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Author | Nord, M.; Semisalova, A.; Kákay, A.; Hlawacek, G.; MacLaren, I.; Liersch, V.; Volkov, O.M.; Makarov, D.; Paterson, G.W.; Potzger, K.; Lindner, J.; Fassbender, J.; McGrouther, D.; Bali, R. | ||||
Title | Strain Anisotropy and Magnetic Domains in Embedded Nanomagnets | Type | A1 Journal article | ||
Year | 2019 | Publication | Small | Abbreviated Journal | Small |
Volume | Issue | Pages | 1904738 | ||
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | Nanoscale modifications of strain and magnetic anisotropy can open pathways to engineering magnetic domains for device applications. A periodic magnetic domain structure can be stabilized in sub‐200 nm wide linear as well as curved magnets, embedded within a flat non‐ferromagnetic thin film. The nanomagnets are produced within a non‐ferromagnetic B2‐ordered Fe60Al40 thin film, where local irradiation by a focused ion beam causes the formation of disordered and strongly ferromagnetic regions of A2 Fe60Al40. An anisotropic lattice relaxation is observed, such that the in‐plane lattice parameter is larger when measured parallel to the magnet short‐axis as compared to its length. This in‐plane structural anisotropy manifests a magnetic anisotropy contribution, generating an easy‐axis parallel to the short axis. The competing effect of the strain and shape anisotropies stabilizes a periodic domain pattern in linear as well as spiral nanomagnets, providing a versatile and geometrically controllable path to engineering the strain and thereby the magnetic anisotropy at the nanoscale. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000495563400001 | Publication Date | 2019-11-11 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1613-6810 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.643 | Times cited | 2 | Open Access | |
Notes | Deutsche Forschungsgemeinschaft, BA5656/1‐1 ; Engineering and Physical Sciences Research Council, EP/M009963/1 ; | Approved | Most recent IF: 8.643 | ||
Call Number | EMAT @ emat @c:irua:164059 | Serial | 5376 | ||
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Author | Mychinko, M.; Skorikov, A.; Albrecht, W.; Sánchez‐Iglesias, A.; Zhuo, X.; Kumar, V.; Liz‐Marzán, L.M.; Bals, S. | ||||
Title | The Influence of Size, Shape, and Twin Boundaries on Heat‐Induced Alloying in Individual Au@Ag Core–Shell Nanoparticles | Type | A1 Journal article | ||
Year | 2021 | Publication | Small | Abbreviated Journal | Small |
Volume | Issue | Pages | 2102348 | ||
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | Environmental conditions during real-world application of bimetallic core–shell nanoparticles (NPs) often include the use of elevated temperatures, which are known to cause elemental redistribution, in turn significantly altering the properties of these nanomaterials. Therefore, a thorough understanding of such processes is of great importance. The recently developed combination of fast electron tomography with in situ heating holders is a powerful approach to investigate heat-induced processes at the single NP level, with high spatial resolution in 3D. In combination with 3D finite-difference diffusion simulations, this method can be used to disclose the influence of various NP parameters on the diffusion dynamics in Au@Ag core–shell systems. A detailed study of the influence of heating on atomic diffusion and alloying for Au@Ag NPs with varying core morphology and crystallographic details is carried out. Whereas the core shape and aspect ratio of the NPs play a minor role, twin boundaries are found to have a strong influence on the elemental diffusion. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000673326600001 | Publication Date | 2021-07-14 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1613-6810 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.643 | Times cited | 8 | Open Access | OpenAccess |
Notes | The funding for this project was provided by European Research Council (ERC Consolidator Grant 815128, REALNANO) and European Commission (grant 731019, EUSMI and grant 26019, ESTEEM). This work was performed under the Maria de Maeztu Units of Excellence Programme-Grant No. MDM-2017-0720, Ministry of Science and Innovation.; sygmaSB | Approved | Most recent IF: 8.643 | ||
Call Number | EMAT @ emat @c:irua:179856 | Serial | 6804 | ||
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Author | Vlasov, I.I.; Shenderova, O.; Turner, S.; Lebedev, O.I.; Basov, A.A.; Sildos, I.; Rähn, M.; Shiryaev, A.A.; Van Tendeloo, G. | ||||
Title | Nitrogen and luminescent nitrogen-vacancy defects in detonation nanodiamond | Type | A1 Journal article | ||
Year | 2010 | Publication | Small | Abbreviated Journal | Small |
Volume | 6 | Issue | 5 | Pages | 687-694 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | An efficient method to investigate the microstructure and spatial distribution of nitrogen and nitrogen-vacancy (N-V) defects in detonation nanodiamond (DND) with primary particle sizes ranging from approximately 3 to 50 nm is presented. Detailed analysis reveals atomic nitrogen concentrations as high as 3 at% in 50% of diamond primary particles with sizes smaller than 6 nm. A non-uniform distribution of nitrogen within larger primary DND particles is also presented, indicating a preference for location within the defective central part or at twin boundaries. A photoluminescence (PL) spectrum with well-pronounced zero-phonon lines related to the N-V centers is demonstrated for the first time for electron-irradiated and annealed DND particles at continuous laser excitation. Combined Raman and PL analysis of DND crystallites dispersed on a Si substrate leads to the conclusion that the observed N-V luminescence originates from primary particles with sizes exceeding 30 nm. These findings demonstrate that by manipulation of the size/nitrogen content in DND there are prospects for mass production of nanodiamond photoemitters based on bright and stable luminescence from nitrogen-related defects. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Weinheim | Editor | ||
Language | Wos | 000275972400013 | Publication Date | 2010-01-27 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1613-6810;1613-6829; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.643 | Times cited | 84 | Open Access | |
Notes | Esteem 026019 | Approved | Most recent IF: 8.643; 2010 IF: 7.336 | ||
Call Number | UA @ lucian @ c:irua:82364 | Serial | 2341 | ||
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Author | Grodzińska, D.; Evers, W.H.; Dorland, R.; van Rijssel, J.; van Huis, M.A.; Meijerink, A.; de Mello Donegá, C.; Vanmaekelbergh, D. | ||||
Title | Two-fold emission from the S-shell of PbSe/CdSe core/shell quantum dots | Type | A1 Journal article | ||
Year | 2011 | Publication | Small | Abbreviated Journal | Small |
Volume | 7 | Issue | 24 | Pages | 3493-3501 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | The optical properties of PbSe/CdSe core/shell quantum dots with core sizes smaller than 4 nm in the 5300 K range are reported. The photoluminescence spectra show two peaks, which become increasingly separated in energy as the core diameter is reduced below 4 nm. It is shown that these peaks are due to intrinsic exciton transitions in each quantum dot, rather than emission from different quantum dot sub-ensembles. Most likely, the energy separation between the peaks is due to inter-valley coupling between the L-points of PbSe. The temperature dependence of the relative intensities of the peaks implies that the two emitting states are not in thermal equilibrium and that dark exciton states must play an important role. | ||||
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Publisher | Place of Publication | Weinheim | Editor | ||
Language | Wos | 000298298300012 | Publication Date | 2011-10-21 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1613-6810; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.643 | Times cited | 23 | Open Access | |
Notes | Approved | Most recent IF: 8.643; 2011 IF: 8.349 | |||
Call Number | UA @ lucian @ c:irua:94371 | Serial | 3781 | ||
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Author | Gengler, R.Y.N.; Toma, L.M.; Pardo, E.; Lloret, F.; Ke, X.; Van Tendeloo, G.; Gournis, D.; Rudolf, P. | ||||
Title | Prussian blue analogues of reduced dimensionality | Type | A1 Journal article | ||
Year | 2012 | Publication | Small | Abbreviated Journal | Small |
Volume | 8 | Issue | 16 | Pages | 2532-2540 |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | Mixed-valence polycyanides (Prussian Blue analogues) possess a rich palette of properties spanning from room-temperature ferromagnetism to zero thermal expansion, which can be tuned by chemical modifications or the application of external stimuli (temperature, pressure, light irradiation). While molecule-based materials can combine physical and chemical properties associated with molecular-scale building blocks, their successful integration into real devices depends primarily on higher-order properties such as crystal size, shape, morphology, and organization. Herein a study of a new reduced-dimensionality system based on Prussian Blue analogues (PBAs) is presented. The system is built up by means of a modified Langmuir-Blodgett technique, where the PBA is synthesized from precursors in a self-limited reaction on a clay mineral surface. The focus of this work is understanding the magnetic properties of the PBAs in different periodic, low-dimensional arrangements, and the influence of the “on surface” synthesis on the final properties and dimensionality of the system. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Weinheim | Editor | ||
Language | Wos | 000307390300012 | Publication Date | 2012-07-03 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1613-6810; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.643 | Times cited | 17 | Open Access | |
Notes | Approved | Most recent IF: 8.643; 2012 IF: 7.823 | |||
Call Number | UA @ lucian @ c:irua:101104 | Serial | 2736 | ||
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Author | Goris, B.; van Huis, M.A.; Bals, S.; Zandbergen, H.W.; Manna, L.; Van Tendeloo, G. | ||||
Title | Thermally induced structural and morphological changes of CdSe/CdS octapods | Type | A1 Journal article | ||
Year | 2012 | Publication | Small | Abbreviated Journal | Small |
Volume | 8 | Issue | 6 | Pages | 937-942 |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | Branched nanostructures are of great interest because of their promising optical and electronic properties. For successful and reliable integration in applications such as photovoltaic devices, the thermal stability of the nanostructures is of major importance. Here the different domains (CdSe cores, CdS pods) of the heterogeneous octapods are shown to have different thermal stabilities, and heating is shown to induce specific shape changes. The octapods are heated from room temperature to 700 °C, and investigated using (analytical and tomographic) transmission electron microscopy (TEM). At low annealing temperatures, pure Cd segregates in droplets at the outside of the octapods, indicating non-stochiometric composition of the octapods. Furthermore, the tips of the pods lose their faceting and become rounded. Further heating to temperatures just below the sublimation temperature induces growth of the zinc blende core at the expense of the wurtzite pods. At higher temperatures, (500700 °C), sublimation of the octapods is observed in real time in the TEM. Three-dimensional tomographic reconstructions reveal that the four pods pointing into the vacuum have a lower thermal stability than the four pods that are in contact with the support. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Weinheim | Editor | ||
Language | Wos | 000301718800021 | Publication Date | 2012-01-31 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1613-6810; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.643 | Times cited | 20 | Open Access | |
Notes | Fwo; Esteem 026019 | Approved | Most recent IF: 8.643; 2012 IF: 7.823 | ||
Call Number | UA @ lucian @ c:irua:95040 | Serial | 3633 | ||
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Author | Ke, X.; Turner, S.; Quintana, M.; Hadad, C.; Montellano-López, A.; Carraro, M.; Sartorel, A.; Bonchio, M.; Prato, M.; Bittencourt, C.; Van Tendeloo, G.; | ||||
Title | Dynamic motion of Ru-polyoxometalate ions (POMs) on functionalized few-layer graphene | Type | A1 Journal article | ||
Year | 2013 | Publication | Small | Abbreviated Journal | Small |
Volume | 9 | Issue | 23 | Pages | 3922-3927 |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | The interaction and stability of Ru4POM on few layer graphene via functional groups is investigated by time-dependent imaging using aberration-corrected transmission electron microscopy. The Ru4POM demonstrates dynamic motion on the graphene surface with its frequency and amplitude of rotation related to the nature of the functional group used. The stability of the Ru4POMgraphene hybrid corroborates its long-term robustness when applied to multielectronic catalytic processes. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Weinheim | Editor | ||
Language | Wos | 000331282400003 | Publication Date | 2013-07-01 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1613-6810; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.643 | Times cited | 16 | Open Access | |
Notes | IAP-7; Countatoms; | Approved | Most recent IF: 8.643; 2013 IF: 7.514 | ||
Call Number | UA @ lucian @ c:irua:115768 | Serial | 763 | ||
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Author | Rehor, I.; Slegerova, J.; Kucka, J.; Proks, V.; Petrakova, V.; Adam, M.P.; Treussart, F.; Turner, S.; Bals, S.; Sacha, P.; Ledvina, M.; Wen, A.M.; Steinmetz, N.F.; Cigler, P.; | ||||
Title | Fluorescent nanodiamonds embedded in biocompatible translucent shells | Type | A1 Journal article | ||
Year | 2014 | Publication | Small | Abbreviated Journal | Small |
Volume | 10 | Issue | 6 | Pages | 1106-1115 |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | High pressure high temperature (HPHT) nanodiamonds (NDs) represent extremely promising materials for construction of fluorescent nanoprobes and nanosensors. However, some properties of bare NDs limit their direct use in these applications: they precipitate in biological solutions, only a limited set of bio-orthogonal conjugation techniques is available and the accessible material is greatly polydisperse in shape. In this work, we encapsulate bright 30-nm fluorescent nanodiamonds (FNDs) in 1020-nm thick translucent (i.e., not altering FND fluorescence) silica shells, yielding monodisperse near-spherical particles of mean diameter 66 nm. High yield modification of the shells with PEG chains stabilizes the particles in ionic solutions, making them applicable in biological environments. We further modify the opposite ends of PEG chains with fluorescent dyes or vectoring peptide using click chemistry. High conversion of this bio-orthogonal coupling yielded circa 2000 dye or peptide molecules on a single FND. We demonstrate the superior properties of these particles by in vitro interaction with human prostate cancer cells: while bare nanodiamonds strongly aggregate in the buffer and adsorb onto the cell membrane, the shell encapsulated NDs do not adsorb nonspecifically and they penetrate inside the cells. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Weinheim | Editor | ||
Language | Wos | 000333538000012 | Publication Date | 2014-02-05 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1613-6810; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.643 | Times cited | 79 | Open Access | Not_Open_Access |
Notes | 262348 ESMI; Hercules; FWO | Approved | Most recent IF: 8.643; 2014 IF: 8.368 | ||
Call Number | UA @ lucian @ c:irua:115566 | Serial | 1234 | ||
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Author | Wang, Y.; Belén Serrano, A.; Sentosun, K.; Bals, S.; Liz-Marzán, L.M. | ||||
Title | Stabilization and encapsulation of gold nanostars mediated by dithiols | Type | A1 Journal article | ||
Year | 2015 | Publication | Small | Abbreviated Journal | Small |
Volume | 11 | Issue | 11 | Pages | 4314-4320 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Surface chemistry plays a pivotal role in regulating the morphology of nanoparticles, maintaining colloidal stability, and mediating the interaction with target analytes toward practical applications such as surface-enhanced Raman scattering (SERS)-based sensing and imaging. The use of a binary ligand mixture composed of 1,4-benzenedithiol (BDT) and hexadecyltrimethylammonium chloride (CTAC) to provide gold nanostars with long-term stability is reported. This is despite BDT being a bifunctional ligand, which usually leads to bridging and loss of colloidal stability. It is found however that neither BDT nor CTAC alone are able to provide sufficient colloidal and chemical stability. BDT-coated Au nanostars are additionally used as seeds to direct the encapsulation with a gold outer shell, leading to the formation of unusual nanostructures including semishell-coated gold nanostars, which are characterized by high-resolution electron microscopy and electron tomography. Finally, BDT is exploited as a probe to reveal the enhanced local electric fields in the different nanostructures, showing that the semishell configuration provides significantly high SERS signals as compared to other coreshell configurations obtained during seeded growth, including full shells. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Weinheim | Editor | ||
Language | Wos | 000360852900009 | Publication Date | 2015-06-02 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1613-6810; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.643 | Times cited | 36 | Open Access | OpenAccess |
Notes | 267867 Plasmaquo; 335078 Colouratom; 262348 Esmi; ECAS_Sara; (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:cannot); | Approved | Most recent IF: 8.643; 2015 IF: 8.368 | ||
Call Number | c:irua:127571 | Serial | 3136 | ||
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Author | Bal, K.M.; Neyts, E.C. | ||||
Title | Direct observation of realistic-temperature fuel combustion mechanisms in atomistic simulations | Type | A1 Journal article | ||
Year | 2016 | Publication | Chemical science | Abbreviated Journal | Chem Sci |
Volume | 7 | Issue | 7 | Pages | 5280-5286 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Atomistic simulations can in principle provide an unbiased description of all mechanisms, intermediates, and products of complex chemical processes. However, due to the severe time scale limitation of conventional simulation techniques, unrealistically high simulation temperatures are usually applied, which are a poor approximation of most practically relevant low-temperature applications. In this work, we demonstrate the direct observation at the atomic scale of the pyrolysis and oxidation of n-dodecane at temperatures as low as 700 K through the use of a novel simulation technique, collective variable-driven hyperdynamics (CVHD). A simulated timescale of up to 39 seconds is reached. Product compositions and dominant mechanisms are found to be strongly temperature-dependent, and are consistent with experiments and kinetic models. These simulations provide a first atomic-level look at the full dynamics of the complicated fuel combustion process at industrially relevant temperatures and time scales, unattainable by conventional molecular dynamics simulations. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000380893900059 | Publication Date | 2016-05-05 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2041-6520 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.668 | Times cited | 22 | Open Access | |
Notes | K. M. B. is funded as PhD fellow (aspirant) of the FWO-Flanders (Fund for Scientic Research-Flanders), Grant 11V8915N. The computational resources and services used in this work were provided by the VSC (Flemish Supercomputer Center) and the HPC infrastructure of the University of Antwerp (CalcUA), funded by the Hercules Foundation and the Flemish Government – department EWI. The authors would also like to thank S. Banerjee for assisting with the interpretation of the experimental results. | Approved | Most recent IF: 8.668 | ||
Call Number | c:irua:134577 c:irua:135670 | Serial | 4105 | ||
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Author | Aussems, D.U.B.; Bal, K. M.; Morgan, T.W.; van de Sanden, M.C.M.; Neyts, E.C. | ||||
Title | Atomistic simulations of graphite etching at realistic time scales | Type | A1 Journal article | ||
Year | 2017 | Publication | Chemical science | Abbreviated Journal | Chem Sci |
Volume | 8 | Issue | 10 | Pages | 7160-7168 |
Keywords | A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Hydrogen–graphite interactions are relevant to a wide variety of applications, ranging from astrophysics to fusion devices and nano-electronics. In order to shed light on these interactions, atomistic simulation using Molecular Dynamics (MD) has been shown to be an invaluable tool. It suffers, however, from severe timescale limitations. In this work we apply the recently developed Collective Variable-Driven Hyperdynamics (CVHD) method to hydrogen etching of graphite for varying inter-impact times up to a realistic value of 1 ms, which corresponds to a flux of 1020 m2 s1. The results show that the erosion yield, hydrogen surface coverage and species distribution are significantly affected by the time between impacts. This can be explained by the higher probability of C–C bond breaking due to the prolonged exposure to thermal stress and the subsequent transition from ion- to thermal-induced etching. This latter regime of thermal-induced etching – chemical erosion – is here accessed for the first time using atomistic simulations. In conclusion, this study demonstrates that accounting for long time-scales significantly affects ion bombardment simulations and should not be neglected in a wide range of conditions, in contrast to what is typically assumed. |
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000411730500055 | Publication Date | 2017-08-24 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2041-6520 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.668 | Times cited | 3 | Open Access | OpenAccess |
Notes | DIFFER is part of the Netherlands Organisation for Scientic Research (NWO). K. M. B. is funded as a PhD fellow (aspirant) of the FWO-Flanders (Fund for Scientic Research-Flanders), Grant 11V8915N. 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. | Approved | Most recent IF: 8.668 | ||
Call Number | PLASMANT @ plasmant @c:irua:145519 | Serial | 4707 | ||
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Author | Bueken, B.; Van Velthoven, N.; Willhammar, T.; Stassin, T.; Stassen, I.; Keen, D.A.; Baron, G.V.; Denayer, J.F.M.; Ameloot, R.; Bals, S.; De Vos, D.; Bennett, T.D. | ||||
Title | Gel-based morphological design of zirconium metal-organic frameworks | Type | A1 Journal article | ||
Year | 2017 | Publication | Chemical science | Abbreviated Journal | Chem Sci |
Volume | 8 | Issue | 8 | Pages | 3939-3948 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | The ability of metal-organic frameworks (MOFs) to gelate under specific synthetic conditions opens up new opportunities in the preparation and shaping of hierarchically porous MOF monoliths, which could be directly implemented for catalytic and adsorptive applications. In this work, we present the first examples of xero-or aerogel monoliths consisting solely of nanoparticles of several prototypical Zr4+-based MOFs: UiO-66-X (X – H, NH2, NO2, (OH)(2)), UiO-67, MOF-801, MOF-808 and NU-1000. High reactant and water concentrations during synthesis were observed to induce the formation of gels, which were converted to monolithic materials by drying in air or supercritical CO2. Electron microscopy, combined with N-2 physisorption experiments, was used to show that irregular nanoparticle packing leads to pure MOF monoliths with hierarchical pore systems, featuring both intraparticle micropores and interparticle mesopores. Finally, UiO-66 gels were shaped into monolithic spheres of 600 mm diameter using an oil-drop method, creating promising candidates for packed-bed catalytic or adsorptive applications, where hierarchical pore systems can greatly mitigate mass transfer limitations. | ||||
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Publisher | Royal Society of Chemistry | Place of Publication | Cambridge | Editor | |
Language | Wos | 000400553000077 | Publication Date | 2017-03-23 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2041-6520 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.668 | Times cited | 168 | Open Access | OpenAccess |
Notes | ; B. B., T. S. and I. S. acknowledge the FWO Flanders (doctoral and post-doctoral grants). T. W. acknowledges a post-doctoral grant from the Swedish Research Council. T. D. B. acknowledges the Royal Society (University Research Fellowship) and Trinity Hall (University of Cambridge) for funding. S. B. and D. D. V. are grateful for funding by Belspo (IAP 7/05 P6/27) and by the FWO Flanders. D. D. V. further acknowledges funding from the European Research Council (project H-CCAT). S. B. acknowledges financial support from the European Research Council (ERC Starting Grant #335078-COLOURATOMS). The authors acknowledge Arnau Carne and Shuhei Furukawa for assistance with supercritical CO<INF>2</INF> extraction, and Charles Ghesquiere for assistance in synthesis. ; Ecas_Sara | Approved | Most recent IF: 8.668 | ||
Call Number | UA @ lucian @ c:irua:152643UA @ admin @ c:irua:152643 | Serial | 5143 | ||
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Author | Van Velthoven, N.; Waitschat, S.; Chavan, S.M.; Liu, P.; Smolders, S.; Vercammen, J.; Bueken, B.; Bals, S.; Lillerud, K.P.; Stock, N.; De Vos, D.E. | ||||
Title | Single-site metal-organic framework catalysts for the oxidative coupling of arenes via C-H/C-H activation | Type | A1 Journal article | ||
Year | 2019 | Publication | Chemical science | Abbreviated Journal | Chem Sci |
Volume | 10 | Issue | 10 | Pages | 3616-3622 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | C-H activation reactions are generally associated with relatively low turnover numbers (TONs) and high catalyst concentrations due to a combination of low catalyst stability and activity, highlighting the need for recyclable heterogeneous catalysts with stable single-atom active sites. In this work, several palladium loaded metal-organic frameworks (MOFs) were tested as single-site catalysts for the oxidative coupling of arenes (e.g. o-xylene) via C-H/C-H activation. Isolation of the palladium active sites on the MOF supports reduced Pd(0) aggregate formation and thus catalyst deactivation, resulting in higher turnover numbers (TONs) compared to the homogeneous benchmark reaction. Notably, a threefold higher TON could be achieved for palladium loaded MOF-808 due to increased catalyst stability and the heterogeneous catalyst could efficiently be reused, resulting in a cumulative TON of 1218 after three runs. Additionally, the palladium single-atom active sites on MOF-808 were successfully identified by Fourier transform infrared (FTIR) and extended X-ray absorption fine structure (EXAFS) spectroscopy. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000463759100017 | Publication Date | 2019-02-18 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2041-6520 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.668 | Times cited | 68 | Open Access | OpenAccess |
Notes | ; The research leading to these results has received funding from the NMBP-01-2016 Program of the European Union's Horizon 2020 Framework Program H2020/2014-2020/under grant agreement no. [720996]. N. V. V., S. S., J. V., B. B. and D. E. D. V. thank the FWO for funding (SB, Aspirant and postdoctoral grants). The electron microscopy work was supported by FWO funding G038116. D. E. D. V. is grateful for KU Leuven support in the frame of the CASAS Metusalem project and a C3 type project. The XAS experiments were performed on beamline BM26A at the European Synchrotron Radiation Facility (ESRF), Grenoble, France. We are grateful to D. Banerjee at the ESRF for providing assistance in using beamline BM26A. Johnson Matthey and S. Bennett are gratefully acknowledged for providing Smopex-102. ; | Approved | Most recent IF: 8.668 | ||
Call Number | UA @ admin @ c:irua:159403 | Serial | 5259 | ||
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Author | De Jong, M.; Sleegers, N.; Kim, J.; Van Durme, F.; Samyn, N.; Wang, J.; De Wael, K. | ||||
Title | Electrochemical fingerprint of street samples for fast on-site screening of cocaine in seized drug powders | Type | A1 Journal article | ||
Year | 2016 | Publication | Chemical science | Abbreviated Journal | Chem Sci |
Volume | Issue | Pages | 1-7 | ||
Keywords | A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) | ||||
Abstract | We report on a wearable fingertip sensor for on-the-spot identification of cocaine and its cutting agents in street samples. Traditionally, on-site screening is performed by means of colour tests which are difficult to interpret and lack selectivity. By presenting the distinct voltammetric response of cocaine, cutting agents, binary mixtures of cocaine and street samples in solution and powder street samples, we were able to elucidate the electrochemical fingerprint of all these compounds. The new electrochemical concept holds considerable promise as an on-site screening method. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000371021900094 | Publication Date | 2016-01-06 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2041-6520 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.668 | Times cited | 37 | Open Access | |
Notes | ; The authors acknowledge BELSPO for funding the APTADRU project (BR/314/PI/ APTADRU). ; | Approved | Most recent IF: 8.668 | ||
Call Number | UA @ admin @ c:irua:130404 | Serial | 5591 | ||
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Author | Yang, T.; Abakumov, A.M.; Hadermann, J.; Van Tendeloo, G.; Nowik, I.; Stephens, P.W.; Hamberger, J.; Tsirlin, A.A.; Ramanujachary, K.V.; Lofland, S.; Croft, M.; Ignatov, A.; Sun, J.; Greenblatt, M. | ||||
Title | _BiMnFe2O6, a polysynthetically twinned hcp MO structure | Type | A1 Journal article | ||
Year | 2010 | Publication | Chemical science | Abbreviated Journal | Chem Sci |
Volume | 1 | Issue | 6 | Pages | 751-762 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | The most efficient use of spatial volume and the lowest potential energies in the metal oxide structures are based on cubic close packing (ccp) or hexagonal close packing (hcp) of anions with cations occupying the interstices. A promising way to tune the composition of close packed oxides and design new compounds is related to fragmenting the parent structure into modules by periodically spaced planar interfaces, such as twin planes at the unit cell scale. The unique crystal chemistry properties of cations with a lone electron pair, such as Bi3+ or Pb2+, when located at interfaces, enables them to act as chemical scissors, to help relieve configurational strain. With this approach, we synthesized a new oxide, BiMnFe2O6, where fragments of the hypothetical hcp oxygen-based MO structure (the NiAs structure type), for the first time, serve as the building modules in a complex transition metal oxide. Mn3+ and Fe3+ ions are randomly distributed in two crystallographically independent sites (M1 and M2). The structure consists of quasi two-dimensional blocks of the 2H hexagonal close packed MO structure cut along the (114) crystal plane of the hcp lattice and stacked along the c axis. The blocks are related by a mirror operation that allows BiMnFe2O6 to be considered as a polysynthetically twinned 2H hcp MO structure. The transition to an AFM state with an incommensurate spin configuration at [similar] 212 K is established by 57Fe Mössbauer spectroscopy, magnetic susceptibility, specific heat and low temperature powder neutron diffraction. | ||||
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Publisher | Royal Society of Chemistry | Place of Publication | Cambridge | Editor | |
Language | Wos | 000283939200013 | Publication Date | 2010-10-12 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2041-6520;2041-6539; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.668 | Times cited | 12 | Open Access | |
Notes | Approved | Most recent IF: 8.668; 2010 IF: NA | |||
Call Number | UA @ lucian @ c:irua:85823 | Serial | 3517 | ||
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Author | Yan, L.; Niu, H.J.; Duong, G.V.; Suchomel, M.R.; Bacsa, J.; Chalker, P.R.; Hadermann, J.; Van Tendeloo, G.; Rosseinsky, M.J. | ||||
Title | Cation ordering within the perovskite block of a six-layer Ruddlesden-Popper oxide from layer-by-layer growth artificial interfaces in complex unit cells | Type | A1 Journal article | ||
Year | 2011 | Publication | Chemical science | Abbreviated Journal | Chem Sci |
Volume | 2 | Issue | 2 | Pages | 261-272 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | The (AO)(ABO3)n Ruddlesden-Popper structure is an archetypal complex oxide consisting of two distinct structural units, an (AO) rock salt layer separating an n-octahedra thick perovskite block. Conventional high-temperature oxide synthesis methods cannot access members with n > 3, but low-temperature layer-by-layer thin film methods allow the preparation of materials with thicker perovskite blocks, exploiting high surface mobility and lattice matching with the substrate. This paper describes the growth of an n = 6 member CaO[(CSMO)2(LCMO)2 (CSMO)2] in which the six unit cell perovskite block is sub-divided into two central La0.67Ca0.33MnO3 (LCMO) and two terminal Ca0.85Sm0.15MnO3 (CSMO) layers to allow stabilization of the rock salt layer and variation of the transition metal charge. | ||||
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Publisher | Royal Society of Chemistry | Place of Publication | Cambridge | Editor | |
Language | Wos | 000286327600010 | Publication Date | 2010-11-06 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2041-6520;2041-6539; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.668 | Times cited | 16 | Open Access | |
Notes | Approved | Most recent IF: 8.668; 2011 IF: 7.525 | |||
Call Number | UA @ lucian @ c:irua:88652 | Serial | 300 | ||
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Author | Alaria, J.; Borisov, P.; Dyer, M.S.; Manning, T.D.; Lepadatu, S.; Cain, M.G.; Mishina, E.D.; Sherstyuk, N.E.; Ilyin, N.A.; Hadermann, J.; Lederman, D.; Claridge, J.B.; Rosseinsky, M.J.; | ||||
Title | Engineered spatial inversion symmetry breaking in an oxide heterostructure built from isosymmetric room-temperature magnetically ordered components | Type | A1 Journal article | ||
Year | 2014 | Publication | Chemical science | Abbreviated Journal | Chem Sci |
Volume | 5 | Issue | 4 | Pages | 1599-1610 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
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Publisher | Royal Society of Chemistry | Place of Publication | Cambridge | Editor | |
Language | Wos | 000332467400044 | Publication Date | 2014-01-20 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2041-6520;2041-6539; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.668 | Times cited | 24 | Open Access | |
Notes | Approved | Most recent IF: 8.668; 2014 IF: 9.211 | |||
Call Number | UA @ lucian @ c:irua:117064 | Serial | 1045 | ||
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Author | Lieberman, C.M.; Filatov, A.S.; Wei, Z.; Rogachev, A.Y.; Abakumov, A.M.; Dikarev, E.V. | ||||
Title | Mixed-valent, heteroleptic homometallic diketonates as templates for the design of volatile heterometallic precursors | Type | A1 Journal article | ||
Year | 2015 | Publication | Chemical science | Abbreviated Journal | Chem Sci |
Volume | 6 | Issue | 6 | Pages | 2835-2842 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | A novel series of mixed-valent, heteroleptic transition metal diketonates that can be utilized as prospective single-source precursors for the low-temperature preparation of oxide materials are reported. The first mixed-valent iron beta-diketonates with different Fe-III/Fe-II ratios have been synthesized by applying the mixed-ligand approach. Based on nearly quantitative reaction yields and analysis of iron-oxygen bonds, these compounds were formulated as [Fe-III(acac)(3)][Fe-II(hfac)(2)] (1) and [Fe-II(hfac)(2)][Fe-III(acac)(3)][Fe-II(hfac)(2)] (2). In the above heteroleptic complexes, the Lewis acidic, coordinatively unsaturated Fe-II centers chelated by two hfac (hexafluoroacetylacetonate) ligands with electron-withdrawing substituents maintain bridging interactions with oxygen atoms of electron-donating acac (acetylacetonate) groups that chelate the neighboring Fe-III atoms. Switching the ligands on Fe-III and Fe-II atoms in starting reagents resulted in the instant ligand exchange between iron centers and in yet another polynuclear homometallic diketonate [Fe-II(hfac)(2)][Fe-III(acac)(2)(hfac)][Fe-II(hfac)(2)] (3) that adheres to the same bonding pattern as in complexes 1 and 2. The proposed synthetic methodology has been extended to design heterometallic diketonates with different M : M' ratios. Homometallic parent molecules have been used as templates to obtain heterometallic mixed-valent [Fe-III(acac)(3)][Mn-II(hfac)(2)] (4) and [Ni-II(hfac)(2)] – [Fe-III(acac)(3)][Ni-II(hfac)(2)] (5) complexes. The combination of two different diketonate ligands with electron-donating and electron-withdrawing substituents was found to be crucial for maintaining the above mixed-valent heterometallic assemblies. Theoretical investigation of two possible “isomers”, [Fe-III(acac)(3)][Mn-II(hfac)(2)] (4) and [Mn-III(acac)(3)][Fe-II(hfac)(2)] (40) provided an additional support for the metal site assignment giving a preference of 9.78 kcal mol(-1) for the molecule 4. Heterometallic complexes obtained in the course of this study have been found to act as effective single-source precursors for the synthesis of mixed-transition metal oxide materials MxM2-xO3 and MxMi-xO. The title highly volatile precursors can be used for the low-temperature preparation of both amorphous and crystalline heterometallic oxides in the form of thin films or nanosized particles that are known to operate as efficient catalysts in oxygen evolution reaction. | ||||
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Publisher | Royal Society of Chemistry | Place of Publication | Cambridge | Editor | |
Language | Wos | 000353223100021 | Publication Date | 2015-02-25 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2041-6520;2041-6539; | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.668 | Times cited | 13 | Open Access | |
Notes | Approved | Most recent IF: 8.668; 2015 IF: 9.211 | |||
Call Number | c:irua:126031 | Serial | 2092 | ||
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Author | Li, C.; Sanli, E.S.; Barragan-Yani, D.; Stange, H.; Heinemann, M.-D.; Greiner, D.; Sigle, W.; Mainz, R.; Albe, K.; Abou-Ras, D.; van Aken, P. A. | ||||
Title | Secondary-Phase-Assisted Grain Boundary Migration in CuInSe2 | Type | A1 Journal article | ||
Year | 2020 | Publication | Physical Review Letters | Abbreviated Journal | Phys Rev Lett |
Volume | 124 | Issue | 9 | Pages | 095702 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Significant structural evolution occurs during the deposition of CuInSe2 solar materials when the Cu content increases. We use in situ heating in a scanning transmission electron microscope to directly observe how grain boundaries migrate during heating, causing nondefected grains to consume highly defected grains. Cu substitutes for In in the near grain boundary regions, turning them into a Cu-Se phase topotactic with the CuInSe2 grain interiors. Together with density functional theory and molecular dynamics calculations, we reveal how this Cu-Se phase makes the grain boundaries highly mobile. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000518464200009 | Publication Date | 2020-03-05 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0031-9007 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.6 | Times cited | Open Access | OpenAccess | |
Notes | Horizon 2020 Framework Programme, 823717—ESTEEM3 ; Max-Planck-Gesellschaft; Helmholtz Virtual Institute; | Approved | Most recent IF: 8.6; 2020 IF: 8.462 | ||
Call Number | UA @ lucian @c:irua:167699 | Serial | 6393 | ||
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Author | Imran, M.; Ramade, J.; Di Stasio, F.; De Franco, M.; Buha, J.; Van Aert, S.; Goldoni, L.; Lauciello, S.; Prato, M.; Infante, I.; Bals, S.; Manna, L. | ||||
Title | Alloy CsCdxPb1–xBr3Perovskite Nanocrystals: The Role of Surface Passivation in Preserving Composition and Blue Emission | Type | A1 Journal article | ||
Year | 2020 | Publication | Chemistry Of Materials | Abbreviated Journal | Chem Mater |
Volume | 32 | Issue | Pages | acs.chemmater.0c03825 | |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Various strategies have been proposed to engineer the band gap of metal halide perovskite nanocrystals (NCs) while preserving their structure and composition and thus ensuring spectral stability of the emission color. An aspect that has only been marginally investigated is how the type of surface passivation influences the structural/color stability of AMX3 perovskite NCs composed of two different M2+ cations. Here, we report the synthesis of blue-emitting Cs-oleate capped CsCdxPb1–xBr3 NCs, which exhibit a cubic perovskite phase containing Cd-rich domains of Ruddlesden–Popper phases (RP phases). The RP domains spontaneously transform into pure orthorhombic perovskite ones upon NC aging, and the emission color of the NCs shifts from blue to green over days. On the other hand, postsynthesis ligand exchange with various Cs-carboxylate or ammonium bromide salts, right after NC synthesis, provides monocrystalline NCs with cubic phase, highlighting the metastability of RP domains. When NCs are treated with Cs-carboxylates (including Cs-oleate), most of the Cd2+ ions are expelled from NCs upon aging, and the NCs phase evolves from cubic to orthorhombic and their emission color changes from blue to green. Instead, when NCs are coated with ammonium bromides, the loss of Cd2+ ions is suppressed and the NCs tend to retain their blue emission (both in colloidal dispersions and in electroluminescent devices), as well as their cubic phase, over time. The improved compositional and structural stability in the latter cases is ascribed to the saturation of surface vacancies, which may act as channels for the expulsion of Cd2+ ions from NCs. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000603288800034 | Publication Date | 2020-12-04 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0897-4756 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.6 | Times cited | 44 | Open Access | OpenAccess |
Notes | European Commission; Fonds Wetenschappelijk Onderzoek, G.0267.18N ; H2020 European Research Council, 770887 815128 851794 ; We acknowledge funding from the FLAG-ERA JTC2019 project PeroGas. S.B., and S.V.A. acknowledges funding from the European Research Council under the European Union’s Horizon 2020 research and innovation program (ERC Consolidator Grants #815128REALNANO and #770887PICOMETRICS) and from the Research Foundation Flanders (FWO, Belgium) through project funding G.0267.18N. F.D.S. acknowledges the funding from ERC starting grant NANOLED (851794). The computational work was carried out on the Dutch National e-infrastructure with the support of the SURF Cooperative; sygma | Approved | Most recent IF: 8.6; 2020 IF: 9.466 | ||
Call Number | EMAT @ emat @c:irua:174004 | Serial | 6659 | ||
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Author | Conti, S.; Perali, A.; Hamilton, A.R.; Milošević, M.V.; Peeters, F.M.; Neilson, D. | ||||
Title | Chester supersolid of spatially indirect excitons in double-layer semiconductor heterostructures | Type | A1 Journal article | ||
Year | 2023 | Publication | Physical review letters | Abbreviated Journal | |
Volume | 130 | Issue | 5 | Pages | 057001-57006 |
Keywords | A1 Journal article; Condensed Matter Theory (CMT) | ||||
Abstract | A supersolid, a counterintuitive quantum state in which a rigid lattice of particles flows without resistance, has to date not been unambiguously realized. Here we reveal a supersolid ground state of excitons in a double-layer semiconductor heterostructure over a wide range of layer separations outside the focus of recent experiments. This supersolid conforms to the original Chester supersolid with one exciton per supersolid site, as distinct from the alternative version reported in cold-atom systems of a periodic density modulation or clustering of the superfluid. We provide the phase diagram augmented by the supersolid. This new phase appears at layer separations much smaller than the predicted exciton normal solid, and it persists up to a solid-solid transition where the quantum phase coherence collapses. The ranges of layer separations and exciton densities in our phase diagram are well within reach of the current experimental capabilities. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000968650900001 | Publication Date | 2023-02-01 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0031-9007; 1079-7114 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.6 | Times cited | 7 | Open Access | Not_Open_Access |
Notes | Approved | Most recent IF: 8.6; 2023 IF: 8.462 | |||
Call Number | UA @ admin @ c:irua:196742 | Serial | 8817 | ||
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Author | van der Sluijs, M.M.; Salzmann, B.B.V.; Arenas Esteban, D.; Li, C.; Jannis, D.; Brafine, L.C.; Laning, T.D.; Reinders, J.W.C.; Hijmans, N.S.A.; Moes, J.R.; Verbeeck, J.; Bals, S.; Vanmaekelbergh, D. | ||||
Title | Study of the Mechanism and Increasing Crystallinity in the Self-Templated Growth of Ultrathin PbS Nanosheets | Type | A1 Journal article | ||
Year | 2023 | Publication | Chemistry of materials | Abbreviated Journal | |
Volume | Issue | Pages | |||
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Colloidal 2D semiconductor nanocrystals, the analogue of solid-state quantum wells, have attracted strong interest in material science and physics. Molar quantities of suspended quantum objects with spectrally pure absorption and emission can be synthesized. For the visible region, CdSe nanoplatelets with atomically precise thickness and tailorable emission have been (almost) perfected. For the near-infrared region, PbS nanosheets (NSs) hold strong promise, but the photoluminescence quantum yield is low and many questions on the crystallinity, atomic structure, intriguing rectangular shape, and formation mechanism remain to be answered. Here, we report on a detailed investigation of the PbS NSs prepared with a lead thiocyanate single source precursor. Atomically resolved HAADF-STEM imaging reveals the presence of defects and small cubic domains in the deformed orthorhombic PbS crystal lattice. Moreover, variations in thickness are observed in the NSs, but only in steps of 2 PbS monolayers. To study the reaction mechanism, a synthesis at a lower temperature allowed for the study of reaction intermediates. Specifically, we studied the evolution of pseudo-crystalline templates towards mature, crystalline PbS NSs. We propose a self-induced templating mechanism based on an oleylamine-lead-thiocyanate (OLAM-Pb-SCN) complex with two Pb-SCN units as a building block; the interactions between the long-chain ligands regulate the crystal structure and possibly the lateral dimensions. | ||||
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Publisher | Place of Publication | Editor | |||
Language | Wos | 000959572100001 | Publication Date | 2023-03-25 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0897-4756 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.6 | Times cited | 2 | Open Access | OpenAccess |
Notes | H2020 Research Infrastructures, 731019 ; H2020 European Research Council, 692691 815128 ; Nederlandse Organisatie voor Wetenschappelijk Onderzoek, 715.016.002 ; | Approved | Most recent IF: 8.6; 2023 IF: 9.466 | ||
Call Number | EMAT @ emat @c:irua:195894 | Serial | 7255 | ||
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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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Language | Wos | 001052093300001 | Publication Date | 2023-08-21 | |
Series Editor | Series Title | Abbreviated Series Title | |||
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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 | ||
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Author | Mulder, J.T.T.; Jenkinson, K.; Toso, S.; Prato, M.; Evers, W.H.H.; Bals, S.; Manna, L.; Houtepen, A.J.J. | ||||
Title | Nucleation and growth of bipyramidal Yb:LiYF₄ nanocrystals : growing up in a hot environment | Type | A1 Journal article | ||
Year | 2023 | Publication | Chemistry of materials | Abbreviated Journal | |
Volume | 35 | Issue | 14 | Pages | 5311-5321 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Lanthanide-doped LiYF4 (Ln:YLF) is commonlyused fora broad variety of optical applications, such as lasing, photon upconversionand optical refrigeration. When synthesized as nanocrystals (NCs),this material is also of interest for biological applications andfundamental physical studies. Until now, it was unclear how Ln:YLFNCs grow from their ionic precursors into tetragonal NCs with a well-defined,bipyramidal shape and uniform dopant distribution. Here, we studythe nucleation and growth of ytterbium-doped LiYF4 (Yb:YLF),as a template for general Ln:YLF NC syntheses. We show that the formationof bipyramidal Yb:YLF NCs is a multistep process starting with theformation of amorphous Yb:YLF spheres. Over time, these spheres growvia Ostwald ripening and crystallize, resulting in bipyramidal Yb:YLFNCs. We further show that prolonged heating of the NCs results inthe degradation of the NCs, observed by the presence of large LiFcubes and small, irregular Yb:YLF NCs. Due to the similarity in chemicalnature of all lanthanide ions our work sheds light on the formationstages of Ln:YLF NCs in general. | ||||
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Language | Wos | 001021474500001 | Publication Date | 2023-07-03 | |
Series Editor | Series Title | Abbreviated Series Title | |||
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ISSN | 0897-4756; 1520-5002 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 8.6 | Times cited | 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). The authors thank Niranjan Saikumar for proof reading the manuscript. | Approved | Most recent IF: 8.6; 2023 IF: 9.466 | ||
Call Number | UA @ admin @ c:irua:197787 | Serial | 8907 | ||
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Author | Mayda, S.; Monico, L.; Krishnan, D.; De Meyer, S.; Cotte, M.; Garrevoet, J.; Falkenberg, G.; Sandu, I.C.A.; Partoens, B.; Lamoen, D.; Romani, A.; Miliani, C.; Verbeeck, J.; Janssens, K. | ||||
Title | A combined experimental and computational approach to understanding CdS pigment oxidation in a renowned early 20th century painting | Type | A1 Journal article | ||
Year | 2023 | Publication | Chemistry of materials | Abbreviated Journal | |
Volume | 35 | Issue | 24 | Pages | 10403-10415 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT); Antwerp X-ray Imaging and Spectroscopy (AXIS) | ||||
Abstract | Cadmium sulfide (CdS)-based yellow pigments have been used in a number of early 20th century artworks, including The Scream series painted by Edvard Munch. Some of these unique paintings are threatened by the discoloration of these CdS-based yellow oil paints because of the oxidation of the original sulfides to sulfates. The experimental data obtained here prove that moisture and cadmium chloride compounds play a key role in promoting such oxidation. To clarify how these two factors effectively prompt the process, we studied the band alignment between CdS, CdCl2, and Cd-(OH)Cl as well as the radicals center dot OH and H3O center dot by density functional theory (DFT) methods. Our results show that a stack of several layers of Cd-(OH)Cl creates a pocket of positive holes at the Cl-terminated surface and a pocket of electrons at the OH-terminated surface by leading in a difference in ionization energy at both surfaces. The resulting band alignment indicates that Cd-(OH)Cl can indeed play the role of an oxidative catalyst for CdS in a moist environment, thus providing an explanation for the experimental evidence. | ||||
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Language | Wos | 001133000900001 | Publication Date | 2023-12-08 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0897-4756; 1520-5002 | ISBN | Additional Links | UA library record; WoS full record | |
Impact Factor | 8.6 | Times cited | Open Access | ||
Notes | The experimental research on the cadmium yellow powders/paint mock-ups and The Scream (ca. 1910) was financially supported by the European Union, research projects IPERION-CH (H2020-INFRAIA-2014-2015, GA no. 654028) and IPERION-HS (H2020-INFRAIA-2019-1, GA no. 871034) and the project AMIS within the program Dipartimenti di Eccellenza 2018-2022 (funded by MUR and the University of Perugia). For the beamtime grants received, the authors thank the ESRF-ID21 beamline (experiments HG64 and HG95), the DESY-P06 beamline, a member of the Helmholtz Association HGF (experiments I-20130221 EC and I-20160126 EC), and the project CALIPSOplus under the GA no. 730872 from the E.U. Framework Programme for Research and Innovation Horizon 2020. All of the staff of the MUNCH Museum (Conservation Department) is acknowledged for their collaboration. The computational resources and services used in this work were provided by the VSC (Flemish Supercomputer Center) and the HPC infrastructure of the University of Antwerp (CalcUA), both funded by the FWO – Vlaanderen and the Flemish Government, Department EWI. | Approved | Most recent IF: 8.6; 2023 IF: 9.466 | ||
Call Number | UA @ admin @ c:irua:202836 | Serial | 8999 | ||
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Author | Shevchenko, V.A.; Glazkova, I.S.; Novichkov, D.A.; Skvortsova, I.; V. Sobolev, A.; Abakumov, A.M.; Presniakov, I.A.; Drozhzhin, O.A.; V. Antipov, E. | ||||
Title | Competition between the Ni and Fe redox in the O3-NaNi1/3Fe1/3Mn1/3O2 cathode material for Na-ion batteries | Type | A1 Journal article | ||
Year | 2023 | Publication | Chemistry of materials | Abbreviated Journal | |
Volume | 35 | Issue | 10 | Pages | 4015-4025 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Sodium-ion batteries are attracting great attention due to their low cost and abundance of sodium. The O3-type NaNi1/3Fe1/3Mn1/3O2 layered oxide material is a promising candidate for positive electrodes (cathodes) in Na-ion batteries. However, its stable electrochemical performance is restricted by the upper voltage limit of 4.0 V (vs Na/Na+), which allows for reversibly removing 0.5-0.55 Na+ per formula unit, corresponding to the capacity of 120-130 mAh.g(-1). Further reduction of sodium content inevitably accelerates capacity degradation, and this issue calls for a detailed study of the redox reactions that accompany the electrochemical (de)intercalation of a large amount of sodium. Here, we present operando and ex situ studies using powder X-ray diffraction and X-ray absorption spectroscopy combined with Fe-57 Mossbauer spectroscopy. Our approach reveals the sequence of the redox transitions that occur during the charge and discharge of O3-NaNi1/3Fe1/3Mn1/3O2. Our data show that in addition to nickel and iron cations oxidizing to M+4, a part of iron transforms into the “3 + delta” state owing to the fast electron exchange Fe3+ + Fe4+ <-> Fe4+ + Fe3+. This process freezes upon cooling the material to 35 K, producing Fe4+ cations, some of which occupy tetrahedral positions. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000985970200001 | Publication Date | 2023-05-04 | |
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 | Open Access | ||
Notes | Approved | Most recent IF: 8.6; 2023 IF: 9.466 | |||
Call Number | UA @ admin @ c:irua:197352 | Serial | 9013 | ||
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Author | Zhou, R.; Neek-Amal, M.; Peeters, F.M.; Bai, B.; Sun, C. | ||||
Title | Interlink between Abnormal Water Imbibition in Hydrophilic and Rapid Flow in Hydrophobic Nanochannels | Type | A1 Journal Article | ||
Year | 2024 | Publication | Physical Review Letters | Abbreviated Journal | Phys. Rev. Lett. |
Volume | 132 | Issue | 18 | Pages | 184001 |
Keywords | A1 Journal Article; CMT | ||||
Abstract | Nanoscale extension and refinement of the Lucas-Washburn model is presented with a detailed analysis of recent experimental data and extensive molecular dynamics simulations to investigate rapid water flow and water imbibition within nanocapillaries. Through a comparative analysis of capillary rise in hydrophilic nanochannels, an unexpected reversal of the anticipated trend, with an abnormal peak, of imbibition length below the size of 3 nm was discovered in hydrophilic nanochannels, surprisingly sharing the same physical origin as the well-known peak observed in flow rate within hydrophobic nanochannels. The extended imbibition model is applicable across diverse spatiotemporal scales and validated against simulation results and existing experimental data for both hydrophilic and hydrophobic | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | Publication Date | 2024-04-30 | ||
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0031-9007 | ISBN | Additional Links | ||
Impact Factor | 8.6 | Times cited | 1 | Open Access | |
Notes | We gratefully acknowledge the financial support pro- vided by the National Natural Science Foundation of China (Projects No. 52488201 and No. 52222606). Part of this project was supported by the Flemish Science Foundations (FWO-Vl) and the Iranian National Science Foundation (No. 4025061 and No. 4021261). | Approved | Most recent IF: 8.6; 2024 IF: 8.462 | ||
Call Number | UA @ lucian @ | Serial | 9122 | ||
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Author | Vandemeulebroucke, D.; Batuk, M.; Hajizadeh, A.; Wastiaux, M.; Roussel, P.; Hadermann, J. | ||||
Title | Incommensurate Modulations and Perovskite Growth in LaxSr2–xMnO4−δAffecting Solid Oxide Fuel Cell Conductivity | Type | A1 Journal Article | ||
Year | 2024 | Publication | Chemistry of Materials | Abbreviated Journal | Chem. Mater. |
Volume | Issue | Pages | |||
Keywords | A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; | ||||
Abstract | Ruddlesden-Popper La????Sr2−????MnO4−???? materials are interesting symmetric solid oxide fuel cell electrodes due to their good redox stability, mixed ionic and electronic conducting behavior and thermal expansion that matches well with common electrolytes. In reducing environments – as at a solid oxide fuel cell anode – the x = 0.5 member, i.e. La0.5Sr1.5MnO4−????, has a much higher total conductivity than compounds with a different La/Sr ratio, although all those compositions have the same K2NiF4-type I4/mmm structure. The origin for this conductivity difference is not yet known in literature. Now, a combination of in-situ and ex-situ 3D electron diffraction, high-resolution imaging, energy-dispersive X-ray analysis and electron energy-loss spectroscopy uncovered clear differences between x=0.25 and x=0.5 in the pristine structure, as well as in the transformations upon high-temperature reduction. In La0.5Sr1.5MnO4−????, Ruddlesden-Popper n=2 layer defects and an amorphous surface layer are present, but not in La0.25Sr1.75MnO4−????. After annealing at 700°C in 5% H2/Ar, La0.25Sr1.75MnO4−???? transforms to a tetragonal 2D incommensurately modulated structure with modulation vectors ⃗????1 = 0.2848(1) · (⃗????* +⃗????*) and ⃗????2 =0.2848(1) · (⃗????* – ⃗????*), whereas La0.5Sr1.5MnO4−???? only partially transforms to an orthorhombic 1D incommensurately modulated structure, with ⃗???? = 0.318(2) · ⃗????*. Perovskite domains grow at the crystal edge at 700°C in 5% H2 or vacuum, due to the higher La concentration on the surface compared to the bulk, which leads to a different thermodynamic equilibrium. Since it is known that a lower degree of oxygen vacancy ordering and a higher amount of perovskite blocks enhance oxygen mobility, those differences in defect structure and structural transformation upon reduction, might all contribute to the higher conductivity of La0.5Sr1.5MnO4−???? in solid oxide fuel cell anode conditions compared to other La/Sr ratios. |
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | English | Wos | 001174840900001 | Publication Date | 2024-02-20 |
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 | Not_Open_Access | |
Notes | Universiteit Antwerpen, BOF TOP 38689 ; Fonds Wetenschappelijk Onderzoek, I003218N ; European Commission NanED, 956099 ; | Approved | Most recent IF: 8.6; 2024 IF: 9.466 | ||
Call Number | EMAT @ emat @c:irua:204354 | Serial | 8997 | ||
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Author | Bai, J.; Wang, J.T.-W.; Rubio, N.; Protti, A.; Heidari, H.; Elgogary, R.; Southern, P.; Al-Jamal, W.' T.; Sosabowski, J.; Shah, A.M.; Bals, S.; Pankhurst, Q.A.; Al-Jamal, K.T. | ||||
Title | Triple-Modal Imaging of Magnetically-Targeted Nanocapsules in Solid TumoursIn Vivo | Type | A1 Journal article | ||
Year | 2016 | Publication | Theranostics | Abbreviated Journal | Theranostics |
Volume | 6 | Issue | 6 | Pages | 342-356 |
Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
Abstract | Triple-modal imaging magnetic nanocapsules, encapsulating hydrophobic superparamagnetic iron oxide nanoparticles, are formulated and used to magnetically target solid tumours after intravenous administration in tumour-bearing mice. The engineered magnetic polymeric nanocapsules m-NCs are ~200 nm in size with negative Zeta potential and shown to be spherical in shape. The loading efficiency of superparamagnetic iron oxide nanoparticles in the m-NC was ~100%. Up to ~3- and ~2.2-fold increase in tumour uptake at 1 and 24 h was achieved, when a static magnetic field was applied to the tumour for 1 hour. m-NCs, with multiple imaging probes (e.g. indocyanine green, superparamagnetic iron oxide nanoparticles and indium-111), were capable of triple-modal imaging (fluorescence/magnetic resonance/nuclear imaging) in vivo. Using triple-modal imaging is to overcome the intrinsic limitations of single modality imaging and provides complementary information on the spatial distribution of the nanocarrier within the tumour. The significant findings of this study could open up new research perspectives in using novel magnetically-responsive nanomaterials in magnetic-drug targeting combined with multi-modal imaging. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000377797200005 | Publication Date | 2015-12-31 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 1838-7640 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.712 | Times cited | 54 | Open Access | OpenAccess |
Notes | The authors would like to thank Prof Robert Hider (King's College London) for useful discussion on the chemical functionalization of the polymers, Mr William Luckhurst (King's College London) on the technical help of AFM measurements and Mr Andrew Cakebread (King's College London) on his technical help of ICP-MS measurements. J.B. acknowledges funding from King's-China Scholarship Council (CSC). J.W. and N.R. acknowledge funding from Biotechnology and Biological Sciences Research Council (BB/J008656/1) and Associated International Cancer Research (12-1054). K.T.AJ. acknowledges funding from EU FP7-ITN Marie-Curie Network programme RADDEL (290023). S.B. acknowledges funding from the European Research Council under the 7th Framework Program (FP7), ERC Starting Grant No. 335078 COLOURATOMS, and the Integrated Infrastructure Initiative No. 262348 European Soft Matter Infrastructure, ESMI.; ECAS_Sara; (ROMEO:green; preprint:; postprint:can ; pdfversion:can); | Approved | Most recent IF: 8.712 | ||
Call Number | c:irua:130058 | Serial | 3995 | ||
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Author | Le, T.-S.; Nguyen, P.-D.; Ngo, H.H.; Bui, X.-T.; Dang, B.-T.; Diels, L.; Bui, H.-H.; Nguyen, M.-T.; Le Quang, D.-T. | ||||
Title | Two-stage anaerobic membrane bioreactor for co-treatment of food waste and kitchen wastewater for biogas production and nutrients recovery | Type | A1 Journal article | ||
Year | 2022 | Publication | Chemosphere | Abbreviated Journal | Chemosphere |
Volume | 309 | Issue | 1 | Pages | 136537-136539 |
Keywords | A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL) | ||||
Abstract | Co-digestion of organic waste and wastewater is receiving increased attention as a plausible waste management approach toward energy recovery. However, traditional anaerobic processes for co-digestion are particularly susceptible to severe organic loading rates (OLRs) under long-term treatment. To enhance technological feasi-bility, this work presented a two-stage Anaerobic Membrane Bioreactor (2 S-AnMBR) composed of a hydrolysis reactor (HR) followed by an anaerobic membrane bioreactor (AnMBR) for long-term co-digestion of food waste and kitchen wastewater. The OLRs were expanded from 4.5, 5.6, and 6.9 kg COD m- 3 d-1 to optimize biogas yield, nitrogen recovery, and membrane fouling at ambient temperatures of 25-32 degrees C. Results showed that specific methane production of UASB was 249 +/- 7 L CH4 kg-1 CODremoved at the OLR of 6.9 kg TCOD m- 3 d-1. Total Chemical Oxygen Demand (TCOD) loss by hydrolysis was 21.6% of the input TCOD load at the hydraulic retention time (HRT) of 2 days. However, low total volatile fatty acid concentrations were found in the AnMBR, indicating that a sufficiently high hydrolysis efficiency could be accomplished with a short HRT. Furthermore, using AnMBR structure consisting of an Upflow Anaerobic Sludge Blanket Reactor (UASB) followed by a side -stream ultrafiltration membrane alleviated cake membrane fouling. The wasted digestate from the AnMBR comprised 42-47% Total Kjeldahl Nitrogen (TKN) and 57-68% total phosphorous loading, making it suitable for use in soil amendments or fertilizers. Finally, the predominance of fine particles (D10 = 0.8 mu m) in the ultra -filtration membrane housing (UFMH) could lead to a faster increase in trans-membrane pressure during the filtration process. | ||||
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Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000866470600004 | Publication Date | 2022-09-20 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 0045-6535; 1879-1298 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.8 | Times cited | Open Access | Not_Open_Access | |
Notes | Approved | Most recent IF: 8.8 | |||
Call Number | UA @ admin @ c:irua:191557 | Serial | 7347 | ||
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