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Author |
Bhaskar, G.; Gvozdetskyi, V.; Batuk, M.; Wiaderek, K.M.; Sun, Y.; Wang, R.; Zhang, C.; Carnahan, S.L.; Wu, X.; Ribeiro, R.A.; Bud'ko, S.L.; Canfield, P.C.; Huang, W.; Rossini, A.J.; Wang, C.-Z.; Ho, K.-M.; Hadermann, J.; Zaikina, J., V |
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Title |
Topochemical deintercalation of Li from layered LiNiB : toward 2D MBene |
Type |
A1 Journal article |
| |
Year |
2021 |
Publication |
Journal Of The American Chemical Society |
Abbreviated Journal |
J Am Chem Soc |
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| |
Volume |
143 |
Issue |
11 |
Pages |
4213-4223 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
The pursuit of two-dimensional (2D) borides, MBenes, has proven to be challenging, not the least because of the lack of a suitable precursor prone to the deintercalation. Here, we studied room-temperature topochemical deintercalation of lithium from the layered polymorphs of the LiNiB compound with a considerable amount of Li stored in between [NiB] layers (33 at. % Li). Deintercalation of Li leads to novel metastable borides (Li similar to 0.5NiB) with unique crystal structures. Partial removal of Li is accomplished by exposing the parent phases to air, water, or dilute HCl under ambient conditions. Scanning transmission electron microscopy and solid-state Li-7 and B-1(1) NMR spectroscopy, combined with X-ray pair distribution function (PDF) analysis and DFT calculations, were utilized to elucidate the novel structures of (Li similar to 0.5NiB) and the mechanism of Li-deintercalation. We have shown that the deintercalation of Li proceeds via a “zip-lock” mechanism, leading to the condensation of single [NiB] layers into double or triple layers bound via covalent bonds, resulting in structural fragments with Li[NiB](2) and Li[NiB](3) compositions. The crystal structure of Li similar to 0.5NiB is best described as an intergrowth of the ordered single [NiB], double [NiB](2), or triple [NiB](3) layers alternating with single Li layers; this explains its structural complexity. The formation of double or triple [NiB] layers induces a change in the magnetic behavior from temperature-independent paramagnets in the parent LiNiB compounds to the spin-glassiness in the deintercalated Li similar to 0.5NiB counterparts. LiNiB compounds showcase the potential to access a plethora of unique materials, including 2D MBenes (NiB). |
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Wos |
000634761500021 |
Publication Date |
2021-03-15 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0002-7863 |
ISBN |
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Additional Links  |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.858 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
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Approved |
Most recent IF: 13.858 |
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Call Number |
UA @ admin @ c:irua:177697 |
Serial |
6790 |
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Author |
Freund, R.; Canossa, S.; Cohen, S.M.; Yan, W.; Deng, H.; Guillerm, V.; Eddaoudi, M.; Madden, D.G.; Fairen-Jimenez, D.; Lyu, H.; Macreadie, L.K.; Ji, Z.; Zhang, Y.; Wang, B.; Haase, F.; Wöll, C.; Zaremba, O.; Andreo, J.; Wuttke, S.; Diercks, C.S. |
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Title |
25 years of Reticular Chemistry |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Angewandte Chemie-International Edition |
Abbreviated Journal |
Angew Chem Int Edit |
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Volume |
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Issue |
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Pages |
anie.202101644 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
At its core, reticular chemistry has translated the precision and expertise of organic and inorganic synthesis to the solid state. While initial excitement over metal‐organic frameworks (MOFs) and covalent organic frameworks (COFs) was undoubtedly fueled by their unprecedented porosity and surface areas, the most profound scientific innovation of the field has been the elaboration of design strategies for the synthesis of extended crystalline solids through strong directional bonds. In this contribution we highlight the different classes of reticular materials that have been developed, how these frameworks can be functionalized and how complexity can be introduced into their backbones. Finally, we show how the structural control over these materials is being extended from the molecular scale to their crystal morphology and shape on the nanoscale, all the way to their shaping on the bulk scale. |
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Wos |
000672037800001 |
Publication Date |
2021-03-29 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1433-7851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
11.994 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 11.994 |
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Call Number |
EMAT @ emat @c:irua:177778 |
Serial |
6743 |
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Author |
MacArthur, K.E.; Yankovich, A.B.; Béché, A.; Luysberg, M.; Brown, H.G.; Findlay, S.D.; Heggen, M.; Allen, L.J. |
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Title |
Optimizing Experimental Conditions for Accurate Quantitative Energy-Dispersive X-ray Analysis of Interfaces at the Atomic Scale |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Microscopy And Microanalysis |
Abbreviated Journal |
Microsc Microanal |
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Volume |
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Issue |
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Pages |
1-15 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
The invention of silicon drift detectors has resulted in an unprecedented improvement in detection efficiency for energy-dispersive X-ray (EDX) spectroscopy in the scanning transmission electron microscope. The result is numerous beautiful atomic-scale maps, which provide insights into the internal structure of a variety of materials. However, the task still remains to understand exactly where the X-ray signal comes from and how accurately it can be quantified. Unfortunately, when crystals are aligned with a low-order zone axis parallel to the incident beam direction, as is necessary for atomic-resolution imaging, the electron beam channels. When the beam becomes localized in this way, the relationship between the concentration of a particular element and its spectroscopic X-ray signal is generally nonlinear. Here, we discuss the combined effect of both spatial integration and sample tilt for ameliorating the effects of channeling and improving the accuracy of EDX quantification. Both simulations and experimental results will be presented for a perovskite-based oxide interface. We examine how the scattering and spreading of the electron beam can lead to erroneous interpretation of interface compositions, and what approaches can be made to improve our understanding of the underlying atomic structure. |
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Place of Publication |
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Editor |
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Wos |
000664532400007 |
Publication Date |
2021-04-12 |
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Series Editor |
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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 |
1431-9276 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
1.891 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
The authors would like to thank Jürgen Schubert for helping to supply the sample and valuable discussions on the topic. K. E. MacArthur and M. Heggen acknowledge the Helmholtz Funding agency and the DFG (grant number HE 7192/1-2) for their financial support of this work. L. J. Allen acknowledges the support of the Alexander von Humboldt Foundation. This research was supported under the Discovery Projects funding scheme of the Australian Research Council (Projects DP140102538 and FT190100619). K.E. MacArthur, A.B. Yankovich and A. Béché acknowledge support from the European Union’s Horizon 2020 research innovation program under grant agreement No. 823717 – ESTEEM3. A.B. Yankovich also acknowledges support from the Materials Science Area of Advance at Chalmers and the Swedish Research Council (VR, under grant No: 2020-04986).; esteem3TA; esteem3reported |
Approved |
Most recent IF: 1.891 |
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Call Number |
EMAT @ emat @c:irua:178129 |
Serial |
6760 |
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Author |
Ghidelli, M.; Orekhov, A.; Bassi, A.L.; Terraneo, G.; Djemia, P.; Abadias, G.; Nord, M.; Béché, A.; Gauquelin, N.; Verbeeck, J.; Raskin, J.-p.; Schryvers, D.; Pardoen, T.; Idrissi, H. |
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Title |
Novel class of nanostructured metallic glass films with superior and tunable mechanical properties |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Acta Materialia |
Abbreviated Journal |
Acta Mater |
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Volume |
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Issue |
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Pages |
116955 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
A novel class of nanostructured Zr50Cu50 (%at.) metallic glass films with superior and tunable mechanical
properties is produced by pulsed laser deposition. The process can be controlled to synthetize a wide
range of film microstructures including dense fully amorphous, amorphous embedded with nanocrystals
and amorphous nano-granular. A unique dense self-assembled nano-laminated atomic arrangement
characterized by alternating Cu-rich and Zr/O-rich nanolayers with different local chemical enrichment
and amorphous or amorphous-crystalline composite nanostructure has been discovered, while
significant in-plane clustering is reported for films synthetized at high deposition pressures. This unique
nanoarchitecture is at the basis of superior mechanical properties including large hardness and elastic
modulus up to 10 and 140 GPa, respectively and outstanding total elongation to failure (>9%), leading to
excellent strength/ductility balance, which can be tuned by playing with the film architecture. These
results pave the way to the synthesis of novel class of engineered nanostructured metallic glass films
with high structural performances attractive for a number of applications in microelectronics and
coating industry. |
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Place of Publication |
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Editor |
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Wos |
000670077800004 |
Publication Date |
2021-05-12 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1359-6454 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
5.301 |
Times cited |
27 |
Open Access |
OpenAccess |
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Notes |
H.I. is mandated by the Belgian National Fund for Scientific Research (FSR-FNRS). This work was supported by the Fonds de la Recherche Scientifique – FNRS under Grant T.0178.19 and Grant CDR– J011320F. We acknowledge funding for the direct electron detector used in the 4D stem studies from the Hercules fund 'Direct electron detector for soft matter TEM' from the Flemish Government J.V acknowledges funding from the European Union's Horizon 2020 research and innovation program under grant agreement No 823717 – ESTEEM3. A.O. has received partial funding from the GOA project “Solarpaint” of the University of Antwerp. A.B. and J.V. acknowledge funding through FWO project G093417N ('Compressed sensing enabling low dose imaging in transmission electron microscopy') from the Flanders Research Fund. M.G. and A.L.B acknowledge Chantelle Ekanem for support in PLD depositions. |
Approved |
Most recent IF: 5.301 |
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Call Number |
EMAT @ emat @c:irua:178142 |
Serial |
6761 |
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Author |
Duarte, M.; Daems, N.; Hereijgers, J.; Arenas Esteban, D.; Bals, S.; Breugelmans, T. |
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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 |
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Volume |
50 |
Issue |
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Pages |
101583-12 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
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. |
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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 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2212-9820 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.292 |
Times cited |
14 |
Open Access |
OpenAccess |
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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 |
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Call Number |
UA @ admin @ c:irua:178151 |
Serial |
6779 |
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Author |
van der Jeught, S.; Muyshondt, P.G.G.; Lobato, I. |
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Title |
Optimized loss function in deep learning profilometry for improved prediction performance |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
JPhys Photonics |
Abbreviated Journal |
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Volume |
3 |
Issue |
2 |
Pages |
024014 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Single-shot structured light profilometry (SLP) aims at reconstructing the 3D height map of an object from a single deformed fringe pattern and has long been the ultimate goal in fringe projection profilometry. Recently, deep learning was introduced into SLP setups to replace the task-specific algorithm of fringe demodulation with a dedicated neural network. Research on deep learning-based profilometry has made considerable progress in a short amount of time due to the rapid development of general neural network strategies and to the transferrable nature of deep learning techniques to a wide array of application fields. The selection of the employed loss function has received very little to no attention in the recently reported deep learning-based SLP setups. In this paper, we demonstrate the significant impact of loss function selection on height map prediction accuracy, we evaluate the performance of a range of commonly used loss functions and we propose a new mixed gradient loss function that yields a higher 3D surface reconstruction accuracy than any previously used loss functions. |
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Place of Publication |
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Language |
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Wos |
000641030000001 |
Publication Date |
2021-03-18 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2515-7647 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
|
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: NA |
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Call Number |
UA @ admin @ c:irua:178171 |
Serial |
6797 |
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Author |
Akamine, H.; Mitsuhara, M.; Nishida, M.; Samaee, V.; Schryvers, D.; Tsukamoto, G.; Kunieda, T.; Fujii, H. |
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Title |
Precipitation behaviors in Ti-2.3 Wt Pct Cu alloy during isothermal and two-step aging |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Metallurgical And Materials Transactions A-Physical Metallurgy And Materials Science |
Abbreviated Journal |
Metall Mater Trans A |
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Volume |
52 |
Issue |
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Pages |
2760-2772 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Time evolution of precipitates related to age-hardening in Ti-2.3 wt pct Cu alloys was investigated by electron microscopy. In isothermal aging at 723 K, the hardness increases continuously owing to precipitation strengthening, whereas in two-step aging where the aging temperature is switched from 673 K to 873 K after 100 hours, the hardness is found to drastically drop after the aging temperature switches. In isothermal aging, metastable and stable precipitates are independently nucleated, whereas characteristic V-shaped clusters of precipitates are observed during the two-step aging. It is revealed by atomic-scale observations that the V-shaped clusters are composed of metastable and stable precipitates and each type of precipitate has a different orientation relationship with the alpha phase: (10 (3) over bar)//(0001)(alpha) and [0 (1) over bar0]//respectively. The drop in hardness during two-step aging can be explained by a synergistic effect of decreased precipitation strengthening and solid solution strengthening. (C) The Minerals, Metals & Materials Society and ASM International 2021 |
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Place of Publication |
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Language |
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Wos |
000644823000001 |
Publication Date |
2021-04-27 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1073-5623 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
1.874 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 1.874 |
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Call Number |
UA @ admin @ c:irua:178222 |
Serial |
6786 |
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Author |
Xi, J.; Yang, S.; Silvioli, L.; Cao, S.; Liu, P.; Chen, Q.; Zhao, Y.; Sun, H.; Hansen, J.N.; Haraldsted, J.-P.B.; Kibsgaard, J.; Rossmeisl, J.; Bals, S.; Wang, S.; Chorkendorff, I. |
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Title |
Highly active, selective, and stable Pd single-atom catalyst anchored on N-doped hollow carbon sphere for electrochemical H₂O₂ synthesis under acidic conditions |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Journal Of Catalysis |
Abbreviated Journal |
J Catal |
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Volume |
393 |
Issue |
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Pages |
313-323 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Single-atom catalysts (SACs) have recently attracted broad scientific interests due to their unique structural feature, the single-atom dispersion. Optimized electronic structure as well as high stability are required for single-atom catalysts to enable efficient electrochemical production of H2O2. Herein, we report a facile synthesis method that stabilizes atomic Pd species on the reduced graphene oxide/Ndoped carbon hollow carbon nanospheres (Pd1/N-C). Pd1/N-C exhibited remarkable electrochemical H2O2 production rate with high faradaic efficiency, reaching 80%. The single-atom structure and its high H2O2 production rate were maintained even after 10,000 cycle stability test. The existence of single-atom Pd as well as its coordination with N species is responsible for its high activity, selectivity, and stability. The N coordination number and substrate doping around Pd atoms are found to be critical for an optimized adsorption energy of intermediate *OOH, resulting in efficient electrochemical H2O2 production. (C) 2020 Elsevier Inc. All rights reserved. |
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Place of Publication |
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Wos |
000640923500003 |
Publication Date |
2020-11-26 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0021-9517 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
6.844 |
Times cited |
40 |
Open Access |
Not_Open_Access |
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| |
Notes |
This research was financially supported by the National Natural Science Foundation of China (No. 51772110), Natural Science Foundation of Hubei Province (No. 2019CFB539), Danmarks Innovationsfond within the ProActivE project (5160-00003B), Villum Foundation V-SUSTAIN grant 9455 to the Villum Center for the Science of Sustainable Fuels and Chemicals, the Carlsberg Foundation grant CF18-0435, the Institutional Research Program (2E30220) of the Korea Institute of Science and Technology (KIST), Shenzhen Science and Technology Plan under Grant (JCYJ20170818160751460) and the Open Project of Key Laboratory of Green Chemical Engineering Process of Ministry of Education (No. GCP20200205). The authors would like to acknowledge the Analytical and Testing Center of Huazhong University of Science and Technology and the Wuhan National Laboratory for Optoelectronics for SEM, TEM, Raman and XPS measurements. |
Approved |
Most recent IF: 6.844 |
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Call Number |
UA @ admin @ c:irua:178321 |
Serial |
6796 |
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Author |
Huvé, M.; Vannier, R.-N.; Nowogrocki, G.; Mairesse, G.; Van Tendeloo, G. |
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Title |
From Bi4V2O11 to Bi4V2O10.66: the VV-VIV transformation in the Aurovillius-type framework |
Type |
A1 Journal article |
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Year |
1996 |
Publication |
Journal of materials chemistry |
Abbreviated Journal |
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Volume |
6 |
Issue |
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Pages |
1339-1345 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
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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 |
A1996VC50700012 |
Publication Date |
2004-04-21 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0959-9428;1364-5501; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
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Times cited |
63 |
Open Access |
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Notes |
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Approved |
PHYSICS, MULTIDISCIPLINARY 6/79 Q1 # |
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Call Number |
UA @ lucian @ c:irua:17847 |
Serial |
1287 |
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Author |
Laffez, P.; Van Tendeloo, G.; Seshadri, R.; Hervieu, M.; Martin, C.; Maignan, A.; Raveau, B. |
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| |
Title |
Microstructural and physical properties of layered manganite oxides related to the magnetoresistive perovskites |
Type |
A1 Journal article |
| |
Year |
1996 |
Publication |
Journal of applied physics |
Abbreviated Journal |
J Appl Phys |
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| |
Volume |
80 |
Issue |
|
Pages |
5850-5856 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
American Institute of Physics |
Place of Publication |
New York, N.Y. |
Editor |
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Language |
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Wos |
A1996VU98700045 |
Publication Date |
2002-07-26 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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| |
ISSN |
0021-8979; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
2.183 |
Times cited |
36 |
Open Access |
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Notes |
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Approved |
no |
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| |
Call Number |
UA @ lucian @ c:irua:17848 |
Serial |
2039 |
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| Permanent link to this record |
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Author |
Skorikov, A. |
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| |
Title |
Fast approaches for investigating 3D elemental distribution in nanomaterials |
Type |
Doctoral thesis |
| |
Year |
2021 |
Publication |
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Abbreviated Journal |
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| |
Volume |
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Issue |
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Pages |
143 p. |
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| |
Keywords |
Doctoral thesis; Electron microscopy for materials research (EMAT) |
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Abstract |
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Publication Date |
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Series Editor |
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Abbreviated Series Title |
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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 |
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Impact Factor |
|
Times cited |
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Open Access |
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Notes |
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Approved |
Most recent IF: NA |
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Call Number |
UA @ admin @ c:irua:178855 |
Serial |
6795 |
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| Permanent link to this record |
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Author |
Pramanik, G.; Kvakova, K.; Thottappali, M.A.; Rais, D.; Pfleger, J.; Greben, M.; El-Zoka, A.; Bals, S.; Dracinsky, M.; Valenta, J.; Cigler, P. |
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Title |
Inverse heavy-atom effect in near infrared photoluminescent gold nanoclusters |
Type |
A1 Journal article |
| |
Year |
2021 |
Publication |
Nanoscale |
Abbreviated Journal |
Nanoscale |
|
| |
Volume |
12 |
Issue |
23 |
Pages |
10462-10467 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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| |
Abstract |
Fluorophores functionalized with heavy elements show enhanced intersystem crossing due to increased spin-orbit coupling, which in turn shortens the fluorescence decay lifetime (tau(PL)). This phenomenon is known as the heavy-atom effect (HAE). Here, we report the observation of increased tau(PL) upon functionalisation of near-infrared photoluminescent gold nanoclusters with iodine. The heavy atom-mediated increase in tau(PL) is in striking contrast with the HAE and referred to as inverse HAE. Femtosecond and nanosecond transient absorption spectroscopy revealed overcompensation of a slight decrease in lifetime of the transition associated with the Au core (ps) by a large increase in the long-lived triplet state lifetime associated with the Au shell, which contributed to the observed inverse HAE. This unique observation of inverse HAE in gold nanoclusters provides the means to enhance the triplet excited state lifetime. |
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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 |
000657052500001 |
Publication Date |
2021-06-30 |
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Series Editor |
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Series Title |
|
Abbreviated Series Title |
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Series Volume |
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Series Issue |
|
Edition |
|
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| |
ISSN |
2040-3364 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
7.367 |
Times cited |
1 |
Open Access |
OpenAccess |
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Notes |
The authors acknowledge support from GACR project no. 18-12533S. G. P. acknowledges support from EUSMI project no. E180200060; J. P. from the Ministry of Education, Youth and Sports of the Czech Republic – Program INTER-EXCELLENCE (LTAUSA19066). |
Approved |
Most recent IF: 7.367 |
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| |
Call Number |
UA @ admin @ c:irua:179052 |
Serial |
6843 |
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| Permanent link to this record |
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Author |
Wang, L.; Li, Y.; Yang, X.-Y.; Zhang, B.-B.; Ninane, N.; Busscher, H.J.; Hu, Z.-Y.; Delneuville, C.; Jiang, N.; Xie, H.; Van Tendeloo, G.; Hasan, T.; Su, B.-L. |
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Title |
Single-cell yolk-shell nanoencapsulation for long-term viability with size-dependent permeability and molecular recognition |
Type |
A1 Journal article |
| |
Year |
2021 |
Publication |
National Science Review |
Abbreviated Journal |
Natl Sci Rev |
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| |
Volume |
8 |
Issue |
4 |
Pages |
|
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Like nanomaterials, bacteria have been unknowingly used for centuries. They hold significant economic potential for fuel and medicinal compound production. Their full exploitation, however, is impeded by low biological activity and stability in industrial reactors. Though cellular encapsulation addresses these limitations, cell survival is usually compromised due to shell-to-cell contacts and low permeability. Here, we report ordered packing of silica nanocolloids with organized, uniform and tunable nanoporosities for single cyanobacterium nanoencapsulation using protamine as an electrostatic template. A space between the capsule shell and the cell is created by controlled internalization of protamine, resulting in a highly ordered porous shell-void-cell structure formation. These unique yolk-shell nano structures provide long-term cell viability with superior photosynthetic activities and resistance in harsh environments. In addition, engineering the colloidal packing allows tunable shell-pore diameter for size-dependent permeability and introduction of new functionalities for specific molecular recognition. Our strategy could significantly enhance the activity and stability of cyanobacteria for various nanobiotechnological applications. |
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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 |
000651827200002 |
Publication Date |
2020-05-07 |
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Series Editor |
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Series Title |
|
Abbreviated Series Title |
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Series Volume |
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Series Issue |
|
Edition |
|
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| |
ISSN |
2095-5138 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
8.843 |
Times cited |
|
Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 8.843 |
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| |
Call Number |
UA @ admin @ c:irua:179085 |
Serial |
6885 |
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| Permanent link to this record |
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Author |
Chee, S.-S.; Greboval, C.; Vale Magalhaes, D.; Ramade, J.; Chu, A.; Qu, J.; Rastogi, P.; Khalili, A.; Dang, T.H.; Dabard, C.; Prado, Y.; Patriarche, G.; Chaste, J.; Rosticher, M.; Bals, S.; Delerue, C.; Lhuillier, E. |
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Title |
Correlating structure and detection properties in HgTe nanocrystal films |
Type |
A1 Journal article |
| |
Year |
2021 |
Publication |
Nano Letters |
Abbreviated Journal |
Nano Lett |
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| |
Volume |
21 |
Issue |
10 |
Pages |
4145-4151 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
HgTe nanocrystals (NCs) enable broadly tunable infrared absorption, now commonly used to design light sensors. This material tends to grow under multipodic shapes and does not present well-defined size distributions. Such point generates traps and reduces the particle packing, leading to a reduced mobility. It is thus highly desirable to comprehensively explore the effect of the shape on their performance. Here, we show, using a combination of electron tomography and tight binding simulations, that the charge dissociation is strong within HgTe NCs, but poorly shape dependent. Then, we design a dual-gate field-effect-transistor made of tripod HgTe NCs and use it to generate a planar p-n junction, offering more tunability than its vertical geometry counterpart. Interestingly, the performance of the tripods is higher than sphere ones, and this can be correlated with a stronger Te excess in the case of sphere shapes which is responsible for a higher hole trap density. |
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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 |
000657242300002 |
Publication Date |
2021-05-06 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1530-6984 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
12.712 |
Times cited |
20 |
Open Access |
OpenAccess |
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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 cleanroom facilities from the “Centrale de Proximité Paris-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 ANR11-IDEX-0004-02, and more specifically within the framework of the Cluster of Excellence MATISSE and also by grants IPERNano2 (ANR-18CE30-0023-01), Copin (ANR-19-CE24- 0022), Frontal (ANR-19-CE09-0017), Graskop (ANR-19- CE09-0026), and NITQuantum (ANR-20-ASTR-0008-01). A.C. thanks Agence innovation defense for Ph.D. funding; sygmaSB |
Approved |
Most recent IF: 12.712 |
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| |
Call Number |
UA @ admin @ c:irua:179127 |
Serial |
6837 |
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| Permanent link to this record |
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Author |
Zhang, Z.; Bourgeois, L.; Zhang, Y.; Rosalie, J.M.; Medhekar, N. |
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Title |
Advanced imaging and simulations of precipitate interfaces in aluminium alloys and their role in phase transformations |
Type |
P1 Proceeding |
| |
Year |
2020 |
Publication |
MATEC web of conferences
T2 – 17th International Conference on Aluminium Alloys (ICAA), October 26-29, 2020 |
Abbreviated Journal |
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Volume |
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Issue |
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Pages |
09003 |
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Keywords |
P1 Proceeding; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Precipitation is accompanied by the formation and migration of heterophase interfaces. Using the combined approach of advanced imaging and atomistic simulations, we studied the precipitate-matrix interfaces in various aluminium alloy systems, aiming to resolve their detailed atomic structures and illuminate their role in phase transformations. |
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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 |
000652552200053 |
Publication Date |
2020-11-05 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
326 |
Series Issue |
|
Edition |
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ISSN |
2261-236x; 2274-7214 |
ISBN |
|
Additional Links |
UA library record; WoS full record |
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Impact Factor |
|
Times cited |
|
Open Access |
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Notes |
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Approved |
Most recent IF: NA |
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Call Number |
UA @ admin @ c:irua:179147 |
Serial |
6851 |
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| Permanent link to this record |
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Author |
Zhou, X.-G.; Yang, C.-Q.; Sang, X.; Li, W.; Wang, L.; Yin, Z.-W.; Han, J.-R.; Li, Y.; Ke, X.; Hu, Z.-Y.; Cheng, Y.-B.; Van Tendeloo, G. |
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Title |
Probing the electron beam-induced structural evolution of halide perovskite thin films by scanning transmission electron microscopy |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Journal Of Physical Chemistry C |
Abbreviated Journal |
J Phys Chem C |
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Volume |
125 |
Issue |
19 |
Pages |
10786-10794 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
A deep understanding of the fine structure at the atomic scale of halide perovskite materials has been limited by their sensitivity to the electron beam that is widely used for structural characterization. The sensitivity of a gamma-CsPbIBr2 perovskite thin film under electron beam irradiation is revealed by scanning transmission electron microscopy (STEM) through a universal large-range electron dose measurement, which is based on discrete single-electron events in the STEM mode. Our research indicates that the gamma-CsPbIBr2 thin film undergoes structural changes with increasing electron overall dose (e(-).A(-2)) rather than dose rate (e(-).A(-2).s(-1)), which suggests that overall dose is the key operative parameter. The electron beam-induced structural evolution of gamma-CsPbIBr2 is monitored by fine control of the electron beam dose, together with the analysis of high-resolution (S)TEM, diffraction, and energy-dispersive X-ray spectroscopy. Our results show that the gamma-CsPbIBr2 phase first forms an intermediate phase [e.g., CsPb(1-x)(IBr)((3-y))] with a superstructure of ordered vacancies in the pristine unit cell, while a fraction of Pb2+ is reduced to Pb-0. As the electron dose increases, Pb nanoparticles precipitate, while the remaining framework forms the Cs2IBr phase, accompanied by some amorphization. This work provides guidelines to minimize electron beam irradiation artifacts for atomic-resolution imaging on CsPbIBr2 thin films. |
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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 |
000655640900061 |
Publication Date |
2021-05-11 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447; 1932-7455 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.536 |
Times cited |
|
Open Access |
Not_Open_Access |
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Notes |
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Approved |
Most recent IF: 4.536 |
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Call Number |
UA @ admin @ c:irua:179187 |
Serial |
6880 |
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| Permanent link to this record |
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Author |
Du, K. |
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Title |
In situ TEM study on the manipulation of ferroelectrics |
Type |
Doctoral thesis |
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Year |
2021 |
Publication |
|
Abbreviated Journal |
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Volume |
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Issue |
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Pages |
91 p. |
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Keywords |
Doctoral thesis; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
The strong correlated oxide systems attract a lot of attentions of scientists recently, the coexistence and interplay between various degrees of freedom, such as charge, spin and orbital, has been demonstrated to induce some fancy physical properties and phenomenon, including metal-insulator transition, high temperature superconductivity, colossal magnetoresistance. As a part of the strong correlated oxide systems, the ferroelectrics is abundant in both physical properties and application. First, if the electric dipole continuously rotating around a stable core then a topological structure is produced. If people could manipulate the topological structure and simultaneously observe the structure evolution, with external field applied on the topological structure, then it is very likely for such kind of ferroelectrics to be the next generation of storage, for it is reported to need low power input and produce high density of storage. In the other hand, in solids, charge polarity can one-to-one correspond to spin polarity phenomenologically, such as ferroelectricity and ferromagnetism, antiferroelectricity and antiferromagnetism, but ferrielectricity and ferrimagnetism kept telling a disparate story in microscopic level. The claimed “ferrielectrics” in existing research is equivalent to ferroelectric ones, thus the findings of such a real irreducible solids would complete the last piece of the ferroelectrics family. While solving the above two questions remain challengeable: the size of topological structure is small (typically below 10 nm), general characterization methods are insufficient for such high demand on space resolution, not to mention manipulating and observing its dynamic behavior at an atomic level. Here, employing the spherical aberration corrected electron microscope, we applied external field (heating and bias) on ferroelectrics. Combined with high-end characterization methods including the high-angle annular dark field (HAADF-STEM) image, Electron Energy Loss Spectroscopy (EELS) and integrated differential phase contrast (iDPC), the dynamic evolution of ferroelectrics are observed and analyzed. The main findings of this paper could be concluded as listed here: (1) PbTiO3(001)// SrTiO3(001) is grown on DyScO3 and SrRuO3 by pusled laser deposition, the atomical EDS mapping results reveal that the interface between PTO and STO is atomically sharp. Increasing the thickness of PTO from 1 uc to 21 uc, the topological structure wihtin PTO layer would transform from a/c domain to wave, vortex and finally flux closure domain. The geometric phase analysis results (GPA) reveal that above topological structures are corresponding to various strain. (2) Combined with in-situ biasing holder, the electric bias was applied on polar vortex, and it evolved from vortex (0 V) to polar wave (2 V) and finally polar down (5 V). EELS analysis was performed and we find that negative charge is gathered at vortex core, which turns the Ti4+ to Ti3+ there. The oxygen vacancy at negative polarization surface and the negative charge at the positive polarization surface realized the polarization screening of polar down domain. (3) Through the atomic inspection and analysis on lattice structure of BaFe2Se3, the near ladders within single unit are found to be different in degree of tetramerization, thus leading to a residual polarization along the a-axis. The further in-situ heating and biasing experiment was conducted on BaFe2Se3, and the strong and weak ladders are proved to be independent for their behavior under external field. This findings distinguishes ferrielectrics from ferroelectrics in solids. |
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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 |
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Impact Factor |
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Times cited |
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Open Access |
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Notes |
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Approved |
Most recent IF: NA |
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Call Number |
UA @ admin @ c:irua:179310 |
Serial |
6842 |
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| Permanent link to this record |
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Author |
De wael, A. |
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Title |
Model-based quantitative scanning transmission electron microscopy for measuring dynamic structural changes at the atomic scale |
Type |
Doctoral thesis |
| |
Year |
2021 |
Publication |
|
Abbreviated Journal |
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Volume |
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Issue |
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Pages |
xiv, 146 p. |
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Keywords |
Doctoral thesis; Electron microscopy for materials research (EMAT) |
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Abstract |
Nanomaterialen kunnen uiterst interessante eigenschappen vertonen voor een verscheidenheid aan veelbelovende toepassingen, gaande van zonnecrème tot batterijen voor elektrische auto’s. Een nanometer is een miljard keer kleiner dan een meter. Op deze schaal kunnen de materiaaleigenschappen volledig verschillen van bulkmaterialen op grotere schaal. Bovendien hangen de eigenschappen van nanomaterialen sterk af van hun exacte grootte en vorm. Kleine verschillen in de posities van de atomen, in de grootte-orde van een picometer (nog eens duizend maal kleiner dan een nanometer), kunnen de fysische eigenschappen al drastisch beïnvloeden. Daarom is een betrouwbare kwantificering van de atomaire structuur van kritisch belang om de evolutie naar materiaalontwerp mogelijk te maken en inzicht te verwerven in de relatie tussen de fysische eigenschappen en de structuur van nanomaterialen. Daarnaast kan de atomaire structuur van nanomaterialen ook veranderen in de loop van de tijd ten gevolge van verschillende fysische processen. Het onderzoek dat in deze thesis gepresenteerd wordt, maakt het mogelijk om de dynamische structuurveranderingen van nanomaterialen betrouwbaar te kwantificeren op atomaire schaal door gebruik te maken van raster transmissie elektronenmicroscopie (STEM). Ik heb dit gerealiseerd door methodes te ontwikkelen waarmee ik het aantal atomen “achter elkaar” kan tellen in elke atoomkolom van een nanomateriaal, en dit op basis van beelden opgenomen met een elektronenmicroscoop. Een belangrijk verschil met telmethodes voor de analyse van een enkel beeld is het schatten van de kans dat een atoomkolom atomen zal verliezen of bijkrijgen van het ene naar het andere beeld in de tijdreeks. Deze kwantitatieve methode kan het ontrafelen van de tijdsafhankelijke structuur-eigenschappen relatie van een nanomateriaal mogelijk maken, wat uiteindelijk kan leiden tot efficiënter design en productie van nanomaterialen voor innovatieve toepassingen. |
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Additional Links |
UA library record |
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Impact Factor |
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Times cited |
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Open Access |
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Notes |
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Approved |
Most recent IF: NA |
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Call Number |
UA @ admin @ c:irua:179514 |
Serial |
6870 |
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Author |
Safdel, A.; Zarei-Hanzaki, A.; Abedi, H.R.; Pourbabak, S.; Schryvers, D.; Basu, R. |
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Title |
Asymmetrical superelastic behavior of thermomechanically processed semi-equiatomic NiTi alloy in tensile and compressive modes of deformation |
Type |
A1 Journal article |
| |
Year |
2021 |
Publication |
Journal Of Alloys And Compounds |
Abbreviated Journal |
J Alloy Compd |
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Volume |
878 |
Issue |
|
Pages |
160443 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
In the present work two different cold working and annealing schemes were utilized, and the asymmetric superelastic response of thermomechanically processed materials were then assessed through cyclic tensile and compressive modes of deformation. The values of transformation stress, transformation strain, and pseudoelastic strain were measured for each treated and solutionized specimens and the asymmetric response was compared. In the solution annealed state, the difference of these parameters at different deformation modes was negligible due to the weak texture of the material, while for thermomechanically treated ones, development of specific deformation and recrystallization texture components was identified to be one of the underlying reasons of intensified asymmetry. The evolved substructure during the thermomechanical processing also played a substantial role in determining the asymmetric response. The presence of fine grains and dense dislocation substructure could hinder the movement of the transformation front, thus limiting the range of transformation. In tensile mode, the transformation stress was lower, but higher transformation strain was achieved, which was discussed relying on the slip activity in specified oriented grains. The lower transformation strain in compression mode led to lower pseudoelastic strain due to the narrow transformation range which finally degraded superelastic response of the material. (C) 2021 Elsevier B.V. All rights reserved. |
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Wos |
000660477400005 |
Publication Date |
2021-05-18 |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0925-8388 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.133 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 3.133 |
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Call Number |
UA @ admin @ c:irua:179564 |
Serial |
6855 |
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Author |
Lebedev, N.; Stehno, M.; Rana, A.; Reith, P.; Gauquelin, N.; Verbeeck, J.; Hilgenkamp, H.; Brinkman, A.; Aarts, J. |
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Title |
Gate-tuned anomalous Hall effect driven by Rashba splitting in intermixed LaAlO3/GdTiO3/SrTiO3 |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Scientific Reports |
Abbreviated Journal |
Sci Rep-Uk |
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Volume |
11 |
Issue |
1 |
Pages |
10726 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
The Anomalous Hall Effect (AHE) is an important quantity in determining the properties and understanding the behaviour of the two-dimensional electron system forming at the interface of SrTiO<sub>3</sub>-based oxide heterostructures. The occurrence of AHE is often interpreted as a signature of ferromagnetism, but it is becoming more and more clear that also paramagnets may contribute to AHE. We studied the influence of magnetic ions by measuring intermixed LaAlO<sub>3</sub>/GdTiO<sub>3</sub>/SrTiO<sub>3</sub>at temperatures below 10 K. We find that, as function of gate voltage, the system undergoes a Lifshitz transition while at the same time an onset of AHE is observed. However, we do not observe clear signs of ferromagnetism. We argue the AHE to be due to the change in Rashba spin-orbit coupling at the Lifshitz transition and conclude that also paramagnetic moments which are easily polarizable at low temperatures and high magnetic fields lead to the presence of AHE, which needs to be taken into account when extracting carrier densities and mobilities. |
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Wos |
000658820100014 |
Publication Date |
2021-05-21 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2045-2322 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.259 |
Times cited |
5 |
Open Access |
OpenAccess |
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Notes |
J.V. and N.G. acknowledge funding from the Geconcentreerde Onderzoekacties (GOA) project “Solarpaint” of the University of Antwerp and the European Union’s horizon 2020 research and innovation programme ESTEEM3 under grant agreement 823717. The Qu-Ant-EM microscope used in this study was partly funded by the Hercules fund from the Flemish Government.; esteem3TA; esteem3reported |
Approved |
Most recent IF: 4.259 |
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Call Number |
EMAT @ emat @c:irua:179608 |
Serial |
6822 |
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Author |
Feng, H.L.; Kang, C.-J.; Manuel, P.; Orlandi, F.; Su, Y.; Chen, J.; Tsujimoto, Y.; Hadermann, J.; Kotliar, G.; Yamaura, K.; McCabe, E.E.; Greenblatt, M. |
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Title |
Antiferromagnetic order breaks inversion symmetry in a metallic double perovskite, Pb₂NiOsO₆ |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Chemistry Of Materials |
Abbreviated Journal |
Chem Mater |
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Volume |
33 |
Issue |
11 |
Pages |
4188-4195 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
A polycrystalline sample of Pb2NiOsO6 was synthesized under high-pressure (6 GPa) and high-temperature (1575 K) conditions. Pb2NiOsO6 crystallizes in a monoclinic double perovskite structure with a centrosymmetric space group P2(1)/n at room temperature. Pb2NiOsO6 is metallic down to 2 K and shows a single antiferromagnetic (AFM) transition at T-N = 58 K. Pb2NiOsO6 is a new example of a metallic and AFM oxide with three-dimensional connectivity. Neutron powder diffraction and first-principles calculation studies indicate that both Ni and Os moments are ordered below T-N and the AFM magnetic order breaks inversion symmetry. This loss of inversion symmetry driven by AFM order is unusual in metallic systems, and the 3d-Sd double-perovskite oxides represent a new class of noncentrosymmetric AFM metallic oxides. |
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Wos |
000661521800032 |
Publication Date |
2021-05-26 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756; 1520-5002 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 9.466 |
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Call Number |
UA @ admin @ c:irua:179679 |
Serial |
6854 |
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Author |
Skorikov, A.; Heyvaert, W.; Albecht, W.; Pelt, D.M.; Bals, S. |
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Title |
Deep learning-based denoising for improved dose efficiency in EDX tomography of nanoparticles |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Nanoscale |
Abbreviated Journal |
Nanoscale |
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Volume |
13 |
Issue |
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Pages |
12242-12249 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
The combination of energy-dispersive X-ray spectroscopy (EDX) and electron tomography is a powerful approach to retrieve the 3D elemental distribution in nanomaterials, providing an unprecedented level of information for complex, multi-component systems, such as semiconductor devices, as well as catalytic and plasmonic nanoparticles. Unfortunately, the applicability of EDX tomography is severely limited because of extremely long acquisition times and high electron irradiation doses required to obtain 3D EDX reconstructions with an adequate signal-to-noise ratio. One possibility to address this limitation is intelligent denoising of experimental data using prior expectations about the objects of interest. Herein, this approach is followed using the deep learning methodology, which currently demonstrates state-of-the-art performance for an increasing number of data processing problems. Design choices for the denoising approach and training data are discussed with a focus on nanoparticle-like objects and extremely noisy signals typical for EDX experiments. Quantitative analysis of the proposed method demonstrates its significantly enhanced performance in comparison to classical denoising approaches. This allows for improving the tradeoff between the reconstruction quality, acquisition time and radiation dose for EDX tomography. The proposed method is therefore especially beneficial for the 3D EDX investigation of electron beam-sensitive materials and studies of nanoparticle transformations. |
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Wos |
000671395800001 |
Publication Date |
2021-07-08 |
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Series Editor |
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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 |
2040-3364 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7.367 |
Times cited |
11 |
Open Access |
OpenAccess |
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Notes |
Nederlandse Organisatie voor Wetenschappelijk Onderzoek, 016.Veni.192.235 ; H2020 European Research Council, 815128 ; H2020 Marie Skłodowska-Curie Actions, 797153 ; H2020 Research Infrastructures, 731019; realnano; sygmaSB |
Approved |
Most recent IF: 7.367 |
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Call Number |
EMAT @ emat @c:irua:179756 |
Serial |
6799 |
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Author |
Albrecht, W.; Arslan Irmak, E.; Altantzis, T.; Pedrazo‐Tardajos, A.; Skorikov, A.; Deng, T.‐S.; van der Hoeven, J.E.S.; van Blaaderen, A.; Van Aert, S.; Bals, S. |
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Title |
3D Atomic‐Scale Dynamics of Laser‐Light‐Induced Restructuring of Nanoparticles Unraveled by Electron Tomography |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Advanced Materials |
Abbreviated Journal |
Adv Mater |
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Volume |
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Issue |
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Pages |
2100972 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
Understanding light–matter interactions in nanomaterials is crucial for
optoelectronic, photonic, and plasmonic applications. Specifically, metal
nanoparticles (NPs) strongly interact with light and can undergo shape
transformations, fragmentation and ablation upon (pulsed) laser excitation.
Despite being vital for technological applications, experimental insight into
the underlying atomistic processes is still lacking due to the complexity of
such measurements. Herein, atomic resolution electron tomography is performed
on the same mesoporous-silica-coated gold nanorod, before and after
femtosecond laser irradiation, to assess the missing information. Combined
with molecular dynamics (MD) simulations based on the experimentally
determined 3D atomic-scale morphology, the complex atomistic rearrangements,
causing shape deformations and defect generation, are unraveled.
These rearrangements are simultaneously driven by surface diffusion, facet
restructuring, and strain formation, and are influenced by subtleties in the
atomic distribution at the surface. |
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Corporate Author |
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Place of Publication |
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Language |
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Wos |
000671662000001 |
Publication Date |
2021-07-11 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0935-9648 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
19.791 |
Times cited |
8 |
Open Access |
OpenAccess |
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Notes |
W.A. and E.A.I. contributed equally to this work. The authors acknowledge funding from the European Research Council under the European Union’s Horizon 2020 research and innovation program (ERC Consolidator Grants No. 815128 – REALNANO and No. 770887 – PICOMETRICS), the European Union’s Seventh Framework Programme (ERC Advanced Grant No. 291667 – HierarSACol), and the European Commission (EUSMI). W.A. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in the Horizon2020 program (Grant 797153, SOPMEN). T.-S.D. acknowledges financial support from the National Science Foundation of China (NSFC, Grant No. 61905056). The authors also acknowledge financial support by the Research Foundation Flanders (FWO Grant G.0267.18N).; sygmaSB |
Approved |
Most recent IF: 19.791 |
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Call Number |
EMAT @ emat @c:irua:179781 |
Serial |
6805 |
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Author |
Arenas-Vivo, A.; Rojas, S.; Ocaña, I.; Torres, A.; Liras, M.; Salles, F.; Arenas-Esteban, D.; Bals, S.; Ávila, D.; Horcajada, P. |
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Title |
Ultrafast reproducible synthesis of a Ag-nanocluster@MOF composite and its superior visible-photocatalytic activity in batch and in continuous flow |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Journal Of Materials Chemistry A |
Abbreviated Journal |
J Mater Chem A |
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Volume |
9 |
Issue |
28 |
Pages |
15704-15713 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
The (photo)catalytic properties of metal–organic frameworks (MOFs) can be enhanced by post-synthetic inclusion of metallic species in their porosity. Due to their extraordinarily high surface area and well defined porous structure, MOFs can be used for the stabilization of metal nanoparticles with adjustable size within their porosity. Originally, we present here an optimized ultrafast photoreduction protocol for the<italic>in situ</italic>synthesis of tiny and monodisperse silver nanoclusters (AgNCs) homogeneously supported on a photoactive porous titanium carboxylate MIL-125-NH<sub>2</sub>MOF. The strong metal–framework interaction between –NH<sub>2</sub>and Ag atoms influences the AgNC growth, leading to the surfactant-free efficient catalyst AgNC@MIL-125-NH<sub>2</sub>with improved visible light absorption. The potential use of AgNC@MIL-125-NH<sub>2</sub>was further tested in challenging applications: (i) the photodegradation of the emerging organic contaminants (EOCs) methylene blue (MB-dye) and sulfamethazine (SMT-antibiotic) in water treatment, and (ii) the catalytic hydrogenation of<italic>p</italic>-nitroaniline (4-NA) to<italic>p</italic>-phenylenediamine (PPD) with industrial interest. It is noteworthy that compared with the pristine MIL-125-NH<sub>2</sub>, the composite presents an improved catalytic activity and stability, being able to photodegrade 92% of MB in 60 min and 96% of SMT in 30 min, and transform 100% of 4-NA to PPD in 30 min. Aside from these very good results, this study describes for the first time the use of a MOF in a visible light continuous flow reactor for wastewater treatment. With only 10 mg of AgNC@MIL-125-NH<sub>2</sub>, high SMT removal efficiency over 70% is maintained after >2 h under water flow conditions found in real wastewater treatment plants, signaling a future real application of MOFs in water remediation. |
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Place of Publication |
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Wos |
000671839200001 |
Publication Date |
2021-06-21 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2050-7488 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
8.867 |
Times cited |
18 |
Open Access |
OpenAccess |
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Notes |
Comunidad de Madrid, CAM PEJD-2016/IND-2828 Talento Modality 2, 2017-T2/IND-5149 ; Secretaría de Estado de Investigación, Desarrollo e Innovación, Raphuel project (ENE2016-79608-C2-1-R) Retos Project MAT2017-84385-R ; Ministerio de Ciencia e Innovación, Juan de la Cierva Incorporación Fellowship (grant agreement no. IJC2019-038894-I) MOFSEIDON project (PID2019-104228RB-I00) Ramón y Cajal, Grant Agreements 2014-15039 and 2015-18677 ; Fundación BBVA, IN[17]CBBQUI_0197 ; H2020 European Research Council, ERC Consolidator Grant REALNANO 815128 Grant Agreement no. 731019 (EUSMI) ; sygmaSB; |
Approved |
Most recent IF: 8.867 |
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Call Number |
EMAT @ emat @c:irua:179791 |
Serial |
6802 |
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Author |
Boschker, H.T.S.; Cook, P.L.M.; Polerecky, L.; Eachambadi, R.T.; Lozano, H.; Hidalgo-Martinez, S.; Khalenkow, D.; Spampinato, V.; Claes, N.; Kundu, P.; Wang, D.; Bals, S.; Sand, K.K.; Cavezza, F.; Hauffman, T.; Bjerg, J.T.; Skirtach, A.G.; Kochan, K.; McKee, M.; Wood, B.; Bedolla, D.; Gianoncelli, A.; Geerlings, N.M.J.; Van Gerven, N.; Remaut, H.; Geelhoed, J.S.; Millan-Solsona, R.; Fumagalli, L.; Nielsen, L.P.; Franquet, A.; Manca, J.V.; Gomila, G.; Meysman, F.J.R. |
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Title |
Efficient long-range conduction in cable bacteria through nickel protein wires |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Nature Communications |
Abbreviated Journal |
Nat Commun |
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Volume |
12 |
Issue |
1 |
Pages |
3996 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Filamentous cable bacteria display long-range electron transport, generating electrical currents over centimeter distances through a highly ordered network of fibers embedded in their cell envelope. The conductivity of these periplasmic wires is exceptionally high for a biological material, but their chemical structure and underlying electron transport mechanism remain unresolved. Here, we combine high-resolution microscopy, spectroscopy, and chemical imaging on individual cable bacterium filaments to demonstrate that the periplasmic wires consist of a conductive protein core surrounded by an insulating protein shell layer. The core proteins contain a sulfur-ligated nickel cofactor, and conductivity decreases when nickel is oxidized or selectively removed. The involvement of nickel as the active metal in biological conduction is remarkable, and suggests a hitherto unknown form of electron transport that enables efficient conduction in centimeter-long protein structures. |
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Wos |
000669944900006 |
Publication Date |
2021-06-28 |
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Series Editor |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2041-1723 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
12.124 |
Times cited |
23 |
Open Access |
OpenAccess |
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Notes |
The authors thank Marlies Neiemeisland for assistance with Raman microscopy, Michiel Kienhuis for assistance with NanoSIMS analysis, Peter Hildebrandt and Diego Millo for helping with the interpretation of the Raman spectra, IONTOF for the Orbitrap Hybrid- SIMS analysis, and Rene Fabregas for helping with finite-element numerical modeling for SDM. H.T.S.B. and F.J.R.M. were financially supported by the Netherlands Organization for Scientific Research (VICI grant 016.VICI.170.072). Research Foundation Flanders supported F.J.R.M., J.V.M., and R.T.E. through FWO grant G031416N, and F.J.R.M. and J.S.G. through FWO grant G038819N. N.M.J.G. is the recipient of a Ph.D. scholarship for teachers from NWO in the Netherlands (grant 023.005.049). The NanoSIMS facility at Utrecht University was financed through a large infrastructure grant by the Netherlands Organization for Scientific Research (NWO, grant no. 175.010.2009.011) and through a Research Infrastructure Fund by the Utrecht University Board. A.G.S. is supported by the Special Research Fund (BOF) of Ghent University (BOF14/IOP/003, BAS094-18, 01IO3618) and FWO (G043219). The ToF-SIMS was funded by FWO Hercules grant (ZW/13/07) to J.V.M. and A.F. H.L., R.M.S., and G.G. were funded by the European Union H2020 Framework Programme (MSCA-ITN-2016) under grant agreement n 721874.EU, the Spanish Agencia Estatal de Investigación and EU FEDER under grant agreements TEC2016-79156-P and TEC2015-72751-EXP, the Generalitat de Catalunya through 2017-SGR1079 grant and CERCA Program. G.G. was recipient of an ICREA Academia Award, and H.L. of a FPI fellowship (BES-2015-074799) from the Agencia Estatal de Investigación/Fondo Social Europeo. L.F. received funding from the European Research Council (grant agreement No. 819417) under the European Union’s Horizon 2020 research and innovation programme. |
Approved |
Most recent IF: 12.124 |
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Call Number |
EMAT @ emat @c:irua:179813 |
Serial |
6803 |
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Author |
Coeck, R.; Meeprasert, J.; Li, G.; Altantzis, T.; Bals, S.; Pidko, E.A.; De Vos, D.E. |
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Title |
Gold and silver-catalyzed reductive amination of aromatic carboxylic acids to benzylic amines |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Acs Catalysis |
Abbreviated Journal |
Acs Catal |
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Volume |
11 |
Issue |
13 |
Pages |
7672-7684 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
The reductive amination of benzoic acid and its derivatives would be an effective addition to current synthesis methods for benzylamine. However, with current technology it is very difficult to keep the aromaticity intact when starting from benzoic acid, and salt wastes are often generated in the process. Here, we report a heterogeneous catalytic system for such a reductive amination, requiring solely H-2 and NH3 as the reactants. The Ag/TiO2 or Au/TiO2 catalysts can be used multiple times, and very little noble metal is required, only 0.025 mol % Au. The catalysts are bifunctional: the support catalyzes the dehydration of both the ammonium carboxylate to the amide and of the amide to the nitrile, while the sites at the metal-support interface promote the hydrogenation of the in situ generated nitrile. Yields of up to 92% benzylamine were obtained. |
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Wos |
000670659900005 |
Publication Date |
2021-06-10 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2155-5435 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
10.614 |
Times cited |
16 |
Open Access |
OpenAccess |
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Notes |
R.C. thanks the FWO for his SB PhD fellowship. D.E.D.V. acknowledges FWO for research project funding, as well as KU Leuven for funding in the Metusalem program Casas. S.B. acknowledges support from the European Research Council (ERC Consolidator grant #815128 REALNANO). T.A. acknowledges funding from the University of Antwerp Research fund (BOF). E.A.P. acknowledges the support from the European Research Council (ERC Consolidator grant #725686 DeliCAT). J.M. acknowledges financial support through the Royal Thai Government Scholarship. DFT calculations on SURFsara supercomputer facilities were performed with support from the Netherlands Organization for Scientific Research (NWO).; sygmaSB |
Approved |
Most recent IF: 10.614 |
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Call Number |
UA @ admin @ c:irua:179851 |
Serial |
6840 |
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Author |
Mychinko, M.; Skorikov, A.; Albrecht, W.; Sánchez‐Iglesias, A.; Zhuo, X.; Kumar, V.; Liz‐Marzán, L.M.; Bals, S. |
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Title |
The Influence of Size, Shape, and Twin Boundaries on Heat‐Induced Alloying in Individual Au@Ag Core–Shell Nanoparticles |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Small |
Abbreviated Journal |
Small |
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Volume |
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Issue |
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Pages |
2102348 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Environmental conditions during real-world application of bimetallic core–shell nanoparticles (NPs) often include the use of elevated temperatures, which are known to cause elemental redistribution, in turn significantly altering the properties of these nanomaterials. Therefore, a thorough understanding of such processes is of great importance. The recently developed combination of fast electron tomography with in situ heating holders is a powerful approach to investigate heat-induced processes at the single NP level, with high spatial resolution in 3D. In combination with 3D finite-difference diffusion simulations, this method can be used to disclose the influence of various NP parameters on the diffusion dynamics in Au@Ag core–shell systems. A detailed study of the influence of heating on atomic diffusion and alloying for Au@Ag NPs with varying core morphology and crystallographic details is carried out. Whereas the core shape and aspect ratio of the NPs play a minor role, twin boundaries are found to have a strong influence on the elemental diffusion. |
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Wos |
000673326600001 |
Publication Date |
2021-07-14 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1613-6810 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
8.643 |
Times cited |
8 |
Open Access |
OpenAccess |
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Notes |
The funding for this project was provided by European Research Council (ERC Consolidator Grant 815128, REALNANO) and European Commission (grant 731019, EUSMI and grant 26019, ESTEEM). This work was performed under the Maria de Maeztu Units of Excellence Programme-Grant No. MDM-2017-0720, Ministry of Science and Innovation.; sygmaSB |
Approved |
Most recent IF: 8.643 |
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Call Number |
EMAT @ emat @c:irua:179856 |
Serial |
6804 |
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| Permanent link to this record |
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Author |
Leinders, G.; Baldinozzi, G.; Ritter, C.; Saniz, R.; Arts, I.; Lamoen, D.; Verwerft, M. |
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Title |
Charge Localization and Magnetic Correlations in the Refined Structure of U3O7 |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Inorganic Chemistry |
Abbreviated Journal |
Inorg Chem |
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Volume |
60 |
Issue |
14 |
Pages |
10550-10564 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Atomic arrangements in the mixed-valence oxide U3O7 are refined from high-resolution neutron scattering data. The crystallographic model describes a long-range structural order in a U60O140 primitive cell (space group P42/n) containing distorted cuboctahedral oxygen clusters. By combining experimental data and electronic structure calculations accounting for spin–orbit interactions, we provide robust evidence of an interplay between charge localization and the magnetic moments carried by the uranium atoms. The calculations predict U3O7 to be a semiconducting solid with a band gap of close to 0.32 eV, and a more pronounced charge-transfer insulator behavior as compared to the well-known Mott insulator UO2. Most uranium ions (56 out of 60) occur in 9-fold and 10-fold coordinated environments, surrounding the oxygen clusters, and have a tetravalent (24 out of 60) or pentavalent (32 out of 60) state. The remaining uranium ions (4 out of 60) are not contiguous to the oxygen cuboctahedra and have a very compact, 8-fold coordinated environment with two short (2 × 1.93(3) Å) “oxo-type” bonds. The higher Hirshfeld charge and the diamagnetic character point to a hexavalent state for these four uranium ions. Hence, the valence state distribution corresponds to 24/60 × U(IV) + 32/60 U(V) + 4/60 U(VI). The tetravalent and pentavalent uranium ions are predicted to carry noncollinear magnetic moments (with amplitudes of 1.6 and 0.8 μB, respectively), resulting in canted ferromagnetic order in characteristic layers within the overall fluorite-related structure. |
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Place of Publication |
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Wos |
000675430900049 |
Publication Date |
2021-07-19 |
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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 |
0020-1669 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.857 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
Financial support for this research was partly provided by the Energy Transition Fund of the Belgian FPS Economy (Project SF-CORMOD – Spent Fuel CORrosion MODeling). This work was performed in part using HPC resources from GENCI-IDRIS (Grants 2020-101450 and 2020-101601), and in part by the VSC (Flemish Supercomputer Center) and the HPC infrastructure of the University of Antwerp (CalcUA), both funded by the FWO-Vlaanderen and the Flemish Government-department EWI. GL thanks E. Suard and C. Schreinemachers for assistance during the neutron scattering experiments at the ILL. GB acknowledges V. Petříček for suggestions on using JANA2006. |
Approved |
Most recent IF: 4.857 |
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Call Number |
EMAT @ emat @c:irua:179907 |
Serial |
6801 |
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Author |
Choukroun, D.; Pacquets, L.; Li, C.; Hoekx, S.; Arnouts, S.; Baert, K.; Hauffman, T.; Bals, S.; Breugelmans, T. |
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Title |
Mapping composition–selectivity relationships of supported sub-10 nm Cu–Ag nanocrystals for high-rate CO₂ electroreduction |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Acs Nano |
Abbreviated Journal |
Acs Nano |
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Volume |
15 |
Issue |
9 |
Pages |
14858-14872 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
Colloidal Cu–Ag nanocrystals measuring less than 10 nm across are promising candidates for integration in hybrid CO2 reduction reaction (CO2RR) interfaces, especially in the context of tandem catalysis and selective multicarbon (C2–C3) product formation. In this work, we vary the synthetic-ligand/copper molar ratio from 0.1 to 1.0 and the silver/copper atomic ratio from 0 to 0.7 and study the variations in the nanocrystals’ size distribution, morphology and reactivity at rates of ≥100 mA cm–2 in a gas-fed recycle electrolyzer operating under neutral to mildly basic conditions (0.1–1.0 M KHCO3). High-resolution electron microscopy and spectroscopy are used in order to characterize the morphology of sub-10 nm Cu–Ag nanodimers and core–shells and to elucidate trends in Ag coverage and surface composition. It is shown that Cu–Ag nanocrystals can be densely dispersed onto a carbon black support without the need for immediate ligand removal or binder addition, which considerably facilitates their application. Although CO2RR product distribution remains an intricate function of time, (kinetic) overpotential and processing conditions, we nevertheless conclude that the ratio of oxygenates to hydrocarbons (which depends primarily on the initial dispersion of the nanocrystals and their composition) rises 3-fold at moderate Ag atom % relative to Cu NCs-based electrodes. Finally, the merits of this particular Cu–Ag/C system and the recycling reactor employed are utilized to obtain maximum C2–C3 partial current densities of 92–140 mA cm–2 at −1.15 VRHE and liquid product concentrations in excess of 0.05 wt % in 1 M KHCO3 after short electrolysis periods. |
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Wos |
000703553600082 |
Publication Date |
2021-08-24 |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
25 |
Open Access |
OpenAccess |
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Notes |
D.C. acknowledges Thomas Kenis for configuring the analytical instrumentation (HPLC/GC-FID/ICP-MS), Hannelore Andries for assistance with ICP-MS measurements, and Dr. Saeid Pourbabak and Dr. Tine Derez for assistance with Cu sputtering. L.P. was supported by Research Foundation of Flanders (FWO 1S56920N). S.B. acknowledges financial support from ERC Consolidator grant number 815128 REALNANO. S.B. and T.B. acknowledge financial support from the university research fund (BOF-GOA-PS ID no. 33928).; sygmaSB |
Approved |
Most recent IF: 13.942 |
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Call Number |
UA @ admin @ c:irua:180305 |
Serial |
6844 |
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Author |
Peng, X.; Peng, H.; Zhao, K.; Zhang, Y.; Xia, F.; Lyu, J.; Van Tendeloo, G.; Sun, C.; Wu, J. |
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Title |
Direct visualization of atomic-scale heterogeneous structure dynamics in MnO₂ nanowires |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Acs Applied Materials & Interfaces |
Abbreviated Journal |
Acs Appl Mater Inter |
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Volume |
13 |
Issue |
28 |
Pages |
33644-33651 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Manganese oxides are attracting great interest owing to their rich polymorphism and multiple valent states, which give rise to a wide range of applications in catalysis, capacitors, ion batteries, and so forth. Most of their functionalities are connected to transitions among the various polymorphisms and Mn valences. However, their atomic-scale dynamics is still a great challenge. Herein, we discovered a strong heterogeneity in the crystalline structure and defects, as well as in the Mn valence state. The transitions are studied by in situ transmission electron microscopy (TEM), and they involve a complex ordering of [MnO6] octahedra as the basic building tunnels. MnO2 nanowires synthesized using solution-based hydrothermal methods usually exhibit a large number of multiple polymorphism impurities with different tunnel sizes. Upon heating, MnO2 nanowires undergo a series of stoichiometric polymorphism changes, followed by oxygen release toward an oxygen-deficient spinel and rock-salt phase. The impurity polymorphism exhibits an abnormally high stability with interesting small-large-small tunnel size transition, which is attributed to a preferential stabilizer (K+) concentration, as well as a strong competition of kinetics and thermodynamics. Our results unveil the complicated intergrowth of polymorphism impurities in MnO2, which provide insights into the heterogeneous kinetics, thermodynamics, and transport properties of the tunnel-based building blocks. |
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Place of Publication |
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Language |
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Wos |
000677540900101 |
Publication Date |
2021-07-08 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1944-8244 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7.504 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
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Approved |
Most recent IF: 7.504 |
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Call Number |
UA @ admin @ c:irua:180450 |
Serial |
6861 |
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