Records |
Author |
Zhuo, X.; Mychinko, M.; Heyvaert, W.; Larios, D.; Obelleiro-Liz, M.; Taboada, J.M.; Bals, S.; Liz-Marzán, L.M. |
Title |
Morphological and Optical Transitions during Micelle-Seeded Chiral Growth on Gold Nanorods |
Type |
A1 Journal article |
Year |
2022 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
Volume |
|
Issue |
|
Pages |
|
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
Chiral plasmonics is a rapidly developing field where breakthroughs and unsolved problems coexist. We have recently reported binary surfactant-assisted seeded growth of chiral gold nanorods (Au NRs) with high chiroptical activity. Such a seeded-growth process involves the use of a chiral cosurfactant that induces micellar helicity, in turn driving the transition from achiral to chiral Au NRs, from both the morphological and the optical points of view. We report herein a detailed study on both transitions, which reveals intermediate states that were hidden so far. The correlation between structure and optical response is carefully analyzed, including the (linear and CD) spectral evolution over time, electron tomography, the impact of NR dimensions on their optical response, the variation of the absorption-to-scattering ratio during the evolution from achiral to chiral Au NRs, and the near-field enhancement related to chiral plasmon modes. Our findings provide further understanding of the growth process of chiral Au NRs and the associated optical changes, which will facilitate further study and applications of chiral nanomaterials. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000878324400001 |
Publication Date |
2022-10-26 |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
Series Volume |
|
Series Issue |
|
Edition |
|
ISSN |
1936-0851 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
17.1 |
Times cited |
17 |
Open Access |
OpenAccess |
Notes |
This work was supported by the European Research Council (ERC-AdG-4DbioSERS-787510 to L.M.L.-M. and ERC-CoG-REALNANO-815128 to S.B.) and the MCIN/AEI/10.13039/501100011033 (Grant PID2020-117779RB-I00). X.Z. acknowledges funding from the Juan de la Cierva fellowship (FJC2018-036104-I) and the University Development Fund (UDF01002665, CUHK-Shenzhen). D.L., M.O.-L., and J.M.T. acknowledge funding from the European Regional Development Fund (ERDF) and the Spanish Ministerio de Ciencia, Innovación y Universidades, under Projects PID2020-116627RB-C21 and PID2020-116627RB-C22, as well as from the ERDF/Galician Regional Government as part of the agreement for funding the Atlantic Research Center for Information and Communication Technologies (atlanTTic) and ERDF/Extremadura Regional Government under Projects IB18073 and GR18055. This work was performed in the framework of the Maria de Maeztu Units of Excellence Program from the Spanish State Research Agency (Grant No. MDM-2017-0720). The authors acknowledge Dr. Guillermo González-Rubio for providing suggestions for synthesis and Dr. Irantzu Llarena for assisting with the CD measurements. |
Approved |
Most recent IF: 17.1 |
Call Number |
EMAT @ emat @c:irua:191815 |
Serial |
7116 |
Permanent link to this record |
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Author |
Sa, J.; Hu, N.; Heyvaert, W.; Van Gordon, K.; Li, H.; Wang, L.; Bals, S.; Liz-Marzán, L.M.; Ni, W. |
Title |
Spontaneous Chirality Evolved at the Au–Ag Interface in Plasmonic Nanorods |
Type |
A1 Journal article |
Year |
2023 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem. Mater. |
Volume |
|
Issue |
|
Pages |
|
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
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. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
001052093300001 |
Publication Date |
2023-08-21 |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
Series Volume |
|
Series Issue |
|
Edition |
|
ISSN |
0897-4756 |
ISBN |
|
Additional Links |
UA library record; WoS full record |
Impact Factor |
8.6 |
Times cited |
|
Open Access |
OpenAccess |
Notes |
The authors acknowledge the financial support from the National Natural Science Foundation of China (grant 22074102). LMLM acknowledges funding from 26 MCIN/AEI/10.13039/501100011033 and “ESF Investing in your future” (Grant PID2020- 117779RB-I00). This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 823717 – ESTEEM3.; Ministerio de Ciencia e Innovaci?n, PID2020-117779RB-I00 ; H2020 Research Infrastructures, 823717 ; European Social Fund, PID2020-117779RB-I00 ; National Natural Science Foundation of China, 22074102 ; |
Approved |
Most recent IF: 8.6; 2023 IF: 9.466 |
Call Number |
EMAT @ emat @c:irua:198151 |
Serial |
8810 |
Permanent link to this record |
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|
|
Author |
Spaeth, P.; Adhikari, S.; Heyvaert, W.; Zhuo, X.; Garcia, I.; Liz-Marzan, L.M.; Bals, S.; Orrit, M.; Albrecht, W. |
Title |
Photothermal circular dichroism measurements of single chiral gold nanoparticles correlated with electron tomography |
Type |
A1 Journal article |
Year |
2022 |
Publication |
ACS Photonics |
Abbreviated Journal |
Acs Photonics |
Volume |
9 |
Issue |
12 |
Pages |
3995-4004 |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
Chemically synthesized metal nanoparticles with morphological chiral features are known to exhibit strong circular dichroism. However, we still lack understanding of the correlation between morphological and chiroptical features of plasmonic nanoparticles. To shed light on that question, single nanoparticle experiments are required. We performed photothermal circular dichroism measurements of single chiral and achiral gold nanoparticles and correlated the chiroptical response to the 3D morphology of the same nanoparticles retrieved by electron tomography. In contrast to an ensemble measurement, we show that individual particles within the ensemble display a broad distribution of strength and handedness of circular dichroism signals. Whereas obvious structural chiral features, such as helical wrinkles, translate into chiroptical ones, nanoparticles with less obvious chiral morphological features can also display strong circular dichroism signals. Interestingly, we find that even seemingly achiral nanoparticles can display large g-factors. The origin of this circular dichroism signal is discussed in terms of plasmonics and other potentially relevant factors. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000884432100001 |
Publication Date |
2022-11-08 |
Series Editor |
|
Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
ISSN |
2330-4022 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
7 |
Times cited |
5 |
Open Access |
OpenAccess |
Notes |
This work was supported by The Netherlands Organisation for Scientific Research (NWO) as part of the Open Technology Program (OTP, Project No. 16008) and by a Spinoza prize (M.O.) . W.A. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020 Program (Grant No. 797153, SOPMEN) . L.M.L.M. acknowledges funding from MCIN/AEI/10.13039/501100011033 (Grants PID2020-117779RB-I00 and MDM-2017-0720) . We thank Dr. Wolfgang L?fer for providing optical equipment. We also acknowledge the European Soft Matter Infrastructure (EUSMI: E201200468) . |
Approved |
Most recent IF: 7 |
Call Number |
UA @ admin @ c:irua:192098 |
Serial |
7331 |
Permanent link to this record |
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|
|
Author |
Sentosun, K.; Sanz Ortiz, M.N.; Batenburg, K.J.; Liz-Marzán, L.M.; Bals, S. |
Title |
Combination of HAADF-STEM and ADF-STEM Tomography for Core-Shell Hybrid Materials |
Type |
A1 Journal article |
Year |
2015 |
Publication |
Particle and particle systems characterization |
Abbreviated Journal |
Part Part Syst Char |
Volume |
32 |
Issue |
32 |
Pages |
1063-1067 |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Vision lab |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
Characterization of core-shell type nanoparticles in 3D by transmission electron microscopy (TEM) can be very challenging. Especially when both heavy and light elements co-exist within the same nanostructure, artefacts in the 3D reconstruction are often present. A representative example would be a particle comprising an anisotropic metallic (Au) nanoparticle coated with a (mesoporous) silica shell. To obtain a reliable 3D characterization of such an object, we propose a dose-efficient strategy to simultaneously acquire high angle annular dark field scanning TEM and annular dark field tilt series for tomography. The 3D reconstruction is further improved by applying an advanced masking and interpolation approach to the acquired data. This new methodology enables us to obtain high quality reconstructions from which also quantitative information can be extracted. This approach is broadly applicable to investigate hybrid core-shell materials. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000368446800003 |
Publication Date |
2015-10-13 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
ISSN |
0934-0866; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
4.474 |
Times cited |
13 |
Open Access |
OpenAccess |
Notes |
S.B. acknowledges financial support from European Research Council (ERC) (ERC Starting Grant #335078-COLOURATOM). L.M. acknowledges funding from the EU, Grant# 310651-2 Self-Assembly in Confined Space (SACS). K.J.B acknowledges financial support from the Netherlands Organisation for Scientific Research (NWO), project number 639.072.005 and NWO CW 700.57.026. Networking support was provided by COST Action MP1207. The authors acknowledge the European Union under the Seventh Framework Program under a contract for an Integrated Infrastructure Initiative, Reference No. 312483-ESTEEM2 for financial support.; esteem2jra4; ECASSara; (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:cannot); |
Approved |
Most recent IF: 4.474; 2015 IF: 3.081 |
Call Number |
c:irua:129590 c:irua:129590 |
Serial |
3967 |
Permanent link to this record |
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Author |
Leroux, F.; Gysemans, M.; Bals, S.; Batenburg, K.J.; Snauwaert, J.; Verbiest, T.; van Haesendonck, C.; Van Tendeloo, G. |
Title |
Three-dimensional characterization of helical silver nanochains mediated by protein assemblies |
Type |
A1 Journal article |
Year |
2010 |
Publication |
Advanced materials |
Abbreviated Journal |
Adv Mater |
Volume |
22 |
Issue |
19 |
Pages |
2193-2197 |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Vision lab |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
Characterization methods for the structural investigation of biotemplates for nanodevices remain widely unexplored, despite the fact that biotemplating methods for nanodevice fabrication are becoming more widespread. In this study several techniques are used to characterize the morphology and 3D distribution of silver nanoparticles deposited on insulin fibrils. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
|
Place of Publication |
Weinheim |
Editor |
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Language |
|
Wos |
000278601400016 |
Publication Date |
2010-03-11 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
ISSN |
0935-9648;1521-4095; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
19.791 |
Times cited |
51 |
Open Access |
|
Notes |
Esteem 026019; Fwo |
Approved |
Most recent IF: 19.791; 2010 IF: NA |
Call Number |
UA @ lucian @ c:irua:83296 |
Serial |
3645 |
Permanent link to this record |
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Author |
di Vece, M.; Bals, S.; Lievens, P.; Van Tendeloo, G. |
Title |
Compositional changes of Pd-Au bimetallic nanoclusters upon hydrogenation |
Type |
A1 Journal article |
Year |
2009 |
Publication |
Physical review : B : solid state |
Abbreviated Journal |
Phys Rev B |
Volume |
80 |
Issue |
12 |
Pages |
125420,1-125420,4 |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
Changes in the size distribution and composition of bimetallic Pd-Au nanoclusters have been observed after hydrogen exposure. This effect is caused by hydrogen-induced Ostwald ripening whereby the hydrogen reduces the binding energy of the cluster atoms leading to their detachment from the cluster. The composition changes due to a difference in mobility of the detached palladium and gold atoms on the surface. Fast palladium atoms contribute to the formation of larger nanoclusters, while the slower gold atoms are confined to the smaller nanoclusters. These transformations in the Pd-Au nanocluster size and composition set a limit for chemical reactions in which such nanoclusters are involved together with hydrogen. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
Lancaster, Pa |
Editor |
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Language |
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Wos |
000270383300121 |
Publication Date |
2009-09-23 |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
Series Volume |
|
Series Issue |
|
Edition |
|
ISSN |
1098-0121;1550-235X; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
3.836 |
Times cited |
28 |
Open Access |
|
Notes |
Fwo; Goa; Iap-Vi; Esteem 026019 |
Approved |
Most recent IF: 3.836; 2009 IF: 3.475 |
Call Number |
UA @ lucian @ c:irua:79232 |
Serial |
445 |
Permanent link to this record |
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Author |
Werner, R.; Raisch, C.; Leca, V.; Ion, V.; Bals, S.; Van Tendeloo, G.; Chasse, T.; Kleiner, R.; Koelle, D. |
Title |
Transport, magnetic, and structural properties of La0.7Ce0.3MnO3 thin films: evidence for hole-doping |
Type |
A1 Journal article |
Year |
2009 |
Publication |
Physical review : B : solid state |
Abbreviated Journal |
Phys Rev B |
Volume |
79 |
Issue |
5 |
Pages |
054416,1-054416,8 |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
Cerium-doped manganite thin films were grown epitaxially by pulsed laser deposition at 720 °C and oxygen pressure pO2=125 Pa and were subjected to different annealing steps. According to x-ray diffraction (XRD) data, the formation of CeO2 as a secondary phase could be avoided for pO28 Pa. However, transmission electron microscopy shows the presence of CeO2 nanoclusters even in those films which appear to be single phase in XRD. With O2 annealing, the metal-to-insulator transition temperature increases, while the saturation magnetization decreases and stays well below the theoretical value for electron-doped La0.7Ce0.3MnO3 with mixed Mn3+/Mn2+ valences. The same trend is observed with decreasing film thickness from 100 to 20 nm, indicating a higher oxygen content for thinner films. Hall measurements on a film which shows a metal-to-insulator transition clearly reveal holes as dominating charge carriers. Combining data from x-ray photoemission spectroscopy, for determination of the oxygen content, and x-ray absorption spectroscopy (XAS), for determination of the hole concentration and cation valences, we find that with increasing oxygen content the hole concentration increases and Mn valences are shifted from 2+ to 4+. The dominating Mn valences in the films are Mn3+ and Mn4+, and only a small amount of Mn2+ ions can be observed by XAS. Mn2+ and Ce4+ XAS signals obtained in surface-sensitive total electron yield mode are strongly reduced in the bulk-sensitive fluorescence mode, which indicates hole-doping in the bulk for those films which do show a metal-to-insulator transition. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
|
Place of Publication |
Lancaster, Pa |
Editor |
|
Language |
|
Wos |
000263815400057 |
Publication Date |
2009-02-13 |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
Series Volume |
|
Series Issue |
|
Edition |
|
ISSN |
1098-0121;1550-235X; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
3.836 |
Times cited |
25 |
Open Access |
|
Notes |
Esteem 026019; Fwo |
Approved |
Most recent IF: 3.836; 2009 IF: 3.475 |
Call Number |
UA @ lucian @ c:irua:76221 |
Serial |
3725 |
Permanent link to this record |
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Author |
Leroux, O.; Leroux, F.; Bagniewska-Zadworna,.; Knox, J.P.; Claeys, M.; Bals, S.; Viane, R.L.L. |
Title |
Ultrastructure and composition of cell wall appositions in the roots of Asplenium (Polypodiales) |
Type |
A1 Journal article |
Year |
2011 |
Publication |
Micron |
Abbreviated Journal |
Micron |
Volume |
42 |
Issue |
8 |
Pages |
863-870 |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
Cell wall appositions (CWAs), formed by the deposition of extra wall material at the contact site with microbial organisms, are an integral part of the response of plants to microbial challenge. Detailed histological studies of CWAs in fern roots do not exist. Using light and electron microscopy we examined the (ultra)structure of CWAs in the outer layers of roots of Asplenium species. All cell walls studded with CWAs were impregnated with yellow-brown pigments. CWAs had different shapes, ranging from warts to elongated branched structures, as observed with scanning and transmission electron microscopy. Ultrastructural study further showed that infecting fungi grow intramurally and that they are immobilized by CWAs when attempting to penetrate intracellularly. Immunolabelling experiments using monoclonal antibodies indicated pectic homogalacturonan, xyloglucan, mannan and cellulose in the CWAs, but tests for lignins and callose were negative. We conclude that these appositions are defense-related structures made of a non-lignified polysaccharide matrix on which phenolic compounds are deposited in order to create a barrier protecting the root against infections. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
|
Place of Publication |
Oxford |
Editor |
|
Language |
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Wos |
000294942600013 |
Publication Date |
2011-06-24 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
ISSN |
0968-4328; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
1.98 |
Times cited |
20 |
Open Access |
|
Notes |
Fwo |
Approved |
Most recent IF: 1.98; 2011 IF: 1.527 |
Call Number |
UA @ lucian @ c:irua:92540 |
Serial |
3798 |
Permanent link to this record |
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Author |
Pietra, F.; van Dijk-Moes, R.J.A.; Ke, X.; Bals, S.; Van Tendeloo, G.; de Mello Donega, C.; Vanmaekelbergh, D. |
Title |
Synthesis of highly luminescent silica-coated CdSe/CdS nanorods |
Type |
A1 Journal article |
Year |
2013 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
Volume |
25 |
Issue |
17 |
Pages |
3427-3434 |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
CdSe(core)/CdS(shell) nanorods (NRs) have been extensively investigated for their unique optical properties, such as high photoluminescence (PL) quantum efficiency (QE) and polarized light emission. The incorporation of these NRs in silica (SiO2) is of high interest, since this renders them processable in polar solvents while increasing their photochemical stability, which would be beneficial for their application in LEDs and as biolabels. We report the synthesis of highly luminescent silica-coated CdSe/CdS NRs, by using the reverse micelle method. The mechanism for the encapsulation of the NRs in silica is unravelled and shown to be strongly influenced by the NR shape and its asymmetry. This is attributed to both the different morphology and the different crystallographic nature of the facets terminating the opposite tips of the NRs. These results lead to the formation of a novel class of NR architectures, whose symmetry can be controlled by tuning the degree of coverage of the silica shell. Interestingly, the encapsulation of the NRs in silica leads to a remarkable increase in their photostability, while preserving their optical properties. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
|
Place of Publication |
Washington, D.C. |
Editor |
|
Language |
|
Wos |
000330097900004 |
Publication Date |
2013-08-13 |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
ISSN |
0897-4756;1520-5002; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
9.466 |
Times cited |
46 |
Open Access |
|
Notes |
262348 ESMI; 246791 COUNTATOMS; Hercules |
Approved |
Most recent IF: 9.466; 2013 IF: 8.535 |
Call Number |
UA @ lucian @ c:irua:110037 |
Serial |
3456 |
Permanent link to this record |
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|
|
Author |
He, Z.; Ke, X.; Bals, S.; Van Tendeloo, G. |
Title |
Direct evidence for the existence of multi-walled carbon nanotubes with hexagonal cross-sections |
Type |
A1 Journal article |
Year |
2012 |
Publication |
Carbon |
Abbreviated Journal |
Carbon |
Volume |
50 |
Issue |
7 |
Pages |
2524-2529 |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
Carbon nanotubes (CNTs) with a polygonal cross-section have been paid increasing attention since their three-dimensional structure is related to specific physical properties, which are found to be different in comparison to CNTs with a circular cross-section. Here, we report the existence of novel multi-walled CNTs yielding walls with a rounded-hexagonal configuration. This structure was directly confirmed for the first time by both cross-sectional transmission electron microscopy and electron tomography. The morphology of the Fe catalytic particle also exhibits hexagonal characteristics, and is proposed as the origin of the formation of the rounded-hexagonal walls of the CNT. This observation is of great importance with respect to the design of polygonal (such as pentagonal or hexagonal) cross-sectional CNTs. By controlling the morphology of the catalytic nanoparticles it will be possible to grow CNTs with desired electronic and mechanical properties. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
Oxford |
Editor |
|
Language |
|
Wos |
000303038400015 |
Publication Date |
2012-02-06 |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
ISSN |
0008-6223; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
6.337 |
Times cited |
8 |
Open Access |
|
Notes |
Fwo |
Approved |
Most recent IF: 6.337; 2012 IF: 5.868 |
Call Number |
UA @ lucian @ c:irua:96956 |
Serial |
711 |
Permanent link to this record |
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|
Author |
Van Velthoven, N.; Waitschat, S.; Chavan, S.M.; Liu, P.; Smolders, S.; Vercammen, J.; Bueken, B.; Bals, S.; Lillerud, K.P.; Stock, N.; De Vos, D.E. |
Title |
Single-site metal-organic framework catalysts for the oxidative coupling of arenes via C-H/C-H activation |
Type |
A1 Journal article |
Year |
2019 |
Publication |
Chemical science |
Abbreviated Journal |
Chem Sci |
Volume |
10 |
Issue |
10 |
Pages |
3616-3622 |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
C-H activation reactions are generally associated with relatively low turnover numbers (TONs) and high catalyst concentrations due to a combination of low catalyst stability and activity, highlighting the need for recyclable heterogeneous catalysts with stable single-atom active sites. In this work, several palladium loaded metal-organic frameworks (MOFs) were tested as single-site catalysts for the oxidative coupling of arenes (e.g. o-xylene) via C-H/C-H activation. Isolation of the palladium active sites on the MOF supports reduced Pd(0) aggregate formation and thus catalyst deactivation, resulting in higher turnover numbers (TONs) compared to the homogeneous benchmark reaction. Notably, a threefold higher TON could be achieved for palladium loaded MOF-808 due to increased catalyst stability and the heterogeneous catalyst could efficiently be reused, resulting in a cumulative TON of 1218 after three runs. Additionally, the palladium single-atom active sites on MOF-808 were successfully identified by Fourier transform infrared (FTIR) and extended X-ray absorption fine structure (EXAFS) spectroscopy. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000463759100017 |
Publication Date |
2019-02-18 |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
Series Volume |
|
Series Issue |
|
Edition |
|
ISSN |
2041-6520 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
8.668 |
Times cited |
68 |
Open Access |
OpenAccess |
Notes |
; The research leading to these results has received funding from the NMBP-01-2016 Program of the European Union's Horizon 2020 Framework Program H2020/2014-2020/under grant agreement no. [720996]. N. V. V., S. S., J. V., B. B. and D. E. D. V. thank the FWO for funding (SB, Aspirant and postdoctoral grants). The electron microscopy work was supported by FWO funding G038116. D. E. D. V. is grateful for KU Leuven support in the frame of the CASAS Metusalem project and a C3 type project. The XAS experiments were performed on beamline BM26A at the European Synchrotron Radiation Facility (ESRF), Grenoble, France. We are grateful to D. Banerjee at the ESRF for providing assistance in using beamline BM26A. Johnson Matthey and S. Bennett are gratefully acknowledged for providing Smopex-102. ; |
Approved |
Most recent IF: 8.668 |
Call Number |
UA @ admin @ c:irua:159403 |
Serial |
5259 |
Permanent link to this record |
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Author |
Ustarroz, J.; Altantzis, T.; Hammons, J.A.; Hubin, A.; Bals, S.; Terryn, H. |
Title |
The role of nanocluster aggregation, coalescence, and recrystallization in the electrochemical deposition of platinum nanostructures |
Type |
A1 Journal article |
Year |
2014 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
Volume |
26 |
Issue |
7 |
Pages |
2396-2406 |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
By using an optimized characterization approach that combines aberration-corrected transmission electron microscopy, electron tomography, and in situ ultrasmall angle X-ray scattering (USAXS), we show that the early stages of Pt electrochemical growth on carbon substrates may be affected by the aggregation, self-alignment, and partial coalescence of nanoclusters of d ≈ 2 nm. The morphology of the resulting nanostructures depends on the degree of coalescence and recrystallization of nanocluster aggregates, which in turn depends on the electrodeposition potential. At low overpotentials, a self-limiting growth mechanism may block the epitaxial growth of primary nanoclusters and results in loose dendritic aggregates. At more negative potentials, the extent of nanocluster coalescence and recrystallization is larger and further growth by atomic incorporation may be allowed. On one hand, this suggests a revision of the VolmerWeber island growth mechanism. Whereas this theory has traditionally assumed direct attachment as the only growth mechanism, it is suggested that nanocluster self-limiting growth, aggregation, and coalescence should also be taken into account during the early stages of nanoscale electrodeposition. On the other hand, depending on the deposition potential, ultrahigh porosities can be achieved, turning electrodeposition in an ideal process for highly active electrocatalyst production without the need of using high surface area carbon supports. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
Washington, D.C. |
Editor |
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Language |
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Wos |
000334572300026 |
Publication Date |
2014-03-10 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
ISSN |
0897-4756;1520-5002; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
9.466 |
Times cited |
55 |
Open Access |
Not_Open_Access |
Notes |
FWO; contract no. FWOAL527 |
Approved |
Most recent IF: 9.466; 2014 IF: 8.354 |
Call Number |
UA @ lucian @ c:irua:116956 |
Serial |
2916 |
Permanent link to this record |
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Author |
Smith, J.D.; Bladt, E.; Burkhart, J.A.C.; Winckelmans, N.; Koczkur, K.M.; Ashberry, H.M.; Bals, S.; Skrabalak, S.E. |
Title |
Defect‐Directed Growth of Symmetrically Branched Metal Nanocrystals |
Type |
A1 Journal article |
Year |
2020 |
Publication |
Angewandte Chemie (International ed. Print) |
Abbreviated Journal |
Angew. Chem. |
Volume |
132 |
Issue |
132 |
Pages |
953-960 |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
Branched plasmonic nanocrystals (NCs) have attracted much attention due to electric field enhancements at their tips. Seeded growth provides routes to NCs with defined branching patterns and, in turn, near‐field distributions with defined symmetries. Here, a systematic analysis was undertaken in which seeds containing different distributions of planar defects were used to grow branched NCs in order to understand how their distributions direct the branching. Characterization of the products by multimode electron tomography and analysis of the NC morphologies at different overgrowth stages indicate that the branching patterns are directed by the seed defects, with the emergence of branches from the seed faces consistent with minimizing volumetric strain energy at the expense of surface energy. These results contrast with growth of branched NCs from single‐crystalline seeds and provide a new platform for the synthesis of symmetrically branched plasmonic NCs. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000505279500063 |
Publication Date |
2020-01-07 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
ISSN |
0044-8249 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
|
Times cited |
|
Open Access |
OpenAccess |
Notes |
The authors thank Samantha Harvey for her initial observations of branched structures, Alexander Chen for his help with SAED, the staff of the Nanoscale Characterization Facility (Dr. Yi Yi),Electron Microscopy Center (Dr. David Morgan and Dr. Barry Stein), and Molecular Strucre Center at Indiana University. J.S. recognizes a fellowship provided by the Indiana Space Grant Consortium. E. B. acknowledges a post-doctoral grant from the Research Foundation Flanders (FWO, Belgium). This project has received funding from the National Science Foundation (award number: 1602476), Research Corporation for Scietific Advancement (2017 Frontiers in Research Excellence and Discovery Award), and the European Union’s Horizon 2020 research and innovation program under grant agreement No 731019 (EUSMI) and No 815128 (REALNANO).; sygma |
Approved |
Most recent IF: NA |
Call Number |
EMAT @ emat @c:irua:166581 |
Serial |
6336 |
Permanent link to this record |
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|
|
Author |
Smith, J.D.; Bladt, E.; Burkhart, J.A.C.; Winckelmans, N.; Koczkur, K.M.; Ashberry, H.M.; Bals, S.; Skrabalak, S.E. |
Title |
Defect-directed growth of symmetrically branched metal nanocrystals |
Type |
A1 Journal article |
Year |
2020 |
Publication |
Angewandte Chemie-International Edition |
Abbreviated Journal |
Angew Chem Int Edit |
Volume |
59 |
Issue |
59 |
Pages |
943-950 |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
Branched plasmonic nanocrystals (NCs) have attracted much attention due to electric field enhancements at their tips. Seeded growth provides routes to NCs with defined branching patterns and, in turn, near-field distributions with defined symmetries. Here, a systematic analysis was undertaken in which seeds containing different distributions of planar defects were used to grow branched NCs in order to understand how their distributions direct the branching. Characterization of the products by multimode electron tomography and analysis of the NC morphologies at different overgrowth stages indicate that the branching patterns are directed by the seed defects, with the emergence of branches from the seed faces consistent with minimizing volumetric strain energy at the expense of surface energy. These results contrast with growth of branched NCs from single-crystalline seeds and provide a new platform for the synthesis of symmetrically branched plasmonic NCs. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000498760200001 |
Publication Date |
2019-11-13 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
ISSN |
1433-7851; 0570-0833 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
16.6 |
Times cited |
23 |
Open Access |
OpenAccess |
Notes |
; The authors thank Samantha Harvey for her initial observations of branched structures, Alexander Chen for his help with SAED, the staff of the Nanoscale Characterization Facility (Dr. Yi Yi), Electron Microscopy Center (Dr. David Morgan and Dr. Barry Stein), and Molecular Structure Center at Indiana University. J.S. recognizes a fellowship provided by the Indiana Space Grant Consortium. E.B. acknowledges a post-doctoral grant from the Research Foundation Flanders (FWO, Belgium). This project has received funding to S.E.S. from the U.S. National Science Foundation (award numbers: 1602476 and 1904499) and Research Corporation for Scientific Advancement (2017 Frontiers in Research Excellence and Discovery Award) as well as to S.B. from the European Union's Horizon 2020 research and innovation program under grant agreement No 731019 (EUSMI) and No 815128 (REALNANO). ; sygma |
Approved |
Most recent IF: 16.6; 2020 IF: 11.994 |
Call Number |
UA @ admin @ c:irua:165124 |
Serial |
6293 |
Permanent link to this record |
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Author |
Goris, B.; van Huis, M.A.; Bals, S.; Zandbergen, H.W.; Manna, L.; Van Tendeloo, G. |
Title |
Thermally induced structural and morphological changes of CdSe/CdS octapods |
Type |
A1 Journal article |
Year |
2012 |
Publication |
Small |
Abbreviated Journal |
Small |
Volume |
8 |
Issue |
6 |
Pages |
937-942 |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
Branched nanostructures are of great interest because of their promising optical and electronic properties. For successful and reliable integration in applications such as photovoltaic devices, the thermal stability of the nanostructures is of major importance. Here the different domains (CdSe cores, CdS pods) of the heterogeneous octapods are shown to have different thermal stabilities, and heating is shown to induce specific shape changes. The octapods are heated from room temperature to 700 °C, and investigated using (analytical and tomographic) transmission electron microscopy (TEM). At low annealing temperatures, pure Cd segregates in droplets at the outside of the octapods, indicating non-stochiometric composition of the octapods. Furthermore, the tips of the pods lose their faceting and become rounded. Further heating to temperatures just below the sublimation temperature induces growth of the zinc blende core at the expense of the wurtzite pods. At higher temperatures, (500700 °C), sublimation of the octapods is observed in real time in the TEM. Three-dimensional tomographic reconstructions reveal that the four pods pointing into the vacuum have a lower thermal stability than the four pods that are in contact with the support. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
Weinheim |
Editor |
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Language |
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Wos |
000301718800021 |
Publication Date |
2012-01-31 |
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 |
|
ISSN |
1613-6810; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
8.643 |
Times cited |
20 |
Open Access |
|
Notes |
Fwo; Esteem 026019 |
Approved |
Most recent IF: 8.643; 2012 IF: 7.823 |
Call Number |
UA @ lucian @ c:irua:95040 |
Serial |
3633 |
Permanent link to this record |
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Author |
Monticelli, O.; Musina, Z.; Russo, S.; Bals, S. |
Title |
On the use of TEM in the characterization of nanocomposites |
Type |
A1 Journal article |
Year |
2007 |
Publication |
Materials letters |
Abbreviated Journal |
Mater Lett |
Volume |
61 |
Issue |
16 |
Pages |
3446-3450 |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
Both an organically modified commercial clay of montmorillonite type (MMT) and its nanocomposites, based either on polyamide 6 (PA6) or an epoxy resin, as matrix polymer, have been characterized by transmission electron microscopy (TEM). Sample micrographs, taken at increasing exposure times (t(e)), have shown the gradual disappearance of clay layers, because of an amorphisation of the MMT crystalline structures caused by prolonged sample exposure to electron beam. Indeed, the above phenomenon, which is mostly evident in the case of intercalated nanocomposites, makes the detection of the layered silicate dispersion in the polymer matrix rather difficult and compels to perform TEM measurements using very short exposure times. Moreover, the microscopy accelerating voltage has turned out to affect sample stability; namely, when decreasing the above parameter, the disappearance of clay structure occurs at lower exposure times. (C) 2006 Elsevier B.V. All rights reserved. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
Amsterdam |
Editor |
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Language |
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Wos |
000247146100034 |
Publication Date |
2006-12-06 |
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 |
|
ISSN |
0167-577X; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
2.572 |
Times cited |
28 |
Open Access |
|
Notes |
|
Approved |
Most recent IF: 2.572; 2007 IF: 1.625 |
Call Number |
UA @ lucian @ c:irua:64757 |
Serial |
2460 |
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. |
Title |
Enabling hydrate-based methane storage under mild operating conditions by periodic mesoporous organosilica nanotubes |
Type |
A1 Journal article |
Year |
2023 |
Publication |
Heliyon |
Abbreviated Journal |
|
Volume |
9 |
Issue |
7 |
Pages |
e17662-14 |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
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. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
001056264100001 |
Publication Date |
2023-06-28 |
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 |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
|
Times cited |
4 |
Open Access |
OpenAccess |
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 |
Call Number |
UA @ admin @ c:irua:199249 |
Serial |
8862 |
Permanent link to this record |
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Author |
Irtem, E.; Arenas Esteban, D.; Duarte, M.; Choukroun, D.; Lee, S.; Ibáñez, M.; Bals, S.; Breugelmans, T. |
Title |
Ligand-Mode Directed Selectivity in Cu–Ag Core–Shell Based Gas Diffusion Electrodes for CO2Electroreduction |
Type |
A1 Journal article |
Year |
2020 |
Publication |
Acs Catalysis |
Abbreviated Journal |
Acs Catal |
Volume |
|
Issue |
|
Pages |
13468-13478 |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
Bimetallic nanoparticles with tailored size and specific composition have shown promise as stable and selective catalysts for electrochemical reduction of CO2 (CO2R) in batch systems. Yet, limited effort was devoted to understand the effect of ligand coverage and postsynthesis treatments on CO2 reduction, especially under industrially applicable conditions, such as at high currents (>100 mA/cm2) using gas diffusion electrodes (GDE) and flow reactors. In this work, Cu–Ag core–shell nanoparticles (11 ± 2 nm) were prepared with three different surface modes: (i) capped with oleylamine, (ii) capped with monoisopropylamine, and (iii) surfactant free with a reducing borohydride agent; Cu–Ag (OAm), Cu–Ag (MIPA), and Cu–Ag (NaBH4), respectively. The ligand exchange and removal was evidenced by infrared spectroscopy (ATR-FTIR) analysis, whereas high-resolution scanning transmission electron microscopy (HAADF-STEM) showed their effect on the interparticle distance and nanoparticle rearrangement. Later on, we developed a process-on-substrate method to track these effects on CO2R. Cu–Ag (OAm) gave a lower on-set potential for hydrocarbon production, whereas Cu–Ag (MIPA) and Cu–Ag (NaBH4) promoted syngas production. The electrochemical impedance and surface area analysis on the well-controlled electrodes showed gradual increases in the electrical conductivity and active surface area after each surface treatment. We found that the increasing amount of the triple phase boundaries (the meeting point for the electron–electrolyte–CO2 reactant) affect the required electrode potential and eventually the C+2e̅/C2e̅ product ratio. This study highlights the importance of the electron transfer to those active sites affected by the capping agents—particularly on larger substrates that are crucial for their industrial application. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000592978900031 |
Publication Date |
2020-11-04 |
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 |
|
ISSN |
2155-5435 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
12.9 |
Times cited |
23 |
Open Access |
OpenAccess |
Notes |
The authors also acknowledge financial support from the University Research Fund (BOF-GOA-PS ID No. 33928). S.L. has received funding from the European Union’s Horizon 2020 research and innovation program under the Marie SkłodowskaCurie Grant Agreement No. 665385. |
Approved |
Most recent IF: 12.9; 2020 IF: 10.614 |
Call Number |
EMAT @ emat @c:irua:173803 |
Serial |
6432 |
Permanent link to this record |
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Author |
Yang, S.; Liu, Z.; An, H.; Arnouts, S.; de Ruiter, J.; Rollier, F.; Bals, S.; Altantzis, T.; Figueiredo, M.C.; Filot, I.A.W.; Hensen, E.J.M.; Weckhuysen, B.M.; van der Stam, W. |
Title |
Near-unity electrochemical CO₂ to CO conversion over Sn-doped copper oxide nanoparticles |
Type |
A1 Journal article |
Year |
2022 |
Publication |
ACS catalysis |
Abbreviated Journal |
Acs Catal |
Volume |
12 |
Issue |
24 |
Pages |
15146-15156 |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
Bimetallic electrocatalysts have emerged as a viable strategy to tune the electrocatalytic CO2 reduction reaction (eCO2RR) for the selective production of valuable base chemicals and fuels. However, obtaining high product selectivity and catalyst stability remain challenging, which hinders the practical application of eCO2RR. In this work, it was found that a small doping concentration of tin (Sn) in copper oxide (CuO) has profound influence on the catalytic performance, boosting the Faradaic efficiency (FE) up to 98% for carbon monoxide (CO) at -0.75 V versus RHE, with prolonged stable performance (FE > 90%) for up to 15 h. Through a combination of ex situ and in situ characterization techniques, the in situ activation and reaction mechanism of the electrocatalyst at work was elucidated. In situ Raman spectroscopy measurements revealed that the binding energy of the crucial adsorbed *CO intermediate was lowered through Sn doping, thereby favoring gaseous CO desorption. This observation was confirmed by density functional theory, which further indicated that hydrogen adsorption and subsequent hydrogen evolution were hampered on the Sn-doped electrocatalysts, resulting in boosted CO formation. It was found that the pristine electrocatalysts consisted of CuO nanoparticles decorated with SnO2 domains, as characterized by ex situ high-resolution scanning transmission electron microscopy and X-ray photoelectron spectroscopy measurements. These pristine nanoparticles were subsequently in situ converted into a catalytically active bimetallic Sn-doped Cu phase. Our work sheds light on the intimate relationship between the bimetallic structure and catalytic behavior, resulting in stable and selective oxide-derived Sn-doped Cu electrocatalysts. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000900052400001 |
Publication Date |
2022-11-28 |
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 |
|
ISSN |
2155-5435 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
12.9 |
Times cited |
16 |
Open Access |
OpenAccess |
Notes |
B.M.W., S.Y., M.C.F., E.J.M.H., and W.v.d.S. acknowledge support from the Strategic UU-TU/e Alliance project ?Joint Centre for Chemergy Research?. S.B. acknowledges support from the European Research Council (ERC Consolidator grant #815128 REALNANO) . Z.L. acknowledges financial support of the China Scholarship Council and the Netherlands Organization for Scientific Research for access to computa-tional resources for carrying out the DFT calculations reported in this work. S.A. and T.A. acknowledge funding from theUniversity of Antwerp Research fund (BOF) . The authors also thank Dr. Jochem Wijten and Joris Janssens (Inorganic Chemistry and Catalysis, Utrecht University) for helpful technical support. Sander Deelen (Faculty of Science, Utrecht University) is acknowledged for the design of the in situ XRD cell. |
Approved |
Most recent IF: 12.9 |
Call Number |
UA @ admin @ c:irua:192742 |
Serial |
7325 |
Permanent link to this record |
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|
|
Author |
Choukroun, D.; Daems, N.; Kenis, T.; Van Everbroeck, T.; Hereijgers, J.; Altantzis, T.; Bals, S.; Cool, P.; Breugelmans, T. |
Title |
Bifunctional nickel-nitrogen-doped-carbon-supported copper electrocatalyst for CO2 reduction |
Type |
A1 Journal article |
Year |
2020 |
Publication |
Journal Of Physical Chemistry C |
Abbreviated Journal |
J Phys Chem C |
Volume |
124 |
Issue |
124 |
Pages |
1369-1381 |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Applied Electrochemistry & Catalysis (ELCAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
Bifunctionality is a key feature of many industrial catalysts, supported metal clusters and particles in particular, and the development of such catalysts for the CO2 reduction reaction (CO2RR) to hydrocarbons and alcohols is gaining traction in light of recent advancements in the field. Carbon-supported Cu nanoparticles are suitable candidates for integration in the state-of-the-art reaction interfaces, and here, we propose, synthesize, and evaluate a bifunctional Ni–N-doped-C-supported Cu electrocatalyst, in which the support possesses active sites for selective CO2 conversion to CO and Cu nanoparticles catalyze either the direct CO2 or CO reduction to hydrocarbons. In this work, we introduce the scientific rationale behind the concept, its applicability, and the challenges with regard to the catalyst. From the practical aspect, the deposition of Cu nanoparticles onto carbon black and Ni–N–C supports via an ammonia-driven deposition precipitation method is reported and explored in more detail using X-ray diffraction, thermogravimetric analysis, and hydrogen temperature-programmed reduction. High-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and energy-dispersive X-ray spectroscopy (EDXS) give further evidence of the presence of Cu-containing nanoparticles on the Ni–N–C supports while revealing an additional relationship between the nanoparticle’s composition and the electrode’s electrocatalytic performance. Compared to the benchmark carbon black-supported Cu catalysts, Ni–N–C-supported Cu delivers up to a 2-fold increase in the partial C2H4 current density at −1.05 VRHE (C1/C2 = 0.67) and a concomitant 10-fold increase of the CO partial current density. The enhanced ethylene production metrics, obtained by virtue of the higher intrinsic activity of the Ni–N–C support, point out toward a synergistic action between the two catalytic functionalities. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000508467700015 |
Publication Date |
2020-01-07 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
ISSN |
1932-7447; 1932-7455 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
3.7 |
Times cited |
24 |
Open Access |
OpenAccess |
Notes |
; N.D. acknowledges sponsoring from the research foundation of Flanders (FWO) in the frame of a postdoctoral grant (12Y3919N N.D.). J.H. greatly acknowledges the Research Foundation Flanders (FWO) for support through a postdoctoral fellowship (28761). T.V.E. and P.C. acknowledge financial support from the EU-Partial-PGMs project (H2020NMP-686086). The authors also acknowledge financial support from the university research fund (BOF-GOA PS ID No. 33928). ; |
Approved |
Most recent IF: 3.7; 2020 IF: 4.536 |
Call Number |
UA @ admin @ c:irua:165326 |
Serial |
6286 |
Permanent link to this record |
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|
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Author |
Ata, I.; Ben Dkhil, S.; Pfannmoeller, M.; Bals, S.; Duche, D.; Simon, J.-J.; Koganezawa, T.; Yoshimoto, N.; Videlot-Ackermann, C.; Margeat, O.; Ackermann, J.; Baeuerle, P. |
Title |
The influence of branched alkyl side chains in A-D-A oligothiophenes on the photovoltaic performance and morphology of solution-processed bulk-heterojunction solar cells |
Type |
A1 Journal article |
Year |
2017 |
Publication |
Organic chemistry frontiers : an international journal of organic chemistry |
Abbreviated Journal |
Org Chem Front |
Volume |
4 |
Issue |
4 |
Pages |
1561-1573 |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
Besides providing sufficient solubility, branched alkyl chains also affect the film-forming and packing properties of organic semiconductors. In order to avoid steric hindrance as it is present in wide-spread alkyl chains comprising a branching point position at the C2-position, i.e., 2-ethylhexyl, the branching point can be moved away from the pi-conjugated backbone. In this report, we study the influence of the modification of the branching point position from the C2-position in 2-hexyldecylamine (1) to the C4-position in 4-hexyldecylamine (2) connected to the central dithieno[3,2-b: 2', 3'-d] pyrrole (DTP) moiety in a well-studied A-D-A oligothiophene on the optoelectronic properties and photovoltaic performance in solution- processed bulk heterojunction solar cells (BHJSCs) with [6,6]-phenyl-C71-butyric acid methyl ester (PC71BM) as the acceptor material. Post-treatment of the photoactive layers is performed via solvent vapor annealing (SVA) in order to improve the film microstructure of the bulk heterojunction. The time evolution of nanoscale morphological changes is followed by combining scanning transmission electron microscopy with low-energy-loss spectroscopic imaging (STEM-SI), solid-state absorption spectroscopy, and two-dimensional grazing incidence X-ray diffraction (2D-GIXRD). Our results show an improvement of the photovoltaic performance that is dependent on the branching point position in the donor oligomer. Optical spacers are utilized to increase light absorption inside the co-oligomer 2-based BHJSCs leading to increased power conversion efficiencies (PCEs) of 8.2% when compared to the corresponding co-oligomer 1-based devices. A STEM-SI analysis of the respective device cross-sections of active layers containing 1 and 2 as donor materials indeed reveals significant differences in their respective active layer morphologies. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
RSC Publishing |
Place of Publication |
London |
Editor |
|
Language |
|
Wos |
000406374800013 |
Publication Date |
2017-05-02 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
ISSN |
2052-4129 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
4.955 |
Times cited |
24 |
Open Access |
OpenAccess |
Notes |
; We acknowledge financial support by the European Commission under the project “SUNFLOWER” (FP7-ICT-2011-7, grant number: 287594) and S.B. acknowledges the ERC Starting Grant Colouratoms (335078). ; |
Approved |
Most recent IF: 4.955 |
Call Number |
UA @ lucian @ c:irua:145176UA @ admin @ c:irua:145176 |
Serial |
4727 |
Permanent link to this record |
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Author |
Liu, P.; Arslan Irmak, E.; De Backer, A.; De wael, A.; Lobato, I.; Béché, A.; Van Aert, S.; Bals, S. |
Title |
Three-dimensional atomic structure of supported Au nanoparticles at high temperature |
Type |
A1 Journal article |
Year |
2021 |
Publication |
Nanoscale |
Abbreviated Journal |
Nanoscale |
Volume |
13 |
Issue |
|
Pages |
|
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
Au nanoparticles (NPs) deposited on CeO2 are extensively used as thermal catalysts since the morphology of the NPs is expected to be stable at elevated temperatures. Although it is well known that the activity of Au NPs depends on their size and surface structure, their three-dimensional (3D) structure at the atomic scale has not been completely characterized as a function of temperature. In this paper, we overcome the limitations of conventional electron tomography by combining atom counting applied to aberration-corrected scanning transmission electron microscopy images and molecular dynamics relaxation. In this manner, we are able to perform an atomic resolution 3D investigation of supported Au NPs. Our results enable us to characterize the 3D equilibrium structure of single NPs as a function of temperature. Moreover, the dynamic 3D structural evolution of the NPs at high temperatures, including surface layer jumping and crystalline transformations, has been studied. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000612999200029 |
Publication Date |
2020-12-29 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
ISSN |
2040-3364 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
7.367 |
Times cited |
13 |
Open Access |
OpenAccess |
Notes |
This work was supported by the European Research Council (Grant 815128 REALNANO to SB, Grant 770887 PICOMETRICS to SVA, Grant 823717 ESTEEM3). The authors acknowledge financial support from the Research Foundation Flanders (FWO, Belgium) through grants to A. D. w. and A. D. B. and project funding G.0267.18N.; sygma; esteem3JRA; esteem3reported |
Approved |
Most recent IF: 7.367 |
Call Number |
EMAT @ emat @c:irua:174858 |
Serial |
6665 |
Permanent link to this record |
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Author |
Filez, M.; Feng, J.-Y.; Minjauw, M.M.; Solano, E.; Poonkottil, N.; Van Daele, M.; Ramachandran, R.K.; Li, C.; Bals, S.; Poelman, H.; Detavernier, C.; Dendooven, J.; Filez, M.; Minjauw, M.; Solano, E.; Poonkottil, N.; Li, C.; Bals, S.; Dendooven, J. |
Title |
Shuffling atomic layer deposition gas sequences to modulate bimetallic thin films and nanoparticle properties |
Type |
A1 Journal article |
Year |
2022 |
Publication |
Chemistry of materials |
Abbreviated Journal |
|
Volume |
|
Issue |
|
Pages |
|
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
Atomic layer deposition (ALD) typically employs metal precursors and co-reactant pulses to deposit thin films in a layer-by-layer fashion. While conventional ABAB-type ALD sequences implement only two functionalities, namely, a metal source and ligand exchange agent, additional functionalities have emerged, including etching and reduction agents. Herein, we construct gas-phase sequences-coined as ALD+-with complex-ities reaching beyond the classic ABAB-type ALD by freely combining multiple functionalities within irregular pulse schemes, e.g., ABCADC. The possibilities of such combinations are explored as a smart strategy to tailor bimetallic thin films and nanoparticle (NP) properties. By doing so, we demonstrate that bimetallic thin films can be tailored with target thickness and through the full compositional range, while the morphology can be flexibly modulated from thin films to NPs by shuI 1ing the pulse sequence. These complex pulse schemes are expected to be broadly applicable but are here explored for Pd-Ru bimetallic thin films and NPs. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000823205700001 |
Publication Date |
2022-06-29 |
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 |
|
Edition |
|
ISSN |
0897-4756; 1520-5002 |
ISBN |
|
Additional Links |
UA library record; WoS full record |
Impact Factor |
|
Times cited |
2 |
Open Access |
OpenAccess |
Notes |
This research was funded by the Research Foundation, Flanders (FWO) , and the Special Research Fund BOF of Ghent University (GOA 01G01019) . M.F. and M.M.M. acknowledge the FWO for a postdoctoral research fellowship (1280621N) . N.P. acknowledges the European Union's Horizon 2020 research and innovation program under the Marie Skiodowska-Curie grant agreement no. 765378. For the GISAXS measurements, the author s received funding from the European Community's Transnational Access Program CALIPSOplus. E.S. acknowledges the Spanish project RTI2018-093996-B-C32 MICINN/FEDER funds. Air Liquide is acknowledged for supporting this research. The authors acknowledge SOLEIL for the provision of synchrotron radiation facilities and would like to thank Dr. Alessandro Coati for assistance in using beamline SiXS. The GIWAXS experiments were performed at NCD-SWEET beamline at ALBA Synchrotron with the collaboration of ALBA staff . |
Approved |
no |
Call Number |
UA @ admin @ c:irua:189541 |
Serial |
8928 |
Permanent link to this record |
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Author |
Cremers, V.; Rampelberg, G.; Baert, K.; Abrahami, S.; Claes, N.; de Oliveira, T.M.; Terryn, H.; Bals, S.; Dendooven, J.; Detavernier, C. |
Title |
Corrosion protection of Cu by atomic layer deposition |
Type |
A1 Journal article |
Year |
2019 |
Publication |
Journal of vacuum science and technology: A: vacuum surfaces and films |
Abbreviated Journal |
J Vac Sci Technol A |
Volume |
37 |
Issue |
37 |
Pages |
060902 |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
Atomic layer deposition (ALD) is a vapor phase technique that is able to deposit uniform, conformal thin films with an excellent thickness control at the atomic scale. 18 nm thick Al2O3 and TiO2 coatings were deposited conformaly and pinhole-free onto micrometer-sized Cu powder, using trimethylaluminum and tetrakis(dimethylamido)titanium(IV), respectively, as a precursor and de-ionized water as a reactant. The capability of the ALD coating to protect the Cu powder against corrosion was investigated. Therefore, the stability of the coatings was studied in solutions with different pH in the range of 0–14, and in situ raman spectroscopy was used to detect the emergence of corrosion products of Cu as an indication that the protective coating starts to fail. Both ALD coatings provide good protection at standard pH values in the range of 5–7. In general, the TiO2 coating shows a better barrier protection against corrosion than the Al2O3 coating. However, for the most extreme pH conditions, pH 0 and pH 14, the TiO2 coating starts also to degrade. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000517925800003 |
Publication Date |
2019-09-19 |
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 |
|
ISSN |
0734-2101 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
1.374 |
Times cited |
7 |
Open Access |
OpenAccess |
Notes |
The authors acknowledge financial support from the Strategic Initiative Materials in Flanders (SIM, SBO-FUNC project) and the Special Research Fund BOF of Ghent University (No. GOA 01G01513). J.D. acknowledges the Research Foundation Flanders (FWO-Vlaanderen) for a postdoctoral fellowship. |
Approved |
Most recent IF: 1.374 |
Call Number |
EMAT @ emat @c:irua:162640 |
Serial |
5361 |
Permanent link to this record |
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Author |
Cremers, V.; Rampelberg, G.; Barhoum, A.; Walters, P.; Claes, N.; Oliveira, T.M. de; Assche, G.V.; Bals, S.; Dendooven, J.; Detavernier, C. |
Title |
Oxidation barrier of Cu and Fe powder by Atomic Layer Deposition |
Type |
A1 Journal article |
Year |
2018 |
Publication |
Surface and coatings technology |
Abbreviated Journal |
Surf Coat Tech |
Volume |
349 |
Issue |
349 |
Pages |
1032-1041 |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
Atomic layer deposition (ALD) is a vapor based technique which allows to deposit uniform, conformal films with a thickness control at the atomic scale. In this research, Al 2 O 3 coatings were deposited on micrometer-sized Fe and Cu powder (particles) using the thermal trimethylaluminum (TMA)/ water (H 2 O) process in a rotary pump-type ALD reactor. Rotation of the powder during deposition was required to obtain a pinhole-free ALD coating. The protective nature of the coating was evaluated by quantifying its effectiveness in protecting the metal particles during oxidative annealing treatments. The Al 2 O 3 coated powders were annealed in ambient air while in-situ thermogravimetric analysis (TGA) and in-situ x-ray diffraction (XRD) data were acquired. The thermal stability of a series of Cu and Fe powder with different Al 2 O 3 thicknesses were determined with TGA. In both samples a clear shift in oxidation temperature is visible. For Cu and Fe powder coated with 25 nm Al 2 O 3 , we observed an increase of the oxidation temperature with 300-400°C. For the Cu powder a thin film of only 8 nm is required to obtain an initial increase in oxidation temperature of 200°C. In contrast, for Fe powder a thicker coating of 25 nm is required. In both cases, the oxidation temperature increases with increasing thickness of the Al 2 O 3 coating. These results illustrate that the Al 2 O 3 thin film, deposited by the thermal ALD process (TMA/H 2 O) can be an efficient and pinhole-free barrier layer for micrometer-sized powder particles, provided that the powder is properly agitated during the process to ensure sufficient vapour-solid interaction. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000441492600108 |
Publication Date |
2018-06-25 |
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 |
|
ISSN |
0257-8972 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
2.589 |
Times cited |
10 |
Open Access |
OpenAccess |
Notes |
The authors acknowledge financial support from the Strategic Initiative Materials in Flanders (SIM, SBO-FUNC project) and the Special Research Fund BOF of Ghent University (GOA 01G01513). J. D. acknowledges the Research Foundation Flanders (FWO-Vlaanderen) for a postdoctoral fellowship. N.C. and S.B. acknowledge financial support from European Research Council (ERC Starting Grant 335078-COLOURATOMS). The authors acknowledge S. Goeteyn for the assistance in preliminary depositions. (ROMEO:green; preprint:; postprint:can ; pdfversion:cannot); ecas_sara |
Approved |
Most recent IF: 2.589 |
Call Number |
EMAT @ emat @c:irua:152174UA @ admin @ c:irua:152174 |
Serial |
4994 |
Permanent link to this record |
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Author |
Dendooven, J.; Devloo-Casier, K.; Ide, M.; Grandfield; Kurttepeli; Ludwig, K.F.; Bals, S.; Van der Voort, P.; Detavernier, C. |
Title |
Atomic layer deposition-based tuning of the pore size in mesoporous thin films studied by in situ grazing incidence small angle X-ray scattering |
Type |
A1 Journal article |
Year |
2014 |
Publication |
Nanoscale |
Abbreviated Journal |
Nanoscale |
Volume |
6 |
Issue |
24 |
Pages |
14991-14998 |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
Atomic layer deposition (ALD) enables the conformal coating of porous materials, making the technique suitable for pore size tuning at the atomic level, e.g., for applications in catalysis, gas separation and sensing. It is, however, not straightforward to obtain information about the conformality of ALD coatings deposited in pores with diameters in the low mesoporous regime (<10 nm). In this work, it is demonstrated that in situ synchrotron based grazing incidence small angle X-ray scattering (GISAXS) can provide valuable information on the change in density and internal surface area during ALD of TiO2 in a porous titania film with small mesopores (3-8 nm). The results are shown to be in good agreement with in situ X-ray fluorescence data representing the evolution of the amount of Ti atoms deposited in the porous film. Analysis of both datasets indicates that the minimum pore diameter that can be achieved by ALD is determined by the size of the Ti-precursor molecule. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
Cambridge |
Editor |
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Language |
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Wos |
000345458200051 |
Publication Date |
2014-10-13 |
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 |
|
ISSN |
2040-3364;2040-3372; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
7.367 |
Times cited |
41 |
Open Access |
OpenAccess |
Notes |
239865 Cocoon; 335078 Colouratom; Fwo; ECAS_Sara; (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:cannot); |
Approved |
Most recent IF: 7.367; 2014 IF: 7.394 |
Call Number |
UA @ lucian @ c:irua:122227 |
Serial |
169 |
Permanent link to this record |
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Author |
Duarte, M.; Daems, N.; Hereijgers, J.; Arenas Esteban, D.; Bals, S.; Breugelmans, T. |
Title |
Enhanced CO2 electroreduction with metal-nitrogen-doped carbons in a continuous flow reactor |
Type |
A1 Journal article |
Year |
2021 |
Publication |
Journal Of Co2 Utilization |
Abbreviated Journal |
J Co2 Util |
Volume |
50 |
Issue |
|
Pages |
101583-12 |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
As part of a mitigation and adaptation approach to increasing carbon dioxide atmospheric concentrations, we report superior performance of various metal-nitrogen-doped carbon catalysts, synthesized using an easily up-scalable method, for the electrochemical reduction to carbon monoxide and/or formate at industrially relevant current densities up to 200 mAcm−2. Altering the embedded transition metal (i.e. Sn, Co, Fe, Mn and Ni) allowed to tune the selectivity towards the desired product. Mn-N-C and Fe-N-C performance was compromised by its high CO* binding energy, while Co-N-C catalyzed preferentially the HER. Ni-N-C and Sn-N-C revealed to be promising electrocatalysts, the latter being evaluated for the first time in a flow reactor. A productivity of 589 L CO m-2 h-1 at -1.39 VRHE with Ni-N-C and 751 g HCOO- m-2 h-1 at -1.47 VRHE with Sn-N-C was achieved with no signs of degradation detected after 24 h of operation at industrially relevant current densities (100 mAcm−2). Stable operation at 200 mAcm−2 led to turnover frequencies for the production of carbon products of up to 5176 h-1. These enhanced productivities, in combination with high stability, constitute an essential step towards the scalability and ultimately towards the economical valorization of CO2 electrolyzers using metal-containing nitrogen-doped catalysts. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000670316000002 |
Publication Date |
2021-05-28 |
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 |
|
Edition |
|
ISSN |
2212-9820 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
4.292 |
Times cited |
14 |
Open Access |
OpenAccess |
Notes |
The authors acknowledge sponsoring from the Research Foundation – Flanders (FWO) in the frame of a post-doctoral grant (12Y3919N – ND). This project was co-funded by the Interreg 2 Seas-Program 2014-2020, co-financed by the European Fund for Regional Development in the frame of subsidiary contract nr. 2S03-019. This work was further performed in the framework of the Catalisti MOT project D2M (“Dioxide to Monoxide (D2M): Innovative catalysis for CO2 to CO conversion”). We thank Lien Pacquets for analyzing the samples with SEM-EDX, Saskia Defoss´e for helping with the N2 physisorption measurements and Kitty Baert (VUB) for analyzing the samples with XPS and Raman. |
Approved |
Most recent IF: 4.292 |
Call Number |
UA @ admin @ c:irua:178151 |
Serial |
6779 |
Permanent link to this record |
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Author |
Greboval, C.; Chu, A.; Vale Magalhaes, D.; Ramade, J.; Qu, J.; Rastogi, P.; Khalili, A.; Chee, S.-S.; Aubin, H.; Vincent, G.; Bals, S.; Delerue, C.; Lhuillier, E. |
Title |
Ferroelectric gating of narrow band-gap nanocrystal arrays with enhanced light-matter coupling |
Type |
A1 Journal article |
Year |
2021 |
Publication |
Acs Photonics |
Abbreviated Journal |
Acs Photonics |
Volume |
8 |
Issue |
1 |
Pages |
259-268 |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
As narrow band gap nanocrystals become a considerable building block for the design of infrared sensors, device design needs to match their actual operating conditions. While in the near and shortwave infrared, room-temperature operation has been demonstrated, longer wavelengths still require low-temperature operations and thus specific design. Here, we discuss how field-effect transistors (FETs) can be compatible with low-temperature detection. To reach this goal, two key developments are proposed. First, we report the gating of nanocrystal films from SrTiO3 which leads to high gate capacitance with leakage and breakdown free operation in the 4-100 K range. Second, we demonstrate that this FET is compatible with a plasmonic resonator whose role is to achieve strong light absorption from a thin film used as the channel of the FET. Combining three resonances, broadband absorption from 1.5 to 3 mu m reaching 30% is demonstrated. Finally, combining gate and enhanced light-matter coupling, we show that detectivity can be as high as 10(12) Jones for a device presenting a 3 mu m cutoff wavelength and 30 K operation. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
|
Wos |
000612567900028 |
Publication Date |
2021-01-10 |
Series Editor |
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Series Title |
|
Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
ISSN |
2330-4022 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
6.756 |
Times cited |
21 |
Open Access |
OpenAccess |
Notes |
The project is supported by ERC Starting Grant BlackQD (Grant No. 756225) and Consolidator Grant Realnano (815128). This project has received funding from the European Commission (Grant 731019, EUSMI). We acknowledge the use of clean-room facilities from the “Centrale de ProximitéParis-Centre”. This work has been supported by the Region Ile-de-France in the framework of DIM Nano-K (Grant dopQD). This work was supported by French state funds managed by the ANR within the Investissements d’Avenir programme under Reference ANR-11-IDEX-0004-02 and, more specifically, within the framework of the Cluster of Excellence MATISSE and also by the Grant IPER-Nano2 (ANR-18CE30-0023-01), Copin (ANR-19-CE24-0022), Frontal (ANR-19-CE09-0017), Graskop (ANR-19-CE09-0026), and NITQuantum. J.Q. thanks Chinese Scholarship Council for Ph.D. Grant, while A.C. thanks Agence Innovation Defense.; sygma |
Approved |
Most recent IF: 6.756 |
Call Number |
UA @ admin @ c:irua:176708 |
Serial |
6725 |
Permanent link to this record |
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Author |
Ding, Y.; Maitra, S.; Arenas Esteban, D.; Bals, S.; Vrielinck, H.; Barakat, T.; Roy, S.; Van Tendeloo, G.; Liu, J.; Li, Y.; Vlad, A.; Su, B.-L. |
Title |
Photochemical production of hydrogen peroxide by digging pro-superoxide radical carbon vacancies in carbon nitride |
Type |
A1 Journal article |
Year |
2022 |
Publication |
Cell reports physical science |
Abbreviated Journal |
|
Volume |
3 |
Issue |
5 |
Pages |
100874-17 |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
Artificial photosynthesis of H2O2, an environmentally friendly oxidant and a clean fuel, holds great promise. However, improving its efficiency and stability for industrial implementation remains highly challenging. Here, we report the visible-light H2O2 artificial photosynthesis by digging pro-superoxide radical carbon vacancies in three-dimensional hierarchical porous g-C3N4 through a simple hydrolysis-freeze-drying-thermal treatment. A significant electronic structure change is revealed upon the implantation of carbon vacancies, broadening visible-light absorption and facilitating the photogenerated charge separation. The strong electron affinity of the carbon vacancies promotes superoxide radical (O-center dot(2)-) formation, significantly boosting the H2O2 photocatalytic production. The developed photocatalyst shows an H2O2 evolution rate of 6287.5 mM g(-1) h(-1) under visible-light irradiation with a long cycling stability being the best-performing photocatalyst among all reported g-C3N4-based systems. Our work provides fundamental insight into highly active and stable photocatalysts with great potential for safe industrial H2O2 production. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000805830100006 |
Publication Date |
2022-04-28 |
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 |
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ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
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Times cited |
12 |
Open Access |
OpenAccess |
Notes |
Y.D. thanks the China Scholarship Council (201808310127) for financial support. This work is financially supported by the National Natural Science Foundation of China (U1663225) , Program for Changjiang Scholars and Innovative Research Team in University (IRT_15R52) of the Chinese Ministry of Education, Program of Introducing Talents of Discipline to Universities-Plan 111 (grant no. B20002) from the Ministry of Science and Technology and the Ministry of Education of China, and the National Key R&D Program of China (2016YFA0202602) . This research was also supported by the European Commission Interreg V France-Wallonie-Vlaanderen project “DepollutAir”. |
Approved |
Most recent IF: NA |
Call Number |
UA @ admin @ c:irua:189706 |
Serial |
7090 |
Permanent link to this record |
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Author |
Bals, S.; Kabius, B.; Haider, M.; Radmilovic, V.; Kisielowski, C. |
Title |
Annular dark field imaging in a TEM |
Type |
A1 Journal article |
Year |
2004 |
Publication |
Solid state communications |
Abbreviated Journal |
Solid State Commun |
Volume |
130 |
Issue |
10 |
Pages |
675-680 |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
Abstract ![sorted by Abstract field, descending order (down)](img/sort_desc.gif) |
Annular objective apertures are fabricated for a CM300 transmission electron microscope using a focused ion beam system. A central beam stop in the back focal plane of the objective lens of the microscope blocks all electrons scattered up to a semi-angle of approximately 20 mrad. In this manner, contributions to the image from Bragg scattering are largely reduced and the image contrast is sensitive to the atomic number Z. Experimentally, we find that single atom scattering cross sections measured with this technique are close to Rutherford scattering values. A comparison between this new method and STEM-HAADF shows that both techniques result in qualitatively similar images although the resolution of ADF-TEM is limited by contrast delocalization caused by the spherical aberration of the objective lens. This problem can be overcome by using an aberration corrected microscope. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
New York, N.Y. |
Editor |
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Language |
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Wos |
000221489300007 |
Publication Date |
2004-04-10 |
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 |
|
ISSN |
0038-1098; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
1.554 |
Times cited |
43 |
Open Access |
|
Notes |
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Approved |
Most recent IF: 1.554; 2004 IF: 1.523 |
Call Number |
UA @ lucian @ c:irua:87584 |
Serial |
132 |
Permanent link to this record |