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Author |
Yang, S.; Liu, Z.; An, H.; Arnouts, S.; de Ruiter, J.; Rollier, F.; Bals, S.; Altantzis, T.; Figueiredo, M.C.; Filot, I.A.W.; Hensen, E.J.M.; Weckhuysen, B.M.; van der Stam, W. |
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Title |
Near-unity electrochemical CO₂ to CO conversion over Sn-doped copper oxide nanoparticles |
Type  |
A1 Journal article |
| |
Year |
2022 |
Publication |
ACS catalysis |
Abbreviated Journal |
Acs Catal |
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| |
Volume |
12 |
Issue |
24 |
Pages |
15146-15156 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
Bimetallic electrocatalysts have emerged as a viable strategy to tune the electrocatalytic CO2 reduction reaction (eCO2RR) for the selective production of valuable base chemicals and fuels. However, obtaining high product selectivity and catalyst stability remain challenging, which hinders the practical application of eCO2RR. In this work, it was found that a small doping concentration of tin (Sn) in copper oxide (CuO) has profound influence on the catalytic performance, boosting the Faradaic efficiency (FE) up to 98% for carbon monoxide (CO) at -0.75 V versus RHE, with prolonged stable performance (FE > 90%) for up to 15 h. Through a combination of ex situ and in situ characterization techniques, the in situ activation and reaction mechanism of the electrocatalyst at work was elucidated. In situ Raman spectroscopy measurements revealed that the binding energy of the crucial adsorbed *CO intermediate was lowered through Sn doping, thereby favoring gaseous CO desorption. This observation was confirmed by density functional theory, which further indicated that hydrogen adsorption and subsequent hydrogen evolution were hampered on the Sn-doped electrocatalysts, resulting in boosted CO formation. It was found that the pristine electrocatalysts consisted of CuO nanoparticles decorated with SnO2 domains, as characterized by ex situ high-resolution scanning transmission electron microscopy and X-ray photoelectron spectroscopy measurements. These pristine nanoparticles were subsequently in situ converted into a catalytically active bimetallic Sn-doped Cu phase. Our work sheds light on the intimate relationship between the bimetallic structure and catalytic behavior, resulting in stable and selective oxide-derived Sn-doped Cu electrocatalysts. |
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Place of Publication |
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Wos |
000900052400001 |
Publication Date |
2022-11-28 |
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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 |
2155-5435 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
12.9 |
Times cited |
16 |
Open Access |
OpenAccess |
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Notes |
B.M.W., S.Y., M.C.F., E.J.M.H., and W.v.d.S. acknowledge support from the Strategic UU-TU/e Alliance project ?Joint Centre for Chemergy Research?. S.B. acknowledges support from the European Research Council (ERC Consolidator grant #815128 REALNANO) . Z.L. acknowledges financial support of the China Scholarship Council and the Netherlands Organization for Scientific Research for access to computa-tional resources for carrying out the DFT calculations reported in this work. S.A. and T.A. acknowledge funding from theUniversity of Antwerp Research fund (BOF) . The authors also thank Dr. Jochem Wijten and Joris Janssens (Inorganic Chemistry and Catalysis, Utrecht University) for helpful technical support. Sander Deelen (Faculty of Science, Utrecht University) is acknowledged for the design of the in situ XRD cell. |
Approved |
Most recent IF: 12.9 |
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Call Number |
UA @ admin @ c:irua:192742 |
Serial |
7325 |
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| Permanent link to this record |
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Author |
Dinger, J.; Friedrich, T.; Reimann, T.; Toepfer, J. |
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Title |
NiMn₂O₄ revisited : temperature-dependent cation distribution from in situ neutron diffraction and thermopower studies |
Type |
A1 Journal article |
| |
Year |
2023 |
Publication |
Journal of the American Ceramic Society |
Abbreviated Journal |
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| |
Volume |
106 |
Issue |
3 |
Pages |
1834-1847 |
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| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
The cation distribution of the negative temperature coefficient (NTC) thermistor spinel NiMn2O4 was studied in the temperature range from 55 to 900 degrees C, using a combined in situ neutron diffraction and thermopower study. Rietveld refinements of in situ neutron diffraction data reveal a temperature dependence of the degree of inversion with an inversion parameter of 0.70(1) at 900 degrees C and 0.87(1) at 55 degrees C. Thermopower measurements were evaluated using a modified Heikes formula, and the [Mn4+]/[Mn3+] ratio on octahedral sites of the spinel structure was calculated considering spin and orbital degeneracy. The inversion degree and disproportionation parameter, determined independently as function of temperature, were used to calculate the cation distribution of NiMn2O4 in the whole temperature range. At high temperature, within the stability range of the spinel, the cation distribution is characterized by a moderate degree of inversion with a concentration of NiB2+${\mathrm{Ni}}\mathrm{B}< |
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Corporate Author |
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Publisher |
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Place of Publication |
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Editor |
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Wos |
000880360600001 |
Publication Date |
2022-10-21 |
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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 |
0002-7820 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
3.9 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 3.9; 2023 IF: 2.841 |
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Call Number |
UA @ admin @ c:irua:192087 |
Serial |
7326 |
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Author |
Vladimirova, N.V.; Frolov, A.S.; Sanchez-Barriga, J.; Clark, O.J.; Matsui, F.; Usachov, D.Y.; Muntwiler, M.; Callaert, C.; Hadermann, J.; Neudachina, V.S.; Tamm, M.E.; Yashina, L.V. |
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Title |
Occupancy of lattice positions probed by X-ray photoelectron diffraction : a case study of tetradymite topological insulators |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Surfaces and interfaces |
Abbreviated Journal |
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Volume |
36 |
Issue |
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Pages |
102516-10 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Occupancy of different structural positions in a crystal lattice often seems to play a key role in material prop-erties. Several experimental techniques have been developed to uncover this issue, all of them being mostly bulk sensitive. However, many materials including topological insulators (TIs), which are among the most intriguing modern materials, are intended to be used in devices as thin films, for which the sublattice occupancy may differ from the bulk. One of the possible approaches to occupancy analysis is X-ray Photoelectron Diffraction (XPD), a structural method in surface science with chemical sensitivity. We applied this method in a case study of Sb2(Te1-xSex)3 mixed crystals, which belong to prototypical TIs. We used high-angle annular dark field (HAADF) scanning transmission electron microscopy (STEM) as a reference method to verify our analysis. We revealed that the XPD data for vacuum cleaved bulk crystals are in excellent agreement with the reference ones. Also, we demonstrate that the anion occupancy near a naturally formed surface can be rather different from that of the bulk. The present results are relevant for a wide range of compositions where the system remains a topological phase, as we ultimately show by probing the transiently occupied topological surface state above the Fermi level by ultrafast photoemission. |
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Wos |
000901694900001 |
Publication Date |
2022-11-28 |
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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 |
2468-0230 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
6.2 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 6.2; 2023 IF: NA |
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Call Number |
UA @ admin @ c:irua:193502 |
Serial |
7327 |
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Author |
Spaeth, P.; Adhikari, S.; Heyvaert, W.; Zhuo, X.; Garcia, I.; Liz-Marzan, L.M.; Bals, S.; Orrit, M.; Albrecht, W. |
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Title |
Photothermal circular dichroism measurements of single chiral gold nanoparticles correlated with electron tomography |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
ACS Photonics |
Abbreviated Journal |
Acs Photonics |
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Volume |
9 |
Issue |
12 |
Pages |
3995-4004 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Chemically synthesized metal nanoparticles with morphological chiral features are known to exhibit strong circular dichroism. However, we still lack understanding of the correlation between morphological and chiroptical features of plasmonic nanoparticles. To shed light on that question, single nanoparticle experiments are required. We performed photothermal circular dichroism measurements of single chiral and achiral gold nanoparticles and correlated the chiroptical response to the 3D morphology of the same nanoparticles retrieved by electron tomography. In contrast to an ensemble measurement, we show that individual particles within the ensemble display a broad distribution of strength and handedness of circular dichroism signals. Whereas obvious structural chiral features, such as helical wrinkles, translate into chiroptical ones, nanoparticles with less obvious chiral morphological features can also display strong circular dichroism signals. Interestingly, we find that even seemingly achiral nanoparticles can display large g-factors. The origin of this circular dichroism signal is discussed in terms of plasmonics and other potentially relevant factors. |
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Corporate Author |
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Thesis |
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Place of Publication |
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Language |
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Wos |
000884432100001 |
Publication Date |
2022-11-08 |
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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 |
2330-4022 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7 |
Times cited |
5 |
Open Access |
OpenAccess |
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Notes |
This work was supported by The Netherlands Organisation for Scientific Research (NWO) as part of the Open Technology Program (OTP, Project No. 16008) and by a Spinoza prize (M.O.) . W.A. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020 Program (Grant No. 797153, SOPMEN) . L.M.L.M. acknowledges funding from MCIN/AEI/10.13039/501100011033 (Grants PID2020-117779RB-I00 and MDM-2017-0720) . We thank Dr. Wolfgang L?fer for providing optical equipment. We also acknowledge the European Soft Matter Infrastructure (EUSMI: E201200468) . |
Approved |
Most recent IF: 7 |
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Call Number |
UA @ admin @ c:irua:192098 |
Serial |
7331 |
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Author |
Smeyers, R.; Milošević, M.V.; Covaci, L. |
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Title |
Strong gate-tunability of flat bands in bilayer graphene due to moiré encapsulation between hBN monolayers |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Nanoscale |
Abbreviated Journal |
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Volume |
15 |
Issue |
9 |
Pages |
4561-4569 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT) |
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Abstract |
When using hexagonal boron-nitride (hBN) as a substrate for graphene, the resulting moire pattern creates secondary Dirac points. By encapsulating a multilayer graphene within aligned hBN sheets the controlled moire stacking may offer even richer benefits. Using advanced tight-binding simulations on atomistically-relaxed heterostructures, here we show that the gap at the secondary Dirac point can be opened in selected moire-stacking configurations, and is independent of any additional vertical gating of the heterostructure. On the other hand, gating can broadly tune the gap at the principal Dirac point, and may thereby strongly compress the first moire mini-band in width against the moire-induced gap at the secondary Dirac point. We reveal that in hBN-encapsulated bilayer graphene this novel mechanism can lead to isolated bands flatter than 10 meV under moderate gating, hence presenting a convenient pathway towards electronically-controlled strongly-correlated states on demand. |
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Corporate Author |
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Wos |
000933052600001 |
Publication Date |
2023-02-07 |
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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 |
2040-3364; 2040-3372 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
6.7 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 6.7; 2023 IF: 7.367 |
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Call Number |
UA @ admin @ c:irua:195249 |
Serial |
7340 |
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Author |
Parzyszek, S.; Tessarolo, J.; Pedrazo-Tardajos, A.; Ortuno, A.M.; Baginski, M.; Bals, S.; Clever, G.H.; Lewandowski, W. |
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Title |
Tunable circularly polarized luminescence via chirality induction and energy transfer from organic films to semiconductor nanocrystals |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
16 |
Issue |
11 |
Pages |
18472-18482 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Circularly polarized luminescent (CPL) films with high dissymmetry factors hold great potential for optoelectronic applications. Herei n , we propose a strategy for achieving strongly dissymetric CPL in nanocomposite films based on chira l i t y induction and energy transfer to semiconductor nanocrystals. First, focusing on a purely organic system, aggregation-induced emission (AIE) and CPL activity of organic liquid crystals (LCs) forming helical nanofilaments was detected, featuring green emission with high dissymmetry factors g(lum) similar to 10(-2). The handedness of helical filaments, and thus the sign of CPL, was controlled via minute amounts of a small chiral organic dopant. Second, nanocomposite films were fabricated by incorporating InP/ZnS semi-conductor quantum dots (QDs) into the LC matri x , which induced the chiral assembly of QDs and endowed them with chiroptical properties. Due to the spectral matching of the components, energy transfer (ET) from LC to QDs was possible enabling a convenient way of tuning CPL wavelengths by varying the LC/QD ratio. As obtained, composite films exhibited absolute glum values up to similar to 10(-2) and thermally on/off switchable luminescence. Overall, we demonstrate the induction of chiroptical properties by the assembly of nonchiral building QDs on the chiral organic template and energy transfer from organic films to QDs, representing a simple and versatile approach to tune the CPL activity of organic materials. |
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Corporate Author |
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Thesis |
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Place of Publication |
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Editor |
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Language |
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Wos |
000883943600001 |
Publication Date |
2022-11-07 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
17.1 |
Times cited |
10 |
Open Access |
OpenAccess |
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Notes |
W.L., S.P., and M.B. acknowledge support from the National Science Center Poland under the OPUS Grant UMO-2019/35/B/ST5/04488. J.T. and G.H.C. acknowledge the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany's Excellence Strategy, Grant EXC 2033-390677874-RESOLV. W.L. acknowledges financial support from the European Commission under the Horizon 2020 Programme by Grant E210400529. S.B. and A.P.-T. acknowledge financial support from the European Commission under the Horizon 2020 Programme by Grant 731019 (EUSMI) and ERC Consolidator Grant 815128 (REALNANO). We thank Elie Benchimol for his help with the CPL measurements. We thank Damian Pociecha for his help in the determination of phase sequences of organic compounds. |
Approved |
Most recent IF: 17.1 |
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Call Number |
UA @ admin @ c:irua:192101 |
Serial |
7345 |
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| Permanent link to this record |
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Author |
Mulder, J.T.; Meijer, M.S.; van Blaaderen, J.J.; du Fosse, I.; Jenkinson, K.; Bals, S.; Manna, L.; Houtepen, A.J. |
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Title |
Understanding and preventing photoluminescence quenching to achieve unity photoluminescence quantum yield in Yb:YLF nanocrystals |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
ACS applied materials and interfaces |
Abbreviated Journal |
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Volume |
15 |
Issue |
2 |
Pages |
3274-3286 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Ytterbium-doped LiYF4 (Yb:YLF) is a commonly used material for laser applications, as a photon upconversion medium, and for optical refrigeration. As nanocrystals (NCs), the material is also of interest for biological and physical applications. Unfortunately, as with most phosphors, with the reduction in size comes a large reduction of the photoluminescence quantum yield (PLQY), which is typically associated with an increase in surface-related PL quenching. Here, we report the synthesis of bipyramidal Yb:YLF NCs with a short axis of similar to 60 nm. We systematically study and remove all sources of PL quenching in these NCs. By chemically removing all traces of water from the reaction mixture, we obtain NCs that exhibit a near-unity PLQY for an Yb3+ concentration below 20%. At higher Yb3+ concentrations, efficient concentration quenching occurs. The surface PL quenching is mitigated by growing an undoped YLF shell around the NC core, resulting in near-unity PLQY values even for fully Yb3+-based LiYbF4 cores. This unambiguously shows that the only remaining quenching sites in core-only Yb:YLF NCs reside on the surface and that concentration quenching is due to energy transfer to the surface. Monte Carlo simulations can reproduce the concentration dependence of the PLQY. Surprisingly, Fo''rster resonance energy transfer does not give satisfactory agreement with the experimental data, whereas nearest-neighbor energy transfer does. This work demonstrates that Yb3+-based nanophosphors can be synthesized with a quality close to that of bulk single crystals. The high Yb3+ concentration in the LiYbF4/LiYF4 core/shell nanocrystals increases the weak Yb3+ absorption, making these materials highly promising for fundamental studies and increasing their effectiveness in bioapplications and optical refrigeration. |
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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 |
000912997300001 |
Publication Date |
2023-01-06 |
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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 |
1944-8244 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.5 |
Times cited |
3 |
Open Access |
OpenAccess |
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Notes |
This project has received funding from the European Union's Horizon 2020 research and innovation program under Grant Agreement No. 766900 (Testing the Large-Scale Limit of Quantum Mechanics). A.J.H. and I.d.F. further acknowledge the European Research Council Horizon 2020 ERC Grant Agreement No. 678004 (Doping on Demand) for financial support. The authors thank Freddy Rabouw and Andries Meijerink (Utrecht University) for very fruitful discussions and extremely useful advice. The author s thank Jos Thieme for his help with the laser setups used . The authors furthermore thank Niranjan Saikumar for proofreading the manuscript. |
Approved |
Most recent IF: 9.5; 2023 IF: 7.504 |
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Call Number |
UA @ admin @ c:irua:194317 |
Serial |
7348 |
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Author |
Yang, C.-Q.; Zhi, R.; Rothmann, M.U.; Xu, Y.-Y.; Li, L.-Q.; Hu, Z.-Y.; Pang, S.; Cheng, Y.-B.; Van Tendeloo, G.; Li, W. |
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Title |
Unveiling the intrinsic structure and intragrain defects of organic-inorganic hybrid perovskites by ultralow dose transmission electron microscopy |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Advanced materials |
Abbreviated Journal |
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Volume |
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Issue |
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Pages |
1-9 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Transmission electron microscopy (TEM) is a powerful tool for unveiling the structural, compositional, and electronic properties of organic-inorganic hybrid perovskites (OIHPs) at the atomic to micrometer length scales. However, the structural and compositional instability of OIHPs under electron beam radiation results in misunderstandings of the microscopic structure-property-performance relationship in OIHP devices. Here, ultralow dose TEM is utilized to identify the mechanism of the electron-beam-induced changes in OHIPs and clarify the cumulative electron dose thresholds (critical dose) of different commercially interesting state-of-the-art OIHPs, including methylammonium lead iodide (MAPbI(3)), formamidinium lead iodide (FAPbI(3)), FA(0.83)Cs(0.17)PbI(3), FA(0.15)Cs(0.85)PbI(3), and MAPb(0.5)Sn(0.5)I(3). The critical dose is related to the composition of the OIHPs, with FA(0.15)Cs(0.85)PbI(3) having the highest critical dose of approximate to 84 e angstrom(-2) and FA(0.83)Cs(0.17)PbI(3) having the lowest critical dose of approximate to 4.2 e angstrom(-2). The electron beam irradiation results in the formation of a superstructure with ordered I and FA vacancies along (c), as identified from the three major crystal axes in cubic FAPbI(3), (c), (c), and (c). The intragrain planar defects in FAPbI(3) are stable, while an obvious modification is observed in FA(0.83)Cs(0.17)PbI(3) under continuous electron beam exposure. This information can serve as a guide for ensuring a reliable understanding of the microstructure of OIHP optoelectronic devices by TEM. |
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Corporate Author |
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Publisher |
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Place of Publication |
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Language |
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Wos |
000950461600001 |
Publication Date |
2023-02-13 |
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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 |
29.4 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
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Approved |
Most recent IF: 29.4; 2023 IF: 19.791 |
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Call Number |
UA @ admin @ c:irua:195116 |
Serial |
7349 |
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| Permanent link to this record |
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Author |
Benedet, M.; Andrea Rizzi, G.; Gasparotto, A.; Gauquelin, N.; Orekhov, A.; Verbeeck, J.; Maccato, C.; Barreca, D. |
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Title |
Functionalization of graphitic carbon nitride systems by cobalt and cobalt-iron oxides boosts solar water oxidation performances |
Type |
A1 Journal article |
| |
Year |
2023 |
Publication |
Applied surface science |
Abbreviated Journal |
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Volume |
618 |
Issue |
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Pages |
156652 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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| |
Abstract |
The ever-increasing energy demand from the world population has made the intensive use of fossil fuels an overarching threat to global environment and human health. An appealing alternative is offered by sunlight-assisted photoelectrochemical water splitting to yield carbon-free hydrogen fuel, but kinetic limitations associated to the oxygen evolution reaction (OER) render the development of cost-effective, eco-friendly and stable electrocatalysts an imperative issue. In the present work, OER catalysts based on graphitic carbon nitride (g-C3N4) were deposited on conducting glass substrates by a simple decantation procedure, followed by functionalization with low amounts of nanostructured CoO and CoFe2O4 by radio frequency (RF)-sputtering, and final annealing under inert atmosphere. A combination of advanced characterization tools was used to investigate the interplay between material features and electrochemical performances. The obtained results highlighted the formation of a p-n junction for the g-C3N4-CoO system, whereas a Z-scheme junction accounted for the remarkable performance enhancement yielded by g-C3N4-CoFe2O4. The intimate contact between the system components also afforded an improved electrocatalyst stability in comparison to various bare and functionalized g-C3N4-based systems. These findings emphasize the importance of tailoring g-C3N4 chemico-physical properties through the dispersion of complementary catalysts to fully exploit its applicative potential. |
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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 |
000950654300001 |
Publication Date |
2023-02-04 |
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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 |
0169-4332 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
6.7 |
Times cited |
11 |
Open Access |
OpenAccess |
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| |
Notes |
The authors gratefully acknowledge financial support from CNR (Progetti di Ricerca @CNR – avviso 2020 – ASSIST), Padova University (P-DiSC#04BIRD2020-UNIPD EUREKA, DOR 2020–2022), AMGA Foundation (NYMPHEA project), INSTM Consortium (INSTM21PDGASPAROTTO – NANOMAT, INSTM21PDBARMAC – ATENA) and the European Union's Horizon 2020 research and innovation program under grant agreement No 823717 – ESTEEM3. The FWO-Hercules fund G0H4316N 'Direct electron detector for soft matter TEM' is also acknowledged. Many thanks are due to Prof. Luca Gavioli (Università Cattolica del Sacro Cuore, Brescia, Italy) and Dr. Riccardo Lorenzin (Department of Chemical Sciences, Padova University, Italy) for their invaluable technical support.; esteem3reported; esteem3TA |
Approved |
Most recent IF: 6.7; 2023 IF: 3.387 |
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| |
Call Number |
EMAT @ emat @c:irua:196150 |
Serial |
7376 |
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| Permanent link to this record |
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| |
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Author |
Verdierre, G.; Gauquelin, N.; Jannis, D.; Birkhölzer, Y.A.; Mallik, S.; Verbeeck, J.; Bibes, M.; Koster, G. |
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Title |
Epitaxial growth of the candidate ferroelectric Rashba material SrBiO3by pulsed laser deposition |
Type |
A1 Journal article |
| |
Year |
2023 |
Publication |
APL materials |
Abbreviated Journal |
|
|
| |
Volume |
11 |
Issue |
3 |
Pages |
031109 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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| |
Abstract |
Among oxides, bismuthates have been gaining much interest due to their unique features. In addition to their superconducting properties, they show potential for applications as topological insulators and as possible spin-to-charge converters. After being first investigated in their bulk form in the 1980s, bismuthates have been successfully grown as thin films. However, most efforts have focused on BaBiO<sub>3</sub>, with SrBiO<sub>3</sub>receiving only little attention. Here, we report the growth of epitaxial films of SrBiO<sub>3</sub>on both TiO<sub>2</sub>-terminated SrTiO<sub>3</sub>and NdO-terminated NdScO<sub>3</sub>substrates by pulsed laser deposition. SrBiO<sub>3</sub>has a pseudocubic lattice constant of ∼4.25 Å and grows relaxed on NdScO<sub>3</sub>. Counter-intuitively, it grows with a slight tensile strain on SrTiO<sub>3</sub>despite a large lattice mismatch, which should induce compressive strain. High-resolution transmission electron microscopy reveals that this occurs as a consequence of structural domain matching, with blocks of 10 SrBiO<sub>3</sub>unit planes matching blocks of 11 SrTiO<sub>3</sub>unit planes. This work provides a framework for the synthesis of high quality perovskite bismuthates films and for the understanding of their interface interactions with homostructural substrates. |
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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 |
000953363800004 |
Publication Date |
2023-03-01 |
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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 |
|
Edition |
|
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| |
ISSN |
2166-532X |
ISBN |
|
Additional Links |
UA library record; WoS full record |
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| |
Impact Factor |
6.1 |
Times cited |
|
Open Access |
OpenAccess |
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| |
Notes |
This work received support from the ERC Advanced grant (Grant No. 833973) “FRESCO” and funding from the European Union’s Horizon 2020 Research and Innovation Program under Grant Agreement No. 823717—ESTEEM3, Van Gogh travel grant, Nuffic, The Netherlands (CF No. 42582SB).; esteem3reported; esteem3TA |
Approved |
Most recent IF: 6.1; 2023 IF: 4.335 |
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| |
Call Number |
EMAT @ emat @c:irua:196135 |
Serial |
7377 |
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| Permanent link to this record |
| |
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| |
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Author |
Benedoue, S.; Benedet, M.; Gasparotto, A.; Gauquelin, N.; Orekhov, A.; Verbeeck, J.; Seraglia, R.; Pagot, G.; Rizzi, G.A.; Balzano, V.; Gavioli, L.; Noto, V.D.; Barreca, D.; Maccato, C. |
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Title |
Insights into the Photoelectrocatalytic Behavior of gCN-Based Anode Materials Supported on Ni Foams |
Type |
A1 Journal article |
| |
Year |
2023 |
Publication |
Nanomaterials |
Abbreviated Journal |
Nanomaterials-Basel |
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| |
Volume |
13 |
Issue |
6 |
Pages |
1035 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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| |
Abstract |
Graphitic carbon nitride (gCN) is a promising n-type semiconductor widely investigated for photo-assisted water splitting, but less studied for the (photo)electrochemical degradation of aqueous organic pollutants. In these fields, attractive perspectives for advancements are offered by a proper engineering of the material properties, e.g., by depositing gCN onto conductive and porous scaffolds, tailoring its nanoscale morphology, and functionalizing it with suitable cocatalysts. The present study reports on a simple and easily controllable synthesis of gCN flakes on Ni foam substrates by electrophoretic deposition (EPD), and on their eventual decoration with Co-based cocatalysts [CoO, CoFe2O4, cobalt phosphate (CoPi)] via radio frequency (RF)-sputtering or electrodeposition. After examining the influence of processing conditions on the material characteristics, the developed systems are comparatively investigated as (photo)anodes for water splitting and photoelectrocatalysts for the degradation of a recalcitrant water pollutant [potassium hydrogen phthalate (KHP)]. The obtained results highlight that while gCN decoration with Co-based cocatalysts boosts water splitting performances, bare gCN as such is more efficient in KHP abatement, due to the occurrence of a different reaction mechanism. The related insights, provided by a multi-technique characterization, may provide valuable guidelines for the implementation of active nanomaterials in environmental remediation and sustainable solar-to-chemical energy conversion. |
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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 |
000960297000001 |
Publication Date |
2023-03-13 |
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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 |
2079-4991 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
5.3 |
Times cited |
3 |
Open Access |
OpenAccess |
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| |
Notes |
The present work was financially supported by CNR (Progetti di Ricerca @CNR—avviso 2020—ASSIST), Padova University (P-DiSC#04BIRD2020-UNIPD EUREKA, DOR 2020–2022), AMGA Foundation (NYMPHEA project), INSTM Consortium (INSTM21PDGASPAROTTO—NANOMAT, INSTM21PDBARMAC—ATENA) and the European Union’s Horizon 2020 research and innovation program under grant agreement No. 823717—ESTEEM3. The FWO-Hercules fund G0H4316N ‘Direct electron detector for soft matter TEM’ is also acknowledged. Many thanks are also due to Dr. Riccardo Lorenzin for his support to experimental activities.; esteem3reported; esteem3TA |
Approved |
Most recent IF: 5.3; 2023 IF: 3.553 |
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| |
Call Number |
EMAT @ emat @c:irua:196115 |
Serial |
7378 |
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| Permanent link to this record |
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Author |
Jain, N.; Hao, Y.; Parekh, U.; Kaltenegger, M.; Pedrazo-Tardajos, A.; Lazzaroni, R.; Resel, R.; Geerts, Y.H.; Bals, S.; Van Aert, S. |
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Title |
Exploring the effects of graphene and temperature in reducing electron beam damage: A TEM and electron diffraction-based quantitative study on Lead Phthalocyanine (PbPc) crystals |
Type |
A1 Journal article |
| |
Year |
2023 |
Publication |
Micron |
Abbreviated Journal |
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| |
Volume |
169 |
Issue |
|
Pages |
103444 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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| |
Abstract |
High-resolution transmission electron microscopy (TEM) of organic crystals, such as Lead Phthalocyanine (PbPc), is very challenging since these materials are prone to electron beam damage leading to the breakdown of the crystal structure during investigation. Quantification of the damage is imperative to enable high-resolution imaging of PbPc crystals with minimum structural changes. In this work, we performed a detailed electron diffraction study to quantitatively measure degradation of PbPc crystals upon electron beam irradiation. Our study is based on the quantification of the fading intensity of the spots in the electron diffraction patterns. At various incident dose rates (e/Å2/s) and acceleration voltages, we experimentally extracted the decay rate (1/s), which directly correlates with the rate of beam damage. In this manner, a value for the critical dose (e/Å2) could be determined, which can be used as a measure to quantify beam damage. Using the same methodology, we explored the influence of cryogenic temperatures, graphene TEM substrates, and graphene encapsulation in prolonging the lifetime of the PbPc crystal structure during TEM investigation. The knowledge obtained by diffraction experiments is then translated to real space high-resolution TEM imaging of PbPc. |
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Corporate Author |
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Thesis |
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Place of Publication |
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Editor |
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Language |
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Wos |
000965998800001 |
Publication Date |
2023-03-21 |
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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 |
0968-4328 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
2.4 |
Times cited |
1 |
Open Access |
OpenAccess |
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| |
Notes |
This work is supported by FWO and FNRS within the 2Dto3D network of the EOS (Excellence of Science) program (grant number 30489208) and ERC-CoGREALNANO-815128 (to Prof. Dr. Sara Bals). N.J. would like to thank Dr. Kunal S. Mali and Dr. Da Wang for useful and interesting discussions on sample preparation procedures. |
Approved |
Most recent IF: 2.4; 2023 IF: 1.98 |
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Call Number |
EMAT @ emat @c:irua:196069 |
Serial |
7379 |
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| Permanent link to this record |
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Author |
Kante, M.V.; Weber, M.L.; Ni, S.; van den Bosch, I.C.G.; van der Minne, E.; Heymann, L.; Falling, L.J.; Gauquelin, N.; Tsvetanova, M.; Cunha, D.M.; Koster, G.; Gunkel, F.; Nemsak, S.; Hahn, H.; Estrada, L.V.; Baeumer, C. |
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Title |
A high-entropy oxide as high-activity electrocatalyst for water oxidation |
Type |
A1 Journal article |
| |
Year |
2023 |
Publication |
ACS nano |
Abbreviated Journal |
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Volume |
17 |
Issue |
6 |
Pages |
5329-5339 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
High-entropy materials are an emerging pathway in the development of high-activity (electro)catalysts because of the inherent tunability and coexistence of multiple potential active sites, which may lead to earth-abundant catalyst materials for energy-efficient electrochemical energy storage. In this report, we identify how the multication composition in high-entropy perovskite oxides (HEO) contributes to high catalytic activity for the oxygen evolution reaction (OER), i.e., the key kinetically limiting half-reaction in several electrochemical energy conversion technologies, including green hydrogen generation. We compare the activity of the (001) facet of LaCr0.2Mn0.2Fe0.2Co0.2Ni0.2O3-delta with the parent compounds (single B-site in the ABO3 perovskite). While the single B-site perovskites roughly follow the expected volcano-type activity trends, the HEO clearly outperforms all of its parent compounds with 17 to 680 times higher currents at a fixed overpotential. As all samples were grown as an epitaxial layer, our results indicate an intrinsic composition-function relationship, avoiding the effects of complex geometries or unknown surface composition. In-depth X-ray photoemission studies reveal a synergistic effect of simultaneous oxidation and reduction of different transition metal cations during the adsorption of reaction intermediates. The surprisingly high OER activity demonstrates that HEOs are a highly attractive, earth-abundant material class for high-activity OER electrocatalysts, possibly allowing the activity to be fine-tuned beyond the scaling limits of mono-or bimetallic oxides. |
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Corporate Author |
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Place of Publication |
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Language |
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Wos |
000953440900001 |
Publication Date |
2023-03-13 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
17.1 |
Times cited |
|
Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 17.1; 2023 IF: 13.942 |
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Call Number |
UA @ admin @ c:irua:196097 |
Serial |
7390 |
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Author |
Cao, M.; Xiong, D.-B.; Tan, Z.; Ji, G.; Amin-Ahmadi, B.; Guo, Q.; Fan, G.; Guo, C.; Li, Z.; Zhang, D. |
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Title |
Aligning graphene in bulk copper : nacre-inspired nanolaminated architecture coupled with in-situ processing for enhanced mechanical properties and high electrical conductivity |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
Carbon |
Abbreviated Journal |
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Volume |
117 |
Issue |
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Pages |
65-74 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Methods used to strengthen metals generally also cause a pronounced decrease in ductility and electrical conductivity. In this work a bioinspired strategy is applied to surmount the dilemma. By assembling copper submicron flakes cladded with in-situ grown graphene, graphene/copper matrix composites with a nanolaminated architecture inspired by a natural nacre have been prepared. Owing to a combined effect-from the bioinspired nanolaminated architecture and improved interfacial bonding, a synergy has been achieved between mechanical strength and ductility as well as electrical conductivity in the graphene/copper matrix composites. With a low volume fraction of only 2.5% of graphene, the composite shows a yield strength and elastic modulus similar to 177% and similar to 25% higher than that of unreinforced copper matrix, respectively, while retains ductility and electrical conductivity comparable to that of pure copper. The bioinspired nanolaminated architecture enhances the efficiencies of two-dimensional (2D) graphene in mechanical strengthening and electrical conducting by aligning graphene to maximize performance for required loading and carrier transporting conditions, and toughens the composites by crack deflection. Meanwhile, in-situ growth of graphene is beneficial for improving interfacial bonding and structural quality of graphene. The strategy sheds light on the development of composites with good combined structural and functional properties. (C) 2017 Elsevier Ltd. All rights reserved. |
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Corporate Author |
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Thesis |
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Place of Publication |
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Language |
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Wos |
000400212100008 |
Publication Date |
2017-02-27 |
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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 |
0008-6223 |
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 |
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Open Access |
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Notes |
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Approved |
no |
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Call Number |
UA @ admin @ c:irua:152635 |
Serial |
7435 |
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Author |
Sanchez-Barriga, J.; Aguilera, I.; Yashina, L., V; Tsukanova, D.Y.; Freyse, F.; Chaika, A.N.; Callaert, C.; Abakumov, A.M.; Hadermann, J.; Varykhalov, A.; Rienks, E.D.L.; Bihlmayer, G.; Blugel, S.; Rader, O. |
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Title |
Anomalous behavior of the electronic structure of (Bi1-xInx)2Se3across the quantum phase transition from topological to trivial insulator |
Type |
A1 Journal article |
| |
Year |
2018 |
Publication |
Physical review B |
Abbreviated Journal |
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| |
Volume |
98 |
Issue |
23 |
Pages |
235110 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Using spin- and angle-resolved photoemission spectroscopy and relativistic many-body calculations, we investigate the evolution of the electronic structure of (Bi1-xInx)(2)Se-3)(2)Se-3 bulk single crystals around the critical point of the trivial to topological insulator quantum-phase transition. By increasing x, we observe how a surface gap opens at the Dirac point of the initially gapless topological surface state of Bi2Se3, leading to the existence of massive fermions. The surface gap monotonically increases for a wide range of x values across the topological and trivial sides of the quantum-phase transition. By means of photon-energy-dependent measurements, we demonstrate that the gapped surface state survives the inversion of the bulk bands which occurs at a critical point near x = 0.055. The surface state exhibits a nonzero in-plane spin polarization which decays exponentially with increasing x, and which persists in both the topological and trivial insulator phases. Our calculations reveal qualitative agreement with the experimental results all across the quantum-phase transition upon the systematic variation of the spin-orbit coupling strength. A non-time-reversal symmetry-breaking mechanism of bulk-mediated scattering processes that increase with decreasing spin-orbit coupling strength is proposed as explanation. |
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Place of Publication |
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Wos |
000452322800003 |
Publication Date |
2018-12-05 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2469-9969; 2469-9950 |
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 |
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Open Access |
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Notes |
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Approved |
no |
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Call Number |
UA @ admin @ c:irua:156240 |
Serial |
7462 |
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| Permanent link to this record |
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Author |
Belik, A.A.; Morozov, V.A.; Deyneko, D.V.; Savon, A.E.; Baryshnikova, O.V.; Zhukovskaya, E.S.; Dorbakov, N.G.; Katsuya, Y.; Tanaka, M.; Stefanovich, S.Y.; Hadermann, J.; Lazoryak, B.I. |
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Title |
Antiferroelectric properties and site occupations ofR3+ cations in Ca8MgR(PO4)7 luminescent host materials |
Type |
A1 Journal article |
| |
Year |
2017 |
Publication |
Journal of alloys and compounds |
Abbreviated Journal |
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Volume |
699 |
Issue |
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Pages |
928-937 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Ca8MgR(PO4)(7) = La, Pr, Nd, Sm-Lu, and Y) phosphates with a beta-Ca-3(PO4)(2) related structure were prepared by a standard solid-state method in air. Second-harmonic generation, differential scanning calorimetry, and dielectric measurements led to the conclusion that all Ca8MgR(PO4)(7) are centrosymmetric and go to another centrosymmetric phase in the course of a first-order antiferroelectric phase transition well above room temperature (RT). High-temperature electron diffraction showed that the symmetry changes from R (3) over barc to R (3) over barm during the phase transition. Structures of Ca8MgR(PO4)(7) at RT were refined by the Rietveld method in centrosymmetric space group R (3) over barc. Mg2+ cations occupy the M5 site; the occupancy of the M1 site by R3+ cations increases monotonically from 0.0389 for R = La to 0.1667 for R = Er-Lu, whereas the occupancy of the M3 site by R3+ cations decreases monotonically from 0.1278 for R = La to 0 for R = Er-Lu. In the case of R = Er-Lu, the M3 site is occupied only by Ca2+ cations. P1O(4) tetrahedra and cations at the M3 site are disordered in the R (3) over barc structure of Ca8MgEu(PO4)(7). Using synchrotron X-ray powder diffraction, we found that annealing conditions do not significantly affect the distribution of Ca2+ and Eu3+ cations between the structure positions of Ca8MgEu(PO4)(7). Luminescent properties of CasMgEu(PO4)(7) powder samples were investigated under near-ultraviolet (n-UV) light. Excitation spectra of CasMgEu(PO4)(7) show the strongest absorption at about 395 nm that matches with commercially available n-UV-emitting GaN-based LED chips. Emission spectra show an intense red emission due to the D-5(0) -> F-7(2) transition of Eu3+. (C) 2016 Elsevier B.V. All rights reserved. |
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Place of Publication |
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Wos |
000393727500129 |
Publication Date |
2016-12-24 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0925-8388 |
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 |
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Open Access |
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Notes |
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Approved |
no |
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Call Number |
UA @ admin @ c:irua:152665 |
Serial |
7464 |
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| Permanent link to this record |
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Author |
Takatsu, H.; Hernandez, O.; Yoshimune, W.; Prestipino, C.; Yamamoto, T.; Tassel, C.; Kobayashi, Y.; Batuk, D.; Shibata, Y.; Abakumov, A.M.; Brown, C.M.; Kageyama, H. |
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Title |
Cubic lead perovskite PbMoO3 with anomalous metallic behavior |
Type |
A1 Journal article |
| |
Year |
2017 |
Publication |
Physical review B |
Abbreviated Journal |
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| |
Volume |
95 |
Issue |
15 |
Pages |
155105 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
A previously unreported Pb-based perovskite PbMoO3 is obtained by high-pressure and high-temperature synthesis. This material crystallizes in the Pm3m cubic structure at room temperature, making it distinct from typical Pb-based perovskite oxides with a structural distortion. PbMoO3 exhibits a metallic behavior down to 0.1 K with an unusual T-sublinear dependence of the electrical resistivity. Moreover, a large specific heat is observed at low temperatures accompanied by a peak in C-P/T-3 around 10 K, in marked contrast to the isostructural metallic system SrMoO3. These transport and thermal properties for PbMoO3, taking into account anomalously large Pb atomic displacements detected through diffraction experiments, are attributed to a low-energy vibrational mode, associated with incoherent off-centering of lone-pair Pb2+ cations. We discuss the unusual behavior of the electrical resistivity in terms of a polaronlike conduction, mediated by the strong coupling between conduction electrons and optical phonons of the local low-energy vibrational mode. |
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Language |
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Wos |
000440605700001 |
Publication Date |
2017-04-04 |
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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 |
2469-9969; 2469-9950 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
|
Times cited |
|
Open Access |
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| |
Notes |
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Approved |
no |
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| |
Call Number |
UA @ admin @ c:irua:167288 |
Serial |
7743 |
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| Permanent link to this record |
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| |
|
Author |
Naberezhnyi, D.; Rumyantseva, M.; Filatova, D.; Batuk, M.; Hadermann, J.; Baranchikov, A.; Khmelevsky, N.; Aksenenko, A.; Konstantinova, E.; Gaskov, A. |
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| |
Title |
Effects of Ag additive in low temperature CO detection with In2O3 based gas sensors |
Type |
A1 Journal article |
| |
Year |
2018 |
Publication |
Nanomaterials |
Abbreviated Journal |
|
|
| |
Volume |
8 |
Issue |
10 |
Pages |
801 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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| |
Abstract |
Nanocomposites In2O3/Ag obtained by ultraviolet (UV) photoreduction and impregnation methods were studied as materials for CO sensors operating in the temperature range 25-250 degrees C. Nanocrystalline In2O3 and In2O3/Ag nanocomposites were characterized by X-ray diffraction (XRD), single-point Brunauer-Emmet-Teller (BET) method, scanning electron microscopy (SEM), transmission electron microscopy (TEM), and high angle annular dark field scanning transmission electron microscopy (HAADF-STEM) with energy dispersive X-ray (EDX) mapping. The active surface sites were investigated using Fourier-transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), electron paramagnetic resonance (EPR) spectroscopy and thermo-programmed reduction with hydrogen (TPR-H-2) method. Sensor measurements in the presence of 15 ppm CO demonstrated that UV treatment leads to a complete loss of In2O3 sensor sensitivity, while In2O3/Ag-UV nanocomposite synthesized by UV photoreduction demonstrates an increased sensor signal to CO at T < 200 degrees C. The observed high sensor response of the In2O3/Ag-UV nanocomposite at room temperature may be due to the realization of an additional mechanism of CO oxidation with participation of surface hydroxyl groups associated via hydrogen bonds. |
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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 |
000451174100057 |
Publication Date |
2018-10-08 |
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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 |
2079-4991 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
|
Times cited |
|
Open Access |
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| |
Notes |
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Approved |
no |
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| |
Call Number |
UA @ admin @ c:irua:156335 |
Serial |
7842 |
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| Permanent link to this record |
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| |
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Author |
Chen, H.; Xiong, Y.; Li, J.; Abed, J.; Wang, D.; Pedrazo-Tardajos, A.; Cao, Y.; Zhang, Y.; Wang, Y.; Shakouri, M.; Xiao, Q.; Hu, Y.; Bals, S.; Sargent, E.H.H.; Su, C.-Y.; Yang, Z. |
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Title |
Epitaxially grown silicon-based single-atom catalyst for visible-light-driven syngas production |
Type |
A1 Journal article |
| |
Year |
2023 |
Publication |
Nature communications |
Abbreviated Journal |
Nat Commun |
|
| |
Volume |
14 |
Issue |
1 |
Pages |
1719-11 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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| |
Abstract |
Despite the natural abundance and promising properties of Si, there are few examples of crystalline Si-based catalysts. Here, the authors report an epitaxial growth method to construct Co single atoms on Si for light driven CO2 reduction to syngas. Improving the dispersion of active sites simultaneous with the efficient harvest of photons is a key priority for photocatalysis. Crystalline silicon is abundant on Earth and has a suitable bandgap. However, silicon-based photocatalysts combined with metal elements has proved challenging due to silicon's rigid crystal structure and high formation energy. Here we report a solid-state chemistry that produces crystalline silicon with well-dispersed Co atoms. Isolated Co sites in silicon are obtained through the in-situ formation of CoSi2 intermediate nanodomains that function as seeds, leading to the production of Co-incorporating silicon nanocrystals at the CoSi2/Si epitaxial interface. As a result, cobalt-on-silicon single-atom catalysts achieve an external quantum efficiency of 10% for CO2-to-syngas conversion, with CO and H-2 yields of 4.7 mol g((Co))(-1) and 4.4 mol g((Co))(-1), respectively. Moreover, the H-2/CO ratio is tunable between 0.8 and 2. This photocatalyst also achieves a corresponding turnover number of 2 x 10(4) for visible-light-driven CO2 reduction over 6 h, which is over ten times higher than previously reported single-atom photocatalysts. |
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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 |
000962607600018 |
Publication Date |
2023-03-28 |
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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 |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
2041-1723 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
16.6 |
Times cited |
6 |
Open Access |
OpenAccess |
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| |
Notes |
This work was supported by the National Natural Science Foundation of China (21821003, 21890380, 21905316), Guangdong Natural Science Foundation (2019A1515011748), the Science and Technology Planning Project of Guangdong Province (2019A050510018), Pearl River Recruitment Program of Talent (2019QN01C108), the EU Infrastructure Project EUSMI (Grant No. E190700310), and Sun Yat-sen University. D.W. acknowledges an Individual Fellowship funded by the Marie-Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (grant 894254 SuprAtom). S.B. and A.P.-T. acknowledge financial support from the European Commission under the Horizon 2020 Programme by grant no. 731019 (EUSMI) and ERC Consolidator grant no. 815128 (REALNANO). This project has received funding from the European Commission Grant (EUSMI E190700310). Synchrotron XAS data described in this paper was performed at the Canadian Light Source, a national research facility of the University of Saskatchewan, which is supported by the Canada Foundation for Innovation (CFI), the Natural Sciences and Engineering Research Council (NSERC), the National Research Council (NRC), the Canadian Institutes of Health Research (CIHR), the Government of Saskatchewan, and the University of Saskatchewan. |
Approved |
Most recent IF: 16.6; 2023 IF: 12.124 |
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| |
Call Number |
UA @ admin @ c:irua:196062 |
Serial |
7932 |
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| Permanent link to this record |
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Author |
Yang, T.; Kong, Y.; Li, K.; Lu, Q.; Wang, Y.; Du, Y.; Schryvers, D. |
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| |
Title |
Quasicrystalline clusters transformed from C14-MgZn₂ nanoprecipitates in Al alloys |
Type |
A1 Journal article |
| |
Year |
2023 |
Publication |
Materials characterization |
Abbreviated Journal |
|
|
| |
Volume |
199 |
Issue |
|
Pages |
112772-112777 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Ultrafine faulty C14-MgZn2 Laves phase precipitates containing quasicrystalline clusters and demonstrating the formation of binary quasicrystalline precipitates with Penrose-like random-tiling were observed in the over-aged FCC matrix of a commercial 7N01 Al-Zn-Mg alloy, using high angle annular dark field scanning transmission electron microscopy. The evolution from C14-Laves phase to quasicrystalline clusters is illustrated, and five-fold symmetry can be found in both real and reciprocal spaces. Our findings reveal the possibility of quasicrystalline formation from Laves phase in a highly plastic metal matrix like Al and demonstrate the structural relationship between Laves phase and quasicrystals. |
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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 |
000954788800001 |
Publication Date |
2023-03-02 |
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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 |
1044-5803 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.7 |
Times cited |
|
Open Access |
Not_Open_Access |
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Notes |
|
Approved |
Most recent IF: 4.7; 2023 IF: 2.714 |
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| |
Call Number |
UA @ admin @ c:irua:196106 |
Serial |
8446 |
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| Permanent link to this record |
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Author |
Alexander, C.T.; Abakumov, A.M.; Forslund, R.P.; Johnston, K.P.; Stevenson, K.J. |
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Title |
Role of the carbon support on the oxygen reduction and evolution activities in LaNiO3 composite electrodes in alkaline solution |
Type |
A1 Journal article |
| |
Year |
2018 |
Publication |
ACS applied energy materials |
Abbreviated Journal |
|
|
| |
Volume |
1 |
Issue |
4 |
Pages |
1549-1558 |
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| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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| |
Abstract |
Metal-air batteries and fuel cells show a great deal of promise in advancing low-cost, high-energy-density charge storage solutions for sustainable energy applications. To improve the activities and stabilities of electrocatalysts for the critical oxygen reduction and evolution reactions (ORR and OER, respectively), a greater understanding is needed of the catalyst/carbon interactions and carbon stability. Herein, we report how LaNiO3 (LNO) supported on nitrogen-doped carbon nanotubes (N-CNT) made from a high-yield synthesis lowers the overpotential for both the OER and ORR markedly to enable a low bifunctional window of 0.81 V at only a 51 mu g cm(-2) mass loading. Furthermore, the addition of LNO to the N-CNTs improves the galvanostatic stability for the OER by almost 2 orders of magnitude. The nanoscale geometries of the perovskites and the CNTs enhance the number of metal-support and charge transfer interactions and thus the activity. We use rotating ring disk electrodes (RRDEs) combined with Tafel slope analysis and ICP-OES to quantitatively separate current contributions from the OER, carbon oxidation, and even anodic iron leaching from carbon nanotubes. |
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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 |
000458705400020 |
Publication Date |
2018-03-28 |
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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 |
2574-0962 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
|
Times cited |
|
Open Access |
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Notes |
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Approved |
no |
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| |
Call Number |
UA @ admin @ c:irua:157642 |
Serial |
8487 |
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| Permanent link to this record |
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Author |
Marikutsa, A.; Yang, L.; Rumyantseva, M.; Batuk, M.; Hadermann, J.; Gaskov, A. |
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Title |
Sensitivity of nanocrystalline tungsten oxide to CO and ammonia gas determined by surface catalysts |
Type |
A1 Journal article |
| |
Year |
2018 |
Publication |
Sensors and actuators : B : chemical |
Abbreviated Journal |
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| |
Volume |
277 |
Issue |
|
Pages |
336-346 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Nanocrystalline tungsten oxide with variable particle size and surface area was synthesized by aqueous deposition and heat treatment for use in resistive gas sensors. Surface modification with 1 wt.% Pd and Ru was performed by impregnation to improve the sensitivity to CO and ammonia. Acid and oxidation surface sites were evaluated by temperature-programmed techniques using probe molecules. The surface acidity dropped with increasing particle size, and was weakly affected by additives. Lower crystallinity of WO3 and the presence of Ru species favoured temperature-programmed reduction of the materials. Modifying WO3 increased its sensitivity, to CO at ambient condition for modification by Pd and to NH3 at elevated temperature for Ru modification. An in situ infrared study of the gas – solid interaction showed that the catalytic additives change the interaction route of tungsten oxide with the target gases and make the reception of detected molecules independent of the semiconductor oxide matrix. |
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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 |
000453066700042 |
Publication Date |
2018-09-09 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
|
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| |
ISSN |
0925-4005 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
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Times cited |
|
Open Access |
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Notes |
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Approved |
no |
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Call Number |
UA @ admin @ c:irua:156219 |
Serial |
8513 |
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| Permanent link to this record |
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Author |
Dubrovinskaia, N.; Dubrovinsky, L.; Solopova, N.A.; Abakumov, A.; Turner, S.; Hanfland, M.; Bykova, E.; Bykov, M.; Prescher, C.; Prakapenka, V.B.; Petitgirard, S.; Chuvashova, I.; Gasharova, B.; Mathis, Y.-L.; Ershov, P.; Snigireva, I.; Snigirev, A. |
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Title |
Terapascal static pressure generation with ultrahigh yield strength nanodiamond |
Type |
A1 Journal article |
| |
Year |
2016 |
Publication |
Science Advances |
Abbreviated Journal |
|
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| |
Volume |
2 |
Issue |
7 |
Pages |
e1600341-12 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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| |
Abstract |
Studies of materials' properties at high and ultrahigh pressures lead to discoveries of unique physical and chemical phenomena and a deeper understanding of matter. In high-pressure research, an achievable static pressure limit is imposed by the strength of available strong materials and design of high-pressure devices. Using a high-pressure and high-temperature technique, we synthesized optically transparent microballs of bulk nanocrystalline diamond, which were found to have an exceptional yield strength (similar to 460 GPa at a confining pressure of similar to 70 GPa) due to the unique microstructure of bulk nanocrystalline diamond. We used the nanodiamond balls in a double-stage diamond anvil cell high-pressure device that allowed us to generate static pressures beyond 1 TPa, as demonstrated by synchrotron x-ray diffraction. Outstanding mechanical properties (strain-dependent elasticity, very high hardness, and unprecedented yield strength) make the nanodiamond balls a unique device for ultrahigh static pressure generation. Structurally isotropic, homogeneous, and made of a low-Z material, they are promising in the field of x-ray optical 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 |
000381805300029 |
Publication Date |
2016-07-21 |
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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 |
2375-2548 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
|
Times cited |
|
Open Access |
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Notes |
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Approved |
no |
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| |
Call Number |
UA @ admin @ c:irua:190527 |
Serial |
8647 |
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| Permanent link to this record |
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Author |
Abakumov, M.A.; Semkina, A.S.; Skorikov, A.S.; Vishnevskiy, D.A.; Ivanova, A.V.; Mironova, E.; Davydova, G.A.; Majouga, A.G.; Chekhonin, V.P. |
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Title |
Toxicity of iron oxide nanoparticles : size and coating effects |
Type |
A1 Journal article |
| |
Year |
2018 |
Publication |
Journal of biochemical and molecular toxicology |
Abbreviated Journal |
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| |
Volume |
32 |
Issue |
12 |
Pages |
e22225 |
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Keywords |
A1 Journal article; Pharmacology. Therapy; Electron microscopy for materials research (EMAT) |
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Abstract |
Toxicological research of novel nanomaterials is a major developmental step of their clinical approval. Since iron oxide magnetic nanoparticles have a great potential in cancer treatment and diagnostics, the investigation of their toxic properties is very topical. In this paper we synthesized bovine serum albumin-coated iron oxide nanoparticles with different sizes and their polyethylene glycol derivative. To prove high biocompatibility of obtained nanoparticles the number of in vitro toxicological tests on human fibroblasts and U251 glioblastoma cells was performed. It was shown that albumin nanoparticles' coating provides a stable and biocompatible shell and prevents cytotoxicity of magnetite core. On long exposure times (48 hours), cytotoxicity of iron oxide nanoparticles takes place due to free radical production, but this toxic effect may be neutralized by using polyethylene glycol modification. |
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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 |
000452532300008 |
Publication Date |
2018-10-06 |
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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 |
|
Edition |
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| |
ISSN |
1095-6670 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
|
Times cited |
|
Open Access |
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Notes |
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Approved |
no |
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Call Number |
UA @ admin @ c:irua:156269 |
Serial |
8684 |
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| Permanent link to this record |
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Author |
Gauquelin, N.; Forte, F.; Jannis, D.; Fittipaldi, R.; Autieri, C.; Cuono, G.; Granata, V.; Lettieri, M.; Noce, C.; Miletto-Granozio, F.; Vecchione, A.; Verbeeck, J.; Cuoco, M. |
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Title |
Pattern Formation by Electric-Field Quench in a Mott Crystal |
Type |
A1 Journal Article |
| |
Year |
2023 |
Publication |
Nano letters |
Abbreviated Journal |
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Volume |
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Issue |
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Pages |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
The control of Mott phase is intertwined with the spatial reorganization of the electronic states. Out-of-equilibrium driving forces typically lead to electronic patterns that are absent at equilibrium, whose nature is however often elusive. Here, we unveil a nanoscale pattern formation in the Ca2 RuO4 Mott insulator. We demonstrate how an applied electric field spatially reconstructs the insulating phase that, uniquely after switching off the electric field, exhibits nanoscale stripe domains. The stripe pattern has regions with inequivalent octahedral distortions that we directly observe through high-resolution scanning transmission electron
microscopy. The nanotexture depends on the orientation of the electric field, it is non-volatile and rewritable. We theoretically simulate the charge and orbital reconstruction induced by a quench dynamics of the applied electric field providing clear-cut mechanisms for the stripe phase formation. Our results open the path for the design of non-volatile electronics based on voltage-controlled nanometric phases. |
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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 |
001012061600001 |
Publication Date |
2023-05-18 |
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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 |
1530-6984 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
10.8 |
Times cited |
2 |
Open Access |
OpenAccess |
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Notes |
This project has received funding from the European Union’s Horizon 2020 research and innova- tion programme under grant agreement No 823717 – ESTEEM3. The Merlin camera used in the experiment received funding from the FWO-Hercules fund G0H4316N ’Direct electron detector 15for soft matter TEM’. C. A. and G. C. are supported by the Foundation for Polish Science through the International Research Agendas program co-financed by the European Union within the Smart Growth Operational Programme. C. A. and G. C. acknowledge the access to the computing facil- ities of the Interdisciplinary Center of Modeling at the University of Warsaw, Grant No. GB84-0, GB84-1 and GB84-7 and GB84-7 and Poznan Supercomputing and Networking Center Grant No. 609.. C. A. and G. C. acknowledge the CINECA award under the ISCRA initiative IsC85 “TOP- MOST” Grant, for the availability of high-performance computing resources and support. We acknoweldge A. Guarino and C. Elia for providing support about the electrical characterization of the sample. M.C., R.F., and A.V. acknowledge support from the EU’s Horizon 2020213 research and innovation program under Grant Agreement No. 964398 (SUPERGATE). |
Approved |
Most recent IF: 10.8; 2023 IF: 12.712 |
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Call Number |
EMAT @ emat @c:irua:196970 |
Serial |
8789 |
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| Permanent link to this record |
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Author |
Samal, D.; Gauquelin, N.; Takamura, Y.; Lobato, I.; Arenholz, E.; Van Aert, S.; Huijben, M.; Zhong, Z.; Verbeeck, J.; Van Tendeloo, G.; Koster, G. |
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Title |
Unusual structural rearrangement and superconductivity in infinite layer cuprate superlattices |
Type |
A1 Journal Article |
| |
Year |
2023 |
Publication |
Physical review materials |
Abbreviated Journal |
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| |
Volume |
7 |
Issue |
5 |
Pages |
054803 |
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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 |
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Editor |
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Language |
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Wos |
001041792100007 |
Publication Date |
2023-05-30 |
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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 |
|
Series Issue |
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Edition |
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| |
ISSN |
2475-9953 |
ISBN |
|
Additional Links |
UA library record; WoS full record |
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| |
Impact Factor |
3.4 |
Times cited |
|
Open Access |
OpenAccess |
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| |
Notes |
Air Force Office of Scientific Research; European Office of Aerospace Research and Development, FA8655-10-1-3077 ; Office of Science, DE-AC02-05CH11231 ; National Science Foundation, DMR-1745450 ; Seventh Framework Programme, 278510 ; Bijzonder Onderzoeksfonds UGent; |
Approved |
Most recent IF: 3.4; 2023 IF: NA |
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Call Number |
EMAT @ emat @c:irua:196973 |
Serial |
8790 |
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| Permanent link to this record |
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Author |
Mary Joy, R.; Pobedinskas, P.; Bourgeois, E.; Chakraborty, T.; Görlitz, J.; Herrmann, D.; Noël, C.; Heupel, J.; Jannis, D.; Gauquelin, N.; D'Haen, J.; Verbeeck, J.; Popov, C.; Houssiau, L.; Becher, C.; Nesládek, M.; Haenen, K. |
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Title |
Germanium vacancy centre formation in CVD nanocrystalline diamond using a solid dopant source |
Type |
A1 Journal Article |
| |
Year |
2023 |
Publication |
Science talks |
Abbreviated Journal |
Science Talks |
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| |
Volume |
5 |
Issue |
|
Pages |
100157 |
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Keywords |
A3 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
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Address |
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Wos |
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Publication Date |
2023-02-09 |
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ISSN |
2772-5693 |
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 |
OpenAccess |
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Approved |
Most recent IF: NA |
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Call Number |
EMAT @ emat @c:irua:196969 |
Serial |
8791 |
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Author |
Kavak, S.; Kadu, A.A.; Claes, N.; Sánchez-Iglesias, A.; Liz-Marzán, L.M.; Batenburg, K.J.; Bals, S. |
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Title |
Quantitative 3D Investigation of Nanoparticle Assemblies by Volumetric Segmentation of Electron Tomography Data Sets |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
The journal of physical chemistry: C : nanomaterials and interfaces |
Abbreviated Journal |
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Volume |
127 |
Issue |
20 |
Pages |
9725-9734 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Morphological characterization of nanoparticle assemblies and hybrid nanomaterials is critical in determining their structure-property relationships as well as in the development of structures with desired properties. Electron tomography has become a widely utilized technique for the three-dimensional characterization of nanoparticle assemblies. However, the extraction of quantitative morphological parameters from the reconstructed volume can be a complex and labor-intensive task. In this study, we aim to overcome this challenge by automating the volumetric segmentation process applied to three-dimensional reconstructions of nanoparticle assemblies. The key to enabling automated characterization is to assess the performance of different volumetric segmentation methods in accurately extracting predefined quantitative descriptors for morphological characterization. In our methodology, we compare the quantitative descriptors obtained through manual segmentation with those obtained through automated segmentation methods, to evaluate their accuracy and effectiveness. To show generality, our study focuses on the characterization of assemblies of CdSe/CdS quantum dots, gold nanospheres and CdSe/CdS encapsulated in polymeric micelles, and silica-coated gold nanorods decorated with both CdSe/CdS or PbS quantum dots. We use two unsupervised segmentation algorithms: the watershed transform and the spherical Hough transform. Our results demonstrate that the choice of automated segmentation method is crucial for accurately extracting the predefined quantitative descriptors. Specifically, the spherical Hough transform exhibits superior performance in accurately extracting quantitative descriptors, such as particle size and interparticle distance, thereby allowing for an objective, efficient, and reliable volumetric segmentation of complex nanoparticle assemblies. |
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Wos |
000991752700001 |
Publication Date |
2023-05-25 |
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Edition |
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ISSN |
1932-7447 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.7 |
Times cited |
2 |
Open Access |
OpenAccess |
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Notes |
Fonds Wetenschappelijk Onderzoek, 1181122N ; Horizon 2020 Framework Programme, 861950 ; H2020 European Research Council, 815128 ; |
Approved |
Most recent IF: 3.7; 2023 IF: 4.536 |
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Call Number |
EMAT @ emat @c:irua:196971 |
Serial |
8793 |
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Author |
Vlasov, E.; Skorikov, A.; Sánchez-Iglesias, A.; Liz-Marzán, L.M.; Verbeeck, J.; Bals, S. |
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Title |
Secondary electron induced current in scanning transmission electron microscopy: an alternative way to visualize the morphology of nanoparticles |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
ACS materials letters |
Abbreviated Journal |
ACS Materials Lett. |
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Volume |
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Issue |
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Pages |
1916-1921 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Electron tomography (ET) is a powerful tool to determine the three-dimensional (3D) structure of nanomaterials in a transmission electron microscope. However, the acquisition of a conventional tilt series for ET is a time-consuming process and can therefore not provide 3D structural information in a time-efficient manner. Here, we propose surface-sensitive secondary electron (SE) imaging as an alternative to ET for the investigation of the morphology of nanomaterials. We use the SE electron beam induced current (SEEBIC) technique that maps the electrical current arising from holes generated by the emission of SEs from the sample. SEEBIC imaging can provide valuable information on the sample morphology with high spatial resolution and significantly shorter throughput times compared with ET. In addition, we discuss the contrast formation mechanisms that aid in the interpretation of SEEBIC data. |
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Wos |
001006191600001 |
Publication Date |
2023-06-12 |
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Edition |
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ISSN |
2639-4979 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
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Times cited |
1 |
Open Access |
OpenAccess |
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Notes |
The funding for this project was provided by European Research Council (ERC Consolidator Grant 815128, REALNANO). J.V. acknowledges the eBEAM project, which is supported by the European Union’s Horizon 2020 research and innovation program under grant agreement no. 101017720 (FET-Proactive EBEAM). L.M.L.-M. acknowledges funding from MCIN/AEI/10.13039/501100011033 (grant # PID2020-117779RB-I00). |
Approved |
Most recent IF: NA |
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Call Number |
EMAT @ emat @c:irua:197004 |
Serial |
8795 |
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Author |
Saniz, R.; Baldinozzi, G.; Arts, I.; Lamoen, D.; Leinders, G.; Verwerft, M. |
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Title |
Charge order, frustration relief, and spin-orbit coupling in U3O8 |
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A1 Journal Article |
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Year |
2023 |
Publication |
Physical review materials |
Abbreviated Journal |
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Volume |
7 |
Issue |
5 |
Pages |
054410 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Research efforts on the description of the low-temperature magnetic order and electronic properties of U3O8 have been inconclusive so far. Reinterpreting neutron scattering results, we use group representation theory to show that the ground state presents collinear out-of-plane magnetic moments, with antiferromagnetic coupling both in-layer and between layers. Charge order relieves the initial geometric frustration, generating a slightly distorted honeycomb sublattice with Néel-type order. The precise knowledge of the characteristics of this magnetic ground state is then used to explain the fine features of the band gap. In this system, spin-orbit coupling (SOC) is of critical importance, as it strongly affects the electronic structure, narrowing the gap by ∼38%, compared to calculations neglecting SOC. The predicted electronic structure actually explains the salient features of recent optical absorption measurements, further demonstrating the excellent agreement between the calculated ground state properties and experiment. |
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Wos |
001041429800007 |
Publication Date |
2023-05-31 |
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ISSN |
2475-9953 |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
3.4 |
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).Fonds Wetenschappelijk Onderzoek; Vlaams Supercomputer Centrum; Universiteit Antwerpen; Vlaamse regering; |
Approved |
Most recent IF: 3.4; 2023 IF: NA |
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Call Number |
EMAT @ emat @c:irua:197043 |
Serial |
8796 |
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