even for fully Yb3+-based LiYbF4 cores. This unambiguously shows that the only remaining quenching sites in core-only Yb:YLF NCs reside on the surface and that concentration quenching is due to energy transfer to the surface. Monte Carlo simulations can reproduce the concentration dependence of the PLQY. Surprisingly, Fo''rster resonance energy transfer does not give satisfactory agreement with the experimental data, whereas nearest-neighbor energy transfer does. This work demonstrates that Yb3+-based nanophosphors can be synthesized with a quality close to that of bulk single crystals. The high Yb3+ concentration in the LiYbF4/LiYF4 core/shell nanocrystals increases the weak Yb3+ absorption, making these materials highly promising for fundamental studies and increasing their effectiveness in bioapplications and optical refrigeration. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000912997300001 | Publication Date | 2023-01-06 | |
| 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 |
OpenAccess |
| Notes | This project has received funding from the European Union's Horizon 2020 research and innovation program under Grant Agreement No. 766900 (Testing the Large-Scale Limit of Quantum Mechanics). A.J.H. and I.d.F. further acknowledge the European Research Council Horizon 2020 ERC Grant Agreement No. 678004 (Doping on Demand) for financial support. The authors thank Freddy Rabouw and Andries Meijerink (Utrecht University) for very fruitful discussions and extremely useful advice. The author s thank Jos Thieme for his help with the laser setups used . The authors furthermore thank Niranjan Saikumar for proofreading the manuscript. | Approved | Most recent IF: 9.5; 2023 IF: 7.504 | ||
| Call Number | UA @ admin @ c:irua:194317 | Serial | 7348 | ||
| Permanent link to this record | |||||
| Author | Benedet, M.; Andrea Rizzi, G.; Gasparotto, A.; Gauquelin, N.; Orekhov, A.; Verbeeck, J.; Maccato, C.; Barreca, D. | ||||
| Title | Functionalization of graphitic carbon nitride systems by cobalt and cobalt-iron oxides boosts solar water oxidation performances | Type | A1 Journal article | ||
| Year | 2023 | Publication | Applied surface science | Abbreviated Journal | |
| Volume | 618 | Issue | Pages | 156652 | |
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
| Abstract | The ever-increasing energy demand from the world population has made the intensive use of fossil fuels an overarching threat to global environment and human health. An appealing alternative is offered by sunlight-assisted photoelectrochemical water splitting to yield carbon-free hydrogen fuel, but kinetic limitations associated to the oxygen evolution reaction (OER) render the development of cost-effective, eco-friendly and stable electrocatalysts an imperative issue. In the present work, OER catalysts based on graphitic carbon nitride (g-C3N4) were deposited on conducting glass substrates by a simple decantation procedure, followed by functionalization with low amounts of nanostructured CoO and CoFe2O4 by radio frequency (RF)-sputtering, and final annealing under inert atmosphere. A combination of advanced characterization tools was used to investigate the interplay between material features and electrochemical performances. The obtained results highlighted the formation of a p-n junction for the g-C3N4-CoO system, whereas a Z-scheme junction accounted for the remarkable performance enhancement yielded by g-C3N4-CoFe2O4. The intimate contact between the system components also afforded an improved electrocatalyst stability in comparison to various bare and functionalized g-C3N4-based systems. These findings emphasize the importance of tailoring g-C3N4 chemico-physical properties through the dispersion of complementary catalysts to fully exploit its applicative potential. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000950654300001 | Publication Date | 2023-02-04 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 0169-4332 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 6.7 | Times cited | 11 | Open Access |
OpenAccess |
| Notes | The authors gratefully acknowledge financial support from CNR (Progetti di Ricerca @CNR – avviso 2020 – ASSIST), Padova University (P-DiSC#04BIRD2020-UNIPD EUREKA, DOR 2020–2022), AMGA Foundation (NYMPHEA project), INSTM Consortium (INSTM21PDGASPAROTTO – NANOMAT, INSTM21PDBARMAC – ATENA) and the European Union's Horizon 2020 research and innovation program under grant agreement No 823717 – ESTEEM3. The FWO-Hercules fund G0H4316N 'Direct electron detector for soft matter TEM' is also acknowledged. Many thanks are due to Prof. Luca Gavioli (Università Cattolica del Sacro Cuore, Brescia, Italy) and Dr. Riccardo Lorenzin (Department of Chemical Sciences, Padova University, Italy) for their invaluable technical support.; esteem3reported; esteem3TA | Approved | Most recent IF: 6.7; 2023 IF: 3.387 | ||
| Call Number | EMAT @ emat @c:irua:196150 | Serial | 7376 | ||
| Permanent link to this record | |||||
| Author | Verdierre, G.; Gauquelin, N.; Jannis, D.; Birkhölzer, Y.A.; Mallik, S.; Verbeeck, J.; Bibes, M.; Koster, G. | ||||
| Title | Epitaxial growth of the candidate ferroelectric Rashba material SrBiO3by pulsed laser deposition | Type | A1 Journal article | ||
| Year | 2023 | Publication | APL materials | Abbreviated Journal | |
| Volume | 11 | Issue | 3 | Pages | 031109 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Among oxides, bismuthates have been gaining much interest due to their unique features. In addition to their superconducting properties, they show potential for applications as topological insulators and as possible spin-to-charge converters. After being first investigated in their bulk form in the 1980s, bismuthates have been successfully grown as thin films. However, most efforts have focused on BaBiO<sub>3</sub>, with SrBiO<sub>3</sub>receiving only little attention. Here, we report the growth of epitaxial films of SrBiO<sub>3</sub>on both TiO<sub>2</sub>-terminated SrTiO<sub>3</sub>and NdO-terminated NdScO<sub>3</sub>substrates by pulsed laser deposition. SrBiO<sub>3</sub>has a pseudocubic lattice constant of ∼4.25 Å and grows relaxed on NdScO<sub>3</sub>. Counter-intuitively, it grows with a slight tensile strain on SrTiO<sub>3</sub>despite a large lattice mismatch, which should induce compressive strain. High-resolution transmission electron microscopy reveals that this occurs as a consequence of structural domain matching, with blocks of 10 SrBiO<sub>3</sub>unit planes matching blocks of 11 SrTiO<sub>3</sub>unit planes. This work provides a framework for the synthesis of high quality perovskite bismuthates films and for the understanding of their interface interactions with homostructural substrates. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000953363800004 | Publication Date | 2023-03-01 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 2166-532X | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 6.1 | Times cited | Open Access |
OpenAccess | |
| Notes | This work received support from the ERC Advanced grant (Grant No. 833973) “FRESCO” and funding from the European Union’s Horizon 2020 Research and Innovation Program under Grant Agreement No. 823717—ESTEEM3, Van Gogh travel grant, Nuffic, The Netherlands (CF No. 42582SB).; esteem3reported; esteem3TA | Approved | Most recent IF: 6.1; 2023 IF: 4.335 | ||
| Call Number | EMAT @ emat @c:irua:196135 | Serial | 7377 | ||
| Permanent link to this record | |||||
| Author | Benedoue, S.; Benedet, M.; Gasparotto, A.; Gauquelin, N.; Orekhov, A.; Verbeeck, J.; Seraglia, R.; Pagot, G.; Rizzi, G.A.; Balzano, V.; Gavioli, L.; Noto, V.D.; Barreca, D.; Maccato, C. | ||||
| Title | Insights into the Photoelectrocatalytic Behavior of gCN-Based Anode Materials Supported on Ni Foams | Type | A1 Journal article | ||
| Year | 2023 | Publication | Nanomaterials | Abbreviated Journal | Nanomaterials-Basel |
| Volume | 13 | Issue | 6 | Pages | 1035 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Graphitic carbon nitride (gCN) is a promising n-type semiconductor widely investigated for photo-assisted water splitting, but less studied for the (photo)electrochemical degradation of aqueous organic pollutants. In these fields, attractive perspectives for advancements are offered by a proper engineering of the material properties, e.g., by depositing gCN onto conductive and porous scaffolds, tailoring its nanoscale morphology, and functionalizing it with suitable cocatalysts. The present study reports on a simple and easily controllable synthesis of gCN flakes on Ni foam substrates by electrophoretic deposition (EPD), and on their eventual decoration with Co-based cocatalysts [CoO, CoFe2O4, cobalt phosphate (CoPi)] via radio frequency (RF)-sputtering or electrodeposition. After examining the influence of processing conditions on the material characteristics, the developed systems are comparatively investigated as (photo)anodes for water splitting and photoelectrocatalysts for the degradation of a recalcitrant water pollutant [potassium hydrogen phthalate (KHP)]. The obtained results highlight that while gCN decoration with Co-based cocatalysts boosts water splitting performances, bare gCN as such is more efficient in KHP abatement, due to the occurrence of a different reaction mechanism. The related insights, provided by a multi-technique characterization, may provide valuable guidelines for the implementation of active nanomaterials in environmental remediation and sustainable solar-to-chemical energy conversion. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000960297000001 | Publication Date | 2023-03-13 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 2079-4991 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 5.3 | Times cited | 3 | Open Access |
OpenAccess |
| Notes | The present work was financially supported by CNR (Progetti di Ricerca @CNR—avviso 2020—ASSIST), Padova University (P-DiSC#04BIRD2020-UNIPD EUREKA, DOR 2020–2022), AMGA Foundation (NYMPHEA project), INSTM Consortium (INSTM21PDGASPAROTTO—NANOMAT, INSTM21PDBARMAC—ATENA) and the European Union’s Horizon 2020 research and innovation program under grant agreement No. 823717—ESTEEM3. The FWO-Hercules fund G0H4316N ‘Direct electron detector for soft matter TEM’ is also acknowledged. Many thanks are also due to Dr. Riccardo Lorenzin for his support to experimental activities.; esteem3reported; esteem3TA | Approved | Most recent IF: 5.3; 2023 IF: 3.553 | ||
| Call Number | EMAT @ emat @c:irua:196115 | Serial | 7378 | ||
| Permanent link to this record | |||||
| Author | Jain, N.; Hao, Y.; Parekh, U.; Kaltenegger, M.; Pedrazo-Tardajos, A.; Lazzaroni, R.; Resel, R.; Geerts, Y.H.; Bals, S.; Van Aert, S. | ||||
| Title | Exploring the effects of graphene and temperature in reducing electron beam damage: A TEM and electron diffraction-based quantitative study on Lead Phthalocyanine (PbPc) crystals | Type | A1 Journal article | ||
| Year | 2023 | Publication | Micron | Abbreviated Journal | |
| Volume | 169 | Issue | Pages | 103444 | |
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
| Abstract | High-resolution transmission electron microscopy (TEM) of organic crystals, such as Lead Phthalocyanine (PbPc), is very challenging since these materials are prone to electron beam damage leading to the breakdown of the crystal structure during investigation. Quantification of the damage is imperative to enable high-resolution imaging of PbPc crystals with minimum structural changes. In this work, we performed a detailed electron diffraction study to quantitatively measure degradation of PbPc crystals upon electron beam irradiation. Our study is based on the quantification of the fading intensity of the spots in the electron diffraction patterns. At various incident dose rates (e/Å2/s) and acceleration voltages, we experimentally extracted the decay rate (1/s), which directly correlates with the rate of beam damage. In this manner, a value for the critical dose (e/Å2) could be determined, which can be used as a measure to quantify beam damage. Using the same methodology, we explored the influence of cryogenic temperatures, graphene TEM substrates, and graphene encapsulation in prolonging the lifetime of the PbPc crystal structure during TEM investigation. The knowledge obtained by diffraction experiments is then translated to real space high-resolution TEM imaging of PbPc. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000965998800001 | Publication Date | 2023-03-21 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 0968-4328 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 2.4 | Times cited | 1 | Open Access |
OpenAccess |
| Notes | This work is supported by FWO and FNRS within the 2Dto3D network of the EOS (Excellence of Science) program (grant number 30489208) and ERC-CoGREALNANO-815128 (to Prof. Dr. Sara Bals). N.J. would like to thank Dr. Kunal S. Mali and Dr. Da Wang for useful and interesting discussions on sample preparation procedures. | Approved | Most recent IF: 2.4; 2023 IF: 1.98 | ||
| Call Number | EMAT @ emat @c:irua:196069 | Serial | 7379 | ||
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| Author | Kante, M.V.; Weber, M.L.; Ni, S.; van den Bosch, I.C.G.; van der Minne, E.; Heymann, L.; Falling, L.J.; Gauquelin, N.; Tsvetanova, M.; Cunha, D.M.; Koster, G.; Gunkel, F.; Nemsak, S.; Hahn, H.; Estrada, L.V.; Baeumer, C. | ||||
| Title | A high-entropy oxide as high-activity electrocatalyst for water oxidation | Type | A1 Journal article | ||
| Year | 2023 | Publication | ACS nano | Abbreviated Journal | |
| Volume | 17 | Issue | 6 | Pages | 5329-5339 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
| Abstract | High-entropy materials are an emerging pathway in the development of high-activity (electro)catalysts because of the inherent tunability and coexistence of multiple potential active sites, which may lead to earth-abundant catalyst materials for energy-efficient electrochemical energy storage. In this report, we identify how the multication composition in high-entropy perovskite oxides (HEO) contributes to high catalytic activity for the oxygen evolution reaction (OER), i.e., the key kinetically limiting half-reaction in several electrochemical energy conversion technologies, including green hydrogen generation. We compare the activity of the (001) facet of LaCr0.2Mn0.2Fe0.2Co0.2Ni0.2O3-delta with the parent compounds (single B-site in the ABO3 perovskite). While the single B-site perovskites roughly follow the expected volcano-type activity trends, the HEO clearly outperforms all of its parent compounds with 17 to 680 times higher currents at a fixed overpotential. As all samples were grown as an epitaxial layer, our results indicate an intrinsic composition-function relationship, avoiding the effects of complex geometries or unknown surface composition. In-depth X-ray photoemission studies reveal a synergistic effect of simultaneous oxidation and reduction of different transition metal cations during the adsorption of reaction intermediates. The surprisingly high OER activity demonstrates that HEOs are a highly attractive, earth-abundant material class for high-activity OER electrocatalysts, possibly allowing the activity to be fine-tuned beyond the scaling limits of mono-or bimetallic oxides. | ||||
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| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000953440900001 | Publication Date | 2023-03-13 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 1936-0851 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 17.1 | Times cited | Open Access |
OpenAccess | |
| Notes | Approved | Most recent IF: 17.1; 2023 IF: 13.942 | |||
| Call Number | UA @ admin @ c:irua:196097 | Serial | 7390 | ||
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| Author | Chen, H.; Xiong, Y.; Li, J.; Abed, J.; Wang, D.; Pedrazo-Tardajos, A.; Cao, Y.; Zhang, Y.; Wang, Y.; Shakouri, M.; Xiao, Q.; Hu, Y.; Bals, S.; Sargent, E.H.H.; Su, C.-Y.; Yang, Z. | ||||
| Title | Epitaxially grown silicon-based single-atom catalyst for visible-light-driven syngas production | Type | A1 Journal article | ||
| Year | 2023 | Publication | Nature communications | Abbreviated Journal | Nat Commun |
| Volume | 14 | Issue | 1 | Pages | 1719-11 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Despite the natural abundance and promising properties of Si, there are few examples of crystalline Si-based catalysts. Here, the authors report an epitaxial growth method to construct Co single atoms on Si for light driven CO2 reduction to syngas. Improving the dispersion of active sites simultaneous with the efficient harvest of photons is a key priority for photocatalysis. Crystalline silicon is abundant on Earth and has a suitable bandgap. However, silicon-based photocatalysts combined with metal elements has proved challenging due to silicon's rigid crystal structure and high formation energy. Here we report a solid-state chemistry that produces crystalline silicon with well-dispersed Co atoms. Isolated Co sites in silicon are obtained through the in-situ formation of CoSi2 intermediate nanodomains that function as seeds, leading to the production of Co-incorporating silicon nanocrystals at the CoSi2/Si epitaxial interface. As a result, cobalt-on-silicon single-atom catalysts achieve an external quantum efficiency of 10% for CO2-to-syngas conversion, with CO and H-2 yields of 4.7 mol g((Co))(-1) and 4.4 mol g((Co))(-1), respectively. Moreover, the H-2/CO ratio is tunable between 0.8 and 2. This photocatalyst also achieves a corresponding turnover number of 2 x 10(4) for visible-light-driven CO2 reduction over 6 h, which is over ten times higher than previously reported single-atom photocatalysts. | ||||
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| Language | Wos | 000962607600018 | Publication Date | 2023-03-28 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 2041-1723 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 16.6 | Times cited | 6 | Open Access |
OpenAccess |
| Notes | This work was supported by the National Natural Science Foundation of China (21821003, 21890380, 21905316), Guangdong Natural Science Foundation (2019A1515011748), the Science and Technology Planning Project of Guangdong Province (2019A050510018), Pearl River Recruitment Program of Talent (2019QN01C108), the EU Infrastructure Project EUSMI (Grant No. E190700310), and Sun Yat-sen University. D.W. acknowledges an Individual Fellowship funded by the Marie-Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (grant 894254 SuprAtom). S.B. and A.P.-T. acknowledge financial support from the European Commission under the Horizon 2020 Programme by grant no. 731019 (EUSMI) and ERC Consolidator grant no. 815128 (REALNANO). This project has received funding from the European Commission Grant (EUSMI E190700310). Synchrotron XAS data described in this paper was performed at the Canadian Light Source, a national research facility of the University of Saskatchewan, which is supported by the Canada Foundation for Innovation (CFI), the Natural Sciences and Engineering Research Council (NSERC), the National Research Council (NRC), the Canadian Institutes of Health Research (CIHR), the Government of Saskatchewan, and the University of Saskatchewan. | Approved | Most recent IF: 16.6; 2023 IF: 12.124 | ||
| Call Number | UA @ admin @ c:irua:196062 | Serial | 7932 | ||
| Permanent link to this record | |||||
| Author | Gauquelin, N.; Forte, F.; Jannis, D.; Fittipaldi, R.; Autieri, C.; Cuono, G.; Granata, V.; Lettieri, M.; Noce, C.; Miletto-Granozio, F.; Vecchione, A.; Verbeeck, J.; Cuoco, M. | ||||
| Title | Pattern Formation by Electric-Field Quench in a Mott Crystal | Type | A1 Journal article | ||
| Year | 2023 | Publication | Nano letters | Abbreviated Journal | |
| Volume | Issue | Pages | |||
| Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
| Abstract | The control of Mott phase is intertwined with the spatial reorganization of the electronic states. Out-of-equilibrium driving forces typically lead to electronic patterns that are absent at equilibrium, whose nature is however often elusive. Here, we unveil a nanoscale pattern formation in the Ca2 RuO4 Mott insulator. We demonstrate how an applied electric field spatially reconstructs the insulating phase that, uniquely after switching off the electric field, exhibits nanoscale stripe domains. The stripe pattern has regions with inequivalent octahedral distortions that we directly observe through high-resolution scanning transmission electron microscopy. The nanotexture depends on the orientation of the electric field, it is non-volatile and rewritable. We theoretically simulate the charge and orbital reconstruction induced by a quench dynamics of the applied electric field providing clear-cut mechanisms for the stripe phase formation. Our results open the path for the design of non-volatile electronics based on voltage-controlled nanometric phases. |
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| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001012061600001 | Publication Date | 2023-05-18 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 1530-6984 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 10.8 | Times cited | 2 | Open Access |
OpenAccess |
| Notes | This project has received funding from the European Union’s Horizon 2020 research and innova- tion programme under grant agreement No 823717 – ESTEEM3. The Merlin camera used in the experiment received funding from the FWO-Hercules fund G0H4316N ’Direct electron detector 15for soft matter TEM’. C. A. and G. C. are supported by the Foundation for Polish Science through the International Research Agendas program co-financed by the European Union within the Smart Growth Operational Programme. C. A. and G. C. acknowledge the access to the computing facil- ities of the Interdisciplinary Center of Modeling at the University of Warsaw, Grant No. GB84-0, GB84-1 and GB84-7 and GB84-7 and Poznan Supercomputing and Networking Center Grant No. 609.. C. A. and G. C. acknowledge the CINECA award under the ISCRA initiative IsC85 “TOP- MOST” Grant, for the availability of high-performance computing resources and support. We acknoweldge A. Guarino and C. Elia for providing support about the electrical characterization of the sample. M.C., R.F., and A.V. acknowledge support from the EU’s Horizon 2020213 research and innovation program under Grant Agreement No. 964398 (SUPERGATE). | Approved | Most recent IF: 10.8; 2023 IF: 12.712 | ||
| Call Number | EMAT @ emat @c:irua:196970 | Serial | 8789 | ||
| Permanent link to this record | |||||
| Author | Samal, D.; Gauquelin, N.; Takamura, Y.; Lobato, I.; Arenholz, E.; Van Aert, S.; Huijben, M.; Zhong, Z.; Verbeeck, J.; Van Tendeloo, G.; Koster, G. | ||||
| Title | Unusual structural rearrangement and superconductivity in infinite layer cuprate superlattices | Type | A1 Journal article | ||
| Year | 2023 | Publication | Physical review materials | Abbreviated Journal | |
| Volume | 7 | Issue | 5 | Pages | 054803 |
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
| Abstract | |||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001041792100007 | Publication Date | 2023-05-30 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 2475-9953 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 3.4 | Times cited | Open Access |
OpenAccess | |
| Notes | Air Force Office of Scientific Research; European Office of Aerospace Research and Development, FA8655-10-1-3077 ; Office of Science, DE-AC02-05CH11231 ; National Science Foundation, DMR-1745450 ; Seventh Framework Programme, 278510 ; Bijzonder Onderzoeksfonds UGent; | Approved | Most recent IF: 3.4; 2023 IF: NA | ||
| Call Number | EMAT @ emat @c:irua:196973 | Serial | 8790 | ||
| Permanent link to this record | |||||
| Author | Mary Joy, R.; Pobedinskas, P.; Bourgeois, E.; Chakraborty, T.; Görlitz, J.; Herrmann, D.; Noël, C.; Heupel, J.; Jannis, D.; Gauquelin, N.; D'Haen, J.; Verbeeck, J.; Popov, C.; Houssiau, L.; Becher, C.; Nesládek, M.; Haenen, K. | ||||
| Title | Germanium vacancy centre formation in CVD nanocrystalline diamond using a solid dopant source | Type | A3 Journal article | ||
| Year | 2023 | Publication | Science talks | Abbreviated Journal | Science Talks |
| Volume | 5 | Issue | Pages | 100157 | |
| Keywords | A3 Journal article; Electron microscopy for materials research (EMAT) | ||||
| Abstract | |||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | Publication Date | 2023-02-09 | ||
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 2772-5693 | ISBN | Additional Links | UA library record | |
| Impact Factor | Times cited | Open Access |
OpenAccess | ||
| Notes | Approved | Most recent IF: NA | |||
| Call Number | EMAT @ emat @c:irua:196969 | Serial | 8791 | ||
| Permanent link to this record | |||||
| Author | Kavak, S.; Kadu, A.A.; Claes, N.; Sánchez-Iglesias, A.; Liz-Marzán, L.M.; Batenburg, K.J.; Bals, S. | ||||
| Title | Quantitative 3D Investigation of Nanoparticle Assemblies by Volumetric Segmentation of Electron Tomography Data Sets | Type | A1 Journal article | ||
| Year | 2023 | Publication | The journal of physical chemistry: C : nanomaterials and interfaces | Abbreviated Journal | |
| Volume | 127 | Issue | 20 | Pages | 9725-9734 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Morphological characterization of nanoparticle assemblies and hybrid nanomaterials is critical in determining their structure-property relationships as well as in the development of structures with desired properties. Electron tomography has become a widely utilized technique for the three-dimensional characterization of nanoparticle assemblies. However, the extraction of quantitative morphological parameters from the reconstructed volume can be a complex and labor-intensive task. In this study, we aim to overcome this challenge by automating the volumetric segmentation process applied to three-dimensional reconstructions of nanoparticle assemblies. The key to enabling automated characterization is to assess the performance of different volumetric segmentation methods in accurately extracting predefined quantitative descriptors for morphological characterization. In our methodology, we compare the quantitative descriptors obtained through manual segmentation with those obtained through automated segmentation methods, to evaluate their accuracy and effectiveness. To show generality, our study focuses on the characterization of assemblies of CdSe/CdS quantum dots, gold nanospheres and CdSe/CdS encapsulated in polymeric micelles, and silica-coated gold nanorods decorated with both CdSe/CdS or PbS quantum dots. We use two unsupervised segmentation algorithms: the watershed transform and the spherical Hough transform. Our results demonstrate that the choice of automated segmentation method is crucial for accurately extracting the predefined quantitative descriptors. Specifically, the spherical Hough transform exhibits superior performance in accurately extracting quantitative descriptors, such as particle size and interparticle distance, thereby allowing for an objective, efficient, and reliable volumetric segmentation of complex nanoparticle assemblies. | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000991752700001 | Publication Date | 2023-05-25 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 1932-7447 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 3.7 | Times cited | 2 | Open Access |
OpenAccess |
| Notes | Fonds Wetenschappelijk Onderzoek, 1181122N ; Horizon 2020 Framework Programme, 861950 ; H2020 European Research Council, 815128 ; | Approved | Most recent IF: 3.7; 2023 IF: 4.536 | ||
| Call Number | EMAT @ emat @c:irua:196971 | Serial | 8793 | ||
| Permanent link to this record | |||||
| Author | Vlasov, E.; Skorikov, A.; Sánchez-Iglesias, A.; Liz-Marzán, L.M.; Verbeeck, J.; Bals, S. | ||||
| Title | Secondary electron induced current in scanning transmission electron microscopy: an alternative way to visualize the morphology of nanoparticles | Type | A1 Journal article | ||
| Year | 2023 | Publication | ACS materials letters | Abbreviated Journal | ACS Materials Lett. |
| Volume | Issue | Pages | 1916-1921 | ||
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Electron tomography (ET) is a powerful tool to determine the three-dimensional (3D) structure of nanomaterials in a transmission electron microscope. However, the acquisition of a conventional tilt series for ET is a time-consuming process and can therefore not provide 3D structural information in a time-efficient manner. Here, we propose surface-sensitive secondary electron (SE) imaging as an alternative to ET for the investigation of the morphology of nanomaterials. We use the SE electron beam induced current (SEEBIC) technique that maps the electrical current arising from holes generated by the emission of SEs from the sample. SEEBIC imaging can provide valuable information on the sample morphology with high spatial resolution and significantly shorter throughput times compared with ET. In addition, we discuss the contrast formation mechanisms that aid in the interpretation of SEEBIC data. | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001006191600001 | Publication Date | 2023-06-12 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 2639-4979 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | Times cited | 1 | Open Access |
OpenAccess | |
| Notes | The funding for this project was provided by European Research Council (ERC Consolidator Grant 815128, REALNANO). J.V. acknowledges the eBEAM project, which is supported by the European Union’s Horizon 2020 research and innovation program under grant agreement no. 101017720 (FET-Proactive EBEAM). L.M.L.-M. acknowledges funding from MCIN/AEI/10.13039/501100011033 (grant # PID2020-117779RB-I00). | Approved | Most recent IF: NA | ||
| Call Number | EMAT @ emat @c:irua:197004 | Serial | 8795 | ||
| Permanent link to this record | |||||
| Author | Saniz, R.; Baldinozzi, G.; Arts, I.; Lamoen, D.; Leinders, G.; Verwerft, M. | ||||
| Title | Charge order, frustration relief, and spin-orbit coupling in U3O8 | Type | A1 Journal article | ||
| Year | 2023 | Publication | Physical review materials | Abbreviated Journal | |
| Volume | 7 | Issue | 5 | Pages | 054410 |
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Research efforts on the description of the low-temperature magnetic order and electronic properties of U3O8 have been inconclusive so far. Reinterpreting neutron scattering results, we use group representation theory to show that the ground state presents collinear out-of-plane magnetic moments, with antiferromagnetic coupling both in-layer and between layers. Charge order relieves the initial geometric frustration, generating a slightly distorted honeycomb sublattice with Néel-type order. The precise knowledge of the characteristics of this magnetic ground state is then used to explain the fine features of the band gap. In this system, spin-orbit coupling (SOC) is of critical importance, as it strongly affects the electronic structure, narrowing the gap by ∼38%, compared to calculations neglecting SOC. The predicted electronic structure actually explains the salient features of recent optical absorption measurements, further demonstrating the excellent agreement between the calculated ground state properties and experiment. | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001041429800007 | Publication Date | 2023-05-31 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 2475-9953 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 3.4 | Times cited | Open Access |
OpenAccess | |
| Notes | Financial support for this research was partly provided by the Energy Transition Fund of the Belgian FPS Economy (Project SF-CORMOD Spent Fuel CORrosion MODeling).Fonds Wetenschappelijk Onderzoek; Vlaams Supercomputer Centrum; Universiteit Antwerpen; Vlaamse regering; | Approved | Most recent IF: 3.4; 2023 IF: NA | ||
| Call Number | EMAT @ emat @c:irua:197043 | Serial | 8796 | ||
| Permanent link to this record | |||||
| Author | Carrasco, S.; Orcajo, G.; Martínez, F.; Imaz, I.; Kavak, S.; Arenas-Esteban, D.; Maspoch, D.; Bals, S.; Calleja, G.; Horcajada, P. | ||||
| Title | Hf/porphyrin-based metal-organic framework PCN-224 for CO2 cycloaddition with epoxides | Type | A1 Journal article | ||
| Year | 2023 | Publication | Materials Today Advances | Abbreviated Journal | |
| Volume | 19 | Issue | Pages | 100390 | |
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Herein, we describe for the first time the synthesis of the highly porous Hf-tetracarboxylate porphyrin-based metal-organic framework (MOF) (Hf)PCN-224(M) (M = H2, Co2+). (Hf)PCN-224(H2) was easily and efficiently prepared following a simple microwave-assisted procedure with good yields (56–67%; space-time yields: 1100–1270 kg m−3·day−1), high crystallinity and phase purity by using trifluoromethanesulfonic acid and benzoic acid as modulators in less than 30 min. By simply introducing a preliminary step (10 min), 5,10,15,20-(tetra-4-carboxyphenyl)porphyrin linker (TCPP) was quantitatively metalated with Co2+ without additional purification and/or time consuming protection/deprotection steps to further obtain (Hf)PCN-224(Co). (Hf)PCN-224(Co) was then tested as catalyst in CO2 cycloaddition reaction with different epoxides to yield cyclic carbonates, showing the best catalytic performance described to date compared to other PCNs, under mild conditions (1 bar CO2, room temperature, 18–24 h). Twelve epoxides were tested, obtaining from moderate to excellent conversions (35–96%). Moreover, this reaction was gram scaled-up (x50) without significant loss of yield to cyclic carbonates. (Hf)PCN-224(Co) maintained its integrity and crystallinity even after 8 consecutive runs, and poisoning was efficiently reverted by a simple thermal treatment (175 °C, 6 h), fully recovering the initial catalytic activity. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001025764000001 | Publication Date | 2023-06-19 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 2590-0498 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 10 | Times cited | 1 | Open Access |
OpenAccess |
| Notes | S.C. acknowledges the European Union's Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie (MSCA-COFUND) grant agreement No 754382 (GOT Energy Talent). S.C. and P.H. acknowledge “Comunidad de Madrid” and European Regional Development Fund-FEDER 2014-2020-OE REACT-UE 1 for their financial support to VIRMOF-CM project associated to R&D projects in response to COVID-19. The authors acknowledge H2020-MSCA-ITN-2019 HeatNMof (ref. 860942), the M-ERA-NET C-MOF-cell (grant PCI2020-111998 funded by MCIN/AEI /10.13039/501100011033 and European Union NextGenerationEU/PRTR) project, and Retos Investigación MOFSEIDON (grant PID2019-104228RB-I00 funded by MCIN/AEI/10.13039/501100011033) project. This work has been also supported by the Regional Government of Madrid (Project ACES2030-CM, S2018/EMT-4319) and the Universidad Rey Juan Carlos IMPULSO Project (grant MATER M − 3000). S.K acknowledges the Flemish Fund for Scientific Research (FWO Vlaanderen) through a PhD research grant (1181122 N). | Approved | Most recent IF: 10; 2023 IF: NA | ||
| Call Number | EMAT @ emat @c:irua:197198 | Serial | 8800 | ||
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| Author | Muravev, V.; Parastaev, A.; van den Bosch, Y.; Ligt, B.; Claes, N.; Bals, S.; Kosinov, N.; Hensen, E.J.M. | ||||
| Title | Size of cerium dioxide support nanocrystals dictates reactivity of highly dispersed palladium catalysts | Type | A1 Journal article | ||
| Year | 2023 | Publication | Science | Abbreviated Journal | |
| Volume | 380 | Issue | 6650 | Pages | 1174-1179 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
| Abstract | The catalytic performance of heterogeneous catalysts can be tuned by modulation of the size and structure of supported transition metals, which are typically regarded as the active sites. In single-atom metal catalysts, the support itself can strongly affect the catalytic properties. Here, we demonstrate that the size of cerium dioxide (CeO2) support governs the reactivity of atomically dispersed palladium (Pd) in carbon monoxide (CO) oxidation. Catalysts with small CeO2 nanocrystals (~4 nanometers) exhibit unusually high activity in a CO-rich reaction feed, whereas catalysts with medium-size CeO2 (~8 nanometers) are preferred for lean conditions. Detailed spectroscopic investigations reveal support size–dependent redox properties of the Pd-CeO2 interface. | ||||
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| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001010846100008 | Publication Date | 2023-06-16 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 0036-8075 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 56.9 | Times cited | 22 | Open Access |
OpenAccess |
| Notes | We thank the staff of the MAX IV Laboratory for time on beamline SPECIES under proposals 20200412 and 20190983; E. Kokkonen and A. Klyushin for assistance with NAP-XPS and RPES experiments conducted at SPECIES; staff of the MAX IV Laboratory for time on beamline BALDER under proposal 20200378; K. Klementiev for assistance with XAS measurements; J. Drnec at the ESRF for providing assistance in using beamline ID31; and V. Perez-Dieste and I. Villar Garcia at the CIRCE beamline at ALBA Synchrotron for help with acquiring preliminary RPES data obtained under proposal 2020024219. The synchrotron-based XRD measurements were performed on beamline ID31 at the European Synchrotron Radiation Facility (ESRF), Grenoble, France. Funding: This work was supported by the Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), a NWO Gravitation program funded by the Ministry of Education, Culture and Science of the Government of the Netherlands (V.M. and E.J.M.H.); the European Research Council (ERC consolidator grant 815128 REALNANO to S.B. and N.C.); and the European Union’s Horizon 2020 Research and Innovation Program (grant 823717–ESTEEM to S.B. and N.C). Research conducted at MAX IV, a Swedish national user facility, is supported by the Swedish Research council under contract 2018-07152, the Swedish Governmental Agency for Innovation Systems under contract 2018-04969, and Formas under contract 2019-02496 (VM). | Approved | Most recent IF: 56.9; 2023 IF: 37.205 | ||
| Call Number | EMAT @ emat @c:irua:197199 | Serial | 8801 | ||
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| Author | Vijayakumar, J.; Savchenko, T.M.; Bracher, D.M.; Lumbeeck, G.; Béché, A.; Verbeeck, J.; Vajda, Š.; Nolting, F.; Vaz, Ca.f.; Kleibert, A. | ||||
| Title | Absence of a pressure gap and atomistic mechanism of the oxidation of pure Co nanoparticles | Type | A1 Journal article | ||
| Year | 2023 | Publication | Nature communications | Abbreviated Journal | Nat Commun |
| Volume | 14 | Issue | 1 | Pages | 174 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Understanding chemical reactivity and magnetism of 3<italic>d</italic>transition metal nanoparticles is of fundamental interest for applications in fields ranging from spintronics to catalysis. Here, we present an atomistic picture of the early stage of the oxidation mechanism and its impact on the magnetism of Co nanoparticles. Our experiments reveal a two-step process characterized by (i) the initial formation of small CoO crystallites across the nanoparticle surface, until their coalescence leads to structural completion of the oxide shell passivating the metallic core; (ii) progressive conversion of the CoO shell to Co<sub>3</sub>O<sub>4</sub>and void formation due to the nanoscale Kirkendall effect. The Co nanoparticles remain highly reactive toward oxygen during phase (i), demonstrating the absence of a pressure gap whereby a low reactivity at low pressures is postulated. Our results provide an important benchmark for the development of theoretical models for the chemical reactivity in catalysis and magnetism during metal oxidation at the nanoscale. | ||||
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| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000955726400021 | Publication Date | 2023-01-12 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 2041-1723 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 16.6 | Times cited | 1 | Open Access |
OpenAccess |
| Notes | Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung, 200021160186 2002153540 ; EC | Horizon 2020 Framework Programme, 810310 823717 ; University of Basel | Swiss Nanoscience Institute, P1502 ; This work is funded by Swiss National Foundation (SNF) (Grants. No 200021160186 and 2002153540) and the Swiss Nanoscience Institut (SNI) (Grant No. SNI P1502). S.V. acknowledges support from the European Union’s Horizon 2020 research and innovation programme under grant agreement no. 810310, which corresponds to the J. Heyrovsky Chair project (“ERA Chair at J. Heyrovský Institute of Physical Chemistry AS CR – The institutional approach towards ERA”). The funders had no role in the preparation of the article. Part of this work was performed at the Surface/Interface: Microscopy (SIM) beamline of the Swiss Light Source (SLS), Paul Scherrer Institut, Villigen, Switzerland. We kindly acknowledge Anja Weber and Elisabeth Müller from PSI for their help in fabricating the sample markers. A.B. and J. Verbeeck received funding from the European Union’s Horizon 2020 Research Infrastructure – Integrating Activities for Advanced Communities under grant agreement No. 823717 – ESTEEM3 reported | Approved | Most recent IF: 16.6; 2023 IF: 12.124 | ||
| Call Number | EMAT @ emat @c:irua:196738 | Serial | 8804 | ||
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| Author | Kelly, S.; Mercer, E.; De Meyer, R.; Ciocarlan, R.-G.; Bals, S.; Bogaerts, A. | ||||
| Title | Microwave plasma-based dry reforming of methane: Reaction performance and carbon formation | Type | A1 Journal article | ||
| Year | 2023 | Publication | Journal of CO2 utilization | Abbreviated Journal | Journal of CO2 Utilization |
| Volume | 75 | Issue | Pages | 102564 | |
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | e investigate atmospheric pressure microwave (MW) plasma (2.45 GHz) conversion in CO2 and CH4 mixtures (i.e., dry reforming of methane, DRM) focusing on reaction performance and carbon formation. Promising energy costs of ~2.8–3.0 eV/molecule or ~11.1–11.9 kJ/L are amongst the best performance to date considering the current state-of-the-art for plasma-based DRM for all types of plasma. The conversion is in the range of ~46–49% and ~55–67% for CO2 and CH4, respectively, producing primarily syngas (i.e., H2 and CO) with H2/CO ratios of ~0.6–1 at CH4 fractions ranging from 30% to 45%. Water is the largest byproduct with levels ranging ~7–14% in the exhaust. Carbon particles visibly impact the plasma at higher CH4 fractions (> 30%), where they become heated and incandescent. Particle luminosity increases with increasing CH4 fractions, with the plasma becoming unstable near a 1:1 mixture (i.e., > 45% CH4). Electron microscopy of the carbon material reveals an agglomerated morphology of pure carbon nanoparticles. The mean particle size is determined as ~20 nm, free of any metal contamination, consistent with the electrode-less MW design. | ||||
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| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001065310000001 | Publication Date | 2023-08-10 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 2212-9820 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 7.7 | Times cited | 6 | Open Access |
OpenAccess |
| Notes | We acknowledge financial support by a European Space Agency (ESA) Open Science Innovation Platform study (contract no. 4000137001/21/NL/GLC/ov), the European Marie Skłodowska-Curie Individual Fellowship ‘‘PENFIX’’ within Horizon 2020 (grant no. 838181), the European Research Council (ERC) under the European Union’s Horizon 2020 Research and Innovation Program (grant no. 810182; SCOPE ERC Synergy project), the Excellence of Science FWOFNRS PLASyntH2 project (FWO grant no. G0I1822N and EOS no. 4000751) and the Methusalem project of the University of Antwerp | Approved | Most recent IF: 7.7; 2023 IF: 4.292 | ||
| Call Number | PLASMANT @ plasmant @c:irua:198155 | Serial | 8807 | ||
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| Author | Arteaga Cardona, F.; Jain, N.; Popescu, R.; Busko, D.; Madirov, E.; Arús, B.A.; Gerthsen, D.; De Backer, A.; Bals, S.; Bruns, O.T.; Chmyrov, A.; Van Aert, S.; Richards, B.S.; Hudry, D. | ||||
| Title | Preventing cation intermixing enables 50% quantum yield in sub-15 nm short-wave infrared-emitting rare-earth based core-shell nanocrystals | Type | A1 Journal article | ||
| Year | 2023 | Publication | Nature communications | Abbreviated Journal | Nat Commun |
| Volume | 14 | Issue | 1 | Pages | 4462 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Short-wave infrared (SWIR) fluorescence could become the new gold standard in optical imaging for biomedical applications due to important advantages such as lack of autofluorescence, weak photon absorption by blood and tissues, and reduced photon scattering coefficient. Therefore, contrary to the visible and NIR regions, tissues become translucent in the SWIR region. Nevertheless, the lack of bright and biocompatible probes is a key challenge that must be overcome to unlock the full potential of SWIR fluorescence. Although rare-earth-based core-shell nanocrystals appeared as promising SWIR probes, they suffer from limited photoluminescence quantum yield (PLQY). The lack of control over the atomic scale organization of such complex materials is one of the main barriers limiting their optical performance. Here, the growth of either homogeneous (α-NaYF<sub>4</sub>) or heterogeneous (CaF<sub>2</sub>) shell domains on optically-active α-NaYF<sub>4</sub>:Yb:Er (with and without Ce<sup>3+</sup>co-doping) core nanocrystals is reported. The atomic scale organization can be controlled by preventing cation intermixing only in heterogeneous core-shell nanocrystals with a dramatic impact on the PLQY. The latter reached 50% at 60 mW/cm<sup>2</sup>; one of the highest reported PLQY values for sub-15 nm nanocrystals. The most efficient nanocrystals were utilized for in vivo imaging above 1450 nm. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001037058500022 | Publication Date | 2023-07-25 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 2041-1723 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 16.6 | Times cited | 1 | Open Access |
OpenAccess |
| Notes | D.H. would like to thank Dominique Ectors (Bruker AXS GmbH, Karlsruhe, Germany) for assistance and discussion on the PXRD data and TOPAS evaluations. The authors would like to acknowledge the financial support provided by the Helmholtz Association via: i) the Professorial Recruitment Initiative Funding (B.S.R.); ii) the Research Field Energy – Program Materials and Technologies for the Energy Transition – Topic 1 Photovoltaics (F.A.C., D.B., E.M., B.S.R., D.H.). This project received funding from the European Union’s Horizon 2020 innovation programme under grant agreement 823717. This work was supported by the European Research Council (grant 770887-PICOMETRICS to S.V.A. and Grant 815128-REALNANO to S.B.). The authors acknowledge financial support from the ResearchFoundation Flanders (FWO, Belgium) through project fundings (G.0346.21 N to S.V.A. and S.B.) and a postdoctoral grant (A.D.B.). The authors (B.A.A., O.T.B. and A.C.) acknowledge funding from the Helmholtz Zentrum München, the DFG-Emmy Noether program (BR 5355/2-1) and from the CZI Deep Tissue Imaging (DTI-0000000248). The authors (O.T.B. and D.H.) would like to thank the Helmholtz Imaging (ZT-I-PF-4-038-BENIGN). | Approved | Most recent IF: 16.6; 2023 IF: 12.124 | ||
| Call Number | EMAT @ emat @c:irua:198158 | Serial | 8808 | ||
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| Author | Sa, J.; Hu, N.; Heyvaert, W.; Van Gordon, K.; Li, H.; Wang, L.; Bals, S.; Liz-Marzán, L.M.; Ni, W. | ||||
| Title | Spontaneous Chirality Evolved at the Au–Ag Interface in Plasmonic Nanorods | Type | A1 Journal article | ||
| Year | 2023 | Publication | Chemistry of materials | Abbreviated Journal | Chem. Mater. |
| Volume | Issue | Pages | |||
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Chiral ligands are considered a required ingredient during the synthesis of dissymmetric plasmonic metal nanocrystals. The mechanism behind the generation of chiral structures involves the formation of high Miller index chiral facets, induced by the adsorption of such chiral ligands. We found however that, chirality can also evolve spontaneously, without the involvement of any chiral ligands, during the co-deposition of Au and Ag on Au nanorods. When using a specific Au/Ag ratio, phase segregation of the two metals leads to an interface within the obtained AuAg shell, which can be exposed by removing the Ag component via oxidative etching. Although a close-to-racemic mixture of chiral Au nanorods with right and left handedness is found in solution, electron tomography analysis evidences left- and righthanded helicities, both at the Au-Ag interface and at the exposed surface of Au NRs after Ag etching. The helicity profile of the NRs indicates dominating inclination angles in a range from 30° to 60°. Single-particle optical characterization also reveals random handedness in the plasmonic response of individual nanorods. We hypothesize that, the origin of chirality is related with symmetry breaking during the co-deposition of Au and Ag, through an initial perturbation in a small region on the Au-Ag interface that eventually leads to chiral segregation throughout the nanocrystal. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001052093300001 | Publication Date | 2023-08-21 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 0897-4756 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 8.6 | Times cited | Open Access |
OpenAccess | |
| Notes | The authors acknowledge the financial support from the National Natural Science Foundation of China (grant 22074102). LMLM acknowledges funding from 26 MCIN/AEI/10.13039/501100011033 and “ESF Investing in your future” (Grant PID2020- 117779RB-I00). This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 823717 – ESTEEM3.; Ministerio de Ciencia e Innovaci?n, PID2020-117779RB-I00 ; H2020 Research Infrastructures, 823717 ; European Social Fund, PID2020-117779RB-I00 ; National Natural Science Foundation of China, 22074102 ; | Approved | Most recent IF: 8.6; 2023 IF: 9.466 | ||
| Call Number | EMAT @ emat @c:irua:198151 | Serial | 8810 | ||
| Permanent link to this record | |||||
| Author | Lobato, I.; De Backer, A.; Van Aert, S. | ||||
| Title | Real-time simulations of ADF STEM probe position-integrated scattering cross-sections for single element fcc crystals in zone axis orientation using a densely connected neural network | Type | A1 Journal article | ||
| Year | 2023 | Publication | Ultramicroscopy | Abbreviated Journal | Ultramicroscopy |
| Volume | 251 | Issue | Pages | 113769 | |
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Quantification of annular dark field (ADF) scanning transmission electron microscopy (STEM) images in terms of composition or thickness often relies on probe-position integrated scattering cross sections (PPISCS). In order to compare experimental PPISCS with theoretically predicted ones, expensive simulations are needed for a given specimen, zone axis orientation, and a variety of microscope settings. The computation time of such simulations can be in the order of hours using a single GPU card. ADF STEM simulations can be efficiently parallelized using multiple GPUs, as the calculation of each pixel is independent of other pixels. However, most research groups do not have the necessary hardware, and, in the best-case scenario, the simulation time will only be reduced proportionally to the number of GPUs used. In this manuscript, we use a learning approach and present a densely connected neural network that is able to perform real-time ADF STEM PPISCS predictions as a function of atomic column thickness for most common face-centered cubic (fcc) crystals (i.e., Al, Cu, Pd, Ag, Pt, Au and Pb) along [100] and [111] zone axis orientations, root-mean-square displacements, and microscope parameters. The proposed architecture is parameter efficient and yields accurate predictions for the PPISCS values for a wide range of input parameters that are commonly used for aberration-corrected transmission electron microscopes. |
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001011617200001 | Publication Date | 2023-06-01 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 0304-3991 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 2.2 | Times cited | Open Access |
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 and G0A7723N) and a postdoctoral grant to A. De Backer. S. Van Aert acknowledges funding from the University of Antwerp Research fund (BOF), Belgium. | Approved | Most recent IF: 2.2; 2023 IF: 2.843 | ||
| Call Number | EMAT @ emat @c:irua:197275 | Serial | 8812 | ||
| Permanent link to this record | |||||
| Author | Denisov, N.; Jannis, D.; Orekhov, A.; Müller-Caspary, K.; Verbeeck, J. | ||||
| Title | Characterization of a Timepix detector for use in SEM acceleration voltage range | Type | A1 Journal article | ||
| Year | 2023 | Publication | Ultramicroscopy | Abbreviated Journal | Ultramicroscopy |
| Volume | 253 | Issue | Pages | 113777 | |
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Hybrid pixel direct electron detectors are gaining popularity in electron microscopy due to their excellent properties. Some commercial cameras based on this technology are relatively affordable which makes them attractive tools for experimentation especially in combination with an SEM setup. To support this, a detector characterization (Modulation Transfer Function, Detective Quantum Efficiency) of an Advacam Minipix and Advacam Advapix detector in the 15–30 keV range was made. In the current work we present images of Point Spread Function, plots of MTF/DQE curves and values of DQE(0) for these detectors. At low beam currents, the silicon detector layer behaviour should be dominant, which could make these findings transferable to any other available detector based on either Medipix2, Timepix or Timepix3 provided the same detector layer is used. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001026912700001 | Publication Date | 2023-06-08 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 0304-3991 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 2.2 | Times cited | Open Access |
OpenAccess | |
| Notes | The authors acknowledge the financial support of the Research Foundation Flanders (FWO, Belgium) project SBO S000121N. The authors are grateful to Dr. Lobato for productive discussion of methods. | Approved | Most recent IF: 2.2; 2023 IF: 2.843 | ||
| Call Number | EMAT @ emat @c:irua:198258 | Serial | 8815 | ||
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| Author | Arenas Esteban, D.; Pacquets, L.; Choukroun, D.; Hoekx, S.; Kadu, A.A.; Schalck, J.; Daems, N.; Breugelmans, T.; Bals, S. | ||||
| Title | 3D characterization of the structural transformation undergone by Cu@Ag core-shell nanoparticles following CO₂ reduction reaction | Type | A1 Journal article | ||
| Year | 2023 | Publication | Chemistry of materials | Abbreviated Journal | |
| Volume | 35 | Issue | 17 | Pages | 6682-6691 |
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) | ||||
| Abstract | The increasing use of metallic nanoparticles (NPs) is significantly advancing the field of electrocatalysis. In particular, Cu/Ag bimetallic interfaces are widely used to enhance the electrochemical CO2 reduction reaction (eCO(2)RR) toward CO and, more recently, C-2 products. However, drastic changes in the product distribution and performance when Cu@Ag core-shell configurations are used can often be observed under electrochemical reaction conditions, especially during the first few minutes of the reaction. Possible structural changes that generate these observations remain underexplored; therefore, the structure-property relationship is hardly understood. In this study, we use electron tomography to investigate the structural transformation mechanism of Cu@Ag core-shells NPs during the critical first minutes of the eCO(2)RR. In this manner, we found that the crystallinity of the Cu seed determines whether the formation of a complete and homogeneous Ag shell is possible. Moreover, by tracking the particles' transformations, we conclude that modifications of the Cu-Ag interface and Cu2O enrichment at the surface of the NPs are key factors contributing to the product generation changes. These insights provide a better understanding of how bimetallic core-shell NPs transform under electrochemical conditions. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001061530700001 | Publication Date | 2023-08-31 | |
| 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 | 1 | Open Access |
OpenAccess |
| Notes | L.P. was supported through a PhD fellowship for strategicbasic research (1S56920N) of the Research Foundation – Flanders(FWO). S.H. was supported through a PhD fellowship for strategic basicresearch (1S42623N) of the Research Foundation – Flanders (FWO).S.B., D.A.E., and A.A.K. acknowledge financial support from ERC Consolidator Grant Number 815128 REALNANO. This research was financed by the researchcouncil of the University of Antwerp (BOF-GOA 33928). | Approved | Most recent IF: 8.6; 2023 IF: 9.466 | ||
| Call Number | UA @ admin @ c:irua:199187 | Serial | 8825 | ||
| Permanent link to this record | |||||
| Author | Sasaki, S.; Giri, S.; Cassidy, S.J.; Dey, S.; Batuk, M.; Vandemeulebroucke, D.; Cibin, G.; Smith, R.I.; Holdship, P.; Grey, C.P.; Hadermann, J.; Clarke, S.J. | ||||
| Title | Anion redox as a means to derive layered manganese oxychalcogenides with exotic intergrowth structures | Type | A1 Journal article | ||
| Year | 2023 | Publication | Nature communications | Abbreviated Journal | |
| Volume | 14 | Issue | 1 | Pages | 2917-11 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Topochemistry enables step-by-step conversions of solid-state materials often leading to metastable structures that retain initial structural motifs. Recent advances in this field revealed many examples where relatively bulky anionic constituents were actively involved in redox reactions during (de)intercalation processes. Such reactions are often accompanied by anion-anion bond formation, which heralds possibilities to design novel structure types disparate from known precursors, in a controlled manner. Here we present the multistep conversion of layered oxychalcogenides Sr(2)MnO(2)Cu(1.5)Ch(2) (Ch=S, Se) into Cu-deintercalated phases where antifluorite type [Cu(1.5)Ch(2)](2.5-) slabs collapsed into two-dimensional arrays of chalcogen dimers. The collapse of the chalcogenide layers on deintercalation led to various stacking types of Sr(2)MnO(2)Ch(2) slabs, which formed polychalcogenide structures unattainable by conventional high-temperature syntheses. Anion-redox topochemistry is demonstrated to be of interest not only for electrochemical applications but also as a means to design complex layered architectures. Low temperature chemical transformations of solids using high-energy intermediates have enabled the synthesis of a new series of layered oxide chalcogenide containing oxidised chalcogenide dimers promising a new range of solids. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001024186000011 | Publication Date | 2023-05-22 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 2041-1723 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 16.6 | Times cited | Open Access |
OpenAccess | |
| Notes | Approved | Most recent IF: 16.6; 2023 IF: 12.124 | |||
| Call Number | UA @ admin @ c:irua:199281 | Serial | 8832 | ||
| Permanent link to this record | |||||
| Author | Liu, J.; Wang, C.; Yu, W.; Zhao, H.; Hu, Z.-Y.; Liu, F.; Hasan, T.; Li, Y.; Van Tendeloo, G.; Li, C.; Su, B.-L. | ||||
| Title | Bioinspired noncyclic transfer pathway electron donors for unprecedented hydrogen production | Type | A1 Journal article | ||
| Year | 2023 | Publication | CCS chemistry | Abbreviated Journal | |
| Volume | 5 | Issue | 6 | Pages | 1470-1482 |
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Electron donors are widely exploited in visible-light photocatalytic hydrogen production. As a typical electron donor pair and often the first choice for hydrogen production, the sodium sulfide-sodium sulfite pair has been extensively used. However, the resultant thiosulfate ions consume the photogenerated electrons to form an undesirable pseudocyclic electron transfer pathway during the photocatalytic process, strongly limiting the solar energy conversion efficiency. Here, we report novel and bioinspired electron donor pairs offering a noncyclic electron transfer pathway that provides more electrons without the consumption of the photogenerated electrons. Compared to the state-of-the-art electron donor pair Na2S-Na2SO3, these novel Na2S-NaH2PO2 and Na2S-NaNO2 electron donor pairs enable an unprecedented enhancement of up to 370% and 140% for average photocatalytic H-2 production over commercial CdS nanoparticles, and they are versatile for a large series of photocatalysts for visible-light water splitting. The discovery of these novel electron donor pairs can lead to a revolution in photocatalysis and is of great significance for industrial visible-light-driven H-2 production. [GRAPHICS] . | ||||
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| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001037091900008 | Publication Date | 2022-06-30 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | ||
| Impact Factor | Times cited | Open Access |
OpenAccess | ||
| Notes | Approved | Most recent IF: NA | |||
| Call Number | UA @ admin @ c:irua:198409 | Serial | 8837 | ||
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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 | 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. | ||||
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| 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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| Author | Wang, Y.; Yuan, Y.; Liao, X.; Van Tendeloo, G.; Zhao, Y.; Sun, C. | ||||
| Title | Chip-based in situ TEM investigation of structural thermal instability in aged layered cathode | Type | A1 Journal article | ||
| Year | 2023 | Publication | Nanoscale Advances | Abbreviated Journal | |
| Volume | 5 | Issue | 16 | Pages | 4182-4190 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Thermally induced oxygen release is an intrinsic structural instability in layered cathodes, which causes thermal runaway issues and becomes increasingly critical with the continuous improvement in energy density. Furthermore, thermal runaway events always occur in electrochemically aged cathodes, where the coupling of the thermal and electrochemical effect remains elusive. Herein, we report the anomalous segregation of cobalt metal in an aged LiCoO2 cathode, which is attributed to the local exposure of the high-energy (100) surface of LiCoO2 and weak interface Co-O dangling bonds significantly promoting the diffusion of Co. The presence of the LCO-Co interface severely aggregated the oxygen release in the form of dramatic Co growth. A unique particle-to-particle oxygen release pathway was also found, starting from the isolated high reduction areas induced by the cycling heterogeneity. This study provides atomistic insight into the robust coupling between the intrinsic structural instability and electrochemical cycling. | ||||
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| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001030149900001 | Publication Date | 2023-07-14 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 2516-0230 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 4.7 | Times cited | Open Access |
OpenAccess | |
| Notes | Approved | Most recent IF: 4.7; 2023 IF: NA | |||
| Call Number | UA @ admin @ c:irua:198281 | Serial | 8841 | ||
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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 | 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. | ||||
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| 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 | Vega-Paredes, M.; Aymerich-Armengol, R.; Arenas Esteban, D.; Marti-Sanchez, S.; Bals, S.; Scheu, C.; Manjon, A.G. | ||||
| Title | Electrochemical stability of rhodium-platinum core-shell nanoparticles : an identical location scanning transmission electron microscopy study | Type | A1 Journal article | ||
| Year | 2023 | Publication | ACS nano | Abbreviated Journal | |
| Volume | 17 | Issue | 17 | Pages | 16943-16951 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Rhodium-platinum core-shell nanoparticleson a carbonsupport (Rh@Pt/C NPs) are promising candidates as anode catalystsfor polymer electrolyte membrane fuel cells. However, their electrochemicalstability needs to be further explored for successful applicationin commercial fuel cells. Here we employ identical location scanningtransmission electron microscopy to track the morphological and compositionalchanges of Rh@Pt/C NPs during potential cycling (10 000 cycles,0.06-0.8 V-RHE, 0.5 H2SO4)down to the atomic level, which are then used for understanding thecurrent evolution occurring during the potential cycles. Our resultsreveal a high stability of the Rh@Pt/C system and point toward particledetachment from the carbon support as the main degradation mechanism. | ||||
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| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001051495900001 | Publication Date | 2023-08-21 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 1936-0851 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 17.1 | Times cited | 2 | Open Access |
OpenAccess |
| Notes | The authors would like to thank C. Bodirsky for providing the samples, N. Rivas Rivas for his corrections on the manuscript, and D. Chatain for providing her expertise on the equilibrium shape of nanoparticles. Special thanks to B. Breitbach for performing the XRD experiments. A.G.M. acknowledges the Grant RYC2021-033479- I funded by MCIN/AEI/10.13039/501100011033 and, as appropriate, by European Union NextGenerationEU/PRTR. | Approved | Most recent IF: 17.1; 2023 IF: 13.942 | ||
| Call Number | UA @ admin @ c:irua:199253 | Serial | 8859 | ||
| Permanent link to this record | |||||