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Author |
Yusupov, M.; Razzokov, J.; Cordeiro, R.M.; Bogaerts, A. |
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Title |
Transport of Reactive Oxygen and Nitrogen Species across Aquaporin: A Molecular Level Picture |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
Oxidative medicine and cellular longevity |
Abbreviated Journal |
Oxid Med Cell Longev |
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Volume |
2019 |
Issue |
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Pages |
1-11 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
Aquaporins (AQPs) are transmembrane proteins that conduct not only water molecules across the cell membrane but also other solutes, such as reactive oxygen and nitrogen species (RONS), produced (among others) by cold atmospheric plasma (CAP). These RONS may induce oxidative stress in the cell interior, which plays a role in cancer treatment. The underlying mechanisms of the transport of RONS across AQPs, however, still remain obscure. We apply molecular dynamics simulations to investigate the permeation of both hydrophilic (H<sub>2</sub>O<sub>2</sub>and OH) and hydrophobic (NO<sub>2</sub>and NO) RONS through AQP1. Our simulations show that these RONS can all penetrate across the pores of AQP1. The permeation free energy barrier of OH and NO is lower than that of H<sub>2</sub>O<sub>2</sub>and NO<sub>2</sub>, indicating that these radicals may have easier access to the pore interior and interact with the amino acid residues of AQP1. We also study the effect of RONS-induced oxidation of both the phospholipids and AQP1 (i.e., sulfenylation of Cys<sub>191</sub>) on the transport of the above-mentioned RONS across AQP1. Both lipid and protein oxidation seem to slightly increase the free energy barrier for H<sub>2</sub>O<sub>2</sub>and NO<sub>2</sub>permeation, while for OH and NO, we do not observe a strong effect of oxidation. The simulation results help to gain insight in the underlying mechanisms of the noticeable rise of CAP-induced RONS in cancer cells, thereby improving our understanding on the role of AQPs in the selective anticancer capacity of CAP. |
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Wos |
000492999000001 |
Publication Date |
2019-06-17 |
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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 |
1942-0900 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.593 |
Times cited |
5 |
Open Access |
OpenAccess |
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Notes |
The authors acknowledge the Turing HPC infrastructure at the CalcUA core facility of the University of Antwerp (UA), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI), and the UA, where all computational work was performed. M.Y. gratefully acknowledges Dr. U. Khalilov for the fruitful discussions. This work was financially supported by the Research Foundation Flanders (FWO) (grant number 1200219N). |
Approved |
Most recent IF: 4.593 |
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Call Number |
PLASMANT @ plasmant @UA @ admin @ c:irua:160118 |
Serial |
5180 |
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Permanent link to this record |
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Author |
Razzokov, J.; Yusupov, M.; Bogaerts, A. |
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Title |
Oxidation destabilizes toxic amyloid beta peptide aggregation |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
Scientific reports |
Abbreviated Journal |
Sci Rep-Uk |
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Volume |
9 |
Issue |
1 |
Pages |
5476 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
The aggregation of insoluble amyloid beta (Aβ) peptides in the brain is known to trigger the onset of neurodegenerative diseases, such as Alzheimer’s disease. In spite of the massive number of investigations, the underlying mechanisms to destabilize the Aβ aggregates are still poorly understood. Some studies indicate the importance of oxidation to destabilize the Aβ aggregates. In particular, oxidation induced by cold atmospheric plasma (CAP) has demonstrated promising results in eliminating these toxic aggregates. In this paper, we investigate the effect of oxidation on the stability of an Aβ pentamer. By means of molecular dynamics simulations and umbrella sampling, we elucidate the conformational changes of Aβ pentamer in the presence of oxidized residues, and we estimate the dissociation free energy of the terminal peptide out of the pentamer form. The calculated dissociation free energy of the terminal peptide is also found to decrease with increasing oxidation. This indicates that Aβ pentamer aggregation becomes less favorable upon oxidation. Our study contributes to a better insight in one of the potential mechanisms for inhibition of toxic Aβ peptide aggregation, which is considered to be the main culprit to Alzheimer’s disease. |
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Wos |
000462990000018 |
Publication Date |
2019-04-02 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2045-2322 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.259 |
Times cited |
5 |
Open Access |
OpenAccess |
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Notes |
M.Y. gratefully acknowledges financial support from the Research Foundation – Flanders (FWO), grant 1200216N and 1200219N. The computational work was carried out using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen (UA), a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the UA. |
Approved |
Most recent IF: 4.259 |
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Call Number |
PLASMANT @ plasmant @UA @ admin @ c:irua:159367 |
Serial |
5182 |
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Permanent link to this record |
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Author |
Ghasemitarei, M.; Yusupov, M.; Razzokov, J.; Shokri, B.; Bogaerts, A. |
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Title |
Transport of cystine across xC-antiporter |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
Archives of biochemistry and biophysics |
Abbreviated Journal |
Arch Biochem Biophys |
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Volume |
664 |
Issue |
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Pages |
117-126 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
Extracellular cystine (CYC) uptake by xC antiporter is important for the cell viability. Especially in cancer cells, the upregulation of xC activity is observed, which protects these cells from intracellular oxidative stress. Hence, inhibition of the CYC uptake may eventually lead to cancer cell death. Up to now, the molecular level mechanism of the CYC uptake by xC antiporter has not been studied in detail. In this study, we applied several different simulation techniques to investigate the transport of CYC through xCT, the light subunit of the xC antiporter, which is responsible for the CYC and glutamate translocation. Specifically, we studied the permeation of CYC across three model systems, i.e., outward facing (OF), occluded (OCC) and inward facing (IF) configurations of xCT. We also investigated the effect of mutation of Cys327 to Ala within xCT, which was also studied experimentally in literature. This allowed us to qualitatively compare our computation results with experimental observations, and thus, to validate our simulations. In summary, our simulations provide a molecular level mechanism of the transport of CYC across the xC antiporter, more specifically, which amino acid residues in the xC antiporter play a key role in the uptake, transport and release of CYC. |
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Wos |
000461411200014 |
Publication Date |
2019-02-07 |
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Series Editor |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0003-9861 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.165 |
Times cited |
3 |
Open Access |
OpenAccess |
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Notes |
Research Foundation − FlandersResearch Foundation − Flanders (FWO), 1200216N 1200219N ; Hercules FoundationHercules Foundation; Flemish GovernmentFlemish Government (department EWI); UAUA; M. Y. gratefully acknowledges financial support from the Research Foundation − Flanders (FWO), grant numbers 1200216N and 1200219N. The computational work was carried out using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen, a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the UA. Finally, we thank A. S. Mashayekh Esfehan and A. Mohseni for their important comments on the manuscript. |
Approved |
Most recent IF: 3.165 |
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Call Number |
PLASMANT @ plasmant @UA @ admin @ c:irua:158571 |
Serial |
5183 |
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Permanent link to this record |
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Author |
Asapu, R.; Claes, N.; Ciocarlan, R.-G.; Minjauw, M.; Detavernier, C.; Cool, P.; Bals, S.; Verbruggen, S.W. |
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Title |
Electron Transfer and Near-Field Mechanisms in Plasmonic Gold-Nanoparticle-Modified TiO2Photocatalytic Systems |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
ACS applied nano materials |
Abbreviated Journal |
ACS Appl. Nano Mater. |
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Volume |
2 |
Issue |
2 |
Pages |
4067-4074 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Sustainable Energy, Air and Water Technology (DuEL) |
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Abstract |
The major mechanism responsible for plasmonic enhancement of titanium dioxide photocatalysis using gold nanoparticles is still under contention. This work introduces an experimental strategy to disentangle the significance of the charge transfer and near-field mechanisms in plasmonic photocatalysis. By controlling the thickness and conductive nature of a nanoparticle shell that acts as a spacer layer separating the plasmonic metal core from the TiO2 surface, field enhancement or charge transfer effects can be selectively repressed or evoked. Layer-by-layer and in situ polymerization methods are used to synthesize gold core–polymer shell nanoparticles with shell thickness control up to the sub-nanometer level. Detailed optical and electrical characterization supported by near-field simulation models corroborate the trends in photocatalytic activity of the different systems. This approach mainly points at an important contribution of the enhanced near field. |
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Wos |
000477917700006 |
Publication Date |
2019-05-31 |
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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 |
2574-0970 |
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 |
32 |
Open Access |
OpenAccess |
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Notes |
This work was supported by Research Foundation Flanders (FWO). P.C. and R-G.C. acknowledge financial support from FWO (Project No. G038215N). N.C. and S.B. acknowledge financial support from the European Research Council (ERC Starting Grant No. 335078-COLOURATOM). |
Approved |
Most recent IF: NA |
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Call Number |
EMAT @ emat @UA @ admin @ c:irua:160579 |
Serial |
5184 |
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Permanent link to this record |
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Author |
Snoeckx, R.; Van Wesenbeeck, K.; Lenaerts, S.; Cha, M.S.; Bogaerts, A. |
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Title |
Suppressing the formation of NOxand N2O in CO2/N2dielectric barrier discharge plasma by adding CH4: scavenger chemistry at work |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
Sustainable Energy & Fuels |
Abbreviated Journal |
Sustainable Energy Fuels |
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Volume |
3 |
Issue |
6 |
Pages |
1388-1395 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Sustainable Energy, Air and Water Technology (DuEL) |
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Abstract |
The need for carbon negative technologies led to the development of a wide array of novel CO<sub>2</sub>conversion techniques. Most of them either rely on high temperatures or generate highly reactive O species, which can lead to the undesirable formation of NO<sub>x</sub>and N<sub>2</sub>O when the CO<sub>2</sub>feeds contain N<sub>2</sub>. Here, we show that, for plasma-based CO<sub>2</sub>conversion, adding a hydrogen source, as a chemical oxygen scavenger, can suppress their formation,<italic>in situ</italic>. This allows the use of low-cost N<sub>2</sub>containing (industrial and direct air capture) feeds, rather than expensive purified CO<sub>2</sub>. To demonstrate this, we add CH<sub>4</sub>to a dielectric barrier discharge plasma used for converting impure CO<sub>2</sub>. We find that when adding a stoichiometric amount of CH<sub>4</sub>, 82% less NO<sub>2</sub>and 51% less NO are formed. An even higher reduction (96 and 63%) can be obtained when doubling this amount. However, in that case the excess radicals promote the formation of by-products, such as HCN, NH<sub>3</sub>and CH<sub>3</sub>OH. Thus, we believe that by using an appropriate amount of chemical scavengers, we can use impure CO<sub>2</sub>feeds, which would bring us closer to ‘real world’ conditions and implementation. |
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Wos |
000469258600021 |
Publication Date |
2019-02-20 |
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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 |
2398-4902 |
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 |
OpenAccess |
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Notes |
Fonds Wetenschappelijk Onderzoek, G0F9618N ; Universiteit Antwerpen; King Abdullah University of Science and Technology, BAS/1/1384-01-01 ;The research reported in this publication was supported by funding from the “Excellence of Science Program” (Fund for Scientic Research Flanders (FWO): grant no. G0F9618N; EOS ID: 30505023). The authors R. S. and M. S. C. acknowledge nancial support from King Abdullah University of Science and Technology (KAUST), under award number BAS/1/1384-01-01. |
Approved |
Most recent IF: NA |
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Call Number |
PLASMANT @ plasmant @UA @ admin @ c:irua:160268 |
Serial |
5188 |
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Permanent link to this record |
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Author |
Marikutsa, A.; Rumyantseva, M.; Gaskov, A.; Batuk, M.; Hadermann, J.; Sarmadian, N.; Saniz, R.; Partoens, B.; Lamoen, D. |
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Title |
Effect of zinc oxide modification by indium oxide on microstructure, adsorbed surface species, and sensitivity to CO |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
Frontiers in materials |
Abbreviated Journal |
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Volume |
6 |
Issue |
6 |
Pages |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT) |
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Abstract |
Additives in semiconductor metal oxides are commonly used to improve sensing behavior of gas sensors. Due to complicated effects of additives on the materials microstructure, adsorption sites and reactivity to target gases the sensing mechanism with modified metal oxides is a matter of thorough research. Herein, we establish the promoting effect of nanocrystalline zinc oxide modification by 1-7 at.% of indium on the sensitivity to CO gas due to improved nanostructure dispersion and concentration of active sites. The sensing materials were synthesized via an aqueous coprecipitation route. Materials composition, particle size and BET area were evaluated using X-ray diffraction, nitrogen adsorption isotherms, high-resolution electron microscopy techniques and EDX-mapping. Surface species of chemisorbed oxygen, OH-groups, and acid sites were characterized by probe molecule techniques and infrared spectroscopy. It was found that particle size of zinc oxide decreased and the BET area increased with the amount of indium oxide. The additive was observed as amorphous indium oxide segregated on agglomerated ZnO nanocrystals. The measured concentration of surface species was higher on In2O3-modified zinc oxide. With the increase of indium oxide content, the sensor response of ZnO/In2O3 to CO was improved. Using in situ infrared spectroscopy, it was shown that oxidation of CO molecules was enhanced on the modified zinc oxide surface. The effect of modifier was attributed to promotion of surface OH-groups and enhancement of CO oxidation on the segregated indium ions, as suggested by DFT in previous work. |
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Wos |
000461540600001 |
Publication Date |
2019-03-15 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2296-8016 |
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 |
11 |
Open Access |
OpenAccess |
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Notes |
; Research was supported by the grant from Russian Science Foundation (project No. 18-73-00071). ; |
Approved |
Most recent IF: NA |
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Call Number |
UA @ admin @ c:irua:158540 |
Serial |
5205 |
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Permanent link to this record |
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Author |
Kim, Y.; Che, F.; Jo, J.W.; Choi, J.; de Arquer, F.P.G.; Voznyy, O.; Sun, B.; Kim, J.; Choi, M.-J.; Quintero-Bermudez, R.; Fan, F.; Tan, C.S.; Bladt, E.; Walters, G.; Proppe, A.H.; Zou, C.; Yuan, H.; Bals, S.; Hofkens, J.; Roeffaers, M.B.J.; Hoogland, S.; Sargent, E.H. |
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Title |
A Facet-Specific Quantum Dot Passivation Strategy for Colloid Management and Efficient Infrared Photovoltaics |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
Advanced materials |
Abbreviated Journal |
Adv Mater |
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Volume |
31 |
Issue |
31 |
Pages |
1805580 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Colloidal nanocrystals combine size- and facet-dependent properties with solution processing. They offer thus a compelling suite of materials for technological applications. Their size- and facet-tunable features are studied in synthesis; however, to exploit their features in optoelectronic devices, it will be essential to translate control over size and facets from the colloid all the way to the film. Larger-diameter colloidal quantum dots (CQDs) offer the attractive possibility of harvesting infrared (IR) solar energy beyond absorption of silicon photovoltaics. These CQDs exhibit facets (nonpolar (100)) undisplayed in small-diameter CQDs; and the materials chemistry of smaller nanocrystals fails consequently to translate to materials for the short-wavelength IR regime. A new colloidal management strategy targeting the passivation of both (100) and (111) facets is demonstrated using distinct choices of cations and anions. The approach leads to narrow-bandgap CQDs with impressive colloidal stability and photoluminescence quantum yield. Photophysical studies confirm a reduction both in Stokes shift (approximate to 47 meV) and Urbach tail (approximate to 29 meV). This approach provides a approximate to 50% increase in the power conversion efficiency of IR photovoltaics compared to controls, and a approximate to 70% external quantum efficiency at their excitonic peak. |
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Wos |
000465600000001 |
Publication Date |
2019-03-12 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0935-9648 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
19.791 |
Times cited |
74 |
Open Access |
OpenAccess |
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Notes |
; Y.K., F.C., J.W.J., and J.C. contributed equally. This work was supported by King Abdullah University of Science and Technology (KAUST, Office of Sponsored Research (OSR), Award No. OSR-2017-CPF-3325) and Ontario Research Fund-Research Excellence program (ORF7-Ministry of Research and Innovation, Ontario Research Fund-Research Excellence Round 7). E.B. gratefully acknowledges financial support by the Research Foundation-Flanders (FWO Vlaanderen). Y.K. received financial support from the DGIST R&D Programs of the Ministry of Science, ICT & Future Planning of Korea (18-ET-01). M.B.J.R. and J.H. acknowledge financial support from the Research Foundation-Flanders (FWO, grants nr ZW15_09-GOH6316 and G.098319N) and the Flemish government through long-term structural funding Methusalem (CASAS2, Meth/15/04). H.Y. acknowledges the Research Foundation-Flanders (FWO) for a postdoctoral fellowship. The authors thank L. Levina, R. Wolowiec, D. Kopilovic, and E. Palmiano for their technical help over the course of this research. ; |
Approved |
Most recent IF: 19.791 |
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Call Number |
UA @ admin @ c:irua:160392 |
Serial |
5239 |
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Permanent link to this record |
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Author |
Becker, M.; Guzzinati, G.; Béché, A.; Verbeeck, J.; Batelaan, H. |
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Title |
Asymmetry and non-dispersivity in the Aharonov-Bohm effect |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
Nature communications |
Abbreviated Journal |
Nat Commun |
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Volume |
10 |
Issue |
10 |
Pages |
1700 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Decades ago, Aharonov and Bohm showed that electrons are affected by electromagnetic potentials in the absence of forces due to fields. Zeilinger's theorem describes this absence of classical force in quantum terms as the “dispersionless” nature of the Aharonov-Bohm effect. Shelankov predicted the presence of a quantum “force” for the same Aharonov-Bohm physical system as elucidated by Berry. Here, we report an experiment designed to test Shelankov's prediction and we provide a theoretical analysis that is intended to elucidate the relation between Shelankov's prediction and Zeilinger's theorem. The experiment consists of the Aharonov-Bohm physical system; free electrons pass a magnetized nanorod and far-field electron diffraction is observed. The diffraction pattern is asymmetric confirming one of Shelankov's predictions and giving indirect experimental evidence for the presence of a quantum “force”. Our theoretical analysis shows that Zeilinger's theorem and Shelankov's result are both special cases of one theorem. |
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Wos |
000464338100011 |
Publication Date |
2019-04-12 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2041-1723 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
12.124 |
Times cited |
12 |
Open Access |
OpenAccess |
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Notes |
; H.B. would like to thank Michael Berry for bringing the presence of a quantum “force” to our attention. A.B., G.G. and J.V. acknowledge support from the European Research Council under the 7th Framework Program (FP7) ERC Starting Grant 278510 VORTEX. G.G. acknowledges support from the Fonds Wetenschappelijk Onderzoek -Vlaanderen (FWO). M.B. and H.B. acknowledge support by the U.S. National Science Foundation under Grant No. 1602755. ; |
Approved |
Most recent IF: 12.124 |
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Call Number |
UA @ admin @ c:irua:159341 |
Serial |
5241 |
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Permanent link to this record |
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Author |
Mefford, J.T.; Kurilovich, A.A.; Saunders, J.; Hardin, W.G.; Abakumov, A.M.; Forslund, R.P.; Bonnefont, A.; Dai, S.; Johnston, K.P.; Stevenson, K.J. |
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Title |
Decoupling the roles of carbon and metal oxides on the electrocatalytic reduction of oxygen on La1-xSrxCoO3-\delta perovskite composite electrodes |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
Physical chemistry, chemical physics |
Abbreviated Journal |
Phys Chem Chem Phys |
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Volume |
21 |
Issue |
6 |
Pages |
3327-3338 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Perovskite oxides are active room-temperature bifunctional oxygen electrocatalysts in alkaline media, capable of performing the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) with lower combined overpotentials relative to their precious metal counterparts. However, their semiconducting nature necessitates the use of activated carbons as conductive supports to generate applicably relevant current densities. In efforts to advance the performance and theory of oxide electrocatalysts, the chemical and physical properties of the oxide material often take precedence over contributions from the conductive additive. In this work, we find that carbon plays an important synergistic role in improving the performance of La1-xSrxCoO3- (0 x 1) electrocatalysts through the activation of O-2 and spillover of radical oxygen intermediates, HO2- and O-2(-), which is further reduced through chemical decomposition of HO2- on the perovskite surface. Through a combination of thin-film rotating disk electrochemical characterization of the hydrogen peroxide intermediate reactions (hydrogen peroxide reduction reaction (HPRR), hydrogen peroxide oxidation reaction (HPOR)) and oxygen reduction reaction (ORR), surface chemical analysis, HR-TEM, and microkinetic modeling on La1-xSrxCoO3- (0 x 1)/carbon (with nitrogen and non-nitrogen doped carbons) composite electrocatalysts, we deconvolute the mechanistic aspects and contributions to reactivity of the oxide and carbon support. |
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Corporate Author |
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Place of Publication |
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Editor |
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Language |
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Wos |
000459584900049 |
Publication Date |
2019-01-18 |
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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 |
1463-9076; 1463-9084 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.123 |
Times cited |
5 |
Open Access |
OpenAccess |
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Notes |
; Financial support for this work was provided by the R. A. Welch Foundation (grants F-1529 and F-1319). S. D. was supported as part of the Fluid Interface Reactions, Structures and Transport (FIRST) Center, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences. ; |
Approved |
Most recent IF: 4.123 |
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Call Number |
UA @ admin @ c:irua:158625 |
Serial |
5244 |
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Permanent link to this record |
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Author |
Gonzalez-Rubio, G.; Kumar, V.; Llombart, P.; Diaz-Nunez, P.; Bladt, E.; Altantzis, T.; Bals, S.; Pena-Rodriguez, O.; Noya, E.G.; MacDowell, L.G.; Guerrero-Martinez, A.; Liz-Marzan, L.M. |
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Title |
Disconnecting Symmetry Breaking from Seeded Growth for the Reproducible Synthesis of High Quality Gold Nanorods |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
13 |
Issue |
13 |
Pages |
4424-4435 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
One of the major difficulties hindering the widespread application of colloidal anisotropic plasmonic nanoparticles is the limited robustness and reproducibility of multistep synthetic methods. We demonstrate herein that the reproducibility and reliability of colloidal gold nanorod (AuNR) synthesis can be greatly improved by disconnecting the symmetry-breaking event from the seeded growth process. We have used a modified silver-assisted seeded growth method in the presence of the surfactant hexadecyltrimethylammonium bromide and n-decanol as a co-surfactant to prepare small AuNRs in high yield, which were then used as seeds for the growth of high quality AuNR colloids. Whereas the use of n-decanol provides a more-rigid micellar system, the growth on anisotropic seeds avoids sources of irreproducibility during the symmetry breaking step, yielding uniform AuNR colloids with narrow plasmon bands, ranging from 600 to 1270 nm, and allowing the fine-tuning of the final dimensions. This method provides a robust route for the preparation of high quality AuNR colloids with tunable morphology, size, and optical response in a reproducible and scalable manner. |
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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 |
000466052900067 |
Publication Date |
2019-04-02 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
100 |
Open Access |
OpenAccess |
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Notes |
; This work has been funded by the Spanish MINECO (grant nos. FIS2017-89361-C3-2-P and MAT2017-86659-R), the Madrid Regional Government (grant no. P2018/NMT-4389) and the Complutense University of Madrid (grant no. PR75/18-21616). Funding is acknowledged from the European Commission (grant no. EUSMI 731019). G.G.-R. acknowledges receipt of FPI Fellowship from the Spanish MINECO. E.B. and T.A. acknowledge postdoctoral grants from the Research Foundation Flanders (FWO). The authors are indebted to Profs. Justin Gooding, Watson Loh, Nicholas Kotov, Deqing Zhang, Mihaela Delcea, Maurizio Prato, and Krishna Ganesh, for providing milli-Q water samples. ; |
Approved |
Most recent IF: 13.942 |
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Call Number |
UA @ admin @ c:irua:160417 |
Serial |
5246 |
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Permanent link to this record |
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Author |
Cassidy, S.J.; Pitcher, M.J.; Lim, J.J.K.; Hadermann, J.; Allen, J.P.; Watson, G.W.; Britto, S.; Chong, E.J.; Free, D.G.; Grey, C.P.; Clarke, S.J. |
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Title |
Layered CeSO and LiCeSO oxide chalcogenides obtained via topotactic oxidative and reductive transformations |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
Inorganic chemistry |
Abbreviated Journal |
Inorg Chem |
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Volume |
58 |
Issue |
6 |
Pages |
3838-3850 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
The chemical accessibility of the Celv oxidation state enables redox chemistry to be performed on the naturally coinagemetal -deficient phases CeM1-xSO (M = Cu, Ag). A metastable black compound with the PbFC1 structure type (space group P4/nmm: a = 3.8396(1) angstrom, c = 6.607(4) angstrom, V = 97.40(6) angstrom(3)) and a composition approaching CeSO is obtained by deintercalation of Ag from CeAg0.8SO. High-resolution transmission electron microscopy reveals the presence of large defect-free regions in CeSO, but stacking faults are also evident which can be incorporated into a quantitative model to account for the severe peak anisotropy evident in all the highresolution X-ray and neutron diffractograms of bulk CeSO samples; these suggest that a few percent of residual Ag remains. A strawcolored compound with the filled PbFCI (i.e., ZrSiCuAs- or HfCuSi2type) structure (space group P4/nmm: a = 3.98171(1) angstrom, c = 8.70913(5) angstrom, V = 138.075(1) angstrom 3) and a composition close to LiCeSO, but with small amounts of residual Ag, is obtained by direct reductive lithiation of CeAga8S0 or by insertion of Li into CeSO using chemical or electrochemical means. Computation of the band structure of pure, stoichiometric CeSO predicts it to be a Ce' compound with the 4f-states lying approximately 1 eV above the sulfide-dominated valence band maximum. Accordingly, the effective magnetic moment per Ce ion measured in the CeSO samples is much reduced from the value found for the Ce3+-containing LiCeSO, and the residual paramagnetism corresponds to the Ce3+ ions remaining due to the presence of residual Ag, which presumably reflects the difficulty of stabilizing Ce' in the presence of sulfide (S2-). Comparison of the behavior of CeCu0.8SO with that of CeCu0.8SO reveals much slower reaction kinetics associated with the Cu,_xS layers, and this enables intermediate CeCui LixSO phases to be isolated. |
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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 |
000461978700036 |
Publication Date |
2019-02-25 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0020-1669 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.857 |
Times cited |
|
Open Access |
OpenAccess |
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Notes |
; We thank the UK EPSRC (EP/M020517/1 and EP/P018874/1), the Leverhulme Trust (RPG-2014-221), and Science Foundation Ireland (Grant 12/IA/1414) for funding and the EPSRC for additional studentship support. We acknowledge the ISIS pulsed neutron and muon source and the Diamond Light Source Ltd. (EE13284 and EE18786) and the ESRF for the award of beam time. We thank Dr. R I. Smith for assistance on the neutron beamlines, Dr. A. Baker and Dr. C. Murray for support on III, and Dr. C. Curls for support on ID31. ; |
Approved |
Most recent IF: 4.857 |
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Call Number |
UA @ admin @ c:irua:159426 |
Serial |
5253 |
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Permanent link to this record |
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Author |
Das, S.; Rata, A.D.; Maznichenko, I., V; Agrestini, I.S.; Pippel, E.; Gauquelin, N.; Verbeeck, J.; Chen, K.; Valvidares, S.M.; Vasili, H.B.; Herrero-Martin, J.; Pellegrin, E.; Nenkov, K.; Herklotz, A.; Ernst, A.; Mertig, I.; Hu, Z.; Doerr, K. |
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Title |
Low-field switching of noncollinear spin texture at La0.7Sr0.3MnO3-SrRuO3interfaces |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
Physical review B |
Abbreviated Journal |
Phys Rev B |
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Volume |
99 |
Issue |
2 |
Pages |
024416 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Interfaces of ferroic oxides can show complex magnetic textures which have strong impact on spintronics devices. This has been demonstrated recently for interfaces with insulating antiferromagnets such as BiFeO3. Here, noncollinear spin textures which can be switched in very low magnetic field are reported for conducting ferromagnetic bilayers of La0.7Sr0.3MnO3-SrRuO3 (LSMO-SRO). The magnetic order and switching are fundamentally different for bilayers coherently grown in reversed stacking sequence. The SRO top layer forms a persistent exchange spring which is antiferromagnetically coupled to LSMO and drives switching in low fields of a few milliteslas. Density functional theory reveals the crucial impact of the interface termination on the strength of Mn-Ru exchange coupling across the interface. The observation of an exchange spring agrees with ultrastrong coupling for the MnO2/SrO termination. Our results demonstrate low-field switching of noncollinear spin textures at an interface between conducting oxides, opening a pathway for manipulating and utilizing electron transport phenomena in controlled spin textures at oxide interfaces. |
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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 |
000455821400005 |
Publication Date |
2019-01-15 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
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 |
3.836 |
Times cited |
19 |
Open Access |
OpenAccess |
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Notes |
; The research in Halle was supported by Deutsche Forschungsgemeinschaft (DFG), SFB 762 Functional Oxide Interfaces (Projects No. A9 and No. B1). K.C. benefited from support of the DFG (Project 600575). Discussions with M. Trassin, M. Ziese, H. M. Christen, E.-J. Guo, F. Grcondciel, M. Bibes, and H. N. Lee are gratefully acknowledged. N. G. and J. V. acknowledge funding under the GOA project “Solarpaint” of the University of Antwerp. The Qu-Ant-EM microscope was partly funded by the Hercules fund from the Flemish Government. ; |
Approved |
Most recent IF: 3.836 |
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Call Number |
UA @ admin @ c:irua:156717 |
Serial |
5255 |
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Permanent link to this record |
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Author |
Van Velthoven, N.; Waitschat, S.; Chavan, S.M.; Liu, P.; Smolders, S.; Vercammen, J.; Bueken, B.; Bals, S.; Lillerud, K.P.; Stock, N.; De Vos, D.E. |
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Title |
Single-site metal-organic framework catalysts for the oxidative coupling of arenes via C-H/C-H activation |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
Chemical science |
Abbreviated Journal |
Chem Sci |
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Volume |
10 |
Issue |
10 |
Pages |
3616-3622 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
C-H activation reactions are generally associated with relatively low turnover numbers (TONs) and high catalyst concentrations due to a combination of low catalyst stability and activity, highlighting the need for recyclable heterogeneous catalysts with stable single-atom active sites. In this work, several palladium loaded metal-organic frameworks (MOFs) were tested as single-site catalysts for the oxidative coupling of arenes (e.g. o-xylene) via C-H/C-H activation. Isolation of the palladium active sites on the MOF supports reduced Pd(0) aggregate formation and thus catalyst deactivation, resulting in higher turnover numbers (TONs) compared to the homogeneous benchmark reaction. Notably, a threefold higher TON could be achieved for palladium loaded MOF-808 due to increased catalyst stability and the heterogeneous catalyst could efficiently be reused, resulting in a cumulative TON of 1218 after three runs. Additionally, the palladium single-atom active sites on MOF-808 were successfully identified by Fourier transform infrared (FTIR) and extended X-ray absorption fine structure (EXAFS) spectroscopy. |
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Place of Publication |
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Editor |
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Language |
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Wos |
000463759100017 |
Publication Date |
2019-02-18 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2041-6520 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
8.668 |
Times cited |
68 |
Open Access |
OpenAccess |
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Notes |
; The research leading to these results has received funding from the NMBP-01-2016 Program of the European Union's Horizon 2020 Framework Program H2020/2014-2020/under grant agreement no. [720996]. N. V. V., S. S., J. V., B. B. and D. E. D. V. thank the FWO for funding (SB, Aspirant and postdoctoral grants). The electron microscopy work was supported by FWO funding G038116. D. E. D. V. is grateful for KU Leuven support in the frame of the CASAS Metusalem project and a C3 type project. The XAS experiments were performed on beamline BM26A at the European Synchrotron Radiation Facility (ESRF), Grenoble, France. We are grateful to D. Banerjee at the ESRF for providing assistance in using beamline BM26A. Johnson Matthey and S. Bennett are gratefully acknowledged for providing Smopex-102. ; |
Approved |
Most recent IF: 8.668 |
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Call Number |
UA @ admin @ c:irua:159403 |
Serial |
5259 |
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Permanent link to this record |
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Author |
Tan, X.; Stephens, P.W.; Hendrickx, M.; Hadermann, J.; Segre, C.U.; Croft, M.; Kang, C.-J.; Deng, Z.; Lapidus, S.H.; Kim, S.W.; Jin, C.; Kotliar, G.; Greenblatt, M. |
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Title |
Tetragonal Cs1.17In0.81Cl3 : a charge-ordered indium halide perovskite derivative |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
31 |
Issue |
6 |
Pages |
1981-1989 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Polycrystalline samples of Cs1.17In0.81Cl3 were prepared by annealing a mixture of CsCl, InCl, and InCl3, stoichiometric for the targeted CsInCl3. Synchrotron powder X-ray diffraction refinement and chemical analysis by energy dispersive X-ray indicated that Cs1.17In0.81Cl3, a tetragonal distorted perovskite derivative (I4/m), is the thermodynamically stable product. The refined unit cell parameters and space group were confirmed by electron diffraction. In the tetragonal structure, In+ and In3+ are located in four different crystallographic sites, consistent with their corresponding bond lengths. In1, In2, and In3 are octahedrally coordinated, whereas In4 is at the center of a pentagonal bipyramid of Cl because of the noncooperative octahedral tilting of In4Cl6. The charged-ordered In+ and In3+ were also confirmed by X-ray absorption and Raman spectroscopy. Cs1.17In0.81Cl3 is the first example of an inorganic halide double perovskite derivative with charged-ordered In+ and In3+. Band structure and optical conductivity calculations were carried out with both generalized gradient approximation (GGA) and modified Becke-Johnson (mBJ) approach; the GGA calculations estimated the band gap and optical band gap to be 2.27 eV and 2.4 eV, respectively. The large and indirect band gap suggests that Cs1.17In0.81Cl3 is not a good candidate for photovoltaic application. |
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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 |
000462950400017 |
Publication Date |
2019-02-19 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
6 |
Open Access |
OpenAccess |
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Notes |
; M.G. and X.T. were supported by the Center for Computational Design of Functional Strongly Correlated Materials and Theoretical Spectroscopy under DOE Grant No. DE-FOA-0001276. M.G. also acknowledges support of NSF-DMR-1507252 grant. G.K. and C.-J.K. were supported by the Air Force Office of Scientific Research. MRCAT operations are supported by the Department of Energy and the MRCAT member institutions. The use of the Advanced Photon Source at the Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. The works at IOPCAS were supported by NSF & MOST of China through research projects. ; |
Approved |
Most recent IF: 9.466 |
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Call Number |
UA @ admin @ c:irua:159413 |
Serial |
5262 |
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Permanent link to this record |
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Author |
Jafarzadeh, A.; Bal, K.M.; Bogaerts, A.; Neyts, E.C. |
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Title |
CO2 activation on TiO2-supported Cu5 and Ni5 nanoclusters : effect of plasma-induced surface charging |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
The journal of physical chemistry: C : nanomaterials and interfaces |
Abbreviated Journal |
J Phys Chem C |
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Volume |
123 |
Issue |
11 |
Pages |
6516-6525 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
Surface charging is an often overlooked factor in many plasma-surface interactions and in particular in plasma catalysis. In this study, we investigate the effect of excess electrons induced by a plasma on the adsorption properties of CO2 on titania-supported Cu-5 and Ni-5 clusters using spin-polarized and dispersion-corrected density functional theory calculations. The effect of excess electrons on the adsorption of Ni and Cu pentamers as well as on CO2 adsorption on a pristine anatase TiO2(101) slab is studied. Our results indicate that adding plasma-induced excess electrons to the system leads to further stabilization of the bent CO2 structure. Also, dissociation of CO2 on charged clusters is energetically more favorable than on neutral clusters. We hypothesize that surface charge is a plausible cause for the synergistic effects sometimes observed in plasma catalysis. |
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Corporate Author |
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Place of Publication |
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Language |
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Wos |
000462260700024 |
Publication Date |
2019-02-21 |
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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 |
1932-7447; 1932-7455 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.536 |
Times cited |
4 |
Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 4.536 |
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Call Number |
UA @ admin @ c:irua:159422 |
Serial |
5281 |
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Permanent link to this record |
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Author |
Tong, Y.; Fu, M.; Bladt, E.; Huang, H.; Richter, A.F.; Wang, K.; Mueller-Buschbaum, P.; Bals, S.; Tamarat, P.; Lounis, B.; Feldmann, J.; Polavarapu, L. |
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Title |
Chemical cutting of perovskite nanowires into single-photon emissive low-aspect-ratio CsPbX3(X = Cl, Br, I) nanorods |
Type |
A1 Journal article |
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Year |
2018 |
Publication |
Angewandte Chemie: international edition in English |
Abbreviated Journal |
Angew Chem Int Edit |
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Volume |
57 |
Issue |
57 |
Pages |
16094-16098 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Post-synthetic shape-transformation processes provide access to colloidal nanocrystal morphologies that are unattainable by direct synthetic routes. Herein, we report our finding about the ligand-induced fragmentation of CsPbBr3 perovskite nanowires (NWs) into low aspect-ratio CsPbX3 (X = Cl, Br and I) nanorods (NRs) during halide ion exchange reaction with PbX2-ligand solution. The shape transformation of NWs-to-NRs resulted in an increase of photoluminescence efficiency owing to a decrease of nonradiative decay rates. Importantly, we found that the perovskite NRs exhibit single photon emission as revealed by photon antibunching measurements, while it is not detected in parent NWs. This work not only reports on the quantum light emission of low aspect ratio perovskite NRs, but also expands our current understanding of shape-dependent optical properties of perovskite nanocrystals. |
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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 |
000452235600024 |
Publication Date |
2018-10-12 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1433-7851; 0570-0833 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
11.994 |
Times cited |
70 |
Open Access |
OpenAccess |
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Notes |
; This work was supported by the Bavarian State Ministry of Science, Research, and Arts through the grant “Solar Technologies go Hybrid (SolTech)”, by the China Scholarship Council (Y.T. and K.W.), by the Horizon 2020 research and innovation program under the Marie Skodowska-Curie Grant Agreement COMPASS No. 691185 and by LMU Munich's Institutional Strategy LMU excellent (L.P., J.F.). M.F., P.T. and B.L. acknowledge the financial support from the French National Agency for Research, the French Excellence Initiative (Idex Bordeaux, LAPHIA Program) and the Institut Universitaire de France. E.B. and S.B. acknowledge the financial support from the European Research Council Starting Grant # 335078-COLOURATOMS. L.P. thank the EU Infrastructure Project EUSMI (European Union's Horizon 2020, grant No 731019). ; |
Approved |
Most recent IF: 11.994 |
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Call Number |
UA @ admin @ c:irua:156246 |
Serial |
5283 |
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Permanent link to this record |
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Author |
Cremers, V.; Rampelberg, G.; Baert, K.; Abrahami, S.; Claes, N.; de Oliveira, T.M.; Terryn, H.; Bals, S.; Dendooven, J.; Detavernier, C. |
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Title |
Corrosion protection of Cu by atomic layer deposition |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
Journal of vacuum science and technology: A: vacuum surfaces and films |
Abbreviated Journal |
J Vac Sci Technol A |
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Volume |
37 |
Issue |
37 |
Pages |
060902 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Atomic layer deposition (ALD) is a vapor phase technique that is able to deposit uniform, conformal thin films with an excellent thickness control at the atomic scale. 18 nm thick Al2O3 and TiO2 coatings were deposited conformaly and pinhole-free onto micrometer-sized Cu powder, using trimethylaluminum and tetrakis(dimethylamido)titanium(IV), respectively, as a precursor and de-ionized water as a reactant. The capability of the ALD coating to protect the Cu powder against corrosion was investigated. Therefore, the stability of the coatings was studied in solutions with different pH in the range of 0–14, and in situ raman spectroscopy was used to detect the emergence of corrosion products of Cu as an indication that the protective coating starts to fail. Both ALD coatings provide good protection at standard pH values in the range of 5–7. In general, the TiO2 coating shows a better barrier protection against corrosion than the Al2O3 coating. However, for the most extreme pH conditions, pH 0 and pH 14, the TiO2 coating starts also to degrade. |
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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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Language |
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Wos |
000517925800003 |
Publication Date |
2019-09-19 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0734-2101 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
1.374 |
Times cited |
7 |
Open Access |
OpenAccess |
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|
Notes |
The authors acknowledge financial support from the Strategic Initiative Materials in Flanders (SIM, SBO-FUNC project) and the Special Research Fund BOF of Ghent University (No. GOA 01G01513). J.D. acknowledges the Research Foundation Flanders (FWO-Vlaanderen) for a postdoctoral fellowship. |
Approved |
Most recent IF: 1.374 |
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Call Number |
EMAT @ emat @c:irua:162640 |
Serial |
5361 |
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Permanent link to this record |
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Author |
Nerl, H.C.; Pokle, A.; Jones, L.; Müller‐Caspary, K.; Bos, K.H.W.; Downing, C.; McCarthy, E.K.; Gauquelin, N.; Ramasse, Q.M.; Lobato, I.; Daly, D.; Idrobo, J.C.; Van Aert, S.; Van Tendeloo, G.; Sanvito, S.; Coleman, J.N.; Cucinotta, C.S.; Nicolosi, V. |
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Title |
Self‐Assembly of Atomically Thin Chiral Copper Heterostructures Templated by Black Phosphorus |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
Advanced functional materials |
Abbreviated Journal |
Adv Funct Mater |
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Volume |
29 |
Issue |
37 |
Pages |
1903120 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
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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 |
000478478400001 |
Publication Date |
2019-07-17 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1616-301X |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
12.124 |
Times cited |
1 |
Open Access |
OpenAccess |
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Notes |
European Research Council, 2DNanoCaps TC2D CoG 3D2DPrint CoG Picometrics grant agreement No. 770887; Engineering and Physical Sciences Research Council, EP/P033555/1 EP/R029431 ; Science Foundation Ireland, HPC1600932 ; |
Approved |
Most recent IF: 12.124 |
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Call Number |
EMAT @ emat @c:irua:161901 |
Serial |
5362 |
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Permanent link to this record |
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Author |
Ramachandran, R.K.; Filez, M.; Solano, E.; Poelman, H.; Minjauw, M.M.; Van Daele, M.; Feng, J.-Y.; La Porta, A.; Altantzis, T.; Fonda, E.; Coati, A.; Garreau, Y.; Bals, S.; Marin, G.B.; Detavernier, C.; Dendooven, J. |
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Title |
Chemical and Structural Configuration of Pt Doped Metal Oxide Thin Films Prepared by Atomic Layer Deposition |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
31 |
Issue |
31 |
Pages |
9673-9683 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
Pt doped semiconducting metal oxides and Pt metal clusters embedded in an oxide matrix are of interest for applications such as catalysis and gas sensing, energy storage and memory devices. Accurate tuning of the dopant level is crucial for adjusting the properties of these materials. Here, a novel atomic layer deposition (ALD) based method for doping Pt into In2O3 in specific, and metals in metal oxides in general, is demonstrated. This approach combines alternating exposures of Pt and In2O3 ALD processes in a single ‘supercycle’, followed by supercycle repetition leading to multilayered nanocomposites. The atomic level control of ALD and its conformal nature make the method suitable for accurate dopant control even on high surface area supports. Oxidation state, local structural environment and crystalline phase of the embedded Pt dopants were obtained by means of X-ray characterization methods and high angle annular dark-field scanning transmission electron microscopy (HAADF-STEM). In addition, this approach allows characterization of the nucleation stages of metal ALD processes, by stacking those states multiple times in an oxide matrix. Regardless of experimental conditions, a few Pt ALD cycles leads to the formation of oxidized Pt species due to their highly dispersed nature, as proven by X-ray absorption spectroscopy (XAS). Grazing-incidence small-angle X-ray scattering (GISAXS) and highresolution scanning transmission electron microscopy, combined with energy dispersive X-ray spectroscopy (HR-STEM/EDXS) show that Pt is evenly distributed in the In2O3 metal oxide matrix without the formation of clusters. For a larger number of Pt ALD
cycles, typ. > 10, the oxidation state gradually evolves towards fully metallic, and metallic Pt clusters are obtained within the In2O3 metal oxide matrix. This work reveals how tuning of the ALD supercycle approach for Pt doping allows controlled engineering of the Pt compositional and structural configuration within a metal oxide matrix. |
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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 |
000502418000010 |
Publication Date |
2019-11-11 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
6 |
Open Access |
OpenAccess |
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Notes |
This research was supported by the Flemish Research Foundation (FWO-Vlaanderen), the Flemish Government (Long term structural funding – Methusalem funding and Medium scale research infrastructure funding-Hercules funding), the Special Research Fund BOF of Ghent University (GOA 01G01513) and the CALIPSO Trans National Access Program funded by the European Commission in supplying financing of travel costs. We are grateful to the SIXS and SAMBA-SOLEIL staff for smoothly running the beamline facilities. J.D. and R.K.R. are postdoctoral fellows of the FWO. |
Approved |
Most recent IF: 9.466 |
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Call Number |
EMAT @ emat @c:irua:164056 |
Serial |
5380 |
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Permanent link to this record |
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Author |
Yang, M.; Chen, H.; Orekhov, A.; Lu, Q.; Lan, X.; Li, K.; Zhang, S.; Song, M.; Kong, Y.; Schryvers, D.; Du, Y. |
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Title |
Quantified contribution of β″ and β′ precipitates to the strengthening of an aged Al–Mg–Si alloy |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Materials Science And Engineering A-Structural Materials Properties Microstructure And Processing |
Abbreviated Journal |
Mat Sci Eng A-Struct |
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Volume |
774 |
Issue |
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Pages |
138776 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
It is generally believed that β00 precipitates, rather than β0 precipitates, are the major strengthening precipitates in
aged Al–Mg–Si alloys. The reason for this difference is not well understood. To clarify this, two samples of the
same Al–Mg–Si alloy but with different aging states were prepared. The under-aged sample only contains nanoprecipitates
of the β00 type, while the peak-aged one contains nearly equal volumes of β00 and β0 precipitates. We
have, for the first time, separated the strengthening effect of the contribution from βʺ and βʹ precipitates,
respectively, by an indirect approach based on high-precision measurements of volume fractions, number densities,
sizes, proportions of the precipitates, their lattice strains, the composition and grain size of the matrix. The
β0 precipitates, which take 45.6% of the total precipitate volume in the peak-aged sample, contribute to the entire
precipitation strengthening by only 31.6%. The main reason why they are less useful compared to β00 precipitates
has been found to be associated with their smaller lattice strains relative to the matrix, which is 0.99% versus
2.10% (for β00 ). |
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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 |
000514747200001 |
Publication Date |
2019-12-04 |
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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 |
0921-5093 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
6.4 |
Times cited |
|
Open Access |
OpenAccess |
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Notes |
National Natural Science Foundation of China, 51531009 51711530713 51501230 ; Central South University, 2018gczd033 ; Flemish Science Foundation, VS.026.18N ; Program for Guangdong Introducing Innovative and Entrepreneurial Teams, 2016ZT06G025 ; Guangdong Natural Science Foundation, 2017B030306014 ; |
Approved |
Most recent IF: 6.4; 2020 IF: 3.094 |
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Call Number |
EMAT @ emat @c:irua:165290 |
Serial |
5440 |
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Permanent link to this record |
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Author |
Peeters, H.; Keulemans, M.; Nuyts, G.; Vanmeert, F.; Li, C.; Minjauw, M.; Detavernier, C.; Bals, S.; Lenaerts, S.; Verbruggen, S.W. |
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Title |
Plasmonic gold-embedded TiO2 thin films as photocatalytic self-cleaning coatings |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Applied Catalysis B-Environmental |
Abbreviated Journal |
Appl Catal B-Environ |
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Volume |
267 |
Issue |
267 |
Pages |
118654 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Sustainable Energy, Air and Water Technology (DuEL) |
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Abstract |
Transparent photocatalytic TiO2 thin films hold great potential in the development of self-cleaning glass sur-
faces, but suffer from a poor visible light response that hinders the application under actual sunlight. To alleviate this problem, the photocatalytic film can be modified with plasmonic nanoparticles that interact very effectively with visible light. Since the plasmonic effect is strongly concentrated in the near surroundings of the nano- particle surface, an approach is presented to embed the plasmonic nanostructures in the TiO2 matrix itself, rather than deposit them loosely on the surface. This way the interaction interface is maximised and the plasmonic effect can be fully exploited. In this study, pre-fabricated gold nanoparticles are made compatible with the organic medium of a TiO2 sol-gel coating suspension, resulting in a one-pot coating suspension. After spin coating, homogeneous, smooth, highly transparent and photoactive gold-embedded anatase thin films are ob- tained. |
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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 |
000518865300002 |
Publication Date |
2020-01-18 |
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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 |
0926-3373 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
22.1 |
Times cited |
57 |
Open Access |
OpenAccess |
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Notes |
H.P. is grateful to the Research Foundation Flanders (FWO) for an aspirant PhD scholarship. |
Approved |
Most recent IF: 22.1; 2020 IF: 9.446 |
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Call Number |
EMAT @ emat @c:irua:165616 |
Serial |
5446 |
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Permanent link to this record |
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Author |
Smith, J.D.; Bladt, E.; Burkhart, J.A.C.; Winckelmans, N.; Koczkur, K.M.; Ashberry, H.M.; Bals, S.; Skrabalak, S.E. |
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Title |
Defect-directed growth of symmetrically branched metal nanocrystals |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Angewandte Chemie-International Edition |
Abbreviated Journal |
Angew Chem Int Edit |
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Volume |
59 |
Issue |
59 |
Pages |
943-950 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Branched plasmonic nanocrystals (NCs) have attracted much attention due to electric field enhancements at their tips. Seeded growth provides routes to NCs with defined branching patterns and, in turn, near-field distributions with defined symmetries. Here, a systematic analysis was undertaken in which seeds containing different distributions of planar defects were used to grow branched NCs in order to understand how their distributions direct the branching. Characterization of the products by multimode electron tomography and analysis of the NC morphologies at different overgrowth stages indicate that the branching patterns are directed by the seed defects, with the emergence of branches from the seed faces consistent with minimizing volumetric strain energy at the expense of surface energy. These results contrast with growth of branched NCs from single-crystalline seeds and provide a new platform for the synthesis of symmetrically branched plasmonic NCs. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000498760200001 |
Publication Date |
2019-11-13 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1433-7851; 0570-0833 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
16.6 |
Times cited |
23 |
Open Access |
OpenAccess |
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Notes |
; The authors thank Samantha Harvey for her initial observations of branched structures, Alexander Chen for his help with SAED, the staff of the Nanoscale Characterization Facility (Dr. Yi Yi), Electron Microscopy Center (Dr. David Morgan and Dr. Barry Stein), and Molecular Structure Center at Indiana University. J.S. recognizes a fellowship provided by the Indiana Space Grant Consortium. E.B. acknowledges a post-doctoral grant from the Research Foundation Flanders (FWO, Belgium). This project has received funding to S.E.S. from the U.S. National Science Foundation (award numbers: 1602476 and 1904499) and Research Corporation for Scientific Advancement (2017 Frontiers in Research Excellence and Discovery Award) as well as to S.B. from the European Union's Horizon 2020 research and innovation program under grant agreement No 731019 (EUSMI) and No 815128 (REALNANO). ; sygma |
Approved |
Most recent IF: 16.6; 2020 IF: 11.994 |
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Call Number |
UA @ admin @ c:irua:165124 |
Serial |
6293 |
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Permanent link to this record |
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Author |
Spreitzer, M.; Klement, D.; Egoavil, R.; Verbeeck, J.; Kovac, J.; Zaloznik, A.; Koster, G.; Van Tendeloo, G.; Suvorov, D.; Rijnders, G. |
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Title |
Growth mechanism of epitaxial SrTiO3 on a (1 x 2) + (2 x 1) reconstructed Sr(1/2 ML)/Si(001) surface |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Journal Of Materials Chemistry C |
Abbreviated Journal |
J Mater Chem C |
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Volume |
8 |
Issue |
2 |
Pages |
518-527 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Sub-monolayer control over the growth at silicon-oxide interfaces is a prerequisite for epitaxial integration of complex oxides with the Si platform, enriching it with a variety of functionalities. However, the control over this integration is hindered by the intense reaction of the constituents. The most suitable buffer material for Si passivation is metallic strontium. When it is overgrown with a layer of SrTiO3 (STO) it can serve as a pseudo-substrate for the integration with functional oxides. In our study we determined a mechanism for epitaxial integration of STO with a (1 x 2) + (2 x 1) reconstructed Sr(1/2 ML)/Si(001) surface using all-pulsed laser deposition (PLD) technology. A detailed analysis of the initial deposition parameters was performed, which enabled us to develop a complete protocol for integration, taking into account the peculiarities of the PLD growth, STO critical thickness, and process thermal budget, in order to kinetically trap the reaction between STO and Si and thus to minimize the thickness of the interface layer. The as-prepared oxide layer exhibits STO(001)8Si(001) out-of-plane and STO[110]8Si[100] in-plane orientation and together with recent advances in large-scale PLD tools these results represent a new technological solution for the implementation of oxide electronics on demand. |
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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 |
000506852400036 |
Publication Date |
2019-10-28 |
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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 |
2050-7526; 2050-7534 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
6.4 |
Times cited |
12 |
Open Access |
OpenAccess |
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Notes |
; The research was financially supported by the Slovenian Research Agency (Project No. P2-0091, J2-9237) and Ministry of Education, Science and Sport of the Republic of Slovenia (SIOX projects). This work was also funded by the European Union Council under the 7th Framework Program grant no. NMP3-LA-2010-246102 IFOX. J. V. and G. V. T. acknowledge funding from the Fund for Scientific Research Flanders under project no. G.0044.13N. ; |
Approved |
Most recent IF: 6.4; 2020 IF: 5.256 |
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Call Number |
UA @ admin @ c:irua:165672 |
Serial |
6298 |
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Permanent link to this record |
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Author |
Wang, J.; Nguyen, M.D.; Gauquelin, N.; Verbeeck, J.; Do, M.T.; Koster, G.; Rijnders, G.; Houwman, E. |
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Title |
On the importance of the work function and electron carrier density of oxide electrodes for the functional properties of ferroelectric capacitors |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Physica Status Solidi-Rapid Research Letters |
Abbreviated Journal |
Phys Status Solidi-R |
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Volume |
14 |
Issue |
14 |
Pages |
1900520 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
It is important to understand the effect of the interfaces between the oxide electrode layers and the ferroelectric layer on the polarization response for optimizing the device performance of all-oxide ferroelectric devices. Herein, the effects of the oxide La0.07Ba0.93SnO3 (LBSO) as an electrode material in an PbZr0.52Ti0.48O3 (PZT) ferroelectric capacitor are compared with those of the more commonly used SrRuO3 (SRO) electrode. SRO (top)/PZT/SRO (bottom), SRO/PZT/LBSO, and SRO/PZT/2 nm SRO/LBSO devices are fabricated. Only marginal differences in crystalline properties, determined by X-ray diffraction and scanning transmission electron microscopy, are found. High-quality polarization loops are obtained, but with a much larger coercive field for the SRO/PZT/LBSO device. In contrast to the SRO/PZT/SRO device, the polarization decreases strongly with increasing field cycling. This fatigue problem can be remedied by inserting a 2 nm SRO layer between PZT and LBSO. It is argued that strongly increased charge injection into the PZT occurs at the bottom interface, because of the low PZT/LBSO interfacial barrier and the much lower carrier density in LBSO, as compared with that in SRO, causing a low dielectric constant, depleted layer in LBSO. The charge injection creates a trapped space charge in the PZT, causing the difference in fatigue behavior. |
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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 |
000506195600001 |
Publication Date |
2019-12-12 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1862-6254 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
2.8 |
Times cited |
6 |
Open Access |
OpenAccess |
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Notes |
; This work was supported by Nederlandse Organisatie voor Wetenschappelijk Onderzoek through grant no.13HTSM01. ; |
Approved |
Most recent IF: 2.8; 2020 IF: 3.032 |
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Call Number |
UA @ admin @ c:irua:165681 |
Serial |
6316 |
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Permanent link to this record |
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Author |
Hinterding, S.O.M.; Berends, A.C.; Kurttepeli, M.; Moret, M.-E.; Meeldijk, J.D.; Bals, S.; van der Stam, W.; de Donega, C.M. |
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Title |
Tailoring Cu+ for Ga3+ cation exchange in Cu2-xS and CuInS2 nanocrystals by controlling the Ga precursor chemistry |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
13 |
Issue |
13 |
Pages |
12880-12893 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Nanoscale cation exchange (CE) has resulted in colloidal nanomaterials that are unattainable by direct synthesis methods. Aliovalent CE is complex and synthetically challenging because the exchange of an unequal number of host and guest cations is required to maintain charge balance. An approach to control aliovalent CE reactions is the use of a single reactant to both supply the guest cation and extract the host cation. Here, we study the application of GaCl3-L complexes [L = trioctylphosphine (TOP), triphenylphosphite (TPP), diphenylphosphine (DPP)] as reactants in the exchange of Cu+ for Ga3+ in Cu2-xS nanocrystals. We find that noncomplexed GaCl3 etches the nanocrystals by S2- extraction, whereas GaCl3-TOP is unreactive. Successful exchange of Cu+ for Ga3+ is only possible when GaCl3 is complexed with either TPP or DPP. This is attributed to the pivotal role of the Cu2-xS-GaCl3-L activated complex that forms at the surface of the nanocrystal at the onset of the CE reaction, which must be such that simultaneous Ga3+ insertion and Cu+ extraction can occur. This requisite is only met if GaCl3 is bound to a phosphine ligand, with a moderate bond strength, to allow facile dissociation of the complex at the nanocrystal surface. The general validity of this mechanism is demonstrated by using GaCl3-DPP to convert CuInS2 into (Cu,Ga,In)S-2 nanocrystals, which increases the photoluminescence quantum yield 10 -fold, while blue -shifting the photoluminescence into the NIR biological window. This highlights the general applicability of the mechanistic insights provided by our work. |
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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 |
000500650000061 |
Publication Date |
2019-10-16 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
27 |
Open Access |
OpenAccess |
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Notes |
; S.O.M.H., W.v.d.S., A.C.B., and C.d.M.D. acknowledge financial support from the division of Chemical Sciences (CW) of The Netherlands Organization for Scientific Research (NWO) under Grant Nos. ECHO.712.012.0001 and ECHO.712.014.001. S.B. acknowledges financial support from the European Research Council (ERC Consolidator Grant No. 815128-REALNANO). S.O.M.H. is supported by The Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation Programme funded by the Ministry of Education, Culture and Science of the government of The Netherlands. DFT calculations were carried out on the Dutch national e-infrastructure with the support of SURF Cooperative. This work was sponsored by NWO Physical Sciences for the use of supercomputer facilities. The authors thank Jessi van der Hoeven for EDS and TEM measurements. ; sygma |
Approved |
Most recent IF: 13.942 |
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Call Number |
UA @ admin @ c:irua:165149 |
Serial |
6324 |
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Permanent link to this record |
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Author |
Tran Phong Le, P.; Hofhuis, K.; Rana, A.; Huijben, M.; Hilgenkamp, H.; Rijnders, G.A.J.H.M.; ten Elshof, J.E.; Koster, G.; Gauquelin, N.; Lumbeeck, G.; Schuessler-Langeheine, C.; Popescu, H.; Fortuna, F.; Smit, S.; Verbeek, X.H.; Araizi-Kanoutas, G.; Mishra, S.; Vaskivskyi, I.; Duerr, H.A.; Golden, M.S. |
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Title |
Tailoring vanadium dioxide film orientation using nanosheets : a combined microscopy, diffraction, transport, and soft X-ray in transmission study |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Advanced Functional Materials |
Abbreviated Journal |
Adv Funct Mater |
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Volume |
30 |
Issue |
1 |
Pages |
1900028 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Vanadium dioxide (VO2) is a much-discussed material for oxide electronics and neuromorphic computing applications. Here, heteroepitaxy of VO2 is realized on top of oxide nanosheets that cover either the amorphous silicon dioxide surfaces of Si substrates or X-ray transparent silicon nitride membranes. The out-of-plane orientation of the VO2 thin films is controlled at will between (011)(M1)/(110)(R) and (-402)(M1)/(002)(R) by coating the bulk substrates with Ti0.87O2 and NbWO6 nanosheets, respectively, prior to VO2 growth. Temperature-dependent X-ray diffraction and automated crystal orientation mapping in microprobe transmission electron microscope mode (ACOM-TEM) characterize the high phase purity, the crystallographic and orientational properties of the VO2 films. Transport measurements and soft X-ray absorption in transmission are used to probe the VO2 metal-insulator transition, showing results of a quality equal to those from epitaxial films on bulk single-crystal substrates. Successful local manipulation of two different VO2 orientations on a single substrate is demonstrated using VO2 grown on lithographically patterned lines of Ti0.87O2 and NbWO6 nanosheets investigated by electron backscatter diffraction. Finally, the excellent suitability of these nanosheet-templated VO2 films for advanced lensless imaging of the metal-insulator transition using coherent soft X-rays is discussed. |
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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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Wos |
000505545800010 |
Publication Date |
2019-10-31 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1616-301x |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
19 |
Times cited |
1 |
Open Access |
OpenAccess |
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Notes |
P.T.P.L. and K.H. contributed equally to this work. The authors thank Mark A. Smithers for performing high-resolution scanning electron microscopy and electron backscattering diffraction. The authors also thank Dr. Nicolas Jaouen for his contribution to the soft X-ray imaging experiments. This work is part of the DESCO research program of the Foundation for Fundamental Research on Matter (FOM), which is part of the Netherlands Organisation for Scientific Research (NWO). P.T.P.L. acknowledges the NWO/CW ECHO grant ECHO.15.CM2.043. N.G. acknowledges funding from the Geconcentreerde Onderzoekacties (GOA) project “Solarpaint” of the University of Antwerp and the FLAG-ERA JTC 2017 project GRAPH-EYE. G.L. acknowledges financial support from the Flemish Research Fund (FWO) under project G.0365.15N. I.V. acknowledges support by the U.S. Department of Energy, Office of Science under Award Number 0000231415. |
Approved |
Most recent IF: 19; 2020 IF: 12.124 |
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Call Number |
UA @ admin @ c:irua:165705 |
Serial |
6325 |
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Permanent link to this record |
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Author |
González-Rubio, G.; Milagres de Oliveira, T.; Albrecht, W.; Díaz-Núñez, P.; Castro-Palacio, J.C.; Prada, A.; González, R.I.; Scarabelli, L.; Bañares, L.; Rivera, A.; Liz-Marzán, L.M.; Peña-Rodríguez, O.; Bals, S.; Guerrero-Martínez, A. |
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Title |
Formation of Hollow Gold Nanocrystals by Nanosecond Laser Irradiation |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Journal Of Physical Chemistry Letters |
Abbreviated Journal |
J Phys Chem Lett |
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Volume |
11 |
Issue |
11 |
Pages |
670-677 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
The irradiation of spherical gold nanoparticles (AuNPs) with nanosecond laser pulses induces shape transformations yielding nanocrystals with an inner cavity. The concentration of the stabilizing surfactant, the use of moderate pulse fluences, and the size of the irradiated AuNPs determine the efficiency of the process and the nature of the void. Hollow nanocrystals are obtained when molecules from the surrounding medium (e.g., water and organic matter derived from the surfactant) are trapped during laser pulse irradiation. These experimental observations suggest the existence of a subtle balance between the heating and cooling processes experienced by the nanocrystals, which induce their expansion and subsequent recrystallization keeping exogenous matter inside. The described approach provides valuable insight into the mechanism of interaction of pulsed nanosecond laser with AuNPs, along with interesting prospects for the development of hollow plasmonic nanoparticles with potential applications related to gas and liquid storage at the nanoscale. |
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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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Language |
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Wos |
000512223400012 |
Publication Date |
2020-02-06 |
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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 |
1948-7185 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
5.7 |
Times cited |
15 |
Open Access |
OpenAccess |
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Notes |
This work has been funded by the Spanish Ministry of Science, Innovation and Universities (MICIU) (Grants RTI2018-095844-B-I00, PGC2018-096444-B-I00, ENE2015-70300-C3-3, and MAT2017-86659-R), the EUROfusion Consortium (Grant ENR-IFE19.CCFE-01) and the Madrid Regional Government (Grants P2018/NMT-4389 and P2018/EMT-4437). This project has received funding from the European Commission (grant 731019, EUSMI & grant 823717, ESTEEM3). The publication is based also upon work from COST Action TUMIEE (CA17126). The facilities provided by the Center for Ultrafast Lasers at Complutense University of Madrid are gratefully acknowledged. The authors also acknowledge the computer resources and technical assistance provided by the Centro de Supercomputacion y Visualizacion de Madrid (CeSViMa). L.M.L.-M. acknowledges the Maria de Maeztu Units of Excellence Program from the Spanish State Research Agency (Grant MDM-2017-0720). This project has also received funding from the European Research Council (ERC Consolidator Grant 815128, REALNANO). W.A. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (Grant 797153, SOPMEN). A.P. and R.I.G. acknowledge the support of FONDECYT under Grants 3190123 and 11180557 and Financiamiento Basal para Centros Cientificos y Tecnologicos de Excelencia FB-0807. This research was partially supported by the supercomputing infrastructure of the NLHPC (ECM-02).; sygma; esteem3JRA; esteem3reported |
Approved |
Most recent IF: 5.7; 2020 IF: 9.353 |
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Call Number |
EMAT @ emat @c:irua:166504 |
Serial |
6334 |
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Permanent link to this record |
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Author |
Smith, J.D.; Bladt, E.; Burkhart, J.A.C.; Winckelmans, N.; Koczkur, K.M.; Ashberry, H.M.; Bals, S.; Skrabalak, S.E. |
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Title |
Defect‐Directed Growth of Symmetrically Branched Metal Nanocrystals |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Angewandte Chemie (International ed. Print) |
Abbreviated Journal |
Angew. Chem. |
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Volume |
132 |
Issue |
132 |
Pages |
953-960 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Branched plasmonic nanocrystals (NCs) have attracted much attention due to electric field enhancements at their tips. Seeded growth provides routes to NCs with defined branching patterns and, in turn, near‐field distributions with defined symmetries. Here, a systematic analysis was undertaken in which seeds containing different distributions of planar defects were used to grow branched NCs in order to understand how their distributions direct the branching. Characterization of the products by multimode electron tomography and analysis of the NC morphologies at different overgrowth stages indicate that the branching patterns are directed by the seed defects, with the emergence of branches from the seed faces consistent with minimizing volumetric strain energy at the expense of surface energy. These results contrast with growth of branched NCs from single‐crystalline seeds and provide a new platform for the synthesis of symmetrically branched plasmonic NCs. |
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Thesis |
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Publisher |
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Place of Publication |
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Wos |
000505279500063 |
Publication Date |
2020-01-07 |
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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 |
0044-8249 |
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 |
OpenAccess |
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Notes |
The authors thank Samantha Harvey for her initial observations of branched structures, Alexander Chen for his help with SAED, the staff of the Nanoscale Characterization Facility (Dr. Yi Yi),Electron Microscopy Center (Dr. David Morgan and Dr. Barry Stein), and Molecular Strucre Center at Indiana University. J.S. recognizes a fellowship provided by the Indiana Space Grant Consortium. E. B. acknowledges a post-doctoral grant from the Research Foundation Flanders (FWO, Belgium). This project has received funding from the National Science Foundation (award number: 1602476), Research Corporation for Scietific Advancement (2017 Frontiers in Research Excellence and Discovery Award), and the European Union’s Horizon 2020 research and innovation program under grant agreement No 731019 (EUSMI) and No 815128 (REALNANO).; sygma |
Approved |
Most recent IF: NA |
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Call Number |
EMAT @ emat @c:irua:166581 |
Serial |
6336 |
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Permanent link to this record |
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Author |
Slaets, J.; Aghaei, M.; Ceulemans, S.; Van Alphen, S.; Bogaerts, A. |
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Title |
CO2and CH4conversion in “real” gas mixtures in a gliding arc plasmatron: how do N2and O2affect the performance? |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Green Chemistry |
Abbreviated Journal |
Green Chem |
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Volume |
22 |
Issue |
4 |
Pages |
1366-1377 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
In this paper we study dry reforming of methane (DRM) in a gliding arc plasmatron (GAP) in the presence of N<sub>2</sub>and O<sub>2</sub>. N<sub>2</sub>is added to create a stable plasma at equal fractions of CO<sub>2</sub>and CH<sub>4</sub>, and because emissions from industrial plants typically contain N<sub>2</sub>, while O<sub>2</sub>is added to enhance the process. We test different gas mixing ratios to evaluate the conversion and energy cost. We obtain conversions between 31 and 52% for CO<sub>2</sub>and between 55 and 99% for CH<sub>4</sub>, with total energy costs between 3.4 and 5.0 eV per molecule, depending on the gas mixture. This is very competitive when benchmarked with the literature. In addition, we present a chemical kinetics model to obtain deeper insight in the underlying plasma chemistry. This allows determination of the major reaction pathways to convert CO<sub>2</sub>and CH<sub>4</sub>, in the presence of O<sub>2</sub>and N<sub>2</sub>, into CO and H<sub>2</sub>. We show that N<sub>2</sub>assists in the CO<sub>2</sub>conversion, but part of the applied energy is also wasted in N<sub>2</sub>excitation. Adding O<sub>2</sub>enhances the CH<sub>4</sub>conversion, and lowers the energy cost, while the CO<sub>2</sub>conversion remains constant, and only slightly drops at the highest O<sub>2</sub>fractions studied, when CH<sub>4</sub>is fully oxidized into CO<sub>2</sub>. |
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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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Language |
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Wos |
000518034000032 |
Publication Date |
2020-01-30 |
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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 |
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Series Issue |
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Edition |
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ISSN |
1463-9262 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.8 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
H2020 European Research Council, 810182 ; Fonds Wetenschappelijk Onderzoek, GoF9618n 12M7118N ; We acknowledge financial support from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No 810182 – SCOPE ERC Synergy project), the Excellence of Science FWO-FNRS project (FWO grant ID GoF9618n, EOS ID 30505023), and the FWO postdoctoral fellowship of M. A. (Grant number 12M7118N). This work was carried out in part using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen, a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (department EWI) and the University of Antwerp. |
Approved |
Most recent IF: 9.8; 2020 IF: 9.125 |
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Call Number |
PLASMANT @ plasmant @c:irua:167136 |
Serial |
6339 |
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Permanent link to this record |
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Author |
Saveleva, V.A.; Wang, L.; Kasian, O.; Batuk, M.; Hadermann, J.; Gallet, J.-j.; Bournel, F.; Alonso-Vante, N.; Ozouf, G.; Beauger, C.; Mayrhofer, K.J.J.; Cherevko, S.; Gago, A.S.; Friedrich, K.A.; Zafeiratos, S.; Savinova, E.R. |
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Title |
Insight into the Mechanisms of High Activity and Stability of Iridium Supported on Antimony-Doped Tin Oxide Aerogel for Anodes of Proton Exchange Membrane Water Electrolyzers |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Acs Catalysis |
Abbreviated Journal |
Acs Catal |
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Volume |
10 |
Issue |
4 |
Pages |
2508-2516 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
The use of high amounts of iridium in industrial proton exchange membrane water electrolysers (PEMWE) could hinder their widespread use for the decarbonisation of society with hydrogen. Non-thermally oxidised Ir nanoparticles supported on antimony-doped tin oxide (SnO2:Sb, ATO) aerogel allow decreasing the use of the precious metal by more than 70 %, while enhancing the electro-catalytic activity and stability. To date the origin of these benefits remains unknown. Here we present clear evidence on the mechanisms that lead to the enhancement of the electrochemical properties of the catalyst. Operando near ambient pressure X-ray photoelectron spectroscopy on membrane electrode assemblies reveals a low degree of Ir oxidation, attributed to the oxygen spill-over from Ir to SnO2:Sb. Furthermore, the formation of highly unstable Ir(III) species is mitigated, while the decrease of Ir dissolution in Ir/SnO2:Sb is confirmed by inductively coupled plasma mass spectrometry (ICP-MS). The mechanisms that lead to the high activity and stability of Ir catalyst supported on SnO2:Sb aerogel for PEMWE are thus unveiled. |
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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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Language |
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Wos |
000516887400011 |
Publication Date |
2020-02-21 |
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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 |
2155-5435 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
12.9 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
The research leading to these results has received funding from the European Union’s Seventh Framework Program (FP7/2007-2013) for Fuel Cell and Hydrogen Joint Technology (FCH JU) Initiative under Grant No. 621237 (INSIDE). In addition, A.S.G. and C.B. thank the European Union’s Horizon 2020 research and innovation programme for funding the project PRETZEL under grant agreement No 779478 and it is supported by FCH JU. Solvay is acknowledged for providing Aquivion membrane and ionomer. |
Approved |
Most recent IF: 12.9; 2020 IF: 10.614 |
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Call Number |
EMAT @ emat @c:irua:167147 |
Serial |
6341 |
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Permanent link to this record |