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Guerrero, R.M.; Lemir, I.D.; Carrasco, S.; Fernández-Ruiz, C.; Kavak, S.; Pizarro, P.; Serrano, D.P.; Bals, S.; Horcajada, P.; Pérez, Y. |
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Title |
Scaling-Up Microwave-Assisted Synthesis of Highly Defective Pd@UiO-66-NH2Catalysts for Selective Olefin Hydrogenation under Ambient Conditions |
Type |
A1 Journal Article |
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Year |
2024 |
Publication |
ACS Applied Materials & Interfaces |
Abbreviated Journal  |
ACS Appl. Mater. Interfaces |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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The need to develop green and cost-effective industrial catalytic processes has led to growing interest in preparing more robust, efficient, and selective heterogeneous catalysts at a large scale. In this regard, microwave-assisted synthesis is a fast method for fabricating heterogeneous catalysts (including metal oxides, zeolites, metal–organic frameworks, and supported metal nanoparticles) with enhanced catalytic properties, enabling synthesis scale-up. Herein, the synthesis of nanosized UiO-66-NH2 was optimized via a microwave-assisted hydrothermal method to obtain defective matrices essential for the stabilization of metal nanoparticles, promoting catalytically active sites for hydrogenation reactions (760 kg·m–3·day–1 space time yield, STY). Then, this protocol was scaled up in a multimodal microwave reactor, reaching 86% yield (ca. 1 g, 1450 kg·m–3·day–1 STY) in only 30 min. Afterward, Pd nanoparticles were formed in situ decorating the nanoMOF by an effective and fast microwave-assisted hydrothermal method, resulting in the formation of Pd@UiO-66-NH2 composites. Both the localization and oxidation states of Pd nanoparticles (NPs) in the MOF were achieved using high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and X-ray photoelectron spectroscopy (XPS), respectively. The optimal composite, loaded with 1.7 wt % Pd, exhibited an extraordinary catalytic activity (>95% yield, 100% selectivity) under mild conditions (1 bar H2, 25 °C, 1 h reaction time), not only in the selective hydrogenation of a variety of single alkenes (1-hexene, 1-octene, 1-tridecene, cyclohexene, and tetraphenyl ethylene) but also in the conversion of a complex mixture of alkenes (i.e., 1-hexene, 1-tridecene, and anethole). The results showed a powerful interaction and synergy between the active phase (Pd NPs) and the catalytic porous scaffold (UiO-66-NH2), which are essential for the selectivity and recyclability. |
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Publication Date |
2024-04-26 |
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ISSN |
1944-8244 |
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Impact Factor |
9.5 |
Times cited |
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Open Access |
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Notes |
The authors gratefully acknowledge financial support from “Comunidad de Madrid” and European Regional Development Fund-FEDER through the project HUB MADRID+CIRCULAR; the State Research Agency (MCIN/AEI /10.13039/501100011033) through the grant with reference number CEX2019-000931-M received in the 2019 call for “Severo Ochoa Centres of Excellence” and “María de Maeztu Units of Excellence” of the State Programme for Knowledge Generation and Scientific and Technological Strengthening of the R&D&I System; and MICIU through the project “NAPOLION” (PID2022-139956OB-I00). S.K. acknowledges the Flemish Fund for Scientific Research (FWO Vlaanderen) through a PhD research grant (1181124N). |
Approved |
Most recent IF: 9.5; 2024 IF: 7.504 |
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Call Number |
EMAT @ emat @ |
Serial |
9126 |
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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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000477917700006 |
Publication Date |
2019-05-31 |
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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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Author |
Bhatia, H.; Keshavarz, M.; Martin, C.; Van Gaal, L.; Zhang, Y.; de Coen, B.; Schrenker, N.J.; Valli, D.; Ottesen, M.; Bremholm, M.; Van de Vondel, J.; Bals, S.; Hofkens, J.; Debroye, E. |
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Title |
Achieving High Moisture Tolerance in Pseudohalide Perovskite Nanocrystals for Light-Emitting Diode Application |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
ACS Applied Optical Materials |
Abbreviated Journal |
ACS Appl. Opt. Mater. |
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Volume |
1 |
Issue |
6 |
Pages |
1184-1191 |
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Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
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Abstract |
The addition of potassium thiocyanate (KSCN) to the FAPbBr3 structure and subsequent post-treatment of nanocrystals (NCs) lead to high quantum confinement, resulting in a photoluminescent quantum yield (PLQY) approaching unity and microsecond decay times. This synergistic approach demonstrated exceptional stability under humid conditions, retaining 70% of the PLQY for over a month, while the untreated NCs degrade within 24 h. Additionally, the devices incorporating the post-treated NCs displayed 1.5% external quantum efficiency (EQE), a 5-fold improvement over untreated devices. These results provide promising opportunities for the use of perovskites in moisture-stable optoelectronics. |
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Publication Date |
2023-06-23 |
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Edition |
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ISSN |
2771-9855 |
ISBN |
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Additional Links |
UA library record |
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Impact Factor |
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Times cited |
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Open Access |
OpenAccess |
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Notes |
Hercules Foundation, HER/11/14 ; European Commission; Ministerio de Ciencia e Innovaci?n, PID2021-128761OA-C22 ; European Regional Development Fund; Vlaamse regering, CASAS2 Meth/15/04 ; Fonds Wetenschappelijk Onderzoek, 1238622N 1514220N 1S45223N G.0B39.15 G.0B49.15 G098319N S002019N ZW15_09-GOH6316 ; Onderzoeksraad, KU Leuven, C14/19/079 db/21/006/bm iBOF-21-085 STG/21/010 ; Junta de Comunidades de Castilla-La Mancha, SBPLY/21/180501/000127 ; H2020 European Research Council, 642196 815128 ; |
Approved |
Most recent IF: NA |
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Call Number |
EMAT @ emat @c:irua:201011 |
Serial |
8975 |
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Author |
Ennaert, T.; Geboers, J.; Gobechiya, E.; Courtin, C.M.; Kurttepeli, M.; Houthoofd, K.; Kirschhock, C.E.A.; Magusin, P.C.M.M.; Bals, S.; Jacobs, P.A.; Sels, B.F. |
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Title |
Conceptual frame rationalizing the self-stabilization of H-USY zeolites in hot liquid water |
Type |
A1 Journal article |
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Year |
2015 |
Publication |
ACS catalysis |
Abbreviated Journal |
Acs Catal |
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Volume |
5 |
Issue |
5 |
Pages |
754-768 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
The wide range of liquid-phase reactions required for the catalytic conversion of biomass compounds into new bioplatform molecules defines a new set of challenges for the development of active, selective, and stable catalysts. The potential of bifunctional Ru/H-USY catalysts for conversions in hot liquid water (HLW) is assessed in terms of physicochemical stability and long-term catalytic performance of acid sites and noble metal functionality, as probed by hydrolytic hydrogenation of cellulose. It is shown that zeolite desilication is the main zeolite degradation mechanism in HLW. USY zeolite stability depends on two main parameters, viz., framework and extra-framework aluminum content. The former protects the zeolite lattice by counteracting hydrolysis of framework bonds, and the latter, when located at the external crystal surface, prevents solubilization of the zeolite framework which is the result of its low water-solubility. Hence, the hot liquid water stability of commercial H-USY zeolites, in contrast to their steam stability, increased with decreasing Si/AI ratio. As a result, mildly steamed USY zeolites containing a high amount of both Al species exhibit the highest resistance to HLW. During an initial period of transformations, Al-rich zeolites form additional protective extra-framework Al species at the outer surface, self-stabilizing the framework. A critical bulk Si/AI ratio of 3 was determined whereby USY zeolites with a lower Si/AI ratio will self-stabilize over time. Besides, due to the initial transformation period, the accessibility of the catalytic active sites is extensively enhanced resulting in a material that is more stable and drastically more accessible to large substrates than the original zeolite. When these findings are applied in the hydrolytic hydrogenation of cellulose, unprecedented nearly quantitative hexitol yields were obtained with a stable catalytic system. |
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000349275300031 |
Publication Date |
2014-12-09 |
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ISSN |
2155-5435;2155-5435; |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
10.614 |
Times cited |
65 |
Open Access |
OpenAccess |
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Notes |
335078 Colouratom; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 10.614; 2015 IF: 9.312 |
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Call Number |
c:irua:125288 |
Serial |
474 |
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Author |
Mei, B.; Wiktor, C.; Turner, S.; Pougin, A.; Van Tendeloo, G.; Fischer, R.A.; Muhler, M.; Strunk, J. |
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Title |
Evidence for metalsupport interactions in Au modified TiOx/SBA-15 materials prepared by photodeposition |
Type |
A1 Journal article |
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Year |
2013 |
Publication |
ACS catalysis |
Abbreviated Journal |
Acs Catal |
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Volume |
3 |
Issue |
12 |
Pages |
3041-3049 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Gold nanoparticles have been efficiently photodeposited onto titanate-loaded SBA-15 (Ti(x)/SBA-15) with different titania coordination. Transmission electron microscopy shows that relatively large Au nanoparticles are photodeposited on the outer surface of the Ti(x)/SBA-15 materials and that TiOx tends to form agglomerates in close proximity to the Au nanoparticles, often forming coreshell Au/TiOx structures. This behavior resembles typical processes observed due to strong-metal support interactions. In the presence of gold, the formation of hydrogen on Ti(x)/SBA-15 during the photodeposition process and the performance in the hydroxylation of terephthalic acid is greatly enhanced. The activity of the Au/Ti(x)/SBA-15 materials is found to depend on the TiOx loading, increasing with a larger amount of initially isolated TiO4 tetrahedra. Samples with initially clustered TiOx species show lower photocatalytic activities. When isolated zinc oxide (ZnOx) species are present on Ti(x)/SBA-15, gold nanoparticles are smaller and well dispersed within the pores. Agglomeration of TiOx species and the formation of Au/TiOx structures is negligible. The dispersion of gold and the formation of Au/TiOx in the SBA-15 matrix seem to depend on the mobility of the TiOx species. The mobility is determined by the initial degree of agglomeration of TiOx. Effective hydrogen evolution requires Au/TiOx coreshell composites as in Au/Ti(x)/SBA-15, whereas hydroxylation of terephthalic acid can also be performed with Au/ZnOx/TiOx/SBA-15 materials. However, isolated TiOx species have to be grafted onto the support prior to the zinc oxide species, providing strong evidence for the necessity of TiOSi bridges for high photocatalytic activity in terephthalic acid hydroxylation. |
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Wos |
000328231400044 |
Publication Date |
2013-11-05 |
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ISSN |
2155-5435;2155-5435; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
10.614 |
Times cited |
22 |
Open Access |
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Notes |
262348 ESMI; FWO; 246791 COUNTATOMS; IAP-PAI; Hercules |
Approved |
Most recent IF: 10.614; 2013 IF: 7.572 |
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Call Number |
UA @ lucian @ c:irua:112502 |
Serial |
1094 |
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Author |
Verduyckt, J.; Van Hoof, M.; De Schouwer, F.; Wolberg, M.; Kurttepeli, M.; Eloy, P.; Gaigneaux, E.M.; Bals, S.; Kirschhock, C.E.A.; De Vos, D.E. |
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Title |
PdPb-catalyzed decarboxylation of proline to pyrrolidine : highly selective formation of a biobased amine in water |
Type |
A1 Journal article |
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Year |
2016 |
Publication |
ACS catalysis |
Abbreviated Journal |
Acs Catal |
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Volume |
6 |
Issue |
6 |
Pages |
7303-7310 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Amino acids have huge potential as platform chemicals in the biobased industry. Pd-catalyzed decarboxylation is a very promising route for the valorization of these natural compounds derived from protein waste or fermentation. We report that the highly abundant and nonessential amino acid L-proline is very reactive in the Pd-catalyzed decarboxylation. Full conversions are obtained with Pd/C and different Pd/MeOx catalysts; this allowed the identification of the different side reactions and the mapping of the reaction network. Due to the high reactivity of pyrrolidine, the selectivity for pyrrolidine was initially low. By carefully modifying Pd/ZrO2 with Pb in a controlled manner-via two incipient wetness impregnation steps-the selectivity increased remarkably. Finally, a thorough investigation of the reaction parameters resulted in an increased activity of this modified catalyst and an even further enhanced selectivity under a low H-2 pressure of 4 bar at 235 degrees C in water. This results in a very selective and sustainable production route for the highly interesting pyrrolidine. |
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Wos |
000387306100005 |
Publication Date |
2016-09-16 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2155-5435 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
10.614 |
Times cited |
27 |
Open Access |
OpenAccess |
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Notes |
; J.V. and F.D.S. thank Fonds Wetenschappelijk Onderzoek (FWO) and Agency for Innovation by Science and Technology (IWT) for doctoral fellowships. D.D.V. acknowledges IWT and FWO for research project funding. D.D.V. and C.E.A.K. acknowledge the Flemish government for long-term structural funding through Methusalem. D.D.V. and S.B. acknowledge Belspo (IAP-PAI 7/05) for financial support. S.B. is grateful for funding by the European Research Council (ERC starting grant no. 335078-COLOURATOMS). The authors also thank the Department of Chemistry, University of Cologne, Germany for use of their XRD equipment. Finally, the assistance of Karel Duerinckx, Werner Wouters, Walter Vermandel, Ivo Stassen, Dries Jonckheere, Sabina Accardo and Bart Bueken with 11-1 NMR, pressure reactors, CO chemisorption, N<INF>2</INF> physisorption, SEM, gas phase FTIR and high-throughput XRD, respectively, is very much appreciated. ; ecas_Sara |
Approved |
Most recent IF: 10.614 |
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Call Number |
UA @ lucian @ c:irua:139171 |
Serial |
4445 |
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Author |
Theofanidis, S.A.; Galvita, V.V.; Poelman, H.; Dharanipragada, N.V.R.A.; Longo, A.; Meledina, M.; Van Tendeloo, G.; Detavernier, C.; Marin, G.B. |
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Title |
Fe-containing magnesium aluminate support for stability and carbon control during methane reforming |
Type |
A1 Journal article |
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Year |
2018 |
Publication |
ACS catalysis |
Abbreviated Journal |
Acs Catal |
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Volume |
8 |
Issue |
7 |
Pages |
5983-5995 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
We report a MgFexAl2-xO4 synthetic spinel, where x varies from 0 to 0.26, as support for Ni-based catalysts, offering stability and carbon control under various conditions of methane reforming. By incorporation of Fe into a magnesium aluminate spine!, a support is created with redox functionality and high thermal stability, as concluded from temporal analysis of products (TAP) experiments and redox cycling, respectively. A diffusion coefficient of 3 x 10(-17) m(2) s(-1) was estimated for lattice oxygen at 993 K from TAP experiments. X-ray diffraction (XRD) and extended X-ray absorption fine structure (EXAFS) modeling identified that the incorporation of iron occurs as Fe3+ in the octahedral sites of the spinel lattice, replacing aluminum. Simulation of the X-ray absorption near edge structure (XANES) spectrum of the reduced support showed that 60 +/- 10% of iron was reduced from 3+ to 2+ at 1073 K, while there was no formation of metallic iron. A series of Ni/MgFexAl2-xO4 catalysts, where x varies from 0 to 0.26, was synthesized and reduced, yielding a supported Ni-Fe alloy. The evolution of the catalyst structure during H-2 temperature-programmed reduction (TPR) and CO2 temperature-programmed oxidation (TPO) was examined using time-resolved in situ XRD and XANES. During reforming, iron in both the support and alloy keeps control of carbon accumulation, as confirmed by O-2-TPO on the spent catalysts. By fine tuning the amount of Fe in MgFexAl2-xO4, a supported alloy was obtained with a Ni/Fe molar ratio of similar to 10, which was active for reforming and stable. By comparison of the performance of Ni-based catalysts with Fe either incorporated into or deposited onto the support, the location of Fe within the support proved crucial for the stability and carbon mitigation under reforming conditions. |
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000438475100034 |
Publication Date |
2018-05-22 |
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Series Issue |
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Edition |
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ISSN |
2155-5435 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
10.614 |
Times cited |
18 |
Open Access |
OpenAccess |
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Notes |
; This work was supported by the FAST industrialization by Catalyst Research and Development (FASTCARD) project, which is a Large Scale Collaborative Project supported by the European Commission in the 7th Framework Programme (GA no 604277), the “Long Term Structural Methusalem Funding by the Flemish Government”, the Interuniversity Attraction Poles Programme, IAP7/5, Belgian State – Belgian Science Policy, and the Fund for Scientific Research Flanders (FWO-Vlaanderen) in supplying financing of travel costs and beam time at the DUBBLE beamline of the ESRF. The authors acknowledge the assistance from the DUBBLE (ESRF, XAS campaign 26-01-1048) and ROCK staff (SOLEIL, proposal 201502561). The authors equally acknowledge support from a public grant overseen by the French National Research Agency (ANR) as part of the “Investissements d'Avenir” program (reference: ANR-10-EQPX-45) for the ROCK beamline and from Lukas Buelens and Rakesh Batchu (Laboratory for Chemical Technology, Ghent University) for the STEM measurements and TAP experiments, respectively. ; |
Approved |
Most recent IF: 10.614 |
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Call Number |
UA @ lucian @ c:irua:153178 |
Serial |
5102 |
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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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Wos |
000516887400011 |
Publication Date |
2020-02-21 |
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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 |
|
Open Access |
OpenAccess |
|
| |
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 |
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| |
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Author |
Mehta, P.; Barboun, P.M.; Engelmann, Y.; Go, D.B.; Bogaerts, A.; Schneider, W.F.; Hicks, J.C. |
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| |
Title |
Plasma-Catalytic Ammonia Synthesis beyond the Equilibrium Limit |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Acs Catalysis |
Abbreviated Journal |
Acs Catal |
|
| |
Volume |
10 |
Issue |
12 |
Pages |
6726-6734 |
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| |
Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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| |
Abstract |
We explore the consequences of nonthermal plasma-activation on product yields in catalytic ammonia synthesis, a reaction that is equilibrium-limited at elevated temperatures. We employ a minimal microkinetic model that incorporates the influence of plasma-activation on N2 dissociation rates to predict NH3 yields into and across the equilibrium-limited regime. NH3 yields are predicted to exceed bulk thermodynamic equilibrium limits on materials that are thermal-rate-limited by N2 dissociation. In all cases, yields revert to bulk equilibrium at temperatures at which thermal reaction rates exceed plasma-activated ones. Beyond-equilibrium NH3 yields are observed in a packed bed dielectric barrier discharge reactor and exhibit sensitivity to catalytic material choice in a way consistent with model predictions. The approach and results highlight the opportunity to exploit synergies between nonthermal plasmas and catalysts to affect transformations at conditions inaccessible through thermal routes. |
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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 |
000543663800015 |
Publication Date |
2020-06-19 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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| |
Series Volume |
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Series Issue |
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Edition |
|
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| |
ISSN |
2155-5435 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
12.9 |
Times cited |
|
Open Access |
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| |
Notes |
University of Notre Dame; Basic Energy Sciences, DE-SC-0016543 ; Air Force Office of Scientific Research, FA9550-18-1- 0157 ; This work was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Sustainable Ammonia Synthesis Program, under Award DE-SC-0016543 and by the U.S. Air Force Office of Scientific Research, under Award FA9550-18-1-0157. P.M. acknowledges support through the Eilers Graduate Fellowship for Energy Related Research from the University of Notre Dame. Computational resources were provided by the Notre Dame Center for Research Computing. We thank the Notre Dame Energy Materials Characterization Facility and the Notre Dame Integrated Imaging Facility for the use of the X-ray diffractometer and the transmission electron microscope, respectively. |
Approved |
Most recent IF: 12.9; 2020 IF: 10.614 |
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| |
Call Number |
PLASMANT @ plasmant @c:irua:170713 |
Serial |
6405 |
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| Permanent link to this record |
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| |
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Author |
Irtem, E.; Arenas Esteban, D.; Duarte, M.; Choukroun, D.; Lee, S.; Ibáñez, M.; Bals, S.; Breugelmans, T. |
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| |
Title |
Ligand-Mode Directed Selectivity in Cu–Ag Core–Shell Based Gas Diffusion Electrodes for CO2Electroreduction |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Acs Catalysis |
Abbreviated Journal |
Acs Catal |
|
| |
Volume |
|
Issue |
|
Pages |
13468-13478 |
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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 |
Bimetallic nanoparticles with tailored size and specific composition have shown promise as stable and selective catalysts for electrochemical reduction of CO2 (CO2R) in batch systems. Yet, limited effort was devoted to understand the effect of ligand coverage and postsynthesis treatments on CO2 reduction, especially under industrially applicable conditions, such as at high currents (>100 mA/cm2) using gas diffusion electrodes (GDE) and flow reactors. In this work, Cu–Ag core–shell nanoparticles (11 ± 2 nm) were prepared with three different surface modes: (i) capped with oleylamine, (ii) capped with monoisopropylamine, and (iii) surfactant free with a reducing borohydride agent; Cu–Ag (OAm), Cu–Ag (MIPA), and Cu–Ag (NaBH4), respectively. The ligand exchange and removal was evidenced by infrared spectroscopy (ATR-FTIR) analysis, whereas high-resolution scanning transmission electron microscopy (HAADF-STEM) showed their effect on the interparticle distance and nanoparticle rearrangement. Later on, we developed a process-on-substrate method to track these effects on CO2R. Cu–Ag (OAm) gave a lower on-set potential for hydrocarbon production, whereas Cu–Ag (MIPA) and Cu–Ag (NaBH4) promoted syngas production. The electrochemical impedance and surface area analysis on the well-controlled electrodes showed gradual increases in the electrical conductivity and active surface area after each surface treatment. We found that the increasing amount of the triple phase boundaries (the meeting point for the electron–electrolyte–CO2 reactant) affect the required electrode potential and eventually the C+2e̅/C2e̅ product ratio. This study highlights the importance of the electron transfer to those active sites affected by the capping agents—particularly on larger substrates that are crucial for their industrial application. |
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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 |
000592978900031 |
Publication Date |
2020-11-04 |
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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 |
|
|
| |
ISSN |
2155-5435 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
12.9 |
Times cited |
23 |
Open Access |
OpenAccess |
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Notes |
The authors also acknowledge financial support from the University Research Fund (BOF-GOA-PS ID No. 33928). S.L. has received funding from the European Union’s Horizon 2020 research and innovation program under the Marie SkłodowskaCurie Grant Agreement No. 665385. |
Approved |
Most recent IF: 12.9; 2020 IF: 10.614 |
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| |
Call Number |
EMAT @ emat @c:irua:173803 |
Serial |
6432 |
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| Permanent link to this record |
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Author |
Van Velthoven, N.; Henrion, M.; Dallenes, J.; Krajnc, A.; Bugaev, A.L.; Liu, P.; Bals, S.; Soldatov, A.; Mali, G.; De Vos, D.E. |
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Title |
S,O-functionalized metal-organic frameworks as heterogeneous single-site catalysts for the oxidative alkenylation of arenes via C- H activation |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Acs Catalysis |
Abbreviated Journal |
Acs Catal |
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| |
Volume |
10 |
Issue |
9 |
Pages |
5077-5085 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Heterogeneous single-site catalysts can combine the R precise active site design of organometallic complexes with the efficient recovery of solid catalysts. Based on recent progress on homogeneous thioether ligands for Pd-catalyzed C-H activation reactions, we here develop a scalable metal-organic framework-based heterogeneous single-site catalyst containing S,O-moieties that increase the catalytic activity of Pd(II) for the oxidative alkenylation of arenes. The structure of the Pd@MOF-808-L1 catalyst was characterized in detail via solid-state nuclear magnetic resonance spectroscopy, N-2 physisorption, and high-angle annular dark field scanning transmission electron microscopy, and the structure of the isolated palladium active sites could be identified by X-ray absorption spectroscopy. A turnover frequency (TOF) of 8.4 h(-1) was reached after 1 h of reaction time, which was 3 times higher than the TOF of standard Pd(OAc)(2), ranking Pd@MOF-808-L1 among the most active heterogeneous catalysts ever reported for the nondirected oxidative alkenylation of arenes. Finally, we showed that the single-site catalyst promotes the oxidative alkenylation of a broad range of electron-rich arenes, and the applicability of this heterogeneous system was demonstrated by the gram-scale synthesis of industrially relevant products. |
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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 |
000530090800026 |
Publication Date |
2020-04-06 |
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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 |
2155-5435 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
12.9 |
Times cited |
37 |
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. and D.E.D.V. thank the FWO for funding (1S32917N and G0F2320N). D.E.D.V. is grateful for KU Leuven's support in the frame of the CASAS Metusalem project and a C3 type project. A.K. and G.M. acknowledge the financial support from the Slovenian Research Agency (research core funding no. P1-0021 and project no. N1-0079). A.L.B and A.V.S. acknowledge Russian Science Foundation grant no. 20-43-01015 for financial support. We thank Alexander Trigub and Alexey Veligzhanin for their support during the beamtime at Kurchatov Institute. We are indebted to Elizaveta Kamyshova and Anna Pnevskaya for their valuable help during EXAFS measurements. P.L. and S.B. thank European Research Council for the ERC Consolidator Grant 815128, REALNANO. Kassem Amro and Guillaume Gracy from Sikemia are gratefully acknowledged for providing ; sygma |
Approved |
Most recent IF: 12.9; 2020 IF: 10.614 |
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| |
Call Number |
UA @ admin @ c:irua:169530 |
Serial |
6598 |
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| Permanent link to this record |
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| |
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Author |
Yang, S.; Liu, Z.; An, H.; Arnouts, S.; de Ruiter, J.; Rollier, F.; Bals, S.; Altantzis, T.; Figueiredo, M.C.; Filot, I.A.W.; Hensen, E.J.M.; Weckhuysen, B.M.; van der Stam, W. |
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Title |
Near-unity electrochemical CO₂ to CO conversion over Sn-doped copper oxide nanoparticles |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
ACS catalysis |
Abbreviated Journal |
Acs Catal |
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| |
Volume |
12 |
Issue |
24 |
Pages |
15146-15156 |
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| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
Bimetallic electrocatalysts have emerged as a viable strategy to tune the electrocatalytic CO2 reduction reaction (eCO2RR) for the selective production of valuable base chemicals and fuels. However, obtaining high product selectivity and catalyst stability remain challenging, which hinders the practical application of eCO2RR. In this work, it was found that a small doping concentration of tin (Sn) in copper oxide (CuO) has profound influence on the catalytic performance, boosting the Faradaic efficiency (FE) up to 98% for carbon monoxide (CO) at -0.75 V versus RHE, with prolonged stable performance (FE > 90%) for up to 15 h. Through a combination of ex situ and in situ characterization techniques, the in situ activation and reaction mechanism of the electrocatalyst at work was elucidated. In situ Raman spectroscopy measurements revealed that the binding energy of the crucial adsorbed *CO intermediate was lowered through Sn doping, thereby favoring gaseous CO desorption. This observation was confirmed by density functional theory, which further indicated that hydrogen adsorption and subsequent hydrogen evolution were hampered on the Sn-doped electrocatalysts, resulting in boosted CO formation. It was found that the pristine electrocatalysts consisted of CuO nanoparticles decorated with SnO2 domains, as characterized by ex situ high-resolution scanning transmission electron microscopy and X-ray photoelectron spectroscopy measurements. These pristine nanoparticles were subsequently in situ converted into a catalytically active bimetallic Sn-doped Cu phase. Our work sheds light on the intimate relationship between the bimetallic structure and catalytic behavior, resulting in stable and selective oxide-derived Sn-doped Cu electrocatalysts. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000900052400001 |
Publication Date |
2022-11-28 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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| |
Series Volume |
|
Series Issue |
|
Edition |
|
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| |
ISSN |
2155-5435 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
12.9 |
Times cited |
16 |
Open Access |
OpenAccess |
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| |
Notes |
B.M.W., S.Y., M.C.F., E.J.M.H., and W.v.d.S. acknowledge support from the Strategic UU-TU/e Alliance project ?Joint Centre for Chemergy Research?. S.B. acknowledges support from the European Research Council (ERC Consolidator grant #815128 REALNANO) . Z.L. acknowledges financial support of the China Scholarship Council and the Netherlands Organization for Scientific Research for access to computa-tional resources for carrying out the DFT calculations reported in this work. S.A. and T.A. acknowledge funding from theUniversity of Antwerp Research fund (BOF) . The authors also thank Dr. Jochem Wijten and Joris Janssens (Inorganic Chemistry and Catalysis, Utrecht University) for helpful technical support. Sander Deelen (Faculty of Science, Utrecht University) is acknowledged for the design of the in situ XRD cell. |
Approved |
Most recent IF: 12.9 |
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| |
Call Number |
UA @ admin @ c:irua:192742 |
Serial |
7325 |
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| Permanent link to this record |
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Author |
Gropp, C.; Canossa, S.; Wuttke, S.; Gándara, F.; Li, Q.; Gagliardi, L.; Yaghi, O.M. |
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Title |
Standard Practices of Reticular Chemistry |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Acs Central Science |
Abbreviated Journal |
Acs Central Sci |
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| |
Volume |
6 |
Issue |
8 |
Pages |
1255-1273 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Since 1995 when the first of metal−organic frameworks was crystallized with the strong bond approach, where metal ions are joined by charged organic linkers exemplified by carboxylates, followed by proof of their porosity in 1998 and ultrahigh porosity in 1999, a revolution in the development of their chemistry has ensued. This is being reinforced by the discovery of two- and three-dimensional covalent organic frameworks in 2005 and 2007. Currently, the chemistry of such porous, crystalline frameworks is collectively referred to as reticular chemistry, which is being practiced in over 100 countries. The involvement of researchers from various backgrounds and fields, and the vast scope of this chemistry and its societal applications, necessitate articulating the “Standard Practices of Reticular Chemistry”. |
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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 |
000566668400005 |
Publication Date |
2020-08-26 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
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| |
ISSN |
2374-7943 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
18.2 |
Times cited |
|
Open Access |
OpenAccess |
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Notes |
S.C. acknowledges the Research Foundation Flanders (FWO) for supporting his research (Project 12ZV120N). |
Approved |
Most recent IF: 18.2; 2020 IF: 7.481 |
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| |
Call Number |
EMAT @ emat @c:irua:172057 |
Serial |
6423 |
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| Permanent link to this record |
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Author |
Yang, C.; Batuk, M.; Jacquet, Q.; Rousse, G.; Yin, W.; Zhang, L.; Hadermann, J.; Abakumov, A.M.; Cibin, G.; Chadwick, A.; Tarascon, J.-M.; Grimaud, A. |
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Title |
Revealing pH-Dependent Activities and Surface Instabilities for Ni-Based Electrocatalysts during the Oxygen Evolution Reaction |
Type |
A1 Journal article |
| |
Year |
2018 |
Publication |
ACS energy letters |
Abbreviated Journal |
Acs Energy Lett |
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Volume |
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Issue |
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Pages |
2884-2890 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Multiple electrochemical processes are involved at the catalyst/ electrolyte interface during the oxygen evolution reaction (OER). With the purpose of elucidating the complexity of surface dynamics upon OER, we systematically studied two Ni-based crystalline oxides (LaNiO3−δ and La2Li0.5Ni0.5O4) and compared them with the state-of-the-art Ni−Fe (oxy)- hydroxide amorphous catalyst. Electrochemical measurements such as rotating ring disk electrode (RRDE) and electrochemical quartz microbalance microscopy (EQCM) coupled with a series of physical characterizations including transmission electron microscopy (TEM) and X-ray absorption spectroscopy (XAS) were conducted to unravel the exact pH effect on both the OER activity and the catalyst stability. We demonstrate that for Ni-based crystalline catalysts the rate for surface degradation depends on the pH and is greater than the rate for surface reconstruction. This behavior is unlike that for the amorphous Ni oxyhydroxide catalyst, which is found to be more stable and pH-independent. |
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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 |
000453805100005 |
Publication Date |
2018-11-08 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2380-8195 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
|
Times cited |
|
Open Access |
Not_Open_Access: Available from 06.11.2019
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Notes |
C.Y., J.-M.T., and A.G. acknowledge funding from the European Research Council (ERC) (FP/2014)/ERC GrantProject 670116-ARPEMA. A.G. acknowledges financial support from the ANR MIDWAY (Project ID ANR-17-CE05- 0008). We acknowledge Diamond Light Source for time awarded to the Energy Materials BAG on Beamline B18, under Proposal sp12559. |
Approved |
Most recent IF: NA |
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Call Number |
EMAT @ emat @c:irua:155046 |
Serial |
5067 |
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| Permanent link to this record |
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Author |
Sánchez-Iglesias, A.; Zhuo, X.; Albrecht, W.; Bals, S.; Liz-Marzán, L.M. |
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Title |
Tuning Size and Seed Position in Small Silver Nanorods |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
ACS materials letters |
Abbreviated Journal |
ACS Materials Lett. |
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| |
Volume |
2 |
Issue |
9 |
Pages |
1246-1250 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000571390700022 |
Publication Date |
2020-09-08 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2639-4979 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
|
Times cited |
9 |
Open Access |
OpenAccess |
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Notes |
Financial support is acknowledged from the European Commission under the Horizon 2020 Programme, by means of Grant Agreement No. 731019 (EUSMI), the ERC Consolidator Grant (No. 815128) (REALNANO), and the ERC Advanced Grant (No. 787510) (4DbioSERS). W.A. acknowledges an Individual Fellowship from the Marie Sklodowska-Curie actions (MSCA), under the EU’s Horizon 2020 program (Grant 797153, SOPMEN). This work was performed under the Maria de Maeztu Units of Excellence Program from the Spanish State Research Agency (Grant No. MDM-2017-0720).; sygma |
Approved |
Most recent IF: NA |
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Call Number |
EMAT @ emat @c:irua:171980 |
Serial |
6439 |
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Author |
Heyvaert, W.; Pedrazo-Tardajos, A.; Kadu, A.; Claes, N.; González-Rubio, G.; Liz-Marzán, L.M.; Albrecht, W.; Bals, S. |
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Title |
Quantification of the Helical Morphology of Chiral Gold Nanorods |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
ACS materials letters |
Abbreviated Journal |
ACS Materials Lett. |
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Volume |
4 |
Issue |
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Pages |
642-649 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Chirality in inorganic nanoparticles and nanostructures has gained increasing scientific interest, because of the possibility to tune their ability to interact differently with left- and right-handed circularly polarized light. In some cases, the optical activity is hypothesized to originate from a chiral morphology of the nanomaterial. However, quantifying the degree of chirality in objects with sizes of tens of nanometers is far from straightforward. Electron tomography offers the possibility to faithfully retrieve the three-dimensional morphology of nanomaterials, but only a qualitative interpretation of the morphology of chiral nanoparticles has been possible so far. We introduce herein a methodology that enables us to quantify the helicity of complex chiral nanomaterials, based on the geometrical properties of a helix. We demonstrate that an analysis at the single particle level can provide significant insights into the origin of chiroptical properties. |
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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 |
000784490000013 |
Publication Date |
2022-03-08 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2639-4979 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
|
Times cited |
11 |
Open Access |
OpenAccess |
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Notes |
S.B. and A.P.-T. gratefully acknowledge funding by the European Research Council (ERC Consolidator Grant #815128-REALNANO) the European Union’s Horizon 2020 research and innovation program under grant agreement #823717ESTEEM3. L.M.L.-M. acknowledges funding from MCIN/ AEI /10.13039/501100011033, grant # PID2020- 117779RB-I00 and the Maria de Maeztu Units of Excellence Program from the Spanish State Research Agency (Grant No. MDM-2017-0720). G.G.-R. thanks the Spanish Spanish Ministerio de Ciencia e Innovación for an FPI (BES-2014- 068972) fellowship.; SygmaSB; esteem3reported; esteem3jra |
Approved |
Most recent IF: NA |
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Call Number |
EMAT @ emat @c:irua:186959 |
Serial |
6956 |
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Author |
Vlasov, E.; Skorikov, A.; Sánchez-Iglesias, A.; Liz-Marzán, L.M.; Verbeeck, J.; Bals, S. |
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Title |
Secondary electron induced current in scanning transmission electron microscopy: an alternative way to visualize the morphology of nanoparticles |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
ACS materials letters |
Abbreviated Journal |
ACS Materials Lett. |
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Volume |
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Issue |
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Pages |
1916-1921 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Electron tomography (ET) is a powerful tool to determine the three-dimensional (3D) structure of nanomaterials in a transmission electron microscope. However, the acquisition of a conventional tilt series for ET is a time-consuming process and can therefore not provide 3D structural information in a time-efficient manner. Here, we propose surface-sensitive secondary electron (SE) imaging as an alternative to ET for the investigation of the morphology of nanomaterials. We use the SE electron beam induced current (SEEBIC) technique that maps the electrical current arising from holes generated by the emission of SEs from the sample. SEEBIC imaging can provide valuable information on the sample morphology with high spatial resolution and significantly shorter throughput times compared with ET. In addition, we discuss the contrast formation mechanisms that aid in the interpretation of SEEBIC data. |
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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 |
001006191600001 |
Publication Date |
2023-06-12 |
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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 |
2639-4979 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
|
Times cited |
1 |
Open Access |
OpenAccess |
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| |
Notes |
The funding for this project was provided by European Research Council (ERC Consolidator Grant 815128, REALNANO). J.V. acknowledges the eBEAM project, which is supported by the European Union’s Horizon 2020 research and innovation program under grant agreement no. 101017720 (FET-Proactive EBEAM). L.M.L.-M. acknowledges funding from MCIN/AEI/10.13039/501100011033 (grant # PID2020-117779RB-I00). |
Approved |
Most recent IF: NA |
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| |
Call Number |
EMAT @ emat @c:irua:197004 |
Serial |
8795 |
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| Permanent link to this record |
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| |
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Author |
Lentijo-Mozo, S.; Tan, R.P.; Garcia-Marcelot, C.; Altantzis, T.; Fazzini, P.F.; Hungria, T.; Cormary, B.; Gallagher, J.R.; Miller, J.T.; Martinez, H.; Schrittwieser, S.; Schotter, J.; Respaud, M.; Bals, S.; Van Tendeloo, G.; Gatel, C.; Soulantica, K. |
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| |
Title |
Air- and water-resistant noble metal coated ferromagnetic cobalt nanorods |
Type |
A1 Journal article |
| |
Year |
2015 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
|
| |
Volume |
9 |
Issue |
9 |
Pages |
2792-2804 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Cobalt nanorods possess ideal magnetic properties for applications requiring magnetically hard nanoparticles. However, their exploitation is undermined by their sensitivity toward oxygen and water, which deteriorates their magnetic properties. The development of a continuous metal shell inert to oxidation could render them stable, opening perspectives not only for already identified applications but also for uses in which contact with air and/or aqueous media is inevitable. However, the direct growth of a conformal noble metal shell on magnetic metals is a challenge. Here, we show that prior treatment of Co nanorods with a tin coordination compound is the crucial step that enables the subsequent growth of a continuous noble metal shell on their surface, rendering them air- and water-resistant, while conserving the monocrystallity, metallicity and the magnetic properties of the Co core. Thus, the as-synthesized coreshell ferromagnetic nanorods combine high magnetization and strong uniaxial magnetic anisotropy, even after exposure to air and water, and hold promise for successful implementation in in vitro biodiagnostics requiring probes of high magnetization and anisotropic shape. |
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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 |
000351791800055 |
Publication Date |
2015-03-03 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
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| |
ISSN |
1936-0851;1936-086X; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
13.942 |
Times cited |
25 |
Open Access |
OpenAccess |
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Notes |
312483 Esteem2; 246791 Countatoms; 335078 Colouratom; esteem2ta; ECASSara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 13.942; 2015 IF: 12.881 |
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Call Number |
c:irua:125380 c:irua:125380 |
Serial |
87 |
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| Permanent link to this record |
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Author |
Javon, E.; Gaceur, M.; Dachraoui, W.; Margeat, O.; Ackermann, J.; Ilenia Saba, M.; Delugas, P.; Mattoni, A.; Bals, S.; Van Tendeloo, G. |
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Title |
Competing forces in the self-assembly of coupled ZnO nanopyramids |
Type |
A1 Journal article |
| |
Year |
2015 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
|
| |
Volume |
9 |
Issue |
9 |
Pages |
3685-3694 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Self-assembly (SA) of nanostructures has recently gained increasing interest. A clear understanding of the process is not straightforward since SA of nanoparticles is a complex multiscale phenomenon including different driving forces. Here, we study the SA between aluminum doped ZnO nanopyramids into couples by combining inorganic chemistry and advanced electron microscopy techniques with atomistic simulations. Our results show that the SA of the coupled nanopyramids is controlled first by morphology, as coupling only occurs in the case of pyramids with well-developed facets of the basal planes. The combination of electron microscopy and atomistic modeling reveals that the coupling is further driven by strong ligandligand interaction between the bases of the pyramids as dominant force, while screening effects due to Al doping or solvent as well as corecore interaction are only minor contributions. Our combined approach provides a deeper understanding of the complex interplay between the interactions at work in the coupled SA of ZnO nanopyramids. |
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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 |
000353867000030 |
Publication Date |
2015-03-12 |
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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 |
1936-0851;1936-086X; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
13.942 |
Times cited |
21 |
Open Access |
OpenAccess |
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| |
Notes |
Esmi; 335078 Colouratom; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 13.942; 2015 IF: 12.881 |
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Call Number |
c:irua:125978 |
Serial |
434 |
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| Permanent link to this record |
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Author |
Rossell, M.D.; Abakumov, A.M.; Ramasse, Q.M.; Erni, R. |
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Title |
Direct evidence of stacking disorder in the mixed ionic-electronic conductor Sr4Fe6O12+\delta |
Type |
A1 Journal article |
| |
Year |
2013 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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| |
Volume |
7 |
Issue |
4 |
Pages |
3078-3085 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Determining the structure-to-property relationship of materials becomes particularly challenging when the material under investigation is dominated by defects and structural disorder. Knowledge on the exact atomic arrangement at the defective structure is required to understand its influence on the functional properties. However, standard diffraction techniques deliver structural information that is averaged over many unit cells. In particular, information about defects and order-disorder phenomena is contained in the coherent diffuse scattering intensity which often is difficult to uniquely interpret. Thus, the examination of the local disorder in materials requires a direct method to study their structure on the atomic level with chemical sensitivity. Using aberration-corrected scanning transmission electron microscopy in combination with atomic-resolution electron energy-loss spectroscopy, we show that the controversial structural arrangement of the Fe2O2+delta layers in the mixed ionic-electronic conducting Sr4Fe6O12+delta perovskite can be unambiguously resolved. Our results provide direct experimental evidence for the presence of a nanomixture of “ordered” and “disordered” domains in an epitaxial Sr4Fe6O12+delta thin film. The most favorable arrangement is the disordered structure and is interpreted as a randomly occurring but well-defined local shift of the Fe-O chains in the Fe2O2+delta layers. By analyzing the electron energy-loss near-edge structure of the different building blocks in the Sr4Fe6O12+delta unit cell we find that the mobile holes in this mixed ionic-electronic conducting oxide are highly localized in the Fe2O2+delta layers, which are responsible for the oxide-ion conductivity. A possible link between disorder and oxygen-ion transport along the Fe2O2+delta layers is proposed by arguing that the disorder can effectively break the oxygen diffusion pathways. |
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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 |
000318143300021 |
Publication Date |
2013-03-04 |
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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 |
1936-0851;1936-086X; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
4 |
Open Access |
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Notes |
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Approved |
Most recent IF: 13.942; 2013 IF: 12.033 |
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Call Number |
UA @ lucian @ c:irua:108476 |
Serial |
713 |
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| Permanent link to this record |
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Author |
Chen, B.; Sahin, H.; Suslu, A.; Ding, L.; Bertoni, M.I.; Peeters, F.M.; Tongay, S. |
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Title |
Environmental changes in MoTe2 excitonic dynamics by defects-activated molecular interaction |
Type |
A1 Journal article |
| |
Year |
2015 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
|
| |
Volume |
9 |
Issue |
9 |
Pages |
5326-5332 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT) |
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Abstract |
Monolayers of group VI transition metal dichalcogenides possess direct gaps in the visible spectrum with the exception of MoTe2, where its gap is suitably located in the infrared region but its stability is of particular interest, as tellurium compounds are acutely sensitive to oxygen exposure. Here, our environmental (time-dependent) measurements reveal two distinct effects on MoTe2 monolayers: For weakly luminescent monolayers, photoluminescence signal and optical contrast disappear, as if they are decomposed, but yet remain intact as evidenced by AFM and Raman measurements. In contrast, strongly luminescent monolayers retain their optical contrast for a prolonged amount of time, while their PL peak blue-shifts and PL intensity saturates to slightly lower values. Our X-ray photoelectron spectroscopy measurements and DFT calculations suggest that the presence of defects and functionalization of these defect sites with O-2 molecules strongly dictate their material properties and aging response by changing the excitonic dynamics due to deep or shallow states that are created within the optical band gap. Presented results not only shed light on environmental effects on fundamental material properties and excitonic dynamics of MoTe2 monolayers but also highlight striking material transformation for metastable 20 systems such as WTe2, silicone, and phosphorene. |
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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 |
000355383000068 |
Publication Date |
2015-04-14 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851;1936-086X; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
13.942 |
Times cited |
150 |
Open Access |
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Notes |
; This work was supported by the Arizona State University seeding program. The authors thank Hui Cai and Kedi Wu for useful discussions. We gratefully acknowledge the use of facilities at the LeRoy Eyring Center for Solid State Science at Arizona State University. This work was supported by the Flemish Science Foundation (FWO-VI) and the Methusalem Foundation of the Flemish government. H.S. is supported by a FWO Pegasus Long Marie Curie Fellowship. ; |
Approved |
Most recent IF: 13.942; 2015 IF: 12.881 |
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Call Number |
c:irua:126441 |
Serial |
1068 |
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| Permanent link to this record |
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Author |
Sanz-Ortiz, M.N.; Sentosun, K.; Bals, S.; Liz-Marzan, L.M. |
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Title |
Templated Growth of Surface Enhanced Raman Scattering -Active Branched Au Nanoparticles within Radial Mesoporous Silica Shells |
Type |
A1 Journal article |
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Year |
2015 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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| |
Volume |
9 |
Issue |
9 |
Pages |
10489-10497 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Noble metal nanoparticles are widely used as probes or substrates for surface-enhanced Raman scattering (SERS), due to their characteristic plasmon resonances in the visible and NIR spectral ranges. Aiming at obtaining a versatile system with high SERS performance we developed the synthesis of quasi-monodisperse, non-aggregated gold nanoparticles protected by radial mesoporous silica shells. The radial channels of such shells were used as templates for the growth of gold tips branching from the cores, thereby improving the plasmonic performance of the particles while favoring the localization of analyte molecules at high electric field regions: close to the tips, inside the pores. The method, which allows control over tip length, was successfully applied to various gold nanoparticle shapes, leading to materials with highly efficient SERS performance. The obtained nanoparticles are stable in ethanol and water upon thermal consolidation and can be safely stored as a powder. |
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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 |
English |
Wos |
000363915300105 |
Publication Date |
2015-09-15 |
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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 |
1936-0851;1936-086X; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
13.942 |
Times cited |
110 |
Open Access |
OpenAccess |
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Notes |
This work has been funded by the European Research Council (ERC Advanced Grant 267867 Plasmaquo and Starting Grant Colouratom). The research leading to these results has received funding from the European Union's Seventh Framework Programme (FP7/2007-2013 under grant agreement no. 312184, SACS). Help from Mert Kurttepeli is acknowledged. Pentatwinned nanorods and nanotriangles were synthesized by L. Scarabelli.; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 13.942; 2015 IF: 12.881 |
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Call Number |
c:irua:129194 |
Serial |
3947 |
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| Permanent link to this record |
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Author |
Tognalii, N.G.; Cortés, E.; Hernández-Nieves, A.D.; Carro, P.; Usaj, G.; Balseiro, C.A.; Vela, M.E.; Salvarezza, R.C.; Fainstein, A. |
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Title |
From single to multiple Ag-layer modification of Au nanocavity substrates : a tunable probe of the chemical surface-enhanced Raman scattering mechanism |
Type |
A1 Journal article |
| |
Year |
2011 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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| |
Volume |
5 |
Issue |
7 |
Pages |
5433-5443 |
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Keywords |
A1 Journal article; Condensed Matter Theory (CMT) |
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Abstract |
We present experimental and computational results that enlighten the mechanisms underlying the chemical contribution to surface-enhanced Raman scattering (SERS). Gold void metallic arrays electrochemically covered either by a Ag monolayer or 10100 Ag layers were modified with a self-assembled monolayer of 4-mercaptopyridine as a molecular Raman probe displaying a rich and unexpected Raman response. A resonant increase of the Raman intensity in the red part of the spectrum is observed that cannot be related to plasmon excitations of the cavity-array. Notably, we find an additional 1020 time increase of the SERS amplification upon deposition of a single Ag layer on the Au substrate, which is, however, almost quenched upon deposition of 10 atomic layers. Further deposition of 100 atomic Ag layers results in a new increase of the SERS signal, consistent with the improved plasmonic efficiency of Ag bulk-like structures. The SERS response as a function of the Ag layer thickness is analyzed in terms of ab initio calculations and a microscopic model for the SERS chemical mechanism based on a resonant charge transfer process between the molecular HOMO state and the Fermi level in the metal surface. We find that a rearrangement of the electronic charge density related to the presence of the Ag monolayer in the Au/Ag/molecule complex causes an increase in the distance between the HOMO center of charge and the metallic image plane that is responsible for the variation of Raman enhancement between the studied substrates. Our results provide a general platform for studying the chemical contribution to SERS, and for enhancing the Raman efficiency of tailored Au-SERS templates through electrochemical modification with Ag films. |
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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 |
000293035200019 |
Publication Date |
2011-06-15 |
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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 |
1936-0851;1936-086X; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
13.942 |
Times cited |
26 |
Open Access |
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Notes |
; We acknowledge financial support from ANPCyT (Argentina, PICT08-1617, PICT08-2236, PICT06-621, PICT-CNPQ-08-0019, PAE 22711, PICT06-01061, PICT06-483) and Project CTQ2008-06017/BQU, Spain. N.G.T, E.C., A.D.H.N., R.C.S, G.U., C.A.B., and A.F. are also at CONICET. M.E.V. is a member of the research career of CIC BsAs. R.C.S., C.A.B., and A.F. are Guggenheim Foundation Fellows. We would like to thank Dr. M. H. Fonticelli for fruitful discussions on the electrochemical measurements and Dr. H. Pastoriza for the help with the SEM measurements. ; |
Approved |
Most recent IF: 13.942; 2011 IF: 11.421 |
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Call Number |
UA @ lucian @ c:irua:91775 |
Serial |
1285 |
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Author |
Sánchez-Iglesias, A.; Grzelczak, M.; Altantzis, T.; Goris, B.; Pérez-Juste, J.; Bals, S.; Van Tendeloo, G.; Donaldson, S.H.; Chmelka, B.F.; Israelachvili, J.N.; Liz-Marzán, L.M.; |
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Title |
Hydrophobic interactions modulate self-assembly of nanoparticles |
Type |
A1 Journal article |
| |
Year |
2012 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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| |
Volume |
6 |
Issue |
12 |
Pages |
11059-11065 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Hydrophobic interactions constitute one of the most important types of nonspecific interactions in biological systems, which emerge when water molecules rearrange as two hydrophobic species come close to each other. The prediction of hydrophobic interactions at the level of nanoparticles (Brownian objects) remains challenging because of uncontrolled diffusive motion of the particles. We describe here a general methodology for solvent-induced, reversible self-assembly of gold nanoparticles into 3D clusters with well-controlled sizes. A theoretical description of the process confirmed that hydrophobic interactions are the main driving force behind nanoparticle aggregation. |
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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 |
000312563600070 |
Publication Date |
2012-11-28 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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| |
ISSN |
1936-0851;1936-086X; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
13.942 |
Times cited |
311 |
Open Access |
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Notes |
267867 Plasma Quo; 246791 Countatoms; 262348 Esmi |
Approved |
Most recent IF: 13.942; 2012 IF: 12.062 |
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Call Number |
UA @ lucian @ c:irua:105292 |
Serial |
1538 |
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| Permanent link to this record |
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Author |
Quintana, M.; López, A.M.; Rapino, S.; Toma, F.M.; Iurlo, M.; Carraro, M.; Sartorel, A.; Maccato, C.; Ke, X.; Bittencourt, C.; Da Ros, T.; Van Tendeloo, G.; Marcaccio, M.; Paolucci, F.; Prato, M.; Bonchio, M.; |
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Title |
Knitting the catalytic pattern of artificial photosynthesis to a hybrid graphene nanotexture |
Type |
A1 Journal article |
| |
Year |
2013 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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| |
Volume |
7 |
Issue |
1 |
Pages |
811-817 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
The artificial leaf project calls for new materials enabling multielectron catalysis with minimal overpotential, high turnover frequency, and long-term stability. Is graphene a better material than carbon nanotubes to enhance water oxidation catalysis for energy applications? Here we show that functionalized graphene with a tailored distribution of polycationic, quaternized, ammonium pendants provides an sp(2) carbon nanoplatform to anchor a totally inorganic tetraruthenate catalyst, mimicking the oxygen evolving center of natural PSII. The resulting hybrid material displays oxygen evolution at overpotential as low as 300 mV at neutral pH with negligible loss of performance after 4 h testing. This multilayer electroactive asset enhances the turnover frequency by 1 order of magnitude with respect to the isolated catalyst, and provides a definite up-grade of the carbon nanotube material, with a similar surface functionalization. Our innovation is based on a noninvasive, synthetic protocol for graphene functionalization that goes beyond the ill-defined oxidation-reduction methods, allowing a definite control of the surface properties. |
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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 |
000314082800088 |
Publication Date |
2012-12-17 |
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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 |
1936-0851;1936-086X; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
13.942 |
Times cited |
69 |
Open Access |
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| |
Notes |
246791 COUNTATOMS; 262348 ESMI; ESF Cost Action NanoTP MP0901 |
Approved |
Most recent IF: 13.942; 2013 IF: 12.033 |
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| |
Call Number |
UA @ lucian @ c:irua:107707 |
Serial |
1766 |
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| Permanent link to this record |
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Author |
Quintana, M.; Ke, X.; Van Tendeloo, G.; Meneghetti, M.; Bittencourt, C.; Prato, M. |
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Title |
Light-induced selective deposition of Au nanoparticles on single-wall carbon nanotubes |
Type |
A1 Journal article |
| |
Year |
2010 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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| |
Volume |
4 |
Issue |
10 |
Pages |
6105-6113 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Novel applications of single-walled carbon nanotubes (SWNT) rely on the development of new strategies to make them easier to handle without affecting their structural properties. In this work, we have selectively deposited Au nanoparticles (Au NP) on SWNT assisted by UV light irradiation. XPS analysis and UV-vis spectroscopy indicate that the deposition occurs at the defects generated after oxidation of the SWNT. By addition of n-dodecylthiol, the separation of oxidized tubes with Au NP (Au-ox-SWNT) from tubes devoid of Au NP (bare tubes, b-SWNT) was achieved. Raman and UV-vis-NIR spectra indicate that UV irradiation induces a faster nucleation of Au NP on metallic SWNT. This new technique can be useful for the preparation of nanohybrid composites with enhanced properties, as increased thermal stability, and to obtain purified SWNT. |
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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 |
000283453700081 |
Publication Date |
2010-09-24 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851;1936-086X; |
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 |
26 |
Open Access |
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Notes |
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Approved |
Most recent IF: 13.942; 2010 IF: 9.865 |
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Call Number |
UA @ lucian @ c:irua:99202 |
Serial |
1819 |
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| Permanent link to this record |
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Author |
Walter, A.L.; Sahin, H.; Jeon, K.J.; Bostwick, A.; Horzum, S.; Koch, R.; Speck, F.; Ostler, M.; Nagel, P.; Merz, M.; Schupler, S.; Moreschini, L.; Chang, Y.J.; Seyller, T.; Peeters, F.M.; Horn, K.; Rotenberg, E.; |
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Title |
Luminescence, patterned metallic regions, and photon-mediated electronic changes in single-sided fluorinated graphene sheets |
Type |
A1 Journal article |
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Year |
2014 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
8 |
Issue |
8 |
Pages |
7801-7808 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT) |
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Abstract |
Single-sided fluorination has been predicted to open an electronic band gap in graphene and to exhibit unique electronic and magnetic properties; however, this has not been substantiated by experimental reports. Our comprehensive experimental and theoretical study of this material on a SiC(0001) substrate shows that single-sided fluorographene exhibits two phases, a stable one with a band gap of similar to 6 eV and a metastable one, induced by UV irradiation, with a band gap of similar to 2.5 eV. The metastable structure, which reverts to the stable “ground-state” phase upon annealing under emission of blue light, in our view is induced by defect states, based on the observation of a nondispersive electronic state at the top of the valence band, not unlike that found in organic molecular layers. Our structural data show that the stable C2F ground state has a “boat” structure, in agreement with our X-ray magnetic circular dichroism data, which show the absence of an ordered magnetic phase. A high flux of UV or X-ray photons removes the fluorine atoms, demonstrating the possibility of lithographically patterning conducting regions into an otherwise semiconducting 2D material. |
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Language |
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Wos |
000340992300025 |
Publication Date |
2014-08-09 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851;1936-086X; |
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 |
23 |
Open Access |
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Notes |
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Approved |
Most recent IF: 13.942; 2014 IF: 12.881 |
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Call Number |
UA @ lucian @ c:irua:119263 |
Serial |
1857 |
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Author |
Felten, A.; Gillon, X.; Gulas, M.; Pireaux, J.-J.; Ke, X.; Van Tendeloo, G.; Bittencourt, C.; Najafi, E.; Hitchcock, A.P. |
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Title |
Measuring point defect density in individual carbon nanotubes using polarization-dependent X-ray microscopy |
Type |
A1 Journal article |
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Year |
2010 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
4 |
Issue |
8 |
Pages |
4431-4436 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
The presence of defects in carbon nanotubes strongly modifies their electrical, mechanical, and chemical properties. It was long thought undesirable, but recent experiments have shown that introduction of structural defects using ion or electron irradiation can lead to novel nanodevices. We demonstrate a method for detecting and quantifying point defect density in individual carbon nanotubes (CNTs) based on measuring the polarization dependence (linear dichroism) of the C 1s → π* transition at specific locations along individual CNTs with a scanning transmission X-ray microscope (STXM). We show that STXM can be used to probe defect density in individual CNTs with high spatial resolution. The quantitative relationship between ion dose, nanotube diameter, and defect density was explored by purposely irradiating selected sections of nanotubes with kiloelectronvolt (keV) Ga+ ions. Our results establish polarization-dependent X-ray microscopy as a new and very powerful characterization technique for carbon nanotubes and other anisotropic nanostructures. |
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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 |
000281052700014 |
Publication Date |
2010-07-07 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851;1936-086X; |
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 |
26 |
Open Access |
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Notes |
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Approved |
Most recent IF: 13.942; 2010 IF: 9.865 |
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Call Number |
UA @ lucian @ c:irua:84734 |
Serial |
1966 |
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Author |
Yan, Y.; Zhou, X.; Jin, H.; Li, C.-Z.; Ke, X.; Van Tendeloo, G.; Liu, K.; Yu, D.; Dressel, M.; Liao, Z.-M. |
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Title |
Surface-Facet-Dependent Phonon Deformation Potential in Individual Strained Topological Insulator Bi2Se3 Nanoribbons |
Type |
A1 Journal article |
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Year |
2015 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
9 |
Issue |
9 |
Pages |
10244-10251 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Strain is an important method to tune the properties of topological insulators. For example, compressive strain can induce superconductivity in Bi2Se3 bulk material. Topological insulator nanostructures are the superior candidates to utilize the unique surface states due to the large surface to volume ratio. Therefore, it is highly desirable to monitor the local strain effects in individual topological insulator nanostructures. Here, we report the systematical micro-Raman spectra of single strained Bi2Se3 nanoribbons with different thicknesses and different surface facets, where four optical modes are resolved in both Stokes and anti-Stokes Raman spectral lines. A striking anisotropy of the strain dependence is observed in the phonon frequency of strained Bi2Se3 nanoribbons grown along the ⟨112̅0⟩ direction. The frequencies of the in-plane Eg2 and out-of-plane A1g1 modes exhibit a nearly linear blue-shift against bending strain when the nanoribbon is bent along the ⟨112̅0⟩ direction with the curved {0001} surface. In this case, the phonon deformation potential of the Eg2 phonon for 100 nm-thick Bi2Se3 nanoribbon is up to 0.94 cm–1/%, which is twice of that in Bi2Se3 bulk material (0.52 cm–1/%). Our results may be valuable for the strain modulation of individual topological insulator nanostructures. |
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Corporate Author |
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Place of Publication |
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Editor |
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Language |
English |
Wos |
000363915300079 |
Publication Date |
2015-09-12 |
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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 |
1936-0851;1936-086X; |
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 |
14 |
Open Access |
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Notes |
Y.Y. would like to thank Xuewen Fu for helpful discussions. This work was supported by MOST (Nos. 2013CB934600, 2013CB932602) and NSFC (Nos. 11274014, 11234001). |
Approved |
Most recent IF: 13.942; 2015 IF: 12.881 |
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Call Number |
c:irua:129216 |
Serial |
3963 |
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Author |
Chen, J.J.; Wang, Q.; Meng, J.; Ke, X.; Van Tendeloo, G.; Bie, Y.Q.; Liu, J.; Liu, K.; Liao, Z.M.; Sun, D.; Yu, D.; |
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Title |
Photovoltaic effect and evidence of carrier multiplication in graphene vertical homojunctions with asymmetrical metal contacts |
Type |
A1 Journal article |
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Year |
2015 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
9 |
Issue |
9 |
Pages |
8851-8858 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Graphene exhibits exciting potentials for high-speed wideband photodetection and high quantum efficiency solar energy harvest because of its broad spectral absorption, fast photoelectric response, and potential carrier multiplication. Although photocurrent can be generated near a metalgraphene interface in lateral devices, the photoactive area is usually limited to a tiny one-dimensional line-like interface region. Here, we report photoelectric devices based on vertical graphene two-dimensional homojunction, which is fabricated via vertically stacking four graphene monolayers with asymmetric metal contacts. The devices show excellent photovoltaic output with excitation wavelength ranging from visible light to mid-infrared. The wavelength dependence of the internal quantum efficiency gives direct evidence of the carrier multiplication effect in graphene. The simple fabrication process, easy scale-up, large photoresponsive active area, and broadband response of the vertical graphene device are very promising for practical applications in optoelectronics and photovoltaics. |
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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 |
000361935800023 |
Publication Date |
2015-08-15 |
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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 |
1936-0851;1936-086X; |
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 |
11 |
Open Access |
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Notes |
246791 Countatoms |
Approved |
Most recent IF: 13.942; 2015 IF: 12.881 |
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Call Number |
c:irua:127689 |
Serial |
2615 |
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| Permanent link to this record |
