| |
Records |
Links  |
|
Author |
Monico, L.; Prati, S.; Sciutto, G.; Catelli, E.; Romani, A.; Balbas, D.Q.; Li, Z.; De Meyer, S.; Nuyts, G.; Janssens, K.; Cotte, M.; Garrevoet, J.; Falkenberg, G.; Tardillo Suarez, V.I.; Tucoulou, R.; Mazzeo, R. |
|
| |
Title |
Development of a multi-method analytical approach based on the combination of synchrotron radiation X-ray micro-analytical techniques and vibrational micro-spectroscopy methods to unveil the causes and mechanism of darkening of “fake-gilded” decorations in a Cimabue painting |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
Journal of analytical atomic spectrometry |
Abbreviated Journal |
J Anal Atom Spectrom |
|
| |
Volume |
37 |
Issue |
1 |
Pages |
114-129 |
|
| |
Keywords |
A1 Journal article; Antwerp X-ray Imaging and Spectroscopy (AXIS) |
|
| |
Abstract |
Redox processes activated by environmental factors have been identified as the main cause of the chromatic alterations of a number of artists' pigments, including the yellow pigment orpiment (As2S3). Although a general comprehension of the mechanisms has been provided through characterization of degradation compounds of As2S3, experimental evidences to prove how other paint components and how different environmental agents influence the formation pathways of specific secondary compounds are still lacking. Thus, it becomes fundamental to develop a methodological strategy which enable achieving a discrimination among the causes affecting the chemical stability of more heterogenous As2S3-based paints and defining the mechanism through which the alteration establishes and evolves, with the ultimate goal of optimizing the preventive conservation measures of unique masterpieces. In this paper, we propose a comprehensive multi-material and multi-method approach based on the combination of synchrotron radiation X-ray micro-analytical techniques (i.e., X-ray diffraction, X-ray fluorescence and X-ray absorption near edge structure spectroscopy at S K-/Ag L-3-/As K-edges) and vibrational micro-spectroscopy methods to unveil the causes and mechanism of darkening of “fake-gilded” decorations in tempera paintings, originally consisting of an unusual mixture of As2S3 and metallic silver (Ag-0). Such degradation process is a not yet understood phenomenon threatening a series of Old Master paintings, including those by the Italian painters Cimabue and Pietro Lorenzetti. The high specificity, sensitivity and lateral resolution of the employed analytical methods allowed providing first-time evidence for the presence of black acanthite (alpha-Ag2S), mimetite [Pb-5(AsO4)(3)Cl] and syngenite [K2Ca(SO4)(2)center dot H2O] as degradation products of the “fake-gilded” decorations in the Maesta by Cimabue (Church of Santa Maria dei Servi, Bologna, Italy). Furthermore, the study of the painting combined with that of tempera paint mock-ups permitted to explore and define the environmental agents and internal factors causing the darkening, by proving that: (i) Ag-0 and moisture are key-factors for triggering the transformation of As2S3 to alpha-Ag2S and As-oxides; (ii) S2--ions arising from the degradation of As2S3 are the main responsible for the formation of alpha-Ag2S; (iii) light exposure strengthens the tendency of the paint components towards alteration. Based on our findings, we finally propose a degradation mechanism of As2S3/Ag-0-based tempera paints. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000722353400001 |
Publication Date |
2021-11-18 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
0267-9477 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
3.4 |
Times cited |
|
Open Access |
OpenAccess |
|
| |
Notes |
|
Approved |
Most recent IF: 3.4 |
|
| |
Call Number |
UA @ admin @ c:irua:184871 |
Serial |
7142 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Mallick, S.; Zhang, W.; Batuk, M.; Gibbs, A.S.; Hadermann, J.; Halasyamani, P.S.; Hayward, M.A. |
|
| |
Title |
The crystal and defect structures of polar KBiNb2O7 |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
Journal of the Chemical Society : Dalton transactions |
Abbreviated Journal |
Dalton T |
|
| |
Volume |
51 |
Issue |
5 |
Pages |
1866-1873 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
KBiNb2O7 was prepared from RbBiNb2O7 by a sequence of cation exchange reactions which first convert RbBiNb2O7 to LiBiNb2O7, before KBiNb2O7 is formed by a further K-for-Li cation exchange. A combination of neutron, synchrotron X-ray and electron diffraction data reveal that KBiNb2O7 adopts a polar, layered, perovskite structure (space group A11m) in which the BiNb2O7 layers are stacked in a (0, ½, z) arrangement, with the K+ cations located in half of the available 10-coordinate interlayer cation sites. The inversion symmetry of the phase is broken by a large displacement of the Bi3+ cations parallel to the y-axis. HAADF-STEM images reveal that KBiNb2O7 exhibits frequent stacking faults which convert the (0. ½, z) layer stacking to (½, 0, z) stacking and vice versa, essentially switching the x- and y-axes of the material. By fitting the complex diffraction peak shape of the SXRD data collected from KBiNb2O7 it is estimated that each layer has approximately an ~11% chance of being defective – a high level which is attributed to the lack of cooperative NbO6 tilting in the material, which limits the lattice strain associated with each fault. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000741540300001 |
Publication Date |
2022-01-05 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
1477-9226 |
ISBN |
|
Additional Links |
UA library record; WoS full record |
|
| |
Impact Factor |
4 |
Times cited |
|
Open Access |
OpenAccess |
|
| |
Notes |
Experiments at the Diamond Light Source were performed as part of the Block Allocation Group award “Oxford/Warwick Solid State Chemistry BAG to probe composition-structure-property relationships in solids” (EE18786). Experiments at the ISIS pulsed neutron facility were supported by a beam time allocation from the STFC (RB 2000148). SM thanks Somerville College for an Oxford Ryniker Lloyd scholarship. PSH and WZ thank the National Science Foundation (DMR-2002319) for support. |
Approved |
Most recent IF: 4 |
|
| |
Call Number |
EMAT @ emat @c:irua:185504 |
Serial |
6951 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Demirkol, Ö.; Sevik, C.; Demiroğlu, I. |
|
| |
Title |
First principles assessment of the phase stability and transition mechanisms of designated crystal structures of pristine and Janus transition metal dichalcogenides |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
Physical chemistry, chemical physics |
Abbreviated Journal |
Phys Chem Chem Phys |
|
| |
Volume |
24 |
Issue |
12 |
Pages |
7430-7441 |
|
| |
Keywords |
A1 Journal article; Condensed Matter Theory (CMT) |
|
| |
Abstract |
Two-dimensional Transition Metal Dichalcogenides (TMDs) possessing extraordinary physical properties at reduced dimensionality have attracted interest due to their promise in electronic and optical device applications. However, TMD monolayers can show a broad range of different properties depending on their crystal phase; for example, H phases are usually semiconductors, while the T phases are metallic. Thus, controlling phase transitions has become critical for device applications. In this study, the energetically low-lying crystal structures of pristine and Janus TMDs are investigated by using ab initio Nudged Elastic Band and molecular dynamics simulations to provide a general explanation for their phase stability and transition properties. Across all materials investigated, the T phase is found to be the least stable and the H phase is the most stable except for WTe2, while the T' and T '' phases change places according to the TMD material. The transition energy barriers are found to be large enough to hint that even the higher energy phases are unlikely to undergo a phase transition to a more stable phase if they can be achieved except for the least stable T phase, which has zero barrier towards the T ' phase. Indeed, in molecular dynamics simulations the thermodynamically least stable T phase transformed into the T ' phase spontaneously while in general no other phase transition was observed up to 2100 K for the other three phases. Thus, the examined T ', T '' and H phases were shown to be mostly stable and do not readily transform into another phase. Furthermore, so-called mixed phase calculations considered in our study explain the experimentally observed lateral hybrid structures and point out that the coexistence of different phases is strongly stable against phase transitions. Indeed, stable complex structures such as metal-semiconductor-metal architectures, which have immense potential to be used in future device applications, are also possible based on our investigation. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000766791000001 |
Publication Date |
2022-02-23 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
1463-9076; 1463-9084 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
3.3 |
Times cited |
|
Open Access |
OpenAccess |
|
| |
Notes |
|
Approved |
Most recent IF: 3.3 |
|
| |
Call Number |
UA @ admin @ c:irua:187184 |
Serial |
7164 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Vervloessem, E.; Gorbanev, Y.; Nikiforov, A.; De Geyter, N.; Bogaerts, A. |
|
| |
Title |
Sustainable NOxproduction from air in pulsed plasma: elucidating the chemistry behind the low energy consumption |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
Green Chemistry |
Abbreviated Journal |
Green Chem |
|
| |
Volume |
24 |
Issue |
2 |
Pages |
916-929 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
|
| |
Abstract |
N-Based fertilisers are paramount to support our still-growing world population. Current industrial N<sub>2</sub>fixation is heavily fossil fuel-dependent, therefore, a lot of work is put into the development of fossil-free pathways. Plasma technology offers a fossil-free and flexible method for N<sub>2</sub>fixation that is compatible with renewable energy sources. We present here a pulsed plasma jet for direct NO<sub><italic>x</italic></sub>production from air. The pulsed power allows for a record-low energy consumption (EC) of 0.42 MJ (mol N)<sup>−1</sup>. This is the lowest reported EC in plasma-based N<sub>2</sub>fixation at atmospheric pressure thus far. We compare our experimental data with plasma chemistry modelling, and obtain very good agreement. Hence, we can use our model to explain the underlying mechanisms responsible for this low EC. The pulsed power and the corresponding pulsed gas temperature are the reason for the very low EC: they provide a strong vibrational–translational non-equilibrium and promote the non-thermal Zeldovich mechanism. This insight is important for the development of the next generation of plasma sources for energy-efficient NO<sub><italic>x</italic></sub>production. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000739578400001 |
Publication Date |
2021-12-22 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
1463-9262 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
9.8 |
Times cited |
|
Open Access |
Not_Open_Access |
|
| |
Notes |
H2020 European Research Council, grant agreement no. 810182 – SCOPE ERC Synergy project ; Herculesstichting; Fonds Wetenschappelijk Onderzoek, EOS ID 30505023 FWO grant ID GoF9618n ; Universiteit Antwerpen; This research was supported by the Excellence of Science FWO-FNRS project (NITROPLASM, FWO grant ID GoF9618n, EOS ID 30505023), the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement no. 810182 – SCOPE ERC Synergy project), and through long-term structural funding (Methusalem). The calculations were performed using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UAntwerpen), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (Department EWI) and the UAntwerpen. We thank E. H. Choi and coworkers from the Plasma Bioscience Research Center (Korea) for providing the Soft Jet plasma source, as well as K. van’t Veer and C. Verheyen for the fruitful discussion on the electron loss fraction calculations. The graphical abstract was designed using resources from Flaticon.com. |
Approved |
Most recent IF: 9.8 |
|
| |
Call Number |
PLASMANT @ plasmant @c:irua:185450 |
Serial |
6906 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Parastaev, A.; Muravev, V.; Osta, E.H.; Kimpel, T.F.; Simons, J.F.M.; van Hoof, A.J.F.; Uslamin, E.; Zhang, L.; Struijs, J.J.C.; Burueva, D.B.; Pokochueva, E.V.; Kovtunov, K.V.; Koptyug, I.V.; Villar-Garcia, I.J.; Escudero, C.; Altantzis, T.; Liu, P.; Béché, A.; Bals, S.; Kosinov, N.; Hensen, E.J.M. |
|
| |
Title |
Breaking structure sensitivity in CO2 hydrogenation by tuning metal–oxide interfaces in supported cobalt nanoparticles |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
Nature Catalysis |
Abbreviated Journal |
Nat Catal |
|
| |
Volume |
5 |
Issue |
11 |
Pages |
1051-1060 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
|
| |
Abstract |
A high dispersion of the active metal phase of transition metals on oxide supports is important when designing efficient heterogeneous catalysts. Besides nanoparticles, clusters and even single metal atoms can be attractive for a wide range of reactions. However, many industrially relevant catalytic transformations suffer from structure sensitivity, where reducing the size of the metal particles below a certain size substantially lowers catalytic performance. A case in point is the low activity of small cobalt nanoparticles in the hydrogenation of CO and CO2. Here we show how engineering of catalytic sites at the metal–oxide interface in cerium oxide–zirconium dioxide (ceria–zirconia)-supported cobalt can overcome this structure sensitivity. Few-atom cobalt clusters dispersed on 3 nm cobalt(II)-oxide particles stabilized by ceria–zirconia yielded a highly active CO2 methanation catalyst with a specific activity higher than that of larger particles under the same conditions. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000884939300006 |
Publication Date |
2022-11-17 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
2520-1158 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
37.8 |
Times cited |
32 |
Open Access |
OpenAccess |
|
| |
Notes |
This research was supported by the Applied and Engineering Sciences division of the Netherlands Organization for Scientific Research through the Alliander (now Qirion) Perspective program on Plasma Conversion of CO2. We acknowledge Diamond Light Source for time on beamline B18 under proposal SP20715-1. This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 823717 – ESTEEM3. S.B. acknowledges support from the European Research Council (ERC Consolidator Grant #815128 REALNANO) and T.A. acknowledges funding from the University of Antwerp Research fund (BOF). A.B. received funding from the European Union under grant agreement No 823717 – ESTEEM3. The authors acknowledge funding through the Hercules grant (FWO, University of Antwerp) I003218N “Infrastructure for imaging nanoscale processes in gas/vapour or liquid environments”. I.V.K., D.B.B., and E.V.P. acknowledge the Russian Ministry of Science and Higher Education (contract 075-15-2021-580) for financial support of parahydrogen-based studies. Experiments using synchrotron radiation XPS were performed at the CIRCE beamline at ALBA Synchrotron with the collaboration of ALBA staff. F. Oropeza Palacio and Rim C.J. van de Poll are acknowledged for the help with RPES measurements.; esteem3reported; esteem3jra |
Approved |
Most recent IF: 37.8 |
|
| |
Call Number |
EMAT @ emat @c:irua:192068 |
Serial |
7230 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Borah, R.; Ninakanti, R.; Bals, S.; Verbruggen, S.W. |
|
| |
Title |
Plasmon resonance of gold and silver nanoparticle arrays in the Kretschmann (attenuated total reflectance) vs. direct incidence configuration |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
Scientific reports |
Abbreviated Journal |
Sci Rep-Uk |
|
| |
Volume |
12 |
Issue |
1 |
Pages |
15738-19 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Sustainable Energy, Air and Water Technology (DuEL) |
|
| |
Abstract |
While the behaviour of plasmonic solid thin films in the Kretschmann (also known as Attenuated Total Reflection, ATR) configuration is well-understood, the use of discrete nanoparticle arrays in this optical configuration is not thoroughly explored. It is important to do so, since close packed plasmonic nanoparticle arrays exhibit exceptionally strong light-matter interactions by plasmonic coupling. The present work elucidates the optical properties of plasmonic Au and Ag nanoparticle arrays in both the direct normal incidence and Kretschmann configuration by numerical models, that are validated experimentally. First, hexagonal close packed Au and Ag nanoparticle films/arrays are obtained by air–liquid interfacial assembly. The numerical models for the rigorous solution of the Maxwell’s equations are validated using experimental optical spectra of these films before systematically investigating various parameters. The individual far-field/near-field optical properties, as well as the plasmon relaxation mechanism of the nanoparticles, vary strongly as the packing density of the array increases. In the Kretschmann configuration, the evanescent fields arising from p – and s -polarized (or TM and TE polarized) incidence have different directional components. The local evanescent field intensity and direction depends on the polarization, angle of incidence and the wavelength of incidence. These factors in the Kretschmann configuration give rise to interesting far-field as well as near-field optical properties. Overall, it is shown that plasmonic nanoparticle arrays in the Kretschmann configuration facilitate strong broadband absorptance without transmission losses, and strong near-field enhancement. The results reported herein elucidate the optical properties of self-assembled nanoparticle films, pinpointing the ideal conditions under which the normal and the Kretschmann configuration can be exploited in multiple light-driven applications. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000858344700048 |
Publication Date |
2022-09-21 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
2045-2322 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
4.6 |
Times cited |
11 |
Open Access |
OpenAccess |
|
| |
Notes |
R.B. acknowledges financial support from the University of Antwerp Special Research Fund (BOF) for a DOCPRO4 doctoral scholarship (Grant FN541100001). |
Approved |
Most recent IF: 4.6 |
|
| |
Call Number |
UA @ admin @ c:irua:190864 |
Serial |
7194 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Vanderveken, F.; Tyberkevych, V.; Talmelli, G.; Sorée, B.; Ciubotaru, F.; Adelmann, C. |
|
| |
Title |
Lumped circuit model for inductive antenna spin-wave transducers |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
Scientific reports |
Abbreviated Journal |
Sci Rep-Uk |
|
| |
Volume |
12 |
Issue |
1 |
Pages |
3796-13 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT) |
|
| |
Abstract |
We derive a lumped circuit model for inductive antenna spin-wave transducers in the vicinity of a ferromagnetic medium. The model considers the antenna's Ohmic resistance, its inductance, as well as the additional inductance due to the excitation of ferromagnetic resonance or spin waves in the ferromagnetic medium. As an example, the additional inductance is discussed for a wire antenna on top of a ferromagnetic waveguide, a structure that is characteristic for many magnonic devices and experiments. The model is used to assess the scaling properties and the energy efficiency of inductive antennas. Issues related to scaling antenna transducers to the nanoscale and possible solutions are also addressed. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000826474600050 |
Publication Date |
2022-03-08 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
2045-2322 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
4.6 |
Times cited |
|
Open Access |
OpenAccess |
|
| |
Notes |
|
Approved |
Most recent IF: 4.6 |
|
| |
Call Number |
UA @ admin @ c:irua:190001 |
Serial |
7180 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Slavkovic, S.; Shoara, A.A.; Churcher, Z.R.; Daems, E.; De Wael, K.; Sobott, F.; Johnson, P.E. |
|
| |
Title |
DNA binding by the antimalarial compound artemisinin |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
Scientific reports |
Abbreviated Journal |
|
|
| |
Volume |
12 |
Issue |
1 |
Pages |
133 |
|
| |
Keywords |
A1 Journal article; Pharmacology. Therapy; Engineering sciences. Technology; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab) |
|
| |
Abstract |
Artemisinin (ART) is a vital medicinal compound that is used alone or as part of a combination therapy against malaria. ART is thought to function by attaching to heme covalently and alkylating a range of proteins. Using a combination of biophysical methods, we demonstrate that ART is bound by three-way junction and duplex containing DNA molecules. Binding of ART by DNA is first shown for the cocaine-binding DNA aptamer and extensively studied using this DNA molecule. Isothermal titration calorimetry methods show that the binding of ART is both entropically and enthalpically driven at physiological NaCl concentration. Native mass spectrometry methods confirm DNA binding and show that a non-covalent complex is formed. Nuclear magnetic resonance spectroscopy shows that ART binds at the three-way junction of the cocaine-binding aptamer, and that binding results in the folding of the structure-switching variant of this aptamer. This structure-switching ability was exploited using the photochrome aptamer switch assay to demonstrate that ART can be detected using this biosensing assay. This study is the first to demonstrate the DNA binding ability of ART and should lay the foundation for further work to study implications of DNA binding for the antimalarial activity of ART. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000740510500120 |
Publication Date |
2022-01-07 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
2045-2322 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
|
Times cited |
|
Open Access |
OpenAccess |
|
| |
Notes |
|
Approved |
no |
|
| |
Call Number |
UA @ admin @ c:irua:184507 |
Serial |
8851 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Zhang, H.; Pryds, N.; Park, D.-S.; Gauquelin, N.; Santucci, S.; Christensen, D., V.; Jannis, D.; Chezganov, D.; Rata, D.A.; Insinga, A.R.; Castelli, I.E.; Verbeeck, J.; Lubomirsky, I.; Muralt, P.; Damjanovic, D.; Esposito, V. |
|
| |
Title |
Atomically engineered interfaces yield extraordinary electrostriction |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
Nature |
Abbreviated Journal |
|
|
| |
Volume |
609 |
Issue |
7928 |
Pages |
695-700 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
Electrostriction is a property of dielectric materials whereby an applied electric field induces a mechanical deformation proportional to the square of that field. The magnitude of the effect is usually minuscule (<10(-19) m(2) V-2 for simple oxides). However, symmetry-breaking phenomena at the interfaces can offer an efficient strategy for the design of new properties(1,2). Here we report an engineered electrostrictive effect via the epitaxial deposition of alternating layers of Gd2O3-doped CeO2 and Er2O3-stabilized delta-Bi2O3 with atomically controlled interfaces on NdGaO3 substrates. The value of the electrostriction coefficient achieved is 2.38 x 10(-14) m(2) V-2, exceeding the best known relaxor ferroelectrics by three orders of magnitude. Our theoretical calculations indicate that this greatly enhanced electrostriction arises from coherent strain imparted by interfacial lattice discontinuity. These artificial heterostructures open a new avenue for the design and manipulation of electrostrictive materials and devices for nano/micro actuation and cutting-edge sensors. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000859073900001 |
Publication Date |
2022-09-21 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
1476-4687 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
|
Times cited |
12 |
Open Access |
OpenAccess |
|
| |
Notes |
This research was supported by the BioWings project, funded by the European Union’s Horizon 2020, Future and Emerging Technologies programme (grant no. 801267), and by the Danish Council for Independent Research Technology and Production Sciences for the DFF—Research Project 2 (grant no. 48293). N.P. and D.V.C. acknowledge funding from Villum Fonden for the NEED project (no. 00027993) and from the Danish Council for Independent Research Technology and Production Sciences for the DFF—Research Project 3 (grant no. 00069 B). V.E. acknowledges funding from Villum Fonden for the IRIDE project (no. 00022862). N.G. and J.V. acknowledge funding from the GOA project ('Solarpaint') of the University of Antwerp. The microscope used in this work was partly funded by the Hercules Fund from the Flemish Government. D.J. acknowledges funding from the FWO Project (no. G093417N) from the Flemish Fund for Scientific Research. D.C. acknowledges TOP/BOF funding from the University of Antwerp. This project has received funding from the European Union’s Horizon 2020 Research Infrastructure—Integrating Activities for Advanced Communities—under grant agreement no. 823717-ESTEEM3. We thank T. D. Pomar and A. J. Bergne for English proofreading.; esteem3reported; esteem3TA |
Approved |
Most recent IF: NA |
|
| |
Call Number |
UA @ admin @ c:irua:190576 |
Serial |
7129 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
De Backer, A.; Van Aert, S.; Faes, C.; Arslan Irmak, E.; Nellist, P.D.; Jones, L. |
|
| |
Title |
Experimental reconstructions of 3D atomic structures from electron microscopy images using a Bayesian genetic algorithm |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
N P J Computational Materials |
Abbreviated Journal |
npj Comput Mater |
|
| |
Volume |
8 |
Issue |
1 |
Pages |
216 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
We introduce a Bayesian genetic algorithm for reconstructing atomic models of monotype crystalline nanoparticles from a single projection using Z-contrast imaging. The number of atoms in a projected atomic column obtained from annular dark field scanning transmission electron microscopy images serves as an input for the initial three-dimensional model. The algorithm minimizes the energy of the structure while utilizing a priori information about the finite precision of the atom-counting results and neighbor-mass relations. The results show promising prospects for obtaining reliable reconstructions of beam-sensitive nanoparticles during dynamical processes from images acquired with sufficiently low incident electron doses. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000866500900001 |
Publication Date |
2022-10-12 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
2057-3960 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
|
Times cited |
|
Open Access |
OpenAccess |
|
| |
Notes |
This work was supported by the European Research Council (Grant 770887 PICOMETRICS to S.V.A. and Grant 823717 ESTEEM3). The authors acknowledge financial support from the Research Foundation Flanders (FWO, Belgium) through project fundings (G.0267.18N, G.0502.18N, G.0346.21N) and a postdoctoral grant to A.D.B. L.J. acknowledges Science Foundation Ireland (SFI – grant number URF/RI/191637), the Royal Society, and the AMBER Centre. The authors acknowledge Aakash Varambhia for his assistance and expertise with the experimental recording and use of characterization facilities within the David Cockayne Centre for Electron Microscopy, Department of Materials, University of Oxford, and in particular the EPSRC (EP/K040375/1 South of England Analytical Electron Microscope).; esteem3reported; esteem3JRA |
Approved |
Most recent IF: NA |
|
| |
Call Number |
EMAT @ emat @c:irua:191398 |
Serial |
7114 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Wang, D.; Hermes, M.; Najmr, S.; Tasios, N.; Grau-Carbonell, A.; Liu, Y.; Bals, S.; Dijkstra, M.; Murray, C.B.; van Blaaderen, A. |
|
| |
Title |
Structural diversity in three-dimensional self-assembly of nanoplatelets by spherical confinement |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
Nature communications |
Abbreviated Journal |
Nat Commun |
|
| |
Volume |
13 |
Issue |
1 |
Pages |
6001-6012 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
Nanoplatelets offer many possibilities to construct advanced materials due to new properties associated with their (semi)two-dimensional shapes. However, precise control of both positional and orientational order of the nanoplatelets in three dimensions, which is required to achieve emerging and collective properties, is challenging to realize. Here, we combine experiments, advanced electron tomography and computer simulations to explore the structure of supraparticles self-assembled from nanoplatelets in slowly drying emulsion droplets. We demonstrate that the rich phase behaviour of nanoplatelets, and its sensitivity to subtle changes in shape and interaction potential can be used to guide the self-assembly into a wide range of different structures, offering precise control over both orientation and position order of the nanoplatelets. Our research is expected to shed light on the design of hierarchically structured metamaterials with distinct shape- and orientation- dependent properties. Nanoplatelets can be used as anisotropic building blocks for constructing novel optoelectronic materials. Here, Wang et al. show a route of assembling nanoplatelets with controllable positional and orientational order in three dimensions facilitated by the surface tension of drying emulsion droplets. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000867312100031 |
Publication Date |
2022-10-12 |
|
| |
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 |
7 |
Open Access |
OpenAccess |
|
| |
Notes |
We thank A. Kadu, M. Chiappini, F. Rabouw, S. Paliwal, X. Xie, C. Xia and Z. Wang for fruitful discussions. D.W. and A.v.B. acknowledge partial financial support from the European Research Council under the European Union's Seventh Framework Programme (FP-2007-2013)/ERC Advanced Grant Agreement 291667 HierarSACol. M.H. was supported by the Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC). D.W. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (grant 894254 SuprAtom). Y.L. acknowledges the Sustainability project between the faculties of Science and Geosciences of Utrecht University. M.D. acknowledges financial support from European Research Council (Grant No. ERC-2019-ADV-H2020 884902 SoftML). S.B. acknowledges financial support from ERC Consolidator Grant No. 815128 REALNANO. C.B.M. acknowledges support for materials synthesis from the Office of Naval Research Multidisciplinary University Research Initiative Award ONR N00014-18-1-2497. The authors acknowledge the EM square center at Utrecht University for the access to the microscopes. |
Approved |
Most recent IF: 16.6 |
|
| |
Call Number |
UA @ admin @ c:irua:191387 |
Serial |
7214 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Cai, J.; Griffin, E.; Guarochico-Moreira, V.H.; Barry, D.; Xin, B.; Yagmurcukardes, M.; Zhang, S.; Geim, A.K.; Peeters, F.M.; Lozada-Hidalgo, M. |
|
| |
Title |
Wien effect in interfacial water dissociation through proton-permeable graphene electrodes |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
Nature communications |
Abbreviated Journal |
Nat Commun |
|
| |
Volume |
13 |
Issue |
1 |
Pages |
5776-5777 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT) |
|
| |
Abstract |
Strong electric fields can accelerate molecular dissociation reactions. The phenomenon known as the Wien effect was previously observed using high-voltage electrolysis cells that produced fields of about 10(7) V m(-1), sufficient to accelerate the dissociation of weakly bound molecules (e.g., organics and weak electrolytes). The observation of the Wien effect for the common case of water dissociation (H2O reversible arrow H+ + OH-) has remained elusive. Here we study the dissociation of interfacial water adjacent to proton-permeable graphene electrodes and observe strong acceleration of the reaction in fields reaching above 10(8) V m(-1). The use of graphene electrodes allows measuring the proton currents arising exclusively from the dissociation of interfacial water, while the electric field driving the reaction is monitored through the carrier density induced in graphene by the same field. The observed exponential increase in proton currents is in quantitative agreement with Onsager's theory. Our results also demonstrate that graphene electrodes can be valuable for the investigation of various interfacial phenomena involving proton transport. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000862552600012 |
Publication Date |
2022-10-01 |
|
| |
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 |
3 |
Open Access |
OpenAccess |
|
| |
Notes |
|
Approved |
Most recent IF: 16.6 |
|
| |
Call Number |
UA @ admin @ c:irua:191575 |
Serial |
7228 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Zhou, Z.; Tan, Y.; Yang, Q.; Bera, A.; Xiong, Z.; Yagmurcukardes, M.; Kim, M.; Zou, Y.; Wang, G.; Mishchenko, A.; Timokhin, I.; Wang, C.; Wang, H.; Yang, C.; Lu, Y.; Boya, R.; Liao, H.; Haigh, S.; Liu, H.; Peeters, F.M.; Li, Y.; Geim, A.K.; Hu, S. |
|
| |
Title |
Gas permeation through graphdiyne-based nanoporous membranes |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
Nature communications |
Abbreviated Journal |
Nat Commun |
|
| |
Volume |
13 |
Issue |
1 |
Pages |
4031-4036 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT) |
|
| |
Abstract |
Nanoporous membranes based on two dimensional materials are predicted to provide highly selective gas transport in combination with extreme permeance. Here we investigate membranes made from multilayer graphdiyne, a graphene-like crystal with a larger unit cell. Despite being nearly a hundred of nanometers thick, the membranes allow fast, Knudsen-type permeation of light gases such as helium and hydrogen whereas heavy noble gases like xenon exhibit strongly suppressed flows. Using isotope and cryogenic temperature measurements, the seemingly conflicting characteristics are explained by a high density of straight-through holes (direct porosity of similar to 0.1%), in which heavy atoms are adsorbed on the walls, partially blocking Knudsen flows. Our work offers important insights into intricate transport mechanisms playing a role at nanoscale. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000918423100001 |
Publication Date |
2022-07-12 |
|
| |
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 |
10 |
Open Access |
OpenAccess |
|
| |
Notes |
|
Approved |
Most recent IF: 16.6 |
|
| |
Call Number |
UA @ admin @ c:irua:194402 |
Serial |
7308 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Toso, S.; Imran, M.; Mugnaioli, E.; Moliterni, A.; Caliandro, R.; Schrenker, N.J.; Pianetti, A.; Zito, J.; Zaccaria, F.; Wu, Y.; Gemmi, M.; Giannini, C.; Brovelli, S.; Infante, I.; Bals, S.; Manna, L. |
|
| |
Title |
Halide perovskites as disposable epitaxial templates for the phase-selective synthesis of lead sulfochloride nanocrystals |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
Nature communications |
Abbreviated Journal |
Nat Commun |
|
| |
Volume |
13 |
Issue |
1 |
Pages |
3976-10 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
Colloidal chemistry grants access to a wealth of materials through simple and mild reactions. However, even few elements can combine in a variety of stoichiometries and structures, potentially resulting in impurities or even wrong products. Similar issues have been long addressed in organic chemistry by using reaction-directing groups, that are added to a substrate to promote a specific product and are later removed. Inspired by such approach, we demonstrate the use of CsPbCl3 perovskite nanocrystals to drive the phase-selective synthesis of two yet unexplored lead sulfochlorides: Pb3S2Cl2 and Pb4S3Cl2. When homogeneously nucleated in solution, lead sulfochlorides form Pb3S2Cl2 nanocrystals. Conversely, the presence of CsPbCl3 triggers the formation of Pb4S3Cl2/CsPbCl3 epitaxial heterostructures. The phase selectivity is guaranteed by the continuity of the cationic subnetwork across the interface, a condition not met in a hypothetical Pb3S2Cl2/CsPbCl3 heterostructure. The perovskite domain is then etched, delivering phase-pure Pb4S3Cl2 nanocrystals that could not be synthesized directly. Phase-selective approaches, such using reaction-directing groups, are often seen in traditional organic chemistry and catalysis. Here authors use perovskite nanocrystals as disposable templates to drive the phase-selective synthesis of two colloidal nanomaterials, the lead sulfohalides Pb3S2Cl2 and Pb4S3Cl2. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000825867200003 |
Publication Date |
2022-07-08 |
|
| |
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 |
15 |
Open Access |
OpenAccess |
|
| |
Notes |
The authors would like to acknowledge Dr. Joka Buha for the help with preliminary tests preceding this project, and Dr. B. M. Aresta and Dr. L. Cassano for their administrative support. The authors acknowledge financial support from the Research Foundation Flanders (FWO) through a postdoctoral fellowship to N.J.S. (FWO Grant No. 1238622N, N.J.S). S.B. acknowledges financial support from the European Commission by ERC Consolidator grant REALNANO (No. 815128, S.B.). L.M. acknowledges financial support from the Italian Ministry of University and Research (MIUR) through the Flag-Era JTC2019 project “Solution-Processed Perovskite/Graphene Nanocomposites for SelfPowered Gas Sensors” (PeroGaS, L.M.). The access to the National Synchrotron Light Source, Brookhaven National Laboratory, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC0298CH10886 (NSLS-II Proposal Number 307441). |
Approved |
Most recent IF: 16.6 |
|
| |
Call Number |
UA @ admin @ c:irua:189684 |
Serial |
7085 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Chen, B.; Gauquelin, N.; Strkalj, N.; Huang, S.; Halisdemir, U.; Nguyen, M.D.; Jannis, D.; Sarott, M.F.; Eltes, F.; Abel, S.; Spreitzer, M.; Fiebig, M.; Trassin, M.; Fompeyrine, J.; Verbeeck, J.; Huijben, M.; Rijnders, G.; Koster, G. |
|
| |
Title |
Signatures of enhanced out-of-plane polarization in asymmetric BaTiO3 superlattices integrated on silicon |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
Nature communications |
Abbreviated Journal |
Nat Commun |
|
| |
Volume |
13 |
Issue |
1 |
Pages |
265 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
In order to bring the diverse functionalities of transition metal oxides into modern electronics, it is imperative to integrate oxide films with controllable properties onto the silicon platform. Here, we present asymmetric LaMnO<sub>3</sub>/BaTiO<sub>3</sub>/SrTiO<sub>3</sub>superlattices fabricated on silicon with layer thickness control at the unit-cell level. By harnessing the coherent strain between the constituent layers, we overcome the biaxial thermal tension from silicon and stabilize<italic>c</italic>-axis oriented BaTiO<sub>3</sub>layers with substantially enhanced tetragonality, as revealed by atomically resolved scanning transmission electron microscopy. Optical second harmonic generation measurements signify a predominant out-of-plane polarized state with strongly enhanced net polarization in the tricolor superlattices, as compared to the BaTiO<sub>3</sub>single film and conventional BaTiO<sub>3</sub>/SrTiO<sub>3</sub>superlattice grown on silicon. Meanwhile, this coherent strain in turn suppresses the magnetism of LaMnO<sub>3</sub>as the thickness of BaTiO<sub>3</sub>increases. Our study raises the prospect of designing artificial oxide superlattices on silicon with tailored functionalities. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000741852200073 |
Publication Date |
2022-01-11 |
|
| |
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 |
11 |
Open Access |
OpenAccess |
|
| |
Notes |
This project has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement No 823717—ESTEEM3. B.C. is sponsored by Shanghai Sailing Program 21YF1410700. J.V. and N.G. acknowledge funding through the GOA project “Solarpaint” of the University of Antwerp. The microscope used in this work was partly funded by the Hercules Fund from the Flemish Government. D.J. acknowledges funding from FWO Project G093417N from the Flemish fund for scientific research. M.T., N.S., M.F.S. and M.F. acknowledge the financial support by the EU European Research Council (Advanced Grant 694955—INSEETO). M.T. acknowledges the Swiss National Science Foundation under Project No. 200021-188414. N.S. acknowledges support under the Swiss National Science Foundation under Project No. P2EZP2-199913. M.S. acknowledges funding from Slovenian Research Agency (Grants No. J2-2510, N2-0149 and P2-0091). B.C. acknowledges Prof. C.D.; Prof. F.Y.; Prof. B.T. and Dr. K.J. for valuable discussions.; esteem3reported; esteem3TA |
Approved |
Most recent IF: 16.6 |
|
| |
Call Number |
EMAT @ emat @c:irua:185179 |
Serial |
6902 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Lopez-Garcia, C.; Canossa, S.; Hadermann, J.; Gorni, G.; Oropeza, F.E.; de la Pena O'Shea, V.A.; Iglesias, M.; Monge, M.A.; Gutierrez-Puebla, E.; Gandara, F. |
|
| |
Title |
Heterometallic molecular complexes act as messenger building units to encode desired metal-atom combinations to multivariate metal-organic frameworks |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
Journal of the American Chemical Society |
Abbreviated Journal |
J Am Chem Soc |
|
| |
Volume |
144 |
Issue |
36 |
Pages |
16262-16266 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
A novel synthetic approach is described for the targeted preparation of multivariate metal-organic frameworks (MTV-MOFs) with specific combinations of metal elements. This methodology is based on the use of molecular complexes that already comprise desired metal-atom combinations, as building units for the MTV-MOF synthesis. These units are transformed into the MOF structural constituents through a ligand/linker exchange process that involves structural modifications while preserving their origina l l y encoded atomic combination. Thus, through the use of heterometalli c ring-shaped molecules combining gallium and nickel or cobalt, we have obtained MOFs with identical combinations of the metal elements, now incorporated in the rod-shaped secondary building unit, as confirmed with a combination of X-ray and electron diffraction, electron microscopy, and X-ray absorption spectroscopy techniques. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000841435900001 |
Publication Date |
2022-08-12 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
0002-7863 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
15 |
Times cited |
|
Open Access |
OpenAccess |
|
| |
Notes |
|
Approved |
Most recent IF: 15 |
|
| |
Call Number |
UA @ admin @ c:irua:190023 |
Serial |
7169 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Zhang, Y.; Qin, S.; Claes, N.; Schilling, W.; Sahoo, P.K.; Ching, H.Y.V.; Jaworski, A.; Lemière, F.; Slabon, A.; Van Doorslaer, S.; Bals, S.; Das, S. |
|
| |
Title |
Direct Solar Energy-Mediated Synthesis of Tertiary Benzylic Alcohols Using a Metal-Free Heterogeneous Photocatalyst |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
ACS Sustainable Chemistry and Engineering |
Abbreviated Journal |
Acs Sustain Chem Eng |
|
| |
Volume |
10 |
Issue |
1 |
Pages |
530-540 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Organic synthesis (ORSY) |
|
| |
Abstract |
Direct hydroxylation via the functionalization of tertiary benzylic C(sp3)-H bond is of great significance for obtaining tertiary alcohols which find wide applications in pharmaceuticals as well as in fine chemical industries. However, current synthetic procedures use toxic reagents and therefore, the development of a sustainable strategy for the synthesis of tertiary benzyl alcohols is highly desirable. To solve this problem, herein, we report a metal-free
heterogeneous photocatalyst to synthesize the hydroxylated products using oxygen as the key reagent. Various benzylic substrates were employed into our mild reaction conditions to afford the desirable products in good to excellent yields. More importantly, gram-scale reaction was achieved via harvesting direct solar energy and exhibited high quantity of the product. The high stability of the catalyst was proved via recycling the catalyst and spectroscopic analyses. Finally, a possible mechanism was proposed based on the EPR and other experimental
evidence. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000736518000001 |
Publication Date |
2022-01-10 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
2168-0485 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
8.4 |
Times cited |
24 |
Open Access |
OpenAccess |
|
| |
Notes |
We thank BOF joint PhD grant (to Y. Z.), Francqui Foundation and FWO research grant (to S.D.), Chinese Scholarship Council (to Y.Z.). A.S. would like to thank the Swedish Energy Agency for financial support (project nr: 5050-1). The SEM microscope was partly funded by the Hercules Fund from the Flemish Government. |
Approved |
Most recent IF: 8.4 |
|
| |
Call Number |
EMAT @ emat @c:irua:184744 |
Serial |
6900 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Spaeth, P.; Adhikari, S.; Heyvaert, W.; Zhuo, X.; Garcia, I.; Liz-Marzan, L.M.; Bals, S.; Orrit, M.; Albrecht, W. |
|
| |
Title |
Photothermal circular dichroism measurements of single chiral gold nanoparticles correlated with electron tomography |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
ACS Photonics |
Abbreviated Journal |
Acs Photonics |
|
| |
Volume |
9 |
Issue |
12 |
Pages |
3995-4004 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
Chemically synthesized metal nanoparticles with morphological chiral features are known to exhibit strong circular dichroism. However, we still lack understanding of the correlation between morphological and chiroptical features of plasmonic nanoparticles. To shed light on that question, single nanoparticle experiments are required. We performed photothermal circular dichroism measurements of single chiral and achiral gold nanoparticles and correlated the chiroptical response to the 3D morphology of the same nanoparticles retrieved by electron tomography. In contrast to an ensemble measurement, we show that individual particles within the ensemble display a broad distribution of strength and handedness of circular dichroism signals. Whereas obvious structural chiral features, such as helical wrinkles, translate into chiroptical ones, nanoparticles with less obvious chiral morphological features can also display strong circular dichroism signals. Interestingly, we find that even seemingly achiral nanoparticles can display large g-factors. The origin of this circular dichroism signal is discussed in terms of plasmonics and other potentially relevant factors. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000884432100001 |
Publication Date |
2022-11-08 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
2330-4022 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
7 |
Times cited |
5 |
Open Access |
OpenAccess |
|
| |
Notes |
This work was supported by The Netherlands Organisation for Scientific Research (NWO) as part of the Open Technology Program (OTP, Project No. 16008) and by a Spinoza prize (M.O.) . W.A. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020 Program (Grant No. 797153, SOPMEN) . L.M.L.M. acknowledges funding from MCIN/AEI/10.13039/501100011033 (Grants PID2020-117779RB-I00 and MDM-2017-0720) . We thank Dr. Wolfgang L?fer for providing optical equipment. We also acknowledge the European Soft Matter Infrastructure (EUSMI: E201200468) . |
Approved |
Most recent IF: 7 |
|
| |
Call Number |
UA @ admin @ c:irua:192098 |
Serial |
7331 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Ehirim, T.J.; Ozoemena, O.C.; Mwonga, P.V.; Haruna, A.B.; Mofokeng, T.P.; De Wael, K.; Ozoemena, K.I. |
|
| |
Title |
Onion-like carbons provide a favorable electrocatalytic platform for the sensitive detection of tramadol drug |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
ACS Omega |
Abbreviated Journal |
|
|
| |
Volume |
7 |
Issue |
51 |
Pages |
47892-47905 |
|
| |
Keywords |
A1 Journal article; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab) |
|
| |
Abstract |
This work reports the first study on the possible application of nanodiamond-derived onion-like carbons (OLCs), in comparison with conductive carbon black (CB), as an electrode platform for the electrocatalytic detection of tramadol (an important drug of abuse). The physicochemical properties of OLCs and CB were determined using X-ray diffraction (XRD), Raman, scanning electron microscopy (SEM), Brunauer-Emmett-Teller (BET), and thermogravimetric analysis (TGA). The OLC exhibits, among others, higher surface area, more surface defects, and higher thermal stability than CB. From the electrochemical analysis (interrogated using cyclic voltammetry, differential pulse voltammetry, and electrochemical impedance spectroscopy), it is shown that an OLC-modified glassy carbon electrode (GCE-OLC) allows faster electron transport and electrocatalysis toward tramadol compared to a GCE-CB. To establish the underlying science behind the high performance of the OLC, theoretical calculations (density functional theory (DFT) simulations) were conducted. DFT predicts that OLC allows for weaker surface binding of tramadol (Ead = -26.656 eV) and faster kinetic energy (K.E. = -155.815 Ha) than CB (Ead = -40.174 eV and -305.322 Ha). The GCE-OLC shows a linear calibration curve for tramadol over the range of similar to 55 to 392 mu M, with high sensitivity (0.0315 mu A/mu M) and low limit of detection (LoD) and quantification (LoQ) (3.8 and 12.7 mu M, respectively). The OLC-modified screen-printed electrode (SPE-OLC) was successfully applied for the sensitive detection of tramadol in real pharmaceutical formulations and human serum. The OLC-based electrochemical sensor promises to be useful for the sensitive and accurate detection of tramadol in clinics, quality control, and routine quantification of tramadol drugs in pharmaceutical formulations. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000903165200001 |
Publication Date |
2022-12-15 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
2470-1343 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
|
Times cited |
|
Open Access |
OpenAccess |
|
| |
Notes |
|
Approved |
no |
|
| |
Call Number |
UA @ admin @ c:irua:193391 |
Serial |
8908 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Zhuo, X.; Mychinko, M.; Heyvaert, W.; Larios, D.; Obelleiro-Liz, M.; Taboada, J.M.; Bals, S.; Liz-Marzán, L.M. |
|
| |
Title |
Morphological and Optical Transitions during Micelle-Seeded Chiral Growth on Gold Nanorods |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
|
| |
Volume |
|
Issue |
|
Pages |
|
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
Chiral plasmonics is a rapidly developing field where breakthroughs and unsolved problems coexist. We have recently reported binary surfactant-assisted seeded growth of chiral gold nanorods (Au NRs) with high chiroptical activity. Such a seeded-growth process involves the use of a chiral cosurfactant that induces micellar helicity, in turn driving the transition from achiral to chiral Au NRs, from both the morphological and the optical points of view. We report herein a detailed study on both transitions, which reveals intermediate states that were hidden so far. The correlation between structure and optical response is carefully analyzed, including the (linear and CD) spectral evolution over time, electron tomography, the impact of NR dimensions on their optical response, the variation of the absorption-to-scattering ratio during the evolution from achiral to chiral Au NRs, and the near-field enhancement related to chiral plasmon modes. Our findings provide further understanding of the growth process of chiral Au NRs and the associated optical changes, which will facilitate further study and applications of chiral nanomaterials. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000878324400001 |
Publication Date |
2022-10-26 |
|
| |
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 |
17 |
Open Access |
OpenAccess |
|
| |
Notes |
This work was supported by the European Research Council (ERC-AdG-4DbioSERS-787510 to L.M.L.-M. and ERC-CoG-REALNANO-815128 to S.B.) and the MCIN/AEI/10.13039/501100011033 (Grant PID2020-117779RB-I00). X.Z. acknowledges funding from the Juan de la Cierva fellowship (FJC2018-036104-I) and the University Development Fund (UDF01002665, CUHK-Shenzhen). D.L., M.O.-L., and J.M.T. acknowledge funding from the European Regional Development Fund (ERDF) and the Spanish Ministerio de Ciencia, Innovación y Universidades, under Projects PID2020-116627RB-C21 and PID2020-116627RB-C22, as well as from the ERDF/Galician Regional Government as part of the agreement for funding the Atlantic Research Center for Information and Communication Technologies (atlanTTic) and ERDF/Extremadura Regional Government under Projects IB18073 and GR18055. This work was performed in the framework of the Maria de Maeztu Units of Excellence Program from the Spanish State Research Agency (Grant No. MDM-2017-0720). The authors acknowledge Dr. Guillermo González-Rubio for providing suggestions for synthesis and Dr. Irantzu Llarena for assisting with the CD measurements. |
Approved |
Most recent IF: 17.1 |
|
| |
Call Number |
EMAT @ emat @c:irua:191815 |
Serial |
7116 |
|
| 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. |
|
| |
Address |
|
|
| |
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 |
Pedrazo-Tardajos, A.; Arslan Irmak, E.; Kumar, V.; Sánchez-Iglesias, A.; Chen, Q.; Wirix, M.; Freitag, B.; Albrecht, W.; Van Aert, S.; Liz-Marzán, L.M.; Bals, S. |
|
| |
Title |
Thermal Activation of Gold Atom Diffusion in Au@Pt Nanorods |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
|
| |
Volume |
|
Issue |
|
Pages |
|
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
Understanding the thermal stability of bimetallic nanoparticles is of vital importance to preserve their functionalities during their use in a variety of applications. In contrast to well-studied bimetallic systems such as Au@Ag, heat-induced morphological and compositional changes in Au@Pt nanoparticles are insufficiently understood, even though Au@Pt is an important material for catalysis. To investigate the thermal instability of Au@Pt nanorods at temperatures below their bulk melting point, we combined in situ heating with two- and three-dimensional electron microscopy techniques, including three-dimensional energy-dispersive X-ray spectroscopy. The experimental results were used as input for molecular dynamics simulations, to unravel the mechanisms behind the morphological transformation of Au@Pt core–shell nanorods. We conclude that thermal stability is influenced not only by the degree of coverage of Pt on Au but also by structural details of the Pt shell. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000819246800001 |
Publication Date |
2022-06-10 |
|
| |
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 |
8 |
Open Access |
OpenAccess |
|
| |
Notes |
S.B., S.V.A., L.M.L.-M. and A.P.-T. acknowledge financial support from the European Commission under the Horizon 2020 Programme by grant nos. 731019 (EUSMI) and 823717 (ESTEEM3) and ERC Consolidator grant nos. 815128 (REALNANO) and 770887 (PICOMETRICS). L.M.L.-M. acknowledges funding from MCIN/AEI/10.13039/501100011033 through grants no. PID2020-117779RB-I00 and Maria de Maeztu Unit of Excellence no. MDM-2017-0720. The authors acknowledge the resources and services used for the simulations in this work were provided by the VSC (Flemish Supercomputer Center), funded by the Research Foundation – Flanders (FWO) and the Flemish Government.; esteem3reported; esteem3JRA |
Approved |
Most recent IF: 17.1 |
|
| |
Call Number |
EMAT @ emat @c:irua:188540 |
Serial |
7072 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Choo, P.; Arenas-Esteban, D.; Jung, I.; Chang, W.J.; Weiss, E.A.; Bals, S.; Odom, T.W. |
|
| |
Title |
Investigating Reaction Intermediates during the Seedless Growth of Gold Nanostars Using Electron Tomography |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
|
| |
Volume |
16 |
Issue |
3 |
Pages |
4408-4414 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
Good’s buffers can act both as nucleating and shape- directing agents during the synthesis of anisotropic gold nanostars (AuNS). Although different Good’s buffers can produce AuNS shapes with branches that are oriented along specific crystallographic directions, the mechanism is not fully understood. This paper reports how an analysis of the intermediate structures during AuNS synthesis from HEPES, EPPS, and MOPS Good’s buffers can provide insight into the formation of seedless AuNS. Electron tomography of AuNS structures quenched at early times (minutes) was used to characterize the morphology of the incipient seeds, and later times were used to construct the growth maps. Through this approach, we identified how the crystallinity and shape of the first structures synthesized with different Good’s buffers determine the final AuNS morphologies. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000780214300084 |
Publication Date |
2022-03-22 |
|
| |
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 |
12 |
Open Access |
OpenAccess |
|
| |
Notes |
This work was supported by the National Science Foundation (NSF) under award NSF CHE-1808502 (P.C. and I.J.). This work made use of the EPIC facility of Northwestern University’s NUANCE Center, which has received support from the SHyNE Resource (NSF ECCS-2025633), the IIN, and Northwestern’s MRSEC program (NSF DMR-1720139). D.A E. and S.B. acknowledge funding from the European Research Council under the European Union’s Horizon 2020 research and innovation program (ERC Consolidator Grants No. 815128 REALNANO and Grant Agreement No. 731019 EUSMI).; sygmaSB |
Approved |
Most recent IF: 17.1 |
|
| |
Call Number |
EMAT @ emat @c:irua:187930 |
Serial |
7055 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Heyvaert, W.; Pedrazo-Tardajos, A.; Kadu, A.; Claes, N.; González-Rubio, G.; Liz-Marzán, L.M.; Albrecht, W.; Bals, S. |
|
| |
Title |
Quantification of the Helical Morphology of Chiral Gold Nanorods |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
ACS materials letters |
Abbreviated Journal |
ACS Materials Lett. |
|
| |
Volume |
4 |
Issue |
|
Pages |
642-649 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
Chirality in inorganic nanoparticles and nanostructures has gained increasing scientific interest, because of the possibility to tune their ability to interact differently with left- and right-handed circularly polarized light. In some cases, the optical activity is hypothesized to originate from a chiral morphology of the nanomaterial. However, quantifying the degree of chirality in objects with sizes of tens of nanometers is far from straightforward. Electron tomography offers the possibility to faithfully retrieve the three-dimensional morphology of nanomaterials, but only a qualitative interpretation of the morphology of chiral nanoparticles has been possible so far. We introduce herein a methodology that enables us to quantify the helicity of complex chiral nanomaterials, based on the geometrical properties of a helix. We demonstrate that an analysis at the single particle level can provide significant insights into the origin of chiroptical properties. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000784490000013 |
Publication Date |
2022-03-08 |
|
| |
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 |
11 |
Open Access |
OpenAccess |
|
| |
Notes |
S.B. and A.P.-T. gratefully acknowledge funding by the European Research Council (ERC Consolidator Grant #815128-REALNANO) the European Union’s Horizon 2020 research and innovation program under grant agreement #823717ESTEEM3. L.M.L.-M. acknowledges funding from MCIN/ AEI /10.13039/501100011033, grant # PID2020- 117779RB-I00 and the Maria de Maeztu Units of Excellence Program from the Spanish State Research Agency (Grant No. MDM-2017-0720). G.G.-R. thanks the Spanish Spanish Ministerio de Ciencia e Innovación for an FPI (BES-2014- 068972) fellowship.; SygmaSB; esteem3reported; esteem3jra |
Approved |
Most recent IF: NA |
|
| |
Call Number |
EMAT @ emat @c:irua:186959 |
Serial |
6956 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Faust, V.; Gruber, W.; Ganigue, R.; Vlaeminck, S.E.; Udert, K.M. |
|
| |
Title |
Nitrous oxide emissions and carbon footprint of decentralized urine fertilizer production by nitrification and distillation |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
ACS ES&T engineering |
Abbreviated Journal |
|
|
| |
Volume |
2 |
Issue |
9 |
Pages |
1745-1755 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL) |
|
| |
Abstract |
Combining partial nitrification, granular activated carbon (GAC) filtration, and distillation is a well-studied approach to convert urine into a fertilizer. To evaluate the environmental sustainability of a technology, the operational carbon footprint and therefore nitrous oxide (N2O) emissions should be known, but N2O emissions from urine nitrification have not been assessed yet. Therefore, N2O emissions of a decentralized urine nitrification reactor were monitored for 1 month. During nitrification, 0.4-1.2% of the total nitrogen load was emitted as N2O-N with an average N2O emission factor (EFN2O) of 0.7%. Additional N2O was produced during anoxic storage between nitrification and GAC filtration with an estimated EFN2O of 0.8%, resulting in an EFN2O of 1.5% for the treatment chain. N2O emissions during nitrification can be mitigated by 60% by avoiding low dissolved oxygen or anoxic conditions and nitrite concentrations above 5 mg-N L-1. Minimizing the hydraulic retention time between nitrification and GAC filtration can reduce N2O formation during intermediate storage by 100%. Overall, the N2O emissions accounted for 45% of the operational carbon footprint of 14 kg-CO2,equiv kg-N-1 for urine fertilizer production. Using electricity from renewable sources and applying the proposed N2O mitigation strategies could potentially lower the carbon footprint by 85%. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000835412700001 |
Publication Date |
2022-07-29 |
|
| |
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:189599 |
Serial |
7182 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Yang, S.; Liu, Z.; An, H.; Arnouts, S.; de Ruiter, J.; Rollier, F.; Bals, S.; Altantzis, T.; Figueiredo, M.C.; Filot, I.A.W.; Hensen, E.J.M.; Weckhuysen, B.M.; van der Stam, W. |
|
| |
Title |
Near-unity electrochemical CO₂ to CO conversion over Sn-doped copper oxide nanoparticles |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
ACS catalysis |
Abbreviated Journal |
Acs Catal |
|
| |
Volume |
12 |
Issue |
24 |
Pages |
15146-15156 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
|
| |
Abstract |
Bimetallic electrocatalysts have emerged as a viable strategy to tune the electrocatalytic CO2 reduction reaction (eCO2RR) for the selective production of valuable base chemicals and fuels. However, obtaining high product selectivity and catalyst stability remain challenging, which hinders the practical application of eCO2RR. In this work, it was found that a small doping concentration of tin (Sn) in copper oxide (CuO) has profound influence on the catalytic performance, boosting the Faradaic efficiency (FE) up to 98% for carbon monoxide (CO) at -0.75 V versus RHE, with prolonged stable performance (FE > 90%) for up to 15 h. Through a combination of ex situ and in situ characterization techniques, the in situ activation and reaction mechanism of the electrocatalyst at work was elucidated. In situ Raman spectroscopy measurements revealed that the binding energy of the crucial adsorbed *CO intermediate was lowered through Sn doping, thereby favoring gaseous CO desorption. This observation was confirmed by density functional theory, which further indicated that hydrogen adsorption and subsequent hydrogen evolution were hampered on the Sn-doped electrocatalysts, resulting in boosted CO formation. It was found that the pristine electrocatalysts consisted of CuO nanoparticles decorated with SnO2 domains, as characterized by ex situ high-resolution scanning transmission electron microscopy and X-ray photoelectron spectroscopy measurements. These pristine nanoparticles were subsequently in situ converted into a catalytically active bimetallic Sn-doped Cu phase. Our work sheds light on the intimate relationship between the bimetallic structure and catalytic behavior, resulting in stable and selective oxide-derived Sn-doped Cu electrocatalysts. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000900052400001 |
Publication Date |
2022-11-28 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
2155-5435 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
12.9 |
Times cited |
16 |
Open Access |
OpenAccess |
|
| |
Notes |
B.M.W., S.Y., M.C.F., E.J.M.H., and W.v.d.S. acknowledge support from the Strategic UU-TU/e Alliance project ?Joint Centre for Chemergy Research?. S.B. acknowledges support from the European Research Council (ERC Consolidator grant #815128 REALNANO) . Z.L. acknowledges financial support of the China Scholarship Council and the Netherlands Organization for Scientific Research for access to computa-tional resources for carrying out the DFT calculations reported in this work. S.A. and T.A. acknowledge funding from theUniversity of Antwerp Research fund (BOF) . The authors also thank Dr. Jochem Wijten and Joris Janssens (Inorganic Chemistry and Catalysis, Utrecht University) for helpful technical support. Sander Deelen (Faculty of Science, Utrecht University) is acknowledged for the design of the in situ XRD cell. |
Approved |
Most recent IF: 12.9 |
|
| |
Call Number |
UA @ admin @ c:irua:192742 |
Serial |
7325 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Nematollahi, P.; Barbiellini, B.; Bansil, A.; Lamoen, D.; Qingying, J.; Mukerjee, S.; Neyts, E.C. |
|
| |
Title |
Identification of a Robust and Durable FeN4CxCatalyst for ORR in PEM Fuel Cells and the Role of the Fifth Ligand |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
ACS catalysis |
Abbreviated Journal |
Acs Catal |
|
| |
Volume |
|
Issue |
|
Pages |
7541-7549 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
|
| |
Abstract |
Although recent studies have advanced the understanding of pyrolyzed
Fe−N−C materials as oxygen reduction reaction (ORR) catalysts, the atomic and
electronic structures of the active sites and their detailed reaction mechanisms still remain unknown. Here, based on first-principles density functional theory (DFT) computations, we discuss the electronic structures of three FeN4 catalytic centers with different local topologies of the surrounding C atoms with a focus on unraveling the mechanism of their ORR activity in acidic electrolytes. Our study brings back a forgotten, synthesized pyridinic Fe−N coordinate to the community’s attention, demonstrating that this catalyst can exhibit excellent activity for promoting direct four-electron ORR through the addition of a fifth ligand such as −NH2, −OH, and −SO4. We also identify sites with good stability properties through the combined use of our DFT calculations and Mössbauer spectroscopy data. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000823193100001 |
Publication Date |
2022-06-10 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
2155-5435 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
12.9 |
Times cited |
|
Open Access |
OpenAccess |
|
| |
Notes |
Basic Energy Sciences, DE-FG02-07ER46352 ; Fonds Wetenschappelijk Onderzoek, 1261721N ; Opetus- ja Kulttuuriministeri?; Department of Energy, DE-EE0008416 ; |
Approved |
Most recent IF: 12.9 |
|
| |
Call Number |
EMAT @ emat @c:irua:189000 |
Serial |
7073 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Cui, Z.; Meng, S.; Yi, Y.; Jafarzadeh, A.; Li, S.; Neyts, E.C.; Hao, Y.; Li, L.; Zhang, X.; Wang, X.; Bogaerts, A. |
|
| |
Title |
Plasma-catalytic methanol synthesis from CO₂ hydrogenation over a supported Cu cluster catalyst : insights into the reaction mechanism |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
Acs Catalysis |
Abbreviated Journal |
Acs Catal |
|
| |
Volume |
12 |
Issue |
2 |
Pages |
1326-1337 |
|
| |
Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
|
| |
Abstract |
Plasma-catalytic CO, hydrogenation for methanol production is gaining increasing interest, but our understanding of its reaction mechanism remains primitive. We present a combined experimental/computational study on plasma-catalytic CO, hydrogenation to CH3OH over a size-selected Cu/gamma-Al2O3 catalyst. Our experiments demonstrate a synergistic effect between the Cu/gamma-Al2O3 catalyst and the CO2/H-2 plasma, achieving a CO2 conversion of 10% at 4 wt % Cu loading and a CH3OH selectivity near 50% further rising to 65% with H2O addition (for a H2O/CO2 ratio of 1). Furthermore, the energy consumption for CH3OH production was more than 20 times lower than with plasma only. We carried out density functional theory calculations over a Cu-13/gamma-Al2O3 model, which reveal that the interfacial sites of the Cu-13 cluster and gamma-Al2O3 support show a bifunctional effect: they not only activate the CO2 molecules but also strongly adsorb key intermediates to promote their hydrogenation further. Reactive plasma species can regulate the catalyst surface reactions via the Eley-Rideal (E-R) mechanism, which accelerates the hydrogenation process and promotes the generation of the key intermediates. H2O can promote the CH3OH desorption by competitive adsorption over the Cu-13/gamma-Al2O3 surface. This study provides new insights into CO2 hydrogenation through plasma catalysis, and it provides inspiration for the conversion of some other small molecules (CH4, N-2, CO, etc.) by plasma catalysis using supported-metal clusters. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000742735600001 |
Publication Date |
2022-01-07 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
2155-5435 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
12.9 |
Times cited |
|
Open Access |
OpenAccess |
|
| |
Notes |
|
Approved |
Most recent IF: 12.9 |
|
| |
Call Number |
UA @ admin @ c:irua:186416 |
Serial |
7192 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Borah, R.; Smets, J.; Ninakanti, R.; Tietze, M.L.; Ameloot, R.; Chigrin, D.N.; Bals, S.; Lenaerts, S.; Verbruggen, S.W. |
|
| |
Title |
Self-assembled ligand-capped plasmonic Au nanoparticle films in the Kretschmann configuration for sensing of volatile organic compounds |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
ACS applied nano materials |
Abbreviated Journal |
|
|
| |
Volume |
5 |
Issue |
8 |
Pages |
acsanm.2c02524-12 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Sustainable Energy, Air and Water Technology (DuEL) |
|
| |
Abstract |
Films of close-packed Au nanoparticles are coupled electrodynamically through their collective plasmon resonances. This collective optical response results in enhanced light–matter interactions, which can be exploited in various applications. Here, we demonstrate their application in sensing volatile organic compounds, using methanol as a test case. Ordered films over several cm2 were obtained by interfacial self-assembly of colloidal Au nanoparticles (∼10 nm diameter) through controlled evaporation of the solvent. Even though isolated nanoparticles of this size are inherently nonscattering, when arranged in a close-packed film the plasmonic coupling results in a strong reflectance and absorbance. The in situ tracking of vapor phase methanol concentration through UV–vis transmission measurements of the nanoparticle film is first demonstrated. Next, in situ ellipsometry of the self-assembled films in the Kretschmann (also known as ATR) configuration is shown to yield enhanced sensitivity, especially with phase difference measurements, Δ. Our study shows the excellent agreement between theoretical models of the spectral response of self-assembled films with experimental in situ sensing experiments. At the same time, the theoretical framework provides the basis for the interpretation of the various observed experimental trends. Combining periodic nanoparticle films with ellipsometry in the Kretschmann configuration is a promising strategy toward highly sensitive and selective plasmonic thin-film devices based on colloidal fabrication methods for volatile organic compound (VOC) sensing applications. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000834348300001 |
Publication Date |
2022-07-27 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
2574-0970 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
5.9 |
Times cited |
11 |
Open Access |
OpenAccess |
|
| |
Notes |
R.B. acknowledges financial support from the University of Antwerp Special Research Fund (BOF) for a DOCPRO4 doctoral scholarship. J.S. acknowledges financial support from the Research Foundation Flanders (FWO) by a Ph.D. fellowship (11H8121N) . M.L.T. acknowledges financial support from the Research Foundation Flanders (FWO) by a senior postdoctoral fellowship (12ZK720N) . |
Approved |
Most recent IF: 5.9 |
|
| |
Call Number |
UA @ admin @ c:irua:189295 |
Serial |
7095 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Pacquets, L.; Van den Hoek, J.; Arenas Esteban, D.; Ciocarlan, R.-G.; Cool, P.; Baert, K.; Hauffman, T.; Daems, N.; Bals, S.; Breugelmans, T. |
|
| |
Title |
Use of nanoscale carbon layers on Ag-based gas diffusion electrodes to promote CO production |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
ACS applied nano materials |
Abbreviated Journal |
|
|
| |
Volume |
5 |
Issue |
6 |
Pages |
7723-7732 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Applied Electrochemistry & Catalysis (ELCAT) |
|
| |
Abstract |
A promising strategy for the inhibition of the hydrogen evolution reaction along with the stabilization of the electrocatalyst in electrochemical CO2 reduction cells involves the application of a nanoscale amorphous carbon layer on top of the active catalyst layer in a gas diffusion electrode. Without modifying the chemical nature of the electrocatalyst itself, these amorphous carbon layers lead to the stabilization of the electrocatalyst, and a significant improvement with respect to the inhibition of the hydrogen evolution reaction was also obtained. The faradaic efficiencies of hydrogen could be reduced from 31.4 to 2.1% after 1 h of electrolysis with a 5 nm thick carbon layer. Furthermore, the impact of the carbon layer thickness (5–30 nm) on this inhibiting effect was investigated. We determined an optimal thickness of 15 nm where the hydrogen evolution reaction was inhibited and a decent stability was obtained. Next, a thickness of 15 nm was selected for durability measurements. Interestingly, these durability measurements revealed the beneficial impact of the carbon layer already after 6 h by suppressing the hydrogen evolution such that an increase of only 37.9% exists compared to 56.9% without the use of an additional carbon layer, which is an improvement of 150%. Since carbon is only applied afterward, it reveals its great potential in terms of electrocatalysis in general. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000818507900001 |
Publication Date |
2022-05-19 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
2574-0970 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
5.9 |
Times cited |
3 |
Open Access |
OpenAccess |
|
| |
Notes |
L.P. was supported through a Ph.D. fellowship strategic basic research (1S56920N) of the Research Foundation-Flanders (FWO). S.B. acknowledges financial support from ERC Consolidator Grant Number 815128 REALNANO. This research was financed by the Research Council of the University of Antwerp (BOF-GOA 33928). P.C. and R.-G.C. acknowledge financial support by FWO Flanders (project no. G038215N). The authors recognize the contribution of S. Pourbabak and T. Derez for the assistance with the Ag and carbon coating, Indah Prihatiningtyas and Bart Van der Bruggen for the assistance with the contact angle measurements, Daniel Choukroun for the use of the in-house-made hybrid flow cell, and Stijn Van den Broeck for his assistance with the FIB measurements. |
Approved |
Most recent IF: 5.9 |
|
| |
Call Number |
UA @ admin @ c:irua:188887 |
Serial |
7099 |
|
| Permanent link to this record |
