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Author |
Hugenschmidt, M.; Jannis, D.; Kadu, A.A.; Grünewald, L.; De Marchi, S.; Perez-Juste, J.; Verbeeck, J.; Van Aert, S.; Bals, S. |
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Title |
Low-dose 4D-STEM tomography for beam-sensitive nanocomposites |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
ACS materials letters |
Abbreviated Journal |
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Volume |
6 |
Issue |
1 |
Pages |
165-173 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Electron tomography is essential for investigating the three-dimensional (3D) structure of nanomaterials. However, many of these materials, such as metal-organic frameworks (MOFs), are extremely sensitive to electron radiation, making it difficult to acquire a series of projection images for electron tomography without inducing electron-beam damage. Another significant challenge is the high contrast in high-angle annular dark field scanning transmission electron microscopy that can be expected for nanocomposites composed of a metal nanoparticle and an MOF. This strong contrast leads to so-called metal artifacts in the 3D reconstruction. To overcome these limitations, we here present low-dose electron tomography based on four-dimensional scanning transmission electron microscopy (4D-STEM) data sets, collected using an ultrafast and highly sensitive direct electron detector. As a proof of concept, we demonstrate the applicability of the method for an Au nanostar embedded in a ZIF-8 MOF, which is of great interest for applications in various fields, including drug delivery. |
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Wos  |
001141178500001 |
Publication Date |
2023-12-11 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2639-4979 |
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Additional Links |
UA library record; WoS full record |
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Times cited |
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Open Access |
Not_Open_Access |
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Notes |
This work was supported by the European Research Council (Grant 815128 REALNANO to S.B., Grant 770887 PICOMETRICS to S.V.A.). J.P.-J. and S.M. acknowledge financial support from the MCIN/AEI/10.13039/501100011033 (Grants No. PID2019-108954RB-I00) and EU Horizon 2020 research and innovation program under grant agreement no. 883390 (SERSing). J.V., S.B., S.V.A., and L.G. acknowledge funding from the Flemish government (iBOF-21-085 PERsist). |
Approved |
no |
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Call Number |
UA @ admin @ c:irua:202771 |
Serial |
9053 |
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Author |
Johnson, G.; Yang, M.Y.; Liu, C.; Zhou, H.; Zuo, X.; Dickie, D.A.; Wang, S.; Gao, W.; Anaclet, B.; Perras, F.A.; Ma, F.; Zeng, C.; Wang, D.; Bals, S.; Dai, S.; Xu, Z.; Liu, G.; Goddard III, W.A.; Zhang, S. |
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Title |
Nanocluster superstructures assembled via surface ligand switching at high temperature |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Nature synthesis |
Abbreviated Journal |
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Volume |
2 |
Issue |
9 |
Pages |
828-837 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Superstructures with nanoscale building blocks, when coupled with precise control of the constituent units, open opportunities in rationally designing and manufacturing desired functional materials. Yet, synthetic strategies for the large-scale production of superstructures are scarce. We report a scalable and generalized approach to synthesizing superstructures assembled from atomically precise Ce24O28(OH)8 and other rare-earth metal-oxide nanoclusters alongside a detailed description of the self-assembly mechanism. Combining operando small-angle X-ray scattering, ex situ molecular and structural characterizations, and molecular dynamics simulations indicates that a high-temperature ligand-switching mechanism, from oleate to benzoate, governs the formation of the nanocluster assembly. The chemical tuning of surface ligands controls superstructure disassembly and reassembly, and furthermore, enables the synthesis of multicomponent superstructures. This synthetic approach, and the accurate mechanistic understanding, are promising for the preparation of superstructures for use in electronics, plasmonics, magnetics and catalysis. Synthesizing superstructures with precisely controlled nanoscale building blocks is challenging. Here the assembly of superstructures is reported from atomically precise Ce24O28(OH)8 and other rare-earth metal-oxide nanoclusters and their multicomponent combinations. A high-temperature ligand-switching mechanism controls the self-assembly. |
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Wos |
001124824000001 |
Publication Date |
2023-05-01 |
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Edition |
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ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
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Times cited |
2 |
Open Access |
Not_Open_Access |
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no |
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Call Number |
UA @ admin @ c:irua:202180 |
Serial |
9060 |
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Author |
Teunissen, J.L.; Braeckevelt, T.; Skvortsova, I.; Guo, J.; Pradhan, B.; Debroye, E.; Roeffaers, M.B.J.; Hofkens, J.; Van Aert, S.; Bals, S.; Rogge, S.M.J.; Van Speybroeck, V. |
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Title |
Additivity of Atomic Strain Fields as a Tool to Strain-Engineering Phase-Stabilized CsPbI3Perovskites |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
The Journal of Physical Chemistry C |
Abbreviated Journal |
J. Phys. Chem. C |
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Volume |
127 |
Issue |
48 |
Pages |
23400-23411 |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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Abstract |
CsPbI3 is a promising perovskite material for photovoltaic applications in its photoactive perovskite or black phase. However, the material degrades to a photovoltaically inactive or yellow phase at room temperature. Various mitigation strategies are currently being developed to increase the lifetime of the black phase, many of which rely on inducing strains in the material that hinder the black-to-yellow phase transition. Physical insight into how these strategies exactly induce strain as well as knowledge of the spatial extent over which these strains impact the material is crucial to optimize these approaches but is still lacking. Herein, we combine machine learning potential-based molecular dynamics simulations with our in silico strain engineering approach to accurately quantify strained large-scale atomic structures on a nanosecond time scale. To this end, we first model the strain fields introduced by atomic substitutions as they form the most elementary strain sources. We demonstrate that the magnitude of the induced strain fields decays exponentially with the distance from the strain source, following a decay rate that is largely independent of the specific substitution. Second, we show that the total strain field induced by multiple strain sources can be predicted to an excellent approximation by summing the strain fields of each individual source. Finally, through a case study, we illustrate how this additive character allows us to explain how complex strain fields, induced by spatially extended strain sources, can be predicted by adequately combining the strain fields caused by local strain sources. Hence, the strain additivity proposed here can be adopted to further our insight into the complex strain behavior in perovskites and to design strain from the atomic level onward to enhance their sought-after phase stability. |
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Wos |
001116862000001 |
Publication Date |
2023-12-07 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
3.7 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
This work was supported by iBOF-21-085 PERsist (Special Research Fund of Ghent University, KU Leuven Research Fund, and the Research Fund of the University of Antwerp). S.M.J.R., T.B., and B.P. acknowledge financial support from the Research Foundation-Flanders (FWO) through two postdoctoral fellow- ships [grant nos. 12T3522N (S.M.J.R.) and 1275521N (B.P.)] and an SB-FWO fellowship [grant no. 1SC1319 (T.B.)]. E.D., M.B.J.R., and J.H. acknowledge financial support from the Research Foundation-Flanders (FWO, grant nos. G.0B39.15, G.0B49.15, G098319N, S002019N, S004322N, and ZW15_09- GOH6316). J.H. acknowledges support from the Flemish government through long-term structural funding Methusalem (CASAS2, Meth/15/04) and the MPI as an MPI fellow. S.V.A. and S.B. acknowledge financial support from the Research Foundation-Flanders (FWO, grant no. G0A7723N). S.M.J.R. and V.V.S. acknowledge funding from the Research Board of Ghent University (BOF). The computational resources and services used in this work were provided by the VSC (Flemish Supercomputer Center), funded by the Research Foundation- Flanders (FWO) and the Flemish Government�department EWI.; KU Leuven, iBOF-21-085 PERsist ; Universiteit Antwerpen, iBOF-21-085 PERsist ; Universiteit Gent, iBOF-21-085 PERsist ; Vlaamse regering, CASAS2, Meth/15/04 ; Fonds Wetenschappelijk Onderzoek, G.0B39.15 G098319N G.0B49.15 1SC1319 12T3522N ZW15 09-GOH6316 G0A7723N 1275521N S004322N S002019N ; |
Approved |
Most recent IF: 3.7; 2023 IF: 4.536 |
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Call Number |
EMAT @ emat @c:irua:202124 |
Serial |
8985 |
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Author |
Manzaneda-Gonzalez, V.; Jenkinson, K.; Pena-Rodriguez, O.; Borrell-Grueiro, O.; Trivino-Sanchez, S.; Banares, L.; Junquera, E.; Espinosa, A.; Gonzalez-Rubio, G.; Bals, S.; Guerrero-Martinez, A. |
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Title |
From multi- to single-hollow trimetallic nanocrystals by ultrafast heating |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Chemistry of materials |
Abbreviated Journal |
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Volume |
35 |
Issue |
22 |
Pages |
9603-9612 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Metal nanocrystals (NCs) display unique physicochemical features that are highly dependent on nanoparticle dimensions, anisotropy, structure, and composition. The development of synthesis methodologies that allow us to tune such parameters finely emerges as crucial for the application of metal NCs in catalysis, optical materials, or biomedicine. Here, we describe a synthetic methodology to fabricate hollow multimetallic heterostructures using a combination of seed-mediated growth routes and femtosecond-pulsed laser irradiation. The envisaged methodology relies on the coreduction of Ag and Pd ions on gold nanorods (Au NRs) to form Au@PdAg core-shell nanostructures containing small cavities at the Au-PdAg interface. The excitation of Au@PdAg NRs with low fluence femtosecond pulses was employed to induce the coalescence and growth of large cavities, forming multihollow anisotropic Au@PdAg nanostructures. Moreover, single-hollow alloy AuPdAg could be achieved in high yield by increasing the irradiation energy. Advanced electron microscopy techniques, energy-dispersive X-ray spectroscopy (EDX) tomography, X-ray absorption near-edge structure (XANES) spectroscopy, and finite differences in the time domain (FDTD) simulations allowed us to characterize the morphology, structure, and elemental distribution of the irradiated NCs in detail. The ability of the reported synthesis route to fabricate multimetallic NCs with unprecedented hollow nanostructures offers attractive prospects for the fabrication of tailored high-entropy alloy nanoparticles. |
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Wos |
001110623500001 |
Publication Date |
2023-11-06 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756; 1520-5002 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
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Times cited |
2 |
Open Access |
OpenAccess |
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Notes |
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no |
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Call Number |
UA @ admin @ c:irua:202144 |
Serial |
9040 |
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Author |
Jenkinson, K.; Spadaro, M.C.; Golovanova, V.; Andreu, T.; Morante, J.R.; Arbiol, J.; Bals, S. |
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Title |
Direct operando visualization of metal support interactions induced by hydrogen spillover during CO₂ hydrogenation |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Advanced materials |
Abbreviated Journal |
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Volume |
35 |
Issue |
51 |
Pages |
2306447-10 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
The understanding of catalyst active sites is a fundamental challenge for the future rational design of optimized and bespoke catalysts. For instance, the partial reduction of Ce4+ surface sites to Ce3+ and the formation of oxygen vacancies are critical for CO2 hydrogenation, CO oxidation, and the water gas shift reaction. Furthermore, metal nanoparticles, the reducible support, and metal support interactions are prone to evolve under reaction conditions; therefore a catalyst structure must be characterized under operando conditions to identify active states and deduce structure-activity relationships. In the present work, temperature-induced morphological and chemical changes in Ni nanoparticle-decorated mesoporous CeO2 by means of in situ quantitative multimode electron tomography and in situ heating electron energy loss spectroscopy, respectively, are investigated. Moreover, operando electron energy loss spectroscopy is employed using a windowed gas cell and reveals the role of Ni-induced hydrogen spillover on active Ce3+ site formation and enhancement of the overall catalytic performance. |
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Wos |
001106139400001 |
Publication Date |
2023-10-22 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0935-9648 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
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Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved |
no |
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Call Number |
UA @ admin @ c:irua:201143 |
Serial |
9022 |
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Author |
de la Croix, T.; Claes, N.; Eyley, S.; Thielemans, W.; Bals, S.; De Vos, D. |
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Title |
Heterogeneous Pt-catalyzed transfer dehydrogenation of long-chain alkanes with ethylene |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
Catalysis Science & Technology |
Abbreviated Journal |
Catal. Sci. Technol. |
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Volume |
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Issue |
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Pages |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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Abstract |
The dehydrogenation of long-chain alkanes to olefins and alkylaromatics is a challenging endothermic reaction, typically requiring harsh conditions which can lead to low selectivity and coking. More favorable thermodynamics can be achieved by using a hydrogen acceptor, such as ethylene. In this work, the potential of heterogeneous platinum catalysts for the transfer dehydrogenation of long-chain alkanes is investigated, using ethylene as a convenient hydrogen acceptor. Pt/C and Pt–Sn/C catalysts were prepared<italic>via</italic>a simple polyol method and characterized with CO pulse chemisorption, HAADF-STEM, and EDX measurements. Conversion of ethylene was monitored<italic>via</italic>gas-phase FTIR, and distribution of liquid products was analyzed<italic>via</italic>GC-FID, GC-MS, and 1H-NMR. Compared to unpromoted Pt/C, Sn-promoted catalysts show lower initial reaction rates, but better resistance to catalyst deactivation, while increasing selectivity towards alkylaromatics. Both reaction products and ethylene were found to inhibit the reaction significantly. At 250 °C for 22 h, TON up to 28 and 86 mol per mol Pt were obtained for Pt/C and PtSn<sub>2</sub>/C, respectively, with olefin selectivities of 94% and 53%. The remaining products were mainly unbranched alkylaromatics. These findings show the potential of simple heterogeneous catalysts in alkane transfer dehydrogenation, for the preparation of valuable olefins and alkylaromatics, or as an essential step in various tandem reactions. |
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Place of Publication |
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Wos |
001104905100001 |
Publication Date |
2023-11-09 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2044-4753 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
5 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
T. de la Croix gratefully acknowledges the support of the Flanders Research Foundation (FWO) under project 11F6622N. D. De Vos is grateful to FWO for support of project G0D3721N, and to KU Leuven for the iBOF project 21/016/C3. S. Bals and N. Claes acknowledge funding from the European Research Council under the European Union’s Horizon 2020 research and innovation program (ERC Consolidator Grant No. 815128- REALNANO). W. Thielemans and S. Eyley thank KU Leuven (grant C14/18/061) and FWO (G0A1219N) for financial support. |
Approved |
Most recent IF: 5; 2023 IF: 5.773 |
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Call Number |
EMAT @ emat @c:irua:201010 |
Serial |
8968 |
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| Permanent link to this record |
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Author |
Van Gordon, K.; Baúlde, S.; Mychinko, M.; Heyvaert, W.; Obelleiro-Liz, M.; Criado, A.; Bals, S.; Liz-Marzán, L.M.; Mosquera, J. |
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Title |
Tuning the Growth of Chiral Gold Nanoparticles Through Rational Design of a Chiral Molecular Inducer |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
Nano Letters |
Abbreviated Journal |
Nano Lett. |
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Volume |
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Issue |
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Pages |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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Abstract |
The bottom-up production of chiral gold nanomaterials holds great potential for the advancement of biosensing and nano-optics, among other applications. Reproducible preparations of colloidal nanomaterials with chiral morphology have been reported, using cosurfactants or chiral inducers such as thiolated amino acids. However, the underlying growth mechanisms for these nanomaterials remain insufficiently understood. We introduce herein a purposely devised chiral inducer, a cysteine modified with a hydrophobic chain, as a versatile chiral inducer. The amphiphilic and chiral features of this molecule provide control over the chiral morphology and the chiroptical signature of the obtained nanoparticles by simply varying the concentration of chiral inducer. These results are supported by circular dichroism and electromagnetic modeling as well as electron tomography to analyze structural evolution at the facet scale. Our observations suggest complex roles for the factors involved in chiral synthesis: the chemical nature of the chiral inducers and the influence of cosurfactants. |
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Wos |
001092787000001 |
Publication Date |
2023-10-25 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1530-6984 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
10.8 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
J.M. Taboada and F. Obelleiro are thanked for support with electromagnetic simulations. The authors acknowledge financial support by the European Research Council (ERC CoG No. 815128 REALNANO to S. Bals; ERC AdG No. 787510, 4DbioSERS to L.M.L.-M.) and from MCIN/AEI/10.13039/501100011033 and “ESF Investing in your future” (Grant PID2020-117779RB-I00 to L.M.L.-M., Grant RYC2020-030183-I to A.C., and Grants RYC2019-027842-I, PID2020-117885GA-I00 to J.M.). |
Approved |
Most recent IF: 10.8; 2023 IF: 12.712 |
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Call Number |
EMAT @ emat @c:irua:200590 |
Serial |
8963 |
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| Permanent link to this record |
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Author |
Ramesha, B.M.; Pawlak, B.; Arenas Esteban, D.; Reekmans, G.; Bals, S.; Marchal, W.; Carleer, R.; Adriaensens, P.; Meynen, V. |
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Title |
Partial hydrolysis of diphosphonate ester during the formation of hybrid Tio₂ nanoparticles : role of acid concentration |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
ChemPhysChem : a European journal of chemical physics and physical chemistry |
Abbreviated Journal |
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Volume |
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Issue |
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Pages |
e202300437-13 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA) |
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Abstract |
In the present work, a method was utilized to control the in‐situ partial hydrolysis of a diphosphonate ester in presence of a titania precursor and in function of acid content and its impact on the hybrid nanoparticles was assessed. The hydrolysis degree of organodiphosphonate ester linkers during the formation of hybrid organic‐inorganic metal oxide nanoparticles, are relatively underexplored . Quantitative solution NMR spectroscopy revealed that during the synthesis of TiO2 nanoparticles, an increase in acid concentration introduces a higher degree of partial hydrolysis of the TEPD linker into diverse acid/ester derivatives of TEPD. Increasing the HCl/Ti ratio from 1 to 3, resulted in an increase in degree of partial hydrolysis of the TEPD linker in solution from 4% to 18.8% under the here applied conditions. As a result of the difference in partial hydrolysis, the linker‐TiO2 bonding was altered. Upon subsequent drying of the colloidal TiO2 solution, different textures, at nanoscale and macroscopic scale, were obtained dependent on the HCl/Ti ratio and thus the degree of hydrolysis of TEPD. Understanding such linker‐TiO2 nanoparticle surface dynamics is crucial for making hybrid organic‐inorganic materials (i.e. (porous) metal phosphonates) employed in applications such as electronic/photonic devices, separation technology and heterogeneous catalysts. |
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Wos |
001071673900001 |
Publication Date |
2023-09-05 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1439-4235; 1439-7641 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
2.9 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
This work was supported by the Research Foundation-Flanders (FWO Vlaanderen) Project G.0121.17 N. The work was further supported by Hasselt University and the Research Foundation – Flanders (FWO Vlaanderen) via the Hercules project AUHL/15/2 – GOH3816 N. V. M. acknowledges the Research Foundation Flanders (FWO) for project K801621 N. B. M. R. acknowledges, Prof. Dr. Christophe Detavernier and Dr. Davy Deduystche (COCOON, Ghent University) for PXRD and VT-XRD measurements, Prof. Dr. Christophe Van De Velde (iPRACS, University of Antwerp) and Dr. Radu Ciocarlan (LADCA, University of Antwerp) for helpful discussions on PXRD measurements and Dr. Nick Gys (University of Antwerp and VITO) for ICP-OES measurements. |
Approved |
Most recent IF: 2.9; 2023 IF: 3.075 |
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Call Number |
UA @ admin @ c:irua:198934 |
Serial |
8911 |
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| Permanent link to this record |
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Author |
Kelly, S.; Mercer, E.; De Meyer, R.; Ciocarlan, R.-G.; Bals, S.; Bogaerts, A. |
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Title |
Microwave plasma-based dry reforming of methane: Reaction performance and carbon formation |
Type |
A1 Journal Article |
| |
Year |
2023 |
Publication |
Journal of CO2 utilization |
Abbreviated Journal |
Journal of CO2 Utilization |
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Volume |
75 |
Issue |
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Pages |
102564 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
e investigate atmospheric pressure microwave (MW) plasma (2.45 GHz) conversion in CO2 and CH4 mixtures (i.e., dry reforming of methane, DRM) focusing on reaction performance and carbon formation. Promising energy costs of ~2.8–3.0 eV/molecule or ~11.1–11.9 kJ/L are amongst the best performance to date considering the current state-of-the-art for plasma-based DRM for all types of plasma. The conversion is in the range of ~46–49% and ~55–67% for CO2 and CH4, respectively, producing primarily syngas (i.e., H2 and CO) with H2/CO ratios of ~0.6–1 at CH4 fractions ranging from 30% to 45%. Water is the largest byproduct with levels ranging ~7–14% in the exhaust. Carbon particles visibly impact the plasma at higher CH4 fractions (> 30%), where they become heated and incandescent. Particle luminosity increases with increasing CH4 fractions, with the plasma becoming unstable near a 1:1 mixture (i.e., > 45% CH4). Electron microscopy of the carbon material reveals an agglomerated morphology of pure carbon nanoparticles. The mean particle size is determined as ~20 nm, free of any metal contamination, consistent with the electrode-less MW design. |
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Corporate Author |
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Place of Publication |
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Editor |
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Wos |
001065310000001 |
Publication Date |
2023-08-10 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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| |
ISSN |
2212-9820 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7.7 |
Times cited |
6 |
Open Access |
OpenAccess |
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| |
Notes |
We acknowledge financial support by a European Space Agency (ESA) Open Science Innovation Platform study (contract no. 4000137001/21/NL/GLC/ov), the European Marie Skłodowska-Curie Individual Fellowship ‘‘PENFIX’’ within Horizon 2020 (grant no. 838181), the European Research Council (ERC) under the European Union’s Horizon 2020 Research and Innovation Program (grant no. 810182; SCOPE ERC Synergy project), the Excellence of Science FWOFNRS PLASyntH2 project (FWO grant no. G0I1822N and EOS no. 4000751) and the Methusalem project of the University of Antwerp |
Approved |
Most recent IF: 7.7; 2023 IF: 4.292 |
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Call Number |
PLASMANT @ plasmant @c:irua:198155 |
Serial |
8807 |
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| Permanent link to this record |
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Author |
Arenas Esteban, D.; Pacquets, L.; Choukroun, D.; Hoekx, S.; Kadu, A.A.; Schalck, J.; Daems, N.; Breugelmans, T.; Bals, S. |
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Title |
3D characterization of the structural transformation undergone by Cu@Ag core-shell nanoparticles following CO₂ reduction reaction |
Type |
A1 Journal article |
| |
Year |
2023 |
Publication |
Chemistry of materials |
Abbreviated Journal |
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| |
Volume |
35 |
Issue |
17 |
Pages |
6682-6691 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
The increasing use of metallic nanoparticles (NPs) is significantly advancing the field of electrocatalysis. In particular, Cu/Ag bimetallic interfaces are widely used to enhance the electrochemical CO2 reduction reaction (eCO(2)RR) toward CO and, more recently, C-2 products. However, drastic changes in the product distribution and performance when Cu@Ag core-shell configurations are used can often be observed under electrochemical reaction conditions, especially during the first few minutes of the reaction. Possible structural changes that generate these observations remain underexplored; therefore, the structure-property relationship is hardly understood. In this study, we use electron tomography to investigate the structural transformation mechanism of Cu@Ag core-shells NPs during the critical first minutes of the eCO(2)RR. In this manner, we found that the crystallinity of the Cu seed determines whether the formation of a complete and homogeneous Ag shell is possible. Moreover, by tracking the particles' transformations, we conclude that modifications of the Cu-Ag interface and Cu2O enrichment at the surface of the NPs are key factors contributing to the product generation changes. These insights provide a better understanding of how bimetallic core-shell NPs transform under electrochemical conditions. |
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Place of Publication |
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Wos |
001061530700001 |
Publication Date |
2023-08-31 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756; 1520-5002 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
8.6 |
Times cited |
1 |
Open Access |
OpenAccess |
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Notes |
L.P. was supported through a PhD fellowship for strategicbasic research (1S56920N) of the Research Foundation – Flanders(FWO). S.H. was supported through a PhD fellowship for strategic basicresearch (1S42623N) of the Research Foundation – Flanders (FWO).S.B., D.A.E., and A.A.K. acknowledge financial support from ERC Consolidator Grant Number 815128 REALNANO. This research was financed by the researchcouncil of the University of Antwerp (BOF-GOA 33928). |
Approved |
Most recent IF: 8.6; 2023 IF: 9.466 |
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Call Number |
UA @ admin @ c:irua:199187 |
Serial |
8825 |
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| Permanent link to this record |
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Author |
Moggia, G.; Hoekx, S.; Daems, N.; Bals, S.; Breugelmans, T. |
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Title |
Synthesis and characterization of a highly electroactive composite based on Au nanoparticles supported on nanoporous activated carbon for electrocatalysis |
Type |
A1 Journal article |
| |
Year |
2023 |
Publication |
ChemElectroChem |
Abbreviated Journal |
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Volume |
|
Issue |
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Pages |
1-11 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
A facile, “one-pot”, chemical approach to synthesize gold-based nanoparticles finely dispersed on porous activated carbon (Norit) was demonstrated in this work. The pH of the synthesis bath played a critical role in determining the optimal gold-carbon interaction, which enabled a successful deposition of the gold nanoparticles onto the carbon matrix with a maximized metal utilization of 93 %. The obtained AuNP/C nanocomposite was characterized using SEM, HAADF-STEM electron tomography and electrochemical techniques. It was found that the Au nanoparticles, with diameters between 5 and 20 nm, were evenly distributed over the carbon matrix, both inside and outside the pores. Electrochemical characterization indicated that the composite had a very large electroactive surface area (EASA), as high as 282.4 m2 gAu-1. By exploiting its very high EASA, the catalyst was intended to boost the productivity of glucaric acid in the electrooxidation of its precursor, gluconic acid. However, cyclic voltammetry experiments revealed a very limited reactivity towards gluconic acid oxidation, due to the spacial hindrance of gluconic acid molecule which prevented diffusion inside the catalyst nanopores. On the other hand, the as-synthesized nanocomposite promises to be effective towards the ORR, and might thus find potential application as anode catalyst for fuel cells as well as for the scalability of all those electrochemical reactions involving small molecules with high diffusivity and catalysed by noble metals (i. e. CO2, CH4, N2, etc..). Electrocatalysis: Gold nanoparticles with diameter between 5 and 20 nm evenly distributed onto porous activated carbon (Norit) were obtained using a facile “one-pot” chemical synthesis technique with very high metal utilization. The AuNP/C nanocomposite was characterized using SEM, HAADF-STEM electron tomography and electrochemical techniques, revealing a very large electroactive surface area (EASA). The figure shows the HAADF-STEM image (a) and the respective EDX elemental distribution (b) for the AuNP/C composite with 9.3 % Au-loading developed in this work (Au is marked in red and C in green).image |
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Place of Publication |
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Wos |
001060398900001 |
Publication Date |
2023-09-08 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2196-0216 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4 |
Times cited |
1 |
Open Access |
OpenAccess |
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Notes |
The research described in this article has not been supported by the Climate, Infrastructure and Environment Executive Agency of the European Commission. The views expressed in this article have not been adopted or in any way approved by the European Commission and do not constitute a statement of the European Commission & apos;s views.r S. Hoekx was supported by Research Foundation Flanders (FWO 1S42623N). The authors would like to thank Prof. Dr. Christophe Vande Velde, University of Antwerp, for the XRD analysis. |
Approved |
Most recent IF: 4; 2023 IF: 4.136 |
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Call Number |
UA @ admin @ c:irua:199210 |
Serial |
8941 |
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| Permanent link to this record |
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Author |
Chen, Q.; Skorikov, A.; van der Hoeven, J.E.S.; van Blaaderen, A.; Albrecht, W.; Perez-Garza, H.H.; Bals, S. |
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Title |
Estimation of temperature homogeneity in MEMS-based heating nanochips via quantitative HAADF-STEM tomography |
Type |
A1 Journal article |
| |
Year |
2023 |
Publication |
Particle and particle systems characterization |
Abbreviated Journal |
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Volume |
41 |
Issue |
2 |
Pages |
1-8 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Sample holders for transmission electron microscopy (TEM) based on micro-electro-mechanical systems (MEMS) have recently become popular for investigating the behavior of nanomaterials under in situ or environmental conditions. The accuracy and reproducibility of these in situ holders are essential to ensure the reliability of experimental results. In addition, the uniformity of an applied temperature trigger across the MEMS chip is a crucial parameter. In this work, it is measured the temperature homogeneity of MEMS-based heating sample supports by locally analyzing the dynamics of heat-induced alloying of Au@Ag nanoparticles located in different regions of the support through quantitative fast high-angle annular dark-field scanning TEM tomography. These results demonstrate the superior temperature homogeneity of a microheater design based on a heating element shaped as a circular spiral with a width decreasing outwards compared to a double spiral-shaped designed microheater. The proposed approach to measure the local temperature homogeneity based on the thermal properties of bimetallic nanoparticles will support the future development of MEMS-based heating supports with improved thermal properties and in situ studies where high precision in the temperature at a certain position is required. This schematic delineates an approach to quantifying potential localized temperature deviation within a nanochip. Employing two comparable nanoparticles as thermal probes in discrete nanochip regions, the alloying kinetics of these nanoparticles are monitorable using in situ quantitative high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) tomography, thus enabling the precise estimation of local temperature deviations.image |
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Corporate Author |
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Place of Publication |
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Wos |
001060394600001 |
Publication Date |
2023-09-08 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0934-0866 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
2.7 |
Times cited |
|
Open Access |
Not_Open_Access |
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Notes |
This project was funded from the European Commission and The Marie Sklodowska-Curie Innovative Training Network MUMMERING (Grant Agreement no. 765604) |
Approved |
Most recent IF: 2.7; 2023 IF: 4.474 |
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Call Number |
UA @ admin @ c:irua:199219 |
Serial |
8863 |
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| Permanent link to this record |
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Author |
Beckwee, E.J.; Watson, G.; Houlleberghs, M.; Arenas Esteban, D.; Bals, S.; Van Der Voort, P.; Breynaert, E.; Martens, J.; Baron, G.V.; Denayer, J.F.M. |
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Title |
Enabling hydrate-based methane storage under mild operating conditions by periodic mesoporous organosilica nanotubes |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Heliyon |
Abbreviated Journal |
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Volume |
9 |
Issue |
7 |
Pages |
e17662-14 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Biomethane is a renewable natural gas substitute produced from biogas. Storage of this sustainable energy vector in confined clathrate hydrates, encapsulated in the pores of a host material, is a highly promising avenue to improve storage capacity and energy efficiency. Herein, a new type of periodic mesoporous organosilica (PMO) nanotubes, referred to as hollow ring PMO (HR-PMO), capable of promoting methane clathrate hydrate formation under mild working conditions (273 K, 3.5 MPa) and at high water loading (5.1 g water/g HR-PMO) is reported. Gravimetric uptake measurements reveal a steep single-stepped isotherm and a noticeably high methane storage capacity (0.55 g methane/g HR-PMO; 0.11 g methane/g water at 3.5 MPa). The large working capacity throughout consecutive pressure-induced clathrate hydrate formationdissociation cycles demonstrates the material's excellent recyclability (97% preservation of capacity). Supported by ex situ cryo-electron tomography and x-ray diffraction, HR-PMO nanotubes are hypothesized to promote clathrate hydrate nucleation and growth by distribution and confinement of water in the mesopores of their outer wall, along the central channels of the nanotubes and on the external nanotube surface. These findings showcase the potential for application of organosilica materials with hierarchical and interconnected pore systems for pressure-based storage of biomethane in confined clathrate hydrates. |
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Wos |
001056264100001 |
Publication Date |
2023-06-28 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2405-8440 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
|
Times cited |
4 |
Open Access |
OpenAccess |
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Notes |
E.J.B., G.W. and M.H. contributed equally to this work. M.H. acknowledges FWO for an FWO-SB fellowship. All authors acknowledge VLAIO for Moonshot funding (ARCLATH, n ? HBC.2019.0110, ARCLATH2, n ? HBC.2021.0254) . J.A.M. acknowledges the Flemish Government for long-term structural funding (Methusalem) and department EWI for infrastructure investment via the Hermes Fund (AH.2016.134) . NMRCoRe acknowledges the Flemish government, department EWI for financial support as International Research Infrastructure (I001321N: Nuclear Magnetic Resonance Spectroscopy Platform for Molecular Water Research) . J.A.M. acknowledges the European Research Council (ERC) for an Advanced Research Grant under the European Union's Horizon 2020 research and innovation program under grant agreement No. 834134 (WATUSO) . S.B acknowledges financial support by the Research Foundation Flanders (FWO grant G.0381.16N) . This project also received funding from the European Union's Horizon 2020 research and innovation program under grant agreement No 731019 (EUSMI) and No 815128 (REALNANO) . |
Approved |
Most recent IF: NA |
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Call Number |
UA @ admin @ c:irua:199249 |
Serial |
8862 |
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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. |
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Title |
Spontaneous Chirality Evolved at the Au–Ag Interface in Plasmonic Nanorods |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem. Mater. |
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Volume |
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Issue |
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Pages |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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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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Wos |
001052093300001 |
Publication Date |
2023-08-21 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756 |
ISBN |
|
Additional Links |
UA library record; WoS full record |
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Impact Factor |
8.6 |
Times cited |
|
Open Access |
OpenAccess |
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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 |
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Call Number |
EMAT @ emat @c:irua:198151 |
Serial |
8810 |
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Author |
Vega-Paredes, M.; Aymerich-Armengol, R.; Arenas Esteban, D.; Marti-Sanchez, S.; Bals, S.; Scheu, C.; Manjon, A.G. |
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Title |
Electrochemical stability of rhodium-platinum core-shell nanoparticles : an identical location scanning transmission electron microscopy study |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
ACS nano |
Abbreviated Journal |
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Volume |
17 |
Issue |
17 |
Pages |
16943-16951 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Rhodium-platinum core-shell nanoparticleson a carbonsupport (Rh@Pt/C NPs) are promising candidates as anode catalystsfor polymer electrolyte membrane fuel cells. However, their electrochemicalstability needs to be further explored for successful applicationin commercial fuel cells. Here we employ identical location scanningtransmission electron microscopy to track the morphological and compositionalchanges of Rh@Pt/C NPs during potential cycling (10 000 cycles,0.06-0.8 V-RHE, 0.5 H2SO4)down to the atomic level, which are then used for understanding thecurrent evolution occurring during the potential cycles. Our resultsreveal a high stability of the Rh@Pt/C system and point toward particledetachment from the carbon support as the main degradation mechanism. |
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Place of Publication |
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Language |
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Wos |
001051495900001 |
Publication Date |
2023-08-21 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
17.1 |
Times cited |
2 |
Open Access |
OpenAccess |
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Notes |
The authors would like to thank C. Bodirsky for providing the samples, N. Rivas Rivas for his corrections on the manuscript, and D. Chatain for providing her expertise on the equilibrium shape of nanoparticles. Special thanks to B. Breitbach for performing the XRD experiments. A.G.M. acknowledges the Grant RYC2021-033479- I funded by MCIN/AEI/10.13039/501100011033 and, as appropriate, by European Union NextGenerationEU/PRTR. |
Approved |
Most recent IF: 17.1; 2023 IF: 13.942 |
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Call Number |
UA @ admin @ c:irua:199253 |
Serial |
8859 |
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Author |
Yang, S.; An, H.; Arnouts, S.; Wang, H.; Yu, X.; de Ruiter, J.; Bals, S.; Altantzis, T.; Weckhuysen, B.M.; van der Stam, W. |
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Title |
Halide-guided active site exposure in bismuth electrocatalysts for selective CO₂ conversion into formic acid |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Nature Catalysis |
Abbreviated Journal |
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Volume |
6 |
Issue |
9 |
Pages |
796-806 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
It remains a challenge to identify the active sites of bismuth catalysts in the electrochemical CO2 reduction reaction. Here we show through in situ characterization that the activation of bismuth oxyhalide electrocatalysts to metallic bismuth is guided by the halides. In situ X-ray diffraction results show that bromide promotes the selective exposure of planar bismuth surfaces, whereas chloride and iodide result in more disordered active sites. Furthermore, we find that bromide-activated bismuth catalysts outperform the chloride and iodide counterparts, achieving high current density (>100 mA cm(-2)) and formic acid selectivity (>90%), suggesting that planar bismuth surfaces are more active for the electrochemical CO2 reduction reaction. In addition, in situ X-ray absorption spectroscopy measurements reveal that the reconstruction proceeds rapidly in chloride-activated bismuth and gradually when bromide is present, facilitating the formation of ordered planar surfaces. These findings show the pivotal role of halogens on selective facet exposure in activated bismuth-based electrocatalysts during the electrochemical CO2 reduction reaction. |
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Wos |
001050367400001 |
Publication Date |
2023-08-17 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2520-1158 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
37.8 |
Times cited |
13 |
Open Access |
OpenAccess |
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Notes |
B.M.W. acknowledges support from the Strategic UU-TU/e Alliance project 'Joint Centre for Chemergy Research' as well as from the Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), an NWO gravitation programme funded by the Ministry of Education, Culture and Science of the government of the Netherlands. S.B. acknowledges support from the European Research Council (ERC Consolidator Grant #815128 REALNANO). S.A. and T.A. acknowledge funding from the University of Antwerp Research fund (BOF). We also thank J. Wijten, J. Janssens and T. Prins (all from the Inorganic Chemistry and Catalysis group, Utrecht University) for helpful technical support. S. Deelen (Faculty of Science, Utrecht University) and L. Wu (Inorganic Chemistry and Catalysis group, Utrecht University) are acknowledged for the design of the in situ XRD cell. We also acknowledge B. Detlefs, P. Glatzel and V. Paidi (ESRF) for the support during the HERFD-XANES measurements on the ID26 beamline of the ESRF. |
Approved |
Most recent IF: 37.8; 2023 IF: NA |
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Call Number |
UA @ admin @ c:irua:199190 |
Serial |
8877 |
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Author |
Zhang, Y.; van Schayck, J.P.; Pedrazo-Tardajos, A.; Claes, N.; Noteborn, W.E.M.; Lu, P.-H.; Duimel, H.; Dunin-Borkowski, R.E.; Bals, S.; Peters, P.J.; Ravelli, R.B.G. |
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Title |
Charging of vitreous samples in cryogenic electron microscopy mitigated by graphene |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
ACS nano |
Abbreviated Journal |
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Volume |
17 |
Issue |
16 |
Pages |
15836-15846 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Cryogenic electronmicroscopy can provide high-resolution reconstructionsof macromolecules embedded in a thin layer of ice from which atomicmodels can be built de novo. However, the interactionbetween the ionizing electron beam and the sample results in beam-inducedmotion and image distortion, which limit the attainable resolutions.Sample charging is one contributing factor of beam-induced motionsand image distortions, which is normally alleviated by including partof the supporting conducting film within the beam-exposed region.However, routine data collection schemes avoid strategies wherebythe beam is not in contact with the supporting film, whose rationaleis not fully understood. Here we characterize electrostatic chargingof vitreous samples, both in imaging and in diffraction mode. We mitigatesample charging by depositing a single layer of conductive grapheneon top of regular EM grids. We obtained high-resolution single-particleanalysis (SPA) reconstructions at 2 & ANGS; when the electron beamonly irradiates the middle of the hole on graphene-coated grids, usingdata collection schemes that previously failed to produce sub 3 & ANGS;reconstructions without the graphene layer. We also observe that theSPA data obtained with the graphene-coated grids exhibit a higher b factor and reduced particle movement compared to dataobtained without the graphene layer. This mitigation of charging couldhave broad implications for various EM techniques, including SPA andcryotomography, and for the study of radiation damage and the developmentof future sample carriers. Furthermore, it may facilitate the explorationof more dose-efficient, scanning transmission EM based SPA techniques. |
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Wos |
001041649900001 |
Publication Date |
2023-08-02 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
17.1 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
We thank H. Nguyen for editing the manuscript. We warmly thank the M4i Microscopy CORE Lab team of FHML Maastricht University (MU) for their support and collaboration and Eve Timlin and Ye Gao (MU) for providing protein samples. Members of the Amsterdam Scientific Instruments team are acknowledged for their Timepix detector support. This work benefited from access to The Netherlands Centre for Electron Nanoscopy (NeCEN) with assistance from Ludovic Renault and Meindert Lamers. The authors acknowledge financial support of the Netherlands Electron Microscopy Infrastructure (NEMI), project number 184.034.014 of the National Roadmap for Large-Scale Research Infrastructure of the Dutch Research Council (NWO), the PPP Allowance made available by Health-Holland, Top Sector Life Sciences & Health, to stimulate public-private partnerships, project 4DEM, number LSHM21029, and the LINK program from the Province of Limburg, The Netherlands, as well as financial support from the European Commission under the Horizon 2020 Programme by grant no. 815128 (REALNANO). |
Approved |
Most recent IF: 17.1; 2023 IF: 13.942 |
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Call Number |
UA @ admin @ c:irua:198376 |
Serial |
8840 |
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| Permanent link to this record |
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Author |
Arteaga Cardona, F.; Jain, N.; Popescu, R.; Busko, D.; Madirov, E.; Arús, B.A.; Gerthsen, D.; De Backer, A.; Bals, S.; Bruns, O.T.; Chmyrov, A.; Van Aert, S.; Richards, B.S.; Hudry, D. |
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Title |
Preventing cation intermixing enables 50% quantum yield in sub-15 nm short-wave infrared-emitting rare-earth based core-shell nanocrystals |
Type |
A1 Journal Article |
| |
Year |
2023 |
Publication |
Nature communications |
Abbreviated Journal |
Nat Commun |
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Volume |
14 |
Issue |
1 |
Pages |
4462 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Short-wave infrared (SWIR) fluorescence could become the new gold standard in optical imaging for biomedical applications due to important advantages such as lack of autofluorescence, weak photon absorption by blood and tissues, and reduced photon scattering coefficient. Therefore, contrary to the visible and NIR regions, tissues become translucent in the SWIR region. Nevertheless, the lack of bright and biocompatible probes is a key challenge that must be overcome to unlock the full potential of SWIR fluorescence. Although rare-earth-based core-shell nanocrystals appeared as promising SWIR probes, they suffer from limited photoluminescence quantum yield (PLQY). The lack of control over the atomic scale organization of such complex materials is one of the main barriers limiting their optical performance. Here, the growth of either homogeneous (α-NaYF<sub>4</sub>) or heterogeneous (CaF<sub>2</sub>) shell domains on optically-active α-NaYF<sub>4</sub>:Yb:Er (with and without Ce<sup>3+</sup>co-doping) core nanocrystals is reported. The atomic scale organization can be controlled by preventing cation intermixing only in heterogeneous core-shell nanocrystals with a dramatic impact on the PLQY. The latter reached 50% at 60 mW/cm<sup>2</sup>; one of the highest reported PLQY values for sub-15 nm nanocrystals. The most efficient nanocrystals were utilized for in vivo imaging above 1450 nm. |
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Wos |
001037058500022 |
Publication Date |
2023-07-25 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2041-1723 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
16.6 |
Times cited |
1 |
Open Access |
OpenAccess |
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Notes |
D.H. would like to thank Dominique Ectors (Bruker AXS GmbH, Karlsruhe, Germany) for assistance and discussion on the PXRD data and TOPAS evaluations. The authors would like to acknowledge the financial support provided by the Helmholtz Association via: i) the Professorial Recruitment Initiative Funding (B.S.R.); ii) the Research Field Energy – Program Materials and Technologies for the Energy Transition – Topic 1 Photovoltaics (F.A.C., D.B., E.M., B.S.R., D.H.). This project received funding from the European Union’s Horizon 2020 innovation programme under grant agreement 823717. This work was supported by the European Research Council (grant 770887-PICOMETRICS to S.V.A. and Grant 815128-REALNANO to S.B.). The authors acknowledge financial support from the ResearchFoundation Flanders (FWO, Belgium) through project fundings (G.0346.21 N to S.V.A. and S.B.) and a postdoctoral grant (A.D.B.). The authors (B.A.A., O.T.B. and A.C.) acknowledge funding from the Helmholtz Zentrum München, the DFG-Emmy Noether program (BR 5355/2-1) and from the CZI Deep Tissue Imaging (DTI-0000000248). The authors (O.T.B. and D.H.) would like to thank the Helmholtz Imaging (ZT-I-PF-4-038-BENIGN). |
Approved |
Most recent IF: 16.6; 2023 IF: 12.124 |
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Call Number |
EMAT @ emat @c:irua:198158 |
Serial |
8808 |
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| Permanent link to this record |
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Author |
Ren, P.; Zhang, T.; Jain, N.; Ching, H.Y.V.; Jaworski, A.; Barcaro, G.; Monti, S.; Silvestre-Albero, J.; Celorrio, V.; Chouhan, L.; Rokicinska, A.; Debroye, E.; Kustrowski, P.; Van Doorslaer, S.; Van Aert, S.; Bals, S.; Das, S. |
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Title |
An atomically dispersed Mn-photocatalyst for generating hydrogen peroxide from seawater via the Water Oxidation Reaction (WOR) |
Type |
A1 Journal article |
| |
Year |
2023 |
Publication |
Journal of the American Chemical Society |
Abbreviated Journal |
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Volume |
145 |
Issue |
30 |
Pages |
16584-16596 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Organic synthesis (ORSY); Theory and Spectroscopy of Molecules and Materials (TSM²) |
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Abstract |
In this work, we have fabricatedan aryl amino-substitutedgraphiticcarbon nitride (g-C3N4) catalyst with atomicallydispersed Mn capable of generating hydrogen peroxide (H2O2) directly from seawater. This new catalyst exhibitedexcellent reactivity, obtaining up to 2230 & mu;M H2O2 in 7 h from alkaline water and up to 1800 & mu;Mfrom seawater under identical conditions. More importantly, the catalystwas quickly recovered for subsequent reuse without appreciable lossin performance. Interestingly, unlike the usual two-electron oxygenreduction reaction pathway, the generation of H2O2 was through a less common two-electron water oxidation reaction(WOR) process in which both the direct and indirect WOR processesoccurred; namely, photoinduced h(+) directly oxidized H2O to H2O2 via a one-step 2e(-) WOR, and photoinduced h(+) first oxidized a hydroxide (OH-) ion to generate a hydroxy radical ((OH)-O-& BULL;), and H2O2 was formed indirectly by thecombination of two (OH)-O-& BULL;. We have characterized thematerial, at the catalytic sites, at the atomic level using electronparamagnetic resonance, X-ray absorption near edge structure, extendedX-ray absorption fine structure, high-resolution transmission electronmicroscopy, X-ray photoelectron spectroscopy, magic-angle spinningsolid-state NMR spectroscopy, and multiscale molecular modeling, combiningclassical reactive molecular dynamics simulations and quantum chemistrycalculations. |
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Wos |
001034983300001 |
Publication Date |
2023-07-24 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0002-7863 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15 |
Times cited |
21 |
Open Access |
Not_Open_Access |
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Notes |
S.D. thanks the IOF grant and Francqui start up grant from the University of Antwerp, Belgium, for the financial support. P.R. thanks CSC and T.Z. thanks FWO for their financial assistance to finish this work. E.D. would like to thank the KU Leuven Research Fund for financial support through STG/21/010. J.S.A. acknowledges financial support from MCIN/AEI/10.13039/501100011033 and EU NextGeneration/PRTR (Project PCI2020-111968/3D-Photocat) and Diamond Synchrotron (rapid access proposal SP32609). This work was supported by the European Research Council (grant 770887-PICOMETRICS to S.V.A. and Grant 815128-REALNANO to S.B.). S.B. and S.V.A. acknowledge financial support from the Research Foundation Flanders (FWO, Belgium, project G.0346.21 N). We also thank Mr. Jian Zhu and Mr. Shahid Ullah Khan from the University of Antwerp, Belgium, for helpful discussions. |
Approved |
Most recent IF: 15; 2023 IF: 13.858 |
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Call Number |
UA @ admin @ c:irua:198426 |
Serial |
8831 |
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Author |
Carrasco, S.; Orcajo, G.; Martínez, F.; Imaz, I.; Kavak, S.; Arenas-Esteban, D.; Maspoch, D.; Bals, S.; Calleja, G.; Horcajada, P. |
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Title |
Hf/porphyrin-based metal-organic framework PCN-224 for CO2 cycloaddition with epoxides |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
Materials Today Advances |
Abbreviated Journal |
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Volume |
19 |
Issue |
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Pages |
100390 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Herein, we describe for the first time the synthesis of the highly porous Hf-tetracarboxylate porphyrin-based metal-organic framework (MOF) (Hf)PCN-224(M) (M = H2, Co2+). (Hf)PCN-224(H2) was easily and efficiently prepared following a simple microwave-assisted procedure with good yields (56–67%; space-time yields: 1100–1270 kg m−3·day−1), high crystallinity and phase purity by using trifluoromethanesulfonic acid and benzoic acid as modulators in less than 30 min. By simply introducing a preliminary step (10 min), 5,10,15,20-(tetra-4-carboxyphenyl)porphyrin linker (TCPP) was quantitatively metalated with Co2+ without additional purification and/or time consuming protection/deprotection steps to further obtain (Hf)PCN-224(Co). (Hf)PCN-224(Co) was then tested as catalyst in CO2 cycloaddition reaction with different epoxides to yield cyclic carbonates, showing the best catalytic performance described to date compared to other PCNs, under mild conditions (1 bar CO2, room temperature, 18–24 h). Twelve epoxides were tested, obtaining from moderate to excellent conversions (35–96%). Moreover, this reaction was gram scaled-up (x50) without significant loss of yield to cyclic carbonates. (Hf)PCN-224(Co) maintained its integrity and crystallinity even after 8 consecutive runs, and poisoning was efficiently reverted by a simple thermal treatment (175 °C, 6 h), fully recovering the initial catalytic activity. |
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Wos |
001025764000001 |
Publication Date |
2023-06-19 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2590-0498 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
10 |
Times cited |
1 |
Open Access |
OpenAccess |
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Notes |
S.C. acknowledges the European Union's Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie (MSCA-COFUND) grant agreement No 754382 (GOT Energy Talent). S.C. and P.H. acknowledge “Comunidad de Madrid” and European Regional Development Fund-FEDER 2014-2020-OE REACT-UE 1 for their financial support to VIRMOF-CM project associated to R&D projects in response to COVID-19. The authors acknowledge H2020-MSCA-ITN-2019 HeatNMof (ref. 860942), the M-ERA-NET C-MOF-cell (grant PCI2020-111998 funded by MCIN/AEI /10.13039/501100011033 and European Union NextGenerationEU/PRTR) project, and Retos Investigación MOFSEIDON (grant PID2019-104228RB-I00 funded by MCIN/AEI/10.13039/501100011033) project. This work has been also supported by the Regional Government of Madrid (Project ACES2030-CM, S2018/EMT-4319) and the Universidad Rey Juan Carlos IMPULSO Project (grant MATER M − 3000). S.K acknowledges the Flemish Fund for Scientific Research (FWO Vlaanderen) through a PhD research grant (1181122 N). |
Approved |
Most recent IF: 10; 2023 IF: NA |
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Call Number |
EMAT @ emat @c:irua:197198 |
Serial |
8800 |
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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. |
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Title |
Nucleation and growth of bipyramidal Yb:LiYF₄ nanocrystals : growing up in a hot environment |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Chemistry of materials |
Abbreviated Journal |
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Volume |
35 |
Issue |
14 |
Pages |
5311-5321 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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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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Place of Publication |
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Wos |
001021474500001 |
Publication Date |
2023-07-03 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756; 1520-5002 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
8.6 |
Times cited |
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Open Access |
OpenAccess |
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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 |
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Call Number |
UA @ admin @ c:irua:197787 |
Serial |
8907 |
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Author |
Panzic, I.; Mandic, V.; Mangalam, J.; Rath, T.; Radovanovic-Peric, F.; Gaboardi, M.; De Coen, B.; Bals, S.; Schrenker, N. |
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Title |
In-situ structural degradation study of quadruple-cation perovskite solar cells with nanostructured charge transfer layer |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Ceramics international |
Abbreviated Journal |
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Volume |
49 |
Issue |
14b |
Pages |
24475-24486 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
We investigated the structural stability of perovskite solar cells (PSCs) in n-i-p configuration comprising a rubidium-caesium-methylammonium-formamidinium (Rb-Cs-MA-FA) lead iodide/bromide perovskite absorber, interfaced with nanostructured ZnO-nanorod (NR) or mesostructured (MS) TiO2 electron transfer layers (ETL). An in-situ setup was established comprising synchrotron grazing incidence diffraction (GID) and Raman spectroscopy as a function of temperature under ambient and isothermal conditions; measurements of current-voltage (IV) characteristics and electron microscopic investigations were conducted discretely.The aging of the solar cells was performed at ambient conditions or at elevated temperatures directly in the in -situ measurement setup. The diffraction depth profiling results point to different degradation rates for different ETLs; moreover, electron microscopy and atomic force microscopy, as well as energy dispersive spectroscopy clarified surface conditions in terms of the extent of the degradation. Scanning transmission electron microscopy of lamellas, derived by dual beam microscopy, revealed that the origin of the degradation lay in the ETL/ absorber interface. For the case of the nanostructured zincite, the perovskite absorber contained many voids, leading to the conclusion that the investigated quadruple perovskite absorber showed limited compatibility with ZnO NR ETL due to a higher number of defects. Morphological defects promoted the absorber degradation and nullified the advantages initially achieved by nanostructuring. The exchange of the ZnO NR ETL with MS TiO2 improved the stability parameters of the absorber layer. |
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Wos |
001021057200001 |
Publication Date |
2022-12-25 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0272-8842; 1873-3956 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
5.2 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
This work has been funded by the projects PZS-2019-02-1555 PV-WALL in Research Cooperability Program of the Croatian Science Foundation funded by the European Union from the European Social Fund under the Operational Programme Efficient Human Resources 2014-2020 (perovskite solar cells) , UIP-2019-04-2367 SLIPPERY SLOPE of the Croatian Science Foundation (nanostructured titania and zincite constituents) , KK.01.2.1.02.0316 “ The development of the technical solution for energy saving using VIS -transparent or semi-transparent and IR-reflective thin-films” by the European Regional Development Fund (ERDF) (characterisation of thin-films) , 20190571 and 20190516 at Elettra Synchrotron, ICM-2019-13220 in Ernst Mach program of the OeAD-GmbH, and E210900588 in the EUSMI program. The group of prof Gregor Trimmel of the ICTM, NAWI Graz, the beam- line scientists of the MCX beamline of the Elettra synchrotron, and FIB- STEM researchers of the Faculty of Science, University of Antwerp, are gratefully acknowledged for collaboration and instrument access. The financial sustenance of the University of Zagreb is gratefully acknowledged. |
Approved |
Most recent IF: 5.2; 2023 IF: 2.986 |
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Call Number |
UA @ admin @ c:irua:197806 |
Serial |
8885 |
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Author |
Muravev, V.; Parastaev, A.; van den Bosch, Y.; Ligt, B.; Claes, N.; Bals, S.; Kosinov, N.; Hensen, E.J.M. |
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Title |
Size of cerium dioxide support nanocrystals dictates reactivity of highly dispersed palladium catalysts |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
Science |
Abbreviated Journal |
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Volume |
380 |
Issue |
6650 |
Pages |
1174-1179 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
The catalytic performance of heterogeneous catalysts can be tuned by modulation of the size and structure of supported transition metals, which are typically regarded as the active sites. In single-atom metal catalysts, the support itself can strongly affect the catalytic properties. Here, we demonstrate that the size of cerium dioxide (CeO2) support governs the reactivity of atomically dispersed palladium (Pd) in carbon monoxide (CO) oxidation. Catalysts with small CeO2 nanocrystals (~4 nanometers) exhibit unusually high activity in a CO-rich reaction feed, whereas catalysts with medium-size CeO2 (~8 nanometers) are preferred for lean conditions. Detailed spectroscopic investigations reveal support size–dependent redox properties of the Pd-CeO2 interface. |
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Wos |
001010846100008 |
Publication Date |
2023-06-16 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0036-8075 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
56.9 |
Times cited |
22 |
Open Access |
OpenAccess |
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Notes |
We thank the staff of the MAX IV Laboratory for time on beamline SPECIES under proposals 20200412 and 20190983; E. Kokkonen and A. Klyushin for assistance with NAP-XPS and RPES experiments conducted at SPECIES; staff of the MAX IV Laboratory for time on beamline BALDER under proposal 20200378; K. Klementiev for assistance with XAS measurements; J. Drnec at the ESRF for providing assistance in using beamline ID31; and V. Perez-Dieste and I. Villar Garcia at the CIRCE beamline at ALBA Synchrotron for help with acquiring preliminary RPES data obtained under proposal 2020024219. The synchrotron-based XRD measurements were performed on beamline ID31 at the European Synchrotron Radiation Facility (ESRF), Grenoble, France. Funding: This work was supported by the Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), a NWO Gravitation program funded by the Ministry of Education, Culture and Science of the Government of the Netherlands (V.M. and E.J.M.H.); the European Research Council (ERC consolidator grant 815128 REALNANO to S.B. and N.C.); and the European Union’s Horizon 2020 Research and Innovation Program (grant 823717–ESTEEM to S.B. and N.C). Research conducted at MAX IV, a Swedish national user facility, is supported by the Swedish Research council under contract 2018-07152, the Swedish Governmental Agency for Innovation Systems under contract 2018-04969, and Formas under contract 2019-02496 (VM). |
Approved |
Most recent IF: 56.9; 2023 IF: 37.205 |
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Call Number |
EMAT @ emat @c:irua:197199 |
Serial |
8801 |
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Author |
Mangnus, M.J.J.; de Wit, J.W.; Vonk, S.J.W.; Geuchies, J.J.; Albrecht, W.; Bals, S.; Houtepen, A.J.; Rabouw, F.T. |
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Title |
High-throughput characterization of single-quantum-dot emission spectra and spectral diffusion by multiparticle spectroscopy |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
ACS Photonics |
Abbreviated Journal |
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Volume |
10 |
Issue |
8 |
Pages |
2688-2698 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
In recent years, quantum dots (QDs) have emerged as bright,color-tunablelight sources for various applications such as light-emitting devices,lasing, and bioimaging. One important next step to advance their applicabilityis to reduce particle-to-particle variations of the emission propertiesas well as fluctuations of a single QD's emission spectrum,also known as spectral diffusion (SD). Characterizing SD is typicallyinefficient as it requires time-consuming measurements at the single-particlelevel. Here, however, we demonstrate multiparticle spectroscopy (MPS)as a high-throughput method to acquire statistically relevant informationabout both fluctuations at the single-particle level and variationsat the level of a synthesis batch. In MPS, we simultaneously measureemission spectra of many (20-100) QDs with a high time resolution.We obtain statistics on single-particle emission line broadening fora batch of traditional CdSe-based core-shell QDs and a batchof the less toxic InP-based core-shell QDs. The CdSe-basedQDs show significantly narrower homogeneous line widths, less SD,and less inhomogeneous broadening than the InP-based QDs. The timescales of SD are longer in the InP-based QDs than in the CdSe-basedQDs. Based on the distributions and correlations in single-particleproperties, we discuss the possible origins of line-width broadeningof the two types of QDs. Our experiments pave the way to large-scale,high-throughput characterization of single-QD emission propertiesand will ultimately contribute to facilitating rational design offuture QD structures. |
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Wos |
001009443500001 |
Publication Date |
2023-06-18 |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2330-4022 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7 |
Times cited |
1 |
Open Access |
OpenAccess |
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Notes |
This work was supported by The Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation Programme funded by the Ministry of Education, Culture and Science of the government of The Netherlands. The electron microscopy experiments at EMAT were supported by the European Commission (EUSMI grant E210100474). |
Approved |
Most recent IF: 7; 2023 IF: 6.756 |
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Call Number |
UA @ admin @ c:irua:197337 |
Serial |
8879 |
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| Permanent link to this record |
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Author |
Vlasov, E.; Skorikov, A.; Sánchez-Iglesias, A.; Liz-Marzán, L.M.; Verbeeck, J.; Bals, S. |
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Title |
Secondary electron induced current in scanning transmission electron microscopy: an alternative way to visualize the morphology of nanoparticles |
Type |
A1 Journal Article |
| |
Year |
2023 |
Publication |
ACS materials letters |
Abbreviated Journal |
ACS Materials Lett. |
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Volume |
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Issue |
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Pages |
1916-1921 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Electron tomography (ET) is a powerful tool to determine the three-dimensional (3D) structure of nanomaterials in a transmission electron microscope. However, the acquisition of a conventional tilt series for ET is a time-consuming process and can therefore not provide 3D structural information in a time-efficient manner. Here, we propose surface-sensitive secondary electron (SE) imaging as an alternative to ET for the investigation of the morphology of nanomaterials. We use the SE electron beam induced current (SEEBIC) technique that maps the electrical current arising from holes generated by the emission of SEs from the sample. SEEBIC imaging can provide valuable information on the sample morphology with high spatial resolution and significantly shorter throughput times compared with ET. In addition, we discuss the contrast formation mechanisms that aid in the interpretation of SEEBIC data. |
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Wos |
001006191600001 |
Publication Date |
2023-06-12 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2639-4979 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
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Times cited |
1 |
Open Access |
OpenAccess |
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Notes |
The funding for this project was provided by European Research Council (ERC Consolidator Grant 815128, REALNANO). J.V. acknowledges the eBEAM project, which is supported by the European Union’s Horizon 2020 research and innovation program under grant agreement no. 101017720 (FET-Proactive EBEAM). L.M.L.-M. acknowledges funding from MCIN/AEI/10.13039/501100011033 (grant # PID2020-117779RB-I00). |
Approved |
Most recent IF: NA |
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Call Number |
EMAT @ emat @c:irua:197004 |
Serial |
8795 |
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| Permanent link to this record |
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Author |
Monai, M.; Jenkinson, K.; Melcherts, A.E.M.; Louwen, J.N.; Irmak, E.A.; Van Aert, S.; Altantzis, T.; Vogt, C.; van der Stam, W.; Duchon, T.; Smid, B.; Groeneveld, E.; Berben, P.; Bals, S.; Weckhuysen, B.M. |
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Title |
Restructuring of titanium oxide overlayers over nickel nanoparticles during catalysis |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Science |
Abbreviated Journal |
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Volume |
380 |
Issue |
6645 |
Pages |
644-651 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
Reducible supports can affect the performance of metal catalysts by the formation of suboxide overlayers upon reduction, a process referred to as the strong metal-support interaction (SMSI). A combination of operando electron microscopy and vibrational spectroscopy revealed that thin TiOx overlayers formed on nickel/titanium dioxide catalysts during 400 degrees C reduction were completely removed under carbon dioxide hydrogenation conditions. Conversely, after 600 degrees C reduction, exposure to carbon dioxide hydrogenation reaction conditions led to only partial reexposure of nickel, forming interfacial sites in contact with TiOx and favoring carbon-carbon coupling by providing a carbon species reservoir. Our findings challenge the conventional understanding of SMSIs and call for more-detailed operando investigations of nanocatalysts at the single-particle level to revisit static models of structure-activity relationships. |
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Wos |
000999020900010 |
Publication Date |
2023-05-11 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0036-8075; 1095-9203 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
56.9 |
Times cited |
29 |
Open Access |
OpenAccess |
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Notes |
This work was supported by BASF and NWO CHIPP (research grant to B.M.W.); the MCEC NWO Gravitation Program (B.M.W.); the ARC-CBBC NWO Program (B.M.W.); the European Research Council (grant 770887 PICOMETRICS to S.V.A.); and the European Research Council (grant 815128 REALNANO to S.B.). |
Approved |
Most recent IF: 56.9; 2023 IF: 37.205 |
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Call Number |
UA @ admin @ c:irua:197432 |
Serial |
8923 |
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Author |
Kavak, S.; Kadu, A.A.; Claes, N.; Sánchez-Iglesias, A.; Liz-Marzán, L.M.; Batenburg, K.J.; Bals, S. |
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Title |
Quantitative 3D Investigation of Nanoparticle Assemblies by Volumetric Segmentation of Electron Tomography Data Sets |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
The journal of physical chemistry: C : nanomaterials and interfaces |
Abbreviated Journal |
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Volume |
127 |
Issue |
20 |
Pages |
9725-9734 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Morphological characterization of nanoparticle assemblies and hybrid nanomaterials is critical in determining their structure-property relationships as well as in the development of structures with desired properties. Electron tomography has become a widely utilized technique for the three-dimensional characterization of nanoparticle assemblies. However, the extraction of quantitative morphological parameters from the reconstructed volume can be a complex and labor-intensive task. In this study, we aim to overcome this challenge by automating the volumetric segmentation process applied to three-dimensional reconstructions of nanoparticle assemblies. The key to enabling automated characterization is to assess the performance of different volumetric segmentation methods in accurately extracting predefined quantitative descriptors for morphological characterization. In our methodology, we compare the quantitative descriptors obtained through manual segmentation with those obtained through automated segmentation methods, to evaluate their accuracy and effectiveness. To show generality, our study focuses on the characterization of assemblies of CdSe/CdS quantum dots, gold nanospheres and CdSe/CdS encapsulated in polymeric micelles, and silica-coated gold nanorods decorated with both CdSe/CdS or PbS quantum dots. We use two unsupervised segmentation algorithms: the watershed transform and the spherical Hough transform. Our results demonstrate that the choice of automated segmentation method is crucial for accurately extracting the predefined quantitative descriptors. Specifically, the spherical Hough transform exhibits superior performance in accurately extracting quantitative descriptors, such as particle size and interparticle distance, thereby allowing for an objective, efficient, and reliable volumetric segmentation of complex nanoparticle assemblies. |
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Wos |
000991752700001 |
Publication Date |
2023-05-25 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.7 |
Times cited |
2 |
Open Access |
OpenAccess |
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Notes |
Fonds Wetenschappelijk Onderzoek, 1181122N ; Horizon 2020 Framework Programme, 861950 ; H2020 European Research Council, 815128 ; |
Approved |
Most recent IF: 3.7; 2023 IF: 4.536 |
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Call Number |
EMAT @ emat @c:irua:196971 |
Serial |
8793 |
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Author |
Ndayirinde, C.; Gorbanev, Y.; Ciocarlan, R.-G.; De Meyer, R.; Smets, A.; Vlasov, E.; Bals, S.; Cool, P.; Bogaerts, A. |
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Title |
Plasma-catalytic ammonia synthesis : packed catalysts act as plasma modifiers |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Catalysis today |
Abbreviated Journal |
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Volume |
419 |
Issue |
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Pages |
114156-12 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
We studied the plasma-catalytic production of NH3 from H2 and N2 in a dielectric barrier discharge plasma reactor using five different Co-based catalysts supported on Al2O3, namely Co/Al2O3, CoCe/Al2O3, CoLa/Al2O3, CoCeLa/Al2O3 and CoCeMg/Al2O3. The catalysts were characterized via several techniques, including SEM-EDX, and their performance was compared. The best performing catalyst was found to be CoLa/Al2O3, but the dif-ferences in NH3 concentration, energy consumption and production rate between the different catalysts were limited under the same conditions (i.e. feed gas, flow rate and ratio, and applied power). At the same time, the plasma properties, such as the plasma power and current profile, varied significantly depending on the catalyst. Taken together, these findings suggest that in the production of NH3 by plasma catalysis, our catalysts act as plasma modifiers, i.e., they change the discharge properties and hence the gas phase plasma chemistry. Importantly, this effect dominates over the direct catalytic effect (as e.g. in thermal catalysis) defined by the chemistry on the catalyst surface. |
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Wos |
000987221300001 |
Publication Date |
2023-04-10 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0920-5861 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
5.3 |
Times cited |
3 |
Open Access |
OpenAccess |
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Notes |
This research was supported by 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 the Methusalem project of the University of Antwerp. We also gratefully acknowledge the NH3-TPD analysis performed by Sander Bossier. |
Approved |
Most recent IF: 5.3; 2023 IF: 4.636 |
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Call Number |
UA @ admin @ c:irua:197268 |
Serial |
8917 |
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Author |
Mosquera, J.; Wang, D.; Bals, S.; Liz-Marzan, L.M. |
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Title |
Surfactant layers on gold nanorods |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Accounts of chemical research |
Abbreviated Journal |
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Volume |
56 |
Issue |
10 |
Pages |
1204-1212 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Gold nanorods (Au NRs) are an exceptionally promising tool in nanotechnology due to three key factors: (i) their strong interaction with electromagnetic radiation, stemming from their plasmonic nature, (ii) the ease with which the resonance frequency of their longitudinal plasmon mode can be tuned from the visible to the near-infrared region of the electromagnetic spect r u m based on their aspect ratio, and (iii) their simple and cost-effective preparation through seed-mediated chemical growth. In this synthetic method, surfactants play a critical role in controlling the size, shape, and colloidal stabi l i t y of Au NRs. For example, surfactants can stabilize specific crystallographic facets during the formation of Au NRs, leading to t h e formation of NRs with specific morphologies. The process of surfactant adsorption onto the NR surface may result in various assemblies of surfactant molecules, such as spherical micelles, elongated micelles, or bilayers. Again, the assembly mode is critical toward determining the further availabi l i t y of the Au NR surface to the surrounding medium. Despite its importance and a great deal of research effort, the interaction between Au NPs and surfactants remains insufficiently understood, because the assembly process is influenced by numerous factors, including the chemical nature of the surfactant, the surface morphology of Au NPs, and solution parameters. Therefore, gaining a more comprehensive understanding of these interactions is essential to unlock the full potential of the seed-mediated growth method and the applications of plasmonic NPs. A plethora of characterization techniques have been applied to reach such an understanding , but many open questions remain. In this Account, we review the current knowledge on the interactions between surfactants and Au NRs. We briefly introduce the state-of-the-art methods for synthesizing Au NRs and highlight the crucial role of cationic surfactants during this process. The self-assembly and organization of surfactants on the Au NR surface is then discussed to better understand their role in seed-mediated growth. Subsequently, we provide examples and elucidate how chemical additives can be used to modulate micellar assemblies, in turn allowing for a finer control over the growth of Au NRs, including chiral NRs. Next, we review the main experimental characterization and computational modeling techniques that have been applied to shed light on the arrangement of surfactants on Au NRs and summarize the advantages and disadvantages for each technique. The Account ends with a “Conclusions and Outlook” section, outlining promising future research directions and developments that we consider are sti l l required, mostly related to the application of electron microscopy in liquid and in 3D. Finally, we remark on the potential of exploiting machine learning techniques to predict synthetic routes for NPs with predefined structures and properties. |
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Wos |
000986447000001 |
Publication Date |
2023-05-08 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0001-4842 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
18.3 |
Times cited |
8 |
Open Access |
OpenAccess |
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Notes |
The authors acknowledge financial support by the European Research Council (ERC CoG No. 815128 REALNANO to S.B.; ERC AdG No. 787510, 4DbioSERS to L.M.L.-M.) , from MCIN/AEI/10.13039/501100011033 and “ESF Investing in your future” (Grant PID2020-117779RB-I00 to L.M.L.-M. and Grants RYC2019-027842-I , PID2020-117885GA-I00 to J.M.) , and by Guangdong Provincial Key Laboratory of Optical Information Materials and Technology (No. 2017B030301007) , National Center for International Research on Green Optoelectronics (No. 2016B01018) , MOE Interna-tional Laboratory for Optical Information Technologies, and the 111 projects. |
Approved |
Most recent IF: 18.3; 2023 IF: 20.268 |
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Call Number |
UA @ admin @ c:irua:196768 |
Serial |
8940 |
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Author |
de la Encarnación, C.; Jungwirth, F.; Vila-Liarte, D.; Renero-Lecuna, C.; Kavak, S.; Orue, I.; Wilhelm, C.; Bals, S.; Henriksen-Lacey, M.; Jimenez de Aberasturi, D.; Liz-Marzán, L.M. |
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Title |
Hybrid core–shell nanoparticles for cell-specific magnetic separation and photothermal heating |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Journal of materials chemistry B : materials for biology and medicine |
Abbreviated Journal |
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Volume |
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Issue |
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Pages |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Hyperthermia, as the process of heating a malignant site above 42 °C to trigger cell death, has emerged as an effective and selective cancer therapy strategy. Various modalities of hyperthermia have been proposed, among which magnetic and photothermal hyperthermia are known to benefit from the use of nanomaterials. In this context, we introduce herein a hybrid colloidal nanostructure comprising plasmonic gold nanorods (AuNRs) covered by a silica shell, onto which iron oxide nanoparticles (IONPs) are subsequently grown. The resulting hybrid nanostructures are responsive to both external magnetic fields and near-infrared irradiation. As a result, they can be applied for the targeted magnetic separation of selected cell populations – upon targeting by antibody functionalization – as well as for photothermal heating. Through this combined functionality, the therapeutic effect of photothermal heating can be enhanced. We demonstrate both the fabrication of the hybrid system and its application for targeted photothermal hyperthermia of human glioblastoma cells. |
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Wos |
000968908400001 |
Publication Date |
2023-04-05 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2050-750X |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7 |
Times cited |
1 |
Open Access |
OpenAccess |
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Notes |
Ministerio de Ciencia e Innovación, PID2019-108854RA-I00 ; H2020 European Research Council, ERC AdG 787510, 4DBIOSERS ERC CoG 815128, REALNANO ; Fonds Wetenschappelijk Onderzoek, PhD research grant 1181122N ; |
Approved |
Most recent IF: 7; 2023 IF: 4.543 |
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Call Number |
EMAT @ emat @c:irua:195879 |
Serial |
7261 |
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| Permanent link to this record |
