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Records |
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Author |
Choukroun, D.; Daems, N.; Kenis, T.; Van Everbroeck, T.; Hereijgers, J.; Altantzis, T.; Bals, S.; Cool, P.; Breugelmans, T. |
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Title |
Bifunctional nickel-nitrogen-doped-carbon-supported copper electrocatalyst for CO2 reduction |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Journal Of Physical Chemistry C |
Abbreviated Journal |
J Phys Chem C |
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Volume |
124 |
Issue |
124 |
Pages |
1369-1381 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
Bifunctionality is a key feature of many industrial catalysts, supported metal clusters and particles in particular, and the development of such catalysts for the CO2 reduction reaction (CO2RR) to hydrocarbons and alcohols is gaining traction in light of recent advancements in the field. Carbon-supported Cu nanoparticles are suitable candidates for integration in the state-of-the-art reaction interfaces, and here, we propose, synthesize, and evaluate a bifunctional Ni–N-doped-C-supported Cu electrocatalyst, in which the support possesses active sites for selective CO2 conversion to CO and Cu nanoparticles catalyze either the direct CO2 or CO reduction to hydrocarbons. In this work, we introduce the scientific rationale behind the concept, its applicability, and the challenges with regard to the catalyst. From the practical aspect, the deposition of Cu nanoparticles onto carbon black and Ni–N–C supports via an ammonia-driven deposition precipitation method is reported and explored in more detail using X-ray diffraction, thermogravimetric analysis, and hydrogen temperature-programmed reduction. High-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and energy-dispersive X-ray spectroscopy (EDXS) give further evidence of the presence of Cu-containing nanoparticles on the Ni–N–C supports while revealing an additional relationship between the nanoparticle’s composition and the electrode’s electrocatalytic performance. Compared to the benchmark carbon black-supported Cu catalysts, Ni–N–C-supported Cu delivers up to a 2-fold increase in the partial C2H4 current density at −1.05 VRHE (C1/C2 = 0.67) and a concomitant 10-fold increase of the CO partial current density. The enhanced ethylene production metrics, obtained by virtue of the higher intrinsic activity of the Ni–N–C support, point out toward a synergistic action between the two catalytic functionalities. |
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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 |
000508467700015 |
Publication Date |
2020-01-07 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447; 1932-7455 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.7 |
Times cited |
24 |
Open Access |
OpenAccess |
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Notes |
; N.D. acknowledges sponsoring from the research foundation of Flanders (FWO) in the frame of a postdoctoral grant (12Y3919N N.D.). J.H. greatly acknowledges the Research Foundation Flanders (FWO) for support through a postdoctoral fellowship (28761). T.V.E. and P.C. acknowledge financial support from the EU-Partial-PGMs project (H2020NMP-686086). The authors also acknowledge financial support from the university research fund (BOF-GOA PS ID No. 33928). ; |
Approved |
Most recent IF: 3.7; 2020 IF: 4.536 |
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Call Number |
UA @ admin @ c:irua:165326 |
Serial |
6286 |
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Permanent link to this record |
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Author |
Yang, S.; Liu, Z.; An, H.; Arnouts, S.; de Ruiter, J.; Rollier, F.; Bals, S.; Altantzis, T.; Figueiredo, M.C.; Filot, I.A.W.; Hensen, E.J.M.; Weckhuysen, B.M.; van der Stam, W. |
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Title |
Near-unity electrochemical CO₂ to CO conversion over Sn-doped copper oxide nanoparticles |
Type |
A1 Journal article |
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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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Corporate Author |
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Place of Publication |
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Editor |
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Wos |
000900052400001 |
Publication Date |
2022-11-28 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2155-5435 |
ISBN |
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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 |
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 |
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 |
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Year |
2020 |
Publication |
Acs Catalysis |
Abbreviated Journal |
Acs Catal |
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Volume |
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Issue |
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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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Corporate Author |
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Place of Publication |
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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 |
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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 |
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 |
Beckwee, E.J.; Watson, G.; Houlleberghs, M.; Arenas Esteban, D.; Bals, S.; Van Der Voort, P.; Breynaert, E.; Martens, J.; Baron, G.V.; Denayer, J.F.M. |
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Title |
Enabling hydrate-based methane storage under mild operating conditions by periodic mesoporous organosilica nanotubes |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Heliyon |
Abbreviated Journal |
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Volume |
9 |
Issue |
7 |
Pages |
e17662-14 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Biomethane is a renewable natural gas substitute produced from biogas. Storage of this sustainable energy vector in confined clathrate hydrates, encapsulated in the pores of a host material, is a highly promising avenue to improve storage capacity and energy efficiency. Herein, a new type of periodic mesoporous organosilica (PMO) nanotubes, referred to as hollow ring PMO (HR-PMO), capable of promoting methane clathrate hydrate formation under mild working conditions (273 K, 3.5 MPa) and at high water loading (5.1 g water/g HR-PMO) is reported. Gravimetric uptake measurements reveal a steep single-stepped isotherm and a noticeably high methane storage capacity (0.55 g methane/g HR-PMO; 0.11 g methane/g water at 3.5 MPa). The large working capacity throughout consecutive pressure-induced clathrate hydrate formationdissociation cycles demonstrates the material's excellent recyclability (97% preservation of capacity). Supported by ex situ cryo-electron tomography and x-ray diffraction, HR-PMO nanotubes are hypothesized to promote clathrate hydrate nucleation and growth by distribution and confinement of water in the mesopores of their outer wall, along the central channels of the nanotubes and on the external nanotube surface. These findings showcase the potential for application of organosilica materials with hierarchical and interconnected pore systems for pressure-based storage of biomethane in confined clathrate hydrates. |
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Thesis |
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Wos |
001056264100001 |
Publication Date |
2023-06-28 |
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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 |
2405-8440 |
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 |
4 |
Open Access |
OpenAccess |
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Notes |
E.J.B., G.W. and M.H. contributed equally to this work. M.H. acknowledges FWO for an FWO-SB fellowship. All authors acknowledge VLAIO for Moonshot funding (ARCLATH, n ? HBC.2019.0110, ARCLATH2, n ? HBC.2021.0254) . J.A.M. acknowledges the Flemish Government for long-term structural funding (Methusalem) and department EWI for infrastructure investment via the Hermes Fund (AH.2016.134) . NMRCoRe acknowledges the Flemish government, department EWI for financial support as International Research Infrastructure (I001321N: Nuclear Magnetic Resonance Spectroscopy Platform for Molecular Water Research) . J.A.M. acknowledges the European Research Council (ERC) for an Advanced Research Grant under the European Union's Horizon 2020 research and innovation program under grant agreement No. 834134 (WATUSO) . S.B acknowledges financial support by the Research Foundation Flanders (FWO grant G.0381.16N) . This project also received funding from the European Union's Horizon 2020 research and innovation program under grant agreement No 731019 (EUSMI) and No 815128 (REALNANO) . |
Approved |
Most recent IF: NA |
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Call Number |
UA @ admin @ c:irua:199249 |
Serial |
8862 |
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Permanent link to this record |
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Author |
Monticelli, O.; Musina, Z.; Russo, S.; Bals, S. |
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Title |
On the use of TEM in the characterization of nanocomposites |
Type |
A1 Journal article |
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Year |
2007 |
Publication |
Materials letters |
Abbreviated Journal |
Mater Lett |
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Volume |
61 |
Issue |
16 |
Pages |
3446-3450 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Both an organically modified commercial clay of montmorillonite type (MMT) and its nanocomposites, based either on polyamide 6 (PA6) or an epoxy resin, as matrix polymer, have been characterized by transmission electron microscopy (TEM). Sample micrographs, taken at increasing exposure times (t(e)), have shown the gradual disappearance of clay layers, because of an amorphisation of the MMT crystalline structures caused by prolonged sample exposure to electron beam. Indeed, the above phenomenon, which is mostly evident in the case of intercalated nanocomposites, makes the detection of the layered silicate dispersion in the polymer matrix rather difficult and compels to perform TEM measurements using very short exposure times. Moreover, the microscopy accelerating voltage has turned out to affect sample stability; namely, when decreasing the above parameter, the disappearance of clay structure occurs at lower exposure times. (C) 2006 Elsevier B.V. All rights reserved. |
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Place of Publication |
Amsterdam |
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Wos |
000247146100034 |
Publication Date |
2006-12-06 |
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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 |
0167-577X; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
2.572 |
Times cited |
28 |
Open Access |
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Notes |
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Approved |
Most recent IF: 2.572; 2007 IF: 1.625 |
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Call Number |
UA @ lucian @ c:irua:64757 |
Serial |
2460 |
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Permanent link to this record |
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Author |
Goris, B.; van Huis, M.A.; Bals, S.; Zandbergen, H.W.; Manna, L.; Van Tendeloo, G. |
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Title |
Thermally induced structural and morphological changes of CdSe/CdS octapods |
Type |
A1 Journal article |
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Year |
2012 |
Publication |
Small |
Abbreviated Journal |
Small |
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Volume |
8 |
Issue |
6 |
Pages |
937-942 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Branched nanostructures are of great interest because of their promising optical and electronic properties. For successful and reliable integration in applications such as photovoltaic devices, the thermal stability of the nanostructures is of major importance. Here the different domains (CdSe cores, CdS pods) of the heterogeneous octapods are shown to have different thermal stabilities, and heating is shown to induce specific shape changes. The octapods are heated from room temperature to 700 °C, and investigated using (analytical and tomographic) transmission electron microscopy (TEM). At low annealing temperatures, pure Cd segregates in droplets at the outside of the octapods, indicating non-stochiometric composition of the octapods. Furthermore, the tips of the pods lose their faceting and become rounded. Further heating to temperatures just below the sublimation temperature induces growth of the zinc blende core at the expense of the wurtzite pods. At higher temperatures, (500700 °C), sublimation of the octapods is observed in real time in the TEM. Three-dimensional tomographic reconstructions reveal that the four pods pointing into the vacuum have a lower thermal stability than the four pods that are in contact with the support. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
Weinheim |
Editor |
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Language |
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Wos |
000301718800021 |
Publication Date |
2012-01-31 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1613-6810; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
8.643 |
Times cited |
20 |
Open Access |
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Notes |
Fwo; Esteem 026019 |
Approved |
Most recent IF: 8.643; 2012 IF: 7.823 |
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Call Number |
UA @ lucian @ c:irua:95040 |
Serial |
3633 |
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Permanent link to this record |
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Author |
Smith, J.D.; Bladt, E.; Burkhart, J.A.C.; Winckelmans, N.; Koczkur, K.M.; Ashberry, H.M.; Bals, S.; Skrabalak, S.E. |
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Title |
Defect-directed growth of symmetrically branched metal nanocrystals |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Angewandte Chemie-International Edition |
Abbreviated Journal |
Angew Chem Int Edit |
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Volume |
59 |
Issue |
59 |
Pages |
943-950 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Branched plasmonic nanocrystals (NCs) have attracted much attention due to electric field enhancements at their tips. Seeded growth provides routes to NCs with defined branching patterns and, in turn, near-field distributions with defined symmetries. Here, a systematic analysis was undertaken in which seeds containing different distributions of planar defects were used to grow branched NCs in order to understand how their distributions direct the branching. Characterization of the products by multimode electron tomography and analysis of the NC morphologies at different overgrowth stages indicate that the branching patterns are directed by the seed defects, with the emergence of branches from the seed faces consistent with minimizing volumetric strain energy at the expense of surface energy. These results contrast with growth of branched NCs from single-crystalline seeds and provide a new platform for the synthesis of symmetrically branched plasmonic NCs. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000498760200001 |
Publication Date |
2019-11-13 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1433-7851; 0570-0833 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
16.6 |
Times cited |
23 |
Open Access |
OpenAccess |
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Notes |
; The authors thank Samantha Harvey for her initial observations of branched structures, Alexander Chen for his help with SAED, the staff of the Nanoscale Characterization Facility (Dr. Yi Yi), Electron Microscopy Center (Dr. David Morgan and Dr. Barry Stein), and Molecular Structure Center at Indiana University. J.S. recognizes a fellowship provided by the Indiana Space Grant Consortium. E.B. acknowledges a post-doctoral grant from the Research Foundation Flanders (FWO, Belgium). This project has received funding to S.E.S. from the U.S. National Science Foundation (award numbers: 1602476 and 1904499) and Research Corporation for Scientific Advancement (2017 Frontiers in Research Excellence and Discovery Award) as well as to S.B. from the European Union's Horizon 2020 research and innovation program under grant agreement No 731019 (EUSMI) and No 815128 (REALNANO). ; sygma |
Approved |
Most recent IF: 16.6; 2020 IF: 11.994 |
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Call Number |
UA @ admin @ c:irua:165124 |
Serial |
6293 |
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Permanent link to this record |
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Author |
Smith, J.D.; Bladt, E.; Burkhart, J.A.C.; Winckelmans, N.; Koczkur, K.M.; Ashberry, H.M.; Bals, S.; Skrabalak, S.E. |
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Title |
Defect‐Directed Growth of Symmetrically Branched Metal Nanocrystals |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Angewandte Chemie (International ed. Print) |
Abbreviated Journal |
Angew. Chem. |
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Volume |
132 |
Issue |
132 |
Pages |
953-960 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Branched plasmonic nanocrystals (NCs) have attracted much attention due to electric field enhancements at their tips. Seeded growth provides routes to NCs with defined branching patterns and, in turn, near‐field distributions with defined symmetries. Here, a systematic analysis was undertaken in which seeds containing different distributions of planar defects were used to grow branched NCs in order to understand how their distributions direct the branching. Characterization of the products by multimode electron tomography and analysis of the NC morphologies at different overgrowth stages indicate that the branching patterns are directed by the seed defects, with the emergence of branches from the seed faces consistent with minimizing volumetric strain energy at the expense of surface energy. These results contrast with growth of branched NCs from single‐crystalline seeds and provide a new platform for the synthesis of symmetrically branched plasmonic NCs. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000505279500063 |
Publication Date |
2020-01-07 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0044-8249 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
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Times cited |
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Open Access |
OpenAccess |
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Notes |
The authors thank Samantha Harvey for her initial observations of branched structures, Alexander Chen for his help with SAED, the staff of the Nanoscale Characterization Facility (Dr. Yi Yi),Electron Microscopy Center (Dr. David Morgan and Dr. Barry Stein), and Molecular Strucre Center at Indiana University. J.S. recognizes a fellowship provided by the Indiana Space Grant Consortium. E. B. acknowledges a post-doctoral grant from the Research Foundation Flanders (FWO, Belgium). This project has received funding from the National Science Foundation (award number: 1602476), Research Corporation for Scietific Advancement (2017 Frontiers in Research Excellence and Discovery Award), and the European Union’s Horizon 2020 research and innovation program under grant agreement No 731019 (EUSMI) and No 815128 (REALNANO).; sygma |
Approved |
Most recent IF: NA |
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Call Number |
EMAT @ emat @c:irua:166581 |
Serial |
6336 |
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Permanent link to this record |
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Author |
Ustarroz, J.; Altantzis, T.; Hammons, J.A.; Hubin, A.; Bals, S.; Terryn, H. |
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Title |
The role of nanocluster aggregation, coalescence, and recrystallization in the electrochemical deposition of platinum nanostructures |
Type |
A1 Journal article |
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Year |
2014 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
26 |
Issue |
7 |
Pages |
2396-2406 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
By using an optimized characterization approach that combines aberration-corrected transmission electron microscopy, electron tomography, and in situ ultrasmall angle X-ray scattering (USAXS), we show that the early stages of Pt electrochemical growth on carbon substrates may be affected by the aggregation, self-alignment, and partial coalescence of nanoclusters of d ≈ 2 nm. The morphology of the resulting nanostructures depends on the degree of coalescence and recrystallization of nanocluster aggregates, which in turn depends on the electrodeposition potential. At low overpotentials, a self-limiting growth mechanism may block the epitaxial growth of primary nanoclusters and results in loose dendritic aggregates. At more negative potentials, the extent of nanocluster coalescence and recrystallization is larger and further growth by atomic incorporation may be allowed. On one hand, this suggests a revision of the VolmerWeber island growth mechanism. Whereas this theory has traditionally assumed direct attachment as the only growth mechanism, it is suggested that nanocluster self-limiting growth, aggregation, and coalescence should also be taken into account during the early stages of nanoscale electrodeposition. On the other hand, depending on the deposition potential, ultrahigh porosities can be achieved, turning electrodeposition in an ideal process for highly active electrocatalyst production without the need of using high surface area carbon supports. |
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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 |
Washington, D.C. |
Editor |
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|
Language |
|
Wos |
000334572300026 |
Publication Date |
2014-03-10 |
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Series Editor |
|
Series Title |
|
Abbreviated Series Title |
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|
|
Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
0897-4756;1520-5002; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
9.466 |
Times cited |
55 |
Open Access |
Not_Open_Access |
|
|
Notes |
FWO; contract no. FWOAL527 |
Approved |
Most recent IF: 9.466; 2014 IF: 8.354 |
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|
Call Number |
UA @ lucian @ c:irua:116956 |
Serial |
2916 |
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Permanent link to this record |
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Author |
Van Velthoven, N.; Waitschat, S.; Chavan, S.M.; Liu, P.; Smolders, S.; Vercammen, J.; Bueken, B.; Bals, S.; Lillerud, K.P.; Stock, N.; De Vos, D.E. |
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Title |
Single-site metal-organic framework catalysts for the oxidative coupling of arenes via C-H/C-H activation |
Type |
A1 Journal article |
|
Year |
2019 |
Publication |
Chemical science |
Abbreviated Journal |
Chem Sci |
|
|
Volume |
10 |
Issue |
10 |
Pages |
3616-3622 |
|
|
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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|
Abstract |
C-H activation reactions are generally associated with relatively low turnover numbers (TONs) and high catalyst concentrations due to a combination of low catalyst stability and activity, highlighting the need for recyclable heterogeneous catalysts with stable single-atom active sites. In this work, several palladium loaded metal-organic frameworks (MOFs) were tested as single-site catalysts for the oxidative coupling of arenes (e.g. o-xylene) via C-H/C-H activation. Isolation of the palladium active sites on the MOF supports reduced Pd(0) aggregate formation and thus catalyst deactivation, resulting in higher turnover numbers (TONs) compared to the homogeneous benchmark reaction. Notably, a threefold higher TON could be achieved for palladium loaded MOF-808 due to increased catalyst stability and the heterogeneous catalyst could efficiently be reused, resulting in a cumulative TON of 1218 after three runs. Additionally, the palladium single-atom active sites on MOF-808 were successfully identified by Fourier transform infrared (FTIR) and extended X-ray absorption fine structure (EXAFS) spectroscopy. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000463759100017 |
Publication Date |
2019-02-18 |
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Series Editor |
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Series Title |
|
Abbreviated Series Title |
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|
Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
2041-6520 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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|
Impact Factor |
8.668 |
Times cited |
68 |
Open Access |
OpenAccess |
|
|
Notes |
; The research leading to these results has received funding from the NMBP-01-2016 Program of the European Union's Horizon 2020 Framework Program H2020/2014-2020/under grant agreement no. [720996]. N. V. V., S. S., J. V., B. B. and D. E. D. V. thank the FWO for funding (SB, Aspirant and postdoctoral grants). The electron microscopy work was supported by FWO funding G038116. D. E. D. V. is grateful for KU Leuven support in the frame of the CASAS Metusalem project and a C3 type project. The XAS experiments were performed on beamline BM26A at the European Synchrotron Radiation Facility (ESRF), Grenoble, France. We are grateful to D. Banerjee at the ESRF for providing assistance in using beamline BM26A. Johnson Matthey and S. Bennett are gratefully acknowledged for providing Smopex-102. ; |
Approved |
Most recent IF: 8.668 |
|
|
Call Number |
UA @ admin @ c:irua:159403 |
Serial |
5259 |
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Permanent link to this record |
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Author |
He, Z.; Ke, X.; Bals, S.; Van Tendeloo, G. |
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Title |
Direct evidence for the existence of multi-walled carbon nanotubes with hexagonal cross-sections |
Type |
A1 Journal article |
|
Year |
2012 |
Publication |
Carbon |
Abbreviated Journal |
Carbon |
|
|
Volume |
50 |
Issue |
7 |
Pages |
2524-2529 |
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|
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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|
Abstract |
Carbon nanotubes (CNTs) with a polygonal cross-section have been paid increasing attention since their three-dimensional structure is related to specific physical properties, which are found to be different in comparison to CNTs with a circular cross-section. Here, we report the existence of novel multi-walled CNTs yielding walls with a rounded-hexagonal configuration. This structure was directly confirmed for the first time by both cross-sectional transmission electron microscopy and electron tomography. The morphology of the Fe catalytic particle also exhibits hexagonal characteristics, and is proposed as the origin of the formation of the rounded-hexagonal walls of the CNT. This observation is of great importance with respect to the design of polygonal (such as pentagonal or hexagonal) cross-sectional CNTs. By controlling the morphology of the catalytic nanoparticles it will be possible to grow CNTs with desired electronic and mechanical properties. |
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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 |
Oxford |
Editor |
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Language |
|
Wos |
000303038400015 |
Publication Date |
2012-02-06 |
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Series Editor |
|
Series Title |
|
Abbreviated Series Title |
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|
Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
0008-6223; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
6.337 |
Times cited |
8 |
Open Access |
|
|
|
Notes |
Fwo |
Approved |
Most recent IF: 6.337; 2012 IF: 5.868 |
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Call Number |
UA @ lucian @ c:irua:96956 |
Serial |
711 |
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Permanent link to this record |
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Author |
Pietra, F.; van Dijk-Moes, R.J.A.; Ke, X.; Bals, S.; Van Tendeloo, G.; de Mello Donega, C.; Vanmaekelbergh, D. |
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Title |
Synthesis of highly luminescent silica-coated CdSe/CdS nanorods |
Type |
A1 Journal article |
|
Year |
2013 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
|
|
Volume |
25 |
Issue |
17 |
Pages |
3427-3434 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
CdSe(core)/CdS(shell) nanorods (NRs) have been extensively investigated for their unique optical properties, such as high photoluminescence (PL) quantum efficiency (QE) and polarized light emission. The incorporation of these NRs in silica (SiO2) is of high interest, since this renders them processable in polar solvents while increasing their photochemical stability, which would be beneficial for their application in LEDs and as biolabels. We report the synthesis of highly luminescent silica-coated CdSe/CdS NRs, by using the reverse micelle method. The mechanism for the encapsulation of the NRs in silica is unravelled and shown to be strongly influenced by the NR shape and its asymmetry. This is attributed to both the different morphology and the different crystallographic nature of the facets terminating the opposite tips of the NRs. These results lead to the formation of a novel class of NR architectures, whose symmetry can be controlled by tuning the degree of coverage of the silica shell. Interestingly, the encapsulation of the NRs in silica leads to a remarkable increase in their photostability, while preserving their optical properties. |
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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 |
Washington, D.C. |
Editor |
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Language |
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Wos |
000330097900004 |
Publication Date |
2013-08-13 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
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ISSN |
0897-4756;1520-5002; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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|
Impact Factor |
9.466 |
Times cited |
46 |
Open Access |
|
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|
Notes |
262348 ESMI; 246791 COUNTATOMS; Hercules |
Approved |
Most recent IF: 9.466; 2013 IF: 8.535 |
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Call Number |
UA @ lucian @ c:irua:110037 |
Serial |
3456 |
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Permanent link to this record |
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Author |
Leroux, O.; Leroux, F.; Bagniewska-Zadworna,.; Knox, J.P.; Claeys, M.; Bals, S.; Viane, R.L.L. |
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Title |
Ultrastructure and composition of cell wall appositions in the roots of Asplenium (Polypodiales) |
Type |
A1 Journal article |
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Year |
2011 |
Publication |
Micron |
Abbreviated Journal |
Micron |
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Volume |
42 |
Issue |
8 |
Pages |
863-870 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Cell wall appositions (CWAs), formed by the deposition of extra wall material at the contact site with microbial organisms, are an integral part of the response of plants to microbial challenge. Detailed histological studies of CWAs in fern roots do not exist. Using light and electron microscopy we examined the (ultra)structure of CWAs in the outer layers of roots of Asplenium species. All cell walls studded with CWAs were impregnated with yellow-brown pigments. CWAs had different shapes, ranging from warts to elongated branched structures, as observed with scanning and transmission electron microscopy. Ultrastructural study further showed that infecting fungi grow intramurally and that they are immobilized by CWAs when attempting to penetrate intracellularly. Immunolabelling experiments using monoclonal antibodies indicated pectic homogalacturonan, xyloglucan, mannan and cellulose in the CWAs, but tests for lignins and callose were negative. We conclude that these appositions are defense-related structures made of a non-lignified polysaccharide matrix on which phenolic compounds are deposited in order to create a barrier protecting the root against infections. |
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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 |
Oxford |
Editor |
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Language |
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Wos |
000294942600013 |
Publication Date |
2011-06-24 |
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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 |
|
Series Issue |
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Edition |
|
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ISSN |
0968-4328; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
1.98 |
Times cited |
20 |
Open Access |
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Notes |
Fwo |
Approved |
Most recent IF: 1.98; 2011 IF: 1.527 |
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Call Number |
UA @ lucian @ c:irua:92540 |
Serial |
3798 |
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Permanent link to this record |
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Author |
Werner, R.; Raisch, C.; Leca, V.; Ion, V.; Bals, S.; Van Tendeloo, G.; Chasse, T.; Kleiner, R.; Koelle, D. |
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Title |
Transport, magnetic, and structural properties of La0.7Ce0.3MnO3 thin films: evidence for hole-doping |
Type |
A1 Journal article |
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Year |
2009 |
Publication |
Physical review : B : solid state |
Abbreviated Journal |
Phys Rev B |
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Volume |
79 |
Issue |
5 |
Pages |
054416,1-054416,8 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Cerium-doped manganite thin films were grown epitaxially by pulsed laser deposition at 720 °C and oxygen pressure pO2=125 Pa and were subjected to different annealing steps. According to x-ray diffraction (XRD) data, the formation of CeO2 as a secondary phase could be avoided for pO28 Pa. However, transmission electron microscopy shows the presence of CeO2 nanoclusters even in those films which appear to be single phase in XRD. With O2 annealing, the metal-to-insulator transition temperature increases, while the saturation magnetization decreases and stays well below the theoretical value for electron-doped La0.7Ce0.3MnO3 with mixed Mn3+/Mn2+ valences. The same trend is observed with decreasing film thickness from 100 to 20 nm, indicating a higher oxygen content for thinner films. Hall measurements on a film which shows a metal-to-insulator transition clearly reveal holes as dominating charge carriers. Combining data from x-ray photoemission spectroscopy, for determination of the oxygen content, and x-ray absorption spectroscopy (XAS), for determination of the hole concentration and cation valences, we find that with increasing oxygen content the hole concentration increases and Mn valences are shifted from 2+ to 4+. The dominating Mn valences in the films are Mn3+ and Mn4+, and only a small amount of Mn2+ ions can be observed by XAS. Mn2+ and Ce4+ XAS signals obtained in surface-sensitive total electron yield mode are strongly reduced in the bulk-sensitive fluorescence mode, which indicates hole-doping in the bulk for those films which do show a metal-to-insulator transition. |
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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 |
Lancaster, Pa |
Editor |
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Language |
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Wos |
000263815400057 |
Publication Date |
2009-02-13 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
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Edition |
|
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ISSN |
1098-0121;1550-235X; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
3.836 |
Times cited |
25 |
Open Access |
|
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|
Notes |
Esteem 026019; Fwo |
Approved |
Most recent IF: 3.836; 2009 IF: 3.475 |
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Call Number |
UA @ lucian @ c:irua:76221 |
Serial |
3725 |
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Permanent link to this record |
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Author |
di Vece, M.; Bals, S.; Lievens, P.; Van Tendeloo, G. |
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Title |
Compositional changes of Pd-Au bimetallic nanoclusters upon hydrogenation |
Type |
A1 Journal article |
|
Year |
2009 |
Publication |
Physical review : B : solid state |
Abbreviated Journal |
Phys Rev B |
|
|
Volume |
80 |
Issue |
12 |
Pages |
125420,1-125420,4 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Changes in the size distribution and composition of bimetallic Pd-Au nanoclusters have been observed after hydrogen exposure. This effect is caused by hydrogen-induced Ostwald ripening whereby the hydrogen reduces the binding energy of the cluster atoms leading to their detachment from the cluster. The composition changes due to a difference in mobility of the detached palladium and gold atoms on the surface. Fast palladium atoms contribute to the formation of larger nanoclusters, while the slower gold atoms are confined to the smaller nanoclusters. These transformations in the Pd-Au nanocluster size and composition set a limit for chemical reactions in which such nanoclusters are involved together with hydrogen. |
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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 |
Lancaster, Pa |
Editor |
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Language |
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Wos |
000270383300121 |
Publication Date |
2009-09-23 |
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Series Editor |
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Series Title |
|
Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
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|
ISSN |
1098-0121;1550-235X; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
3.836 |
Times cited |
28 |
Open Access |
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|
Notes |
Fwo; Goa; Iap-Vi; Esteem 026019 |
Approved |
Most recent IF: 3.836; 2009 IF: 3.475 |
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Call Number |
UA @ lucian @ c:irua:79232 |
Serial |
445 |
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Permanent link to this record |
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Author |
Leroux, F.; Gysemans, M.; Bals, S.; Batenburg, K.J.; Snauwaert, J.; Verbiest, T.; van Haesendonck, C.; Van Tendeloo, G. |
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Title |
Three-dimensional characterization of helical silver nanochains mediated by protein assemblies |
Type |
A1 Journal article |
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Year |
2010 |
Publication |
Advanced materials |
Abbreviated Journal |
Adv Mater |
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Volume |
22 |
Issue |
19 |
Pages |
2193-2197 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Vision lab |
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Abstract |
Characterization methods for the structural investigation of biotemplates for nanodevices remain widely unexplored, despite the fact that biotemplating methods for nanodevice fabrication are becoming more widespread. In this study several techniques are used to characterize the morphology and 3D distribution of silver nanoparticles deposited on insulin fibrils. |
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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 |
Weinheim |
Editor |
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Language |
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Wos |
000278601400016 |
Publication Date |
2010-03-11 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
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ISSN |
0935-9648;1521-4095; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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|
Impact Factor |
19.791 |
Times cited |
51 |
Open Access |
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|
Notes |
Esteem 026019; Fwo |
Approved |
Most recent IF: 19.791; 2010 IF: NA |
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Call Number |
UA @ lucian @ c:irua:83296 |
Serial |
3645 |
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Permanent link to this record |
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Author |
Sentosun, K.; Sanz Ortiz, M.N.; Batenburg, K.J.; Liz-Marzán, L.M.; Bals, S. |
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Title |
Combination of HAADF-STEM and ADF-STEM Tomography for Core-Shell Hybrid Materials |
Type |
A1 Journal article |
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Year |
2015 |
Publication |
Particle and particle systems characterization |
Abbreviated Journal |
Part Part Syst Char |
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Volume |
32 |
Issue |
32 |
Pages |
1063-1067 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Vision lab |
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Abstract |
Characterization of core-shell type nanoparticles in 3D by transmission electron microscopy (TEM) can be very challenging. Especially when both heavy and light elements co-exist within the same nanostructure, artefacts in the 3D reconstruction are often present. A representative example would be a particle comprising an anisotropic metallic (Au) nanoparticle coated with a (mesoporous) silica shell. To obtain a reliable 3D characterization of such an object, we propose a dose-efficient strategy to simultaneously acquire high angle annular dark field scanning TEM and annular dark field tilt series for tomography. The 3D reconstruction is further improved by applying an advanced masking and interpolation approach to the acquired data. This new methodology enables us to obtain high quality reconstructions from which also quantitative information can be extracted. This approach is broadly applicable to investigate hybrid core-shell materials. |
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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 |
000368446800003 |
Publication Date |
2015-10-13 |
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Series Editor |
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Series Title |
|
Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
0934-0866; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
4.474 |
Times cited |
13 |
Open Access |
OpenAccess |
|
|
Notes |
S.B. acknowledges financial support from European Research Council (ERC) (ERC Starting Grant #335078-COLOURATOM). L.M. acknowledges funding from the EU, Grant# 310651-2 Self-Assembly in Confined Space (SACS). K.J.B acknowledges financial support from the Netherlands Organisation for Scientific Research (NWO), project number 639.072.005 and NWO CW 700.57.026. Networking support was provided by COST Action MP1207. The authors acknowledge the European Union under the Seventh Framework Program under a contract for an Integrated Infrastructure Initiative, Reference No. 312483-ESTEEM2 for financial support.; esteem2jra4; ECASSara; (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:cannot); |
Approved |
Most recent IF: 4.474; 2015 IF: 3.081 |
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Call Number |
c:irua:129590 c:irua:129590 |
Serial |
3967 |
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Permanent link to this record |
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Author |
Spaeth, P.; Adhikari, S.; Heyvaert, W.; Zhuo, X.; Garcia, I.; Liz-Marzan, L.M.; Bals, S.; Orrit, M.; Albrecht, W. |
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Title |
Photothermal circular dichroism measurements of single chiral gold nanoparticles correlated with electron tomography |
Type |
A1 Journal article |
|
Year |
2022 |
Publication |
ACS Photonics |
Abbreviated Journal |
Acs Photonics |
|
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Volume |
9 |
Issue |
12 |
Pages |
3995-4004 |
|
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Chemically synthesized metal nanoparticles with morphological chiral features are known to exhibit strong circular dichroism. However, we still lack understanding of the correlation between morphological and chiroptical features of plasmonic nanoparticles. To shed light on that question, single nanoparticle experiments are required. We performed photothermal circular dichroism measurements of single chiral and achiral gold nanoparticles and correlated the chiroptical response to the 3D morphology of the same nanoparticles retrieved by electron tomography. In contrast to an ensemble measurement, we show that individual particles within the ensemble display a broad distribution of strength and handedness of circular dichroism signals. Whereas obvious structural chiral features, such as helical wrinkles, translate into chiroptical ones, nanoparticles with less obvious chiral morphological features can also display strong circular dichroism signals. Interestingly, we find that even seemingly achiral nanoparticles can display large g-factors. The origin of this circular dichroism signal is discussed in terms of plasmonics and other potentially relevant factors. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000884432100001 |
Publication Date |
2022-11-08 |
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Series Editor |
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Series Title |
|
Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
2330-4022 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
7 |
Times cited |
5 |
Open Access |
OpenAccess |
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Notes |
This work was supported by The Netherlands Organisation for Scientific Research (NWO) as part of the Open Technology Program (OTP, Project No. 16008) and by a Spinoza prize (M.O.) . W.A. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020 Program (Grant No. 797153, SOPMEN) . L.M.L.M. acknowledges funding from MCIN/AEI/10.13039/501100011033 (Grants PID2020-117779RB-I00 and MDM-2017-0720) . We thank Dr. Wolfgang L?fer for providing optical equipment. We also acknowledge the European Soft Matter Infrastructure (EUSMI: E201200468) . |
Approved |
Most recent IF: 7 |
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Call Number |
UA @ admin @ c:irua:192098 |
Serial |
7331 |
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Permanent link to this record |
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Author |
Sa, J.; Hu, N.; Heyvaert, W.; Van Gordon, K.; Li, H.; Wang, L.; Bals, S.; Liz-Marzán, L.M.; Ni, W. |
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Title |
Spontaneous Chirality Evolved at the Au–Ag Interface in Plasmonic Nanorods |
Type |
A1 Journal Article |
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Year |
2023 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem. Mater. |
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Volume |
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Issue |
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Pages |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Chiral ligands are considered a required ingredient during the synthesis of dissymmetric plasmonic metal nanocrystals. The mechanism behind the generation of chiral structures involves the formation of high Miller index chiral facets, induced by the adsorption of such chiral ligands. We found however that, chirality can also evolve spontaneously, without the involvement of any chiral ligands, during the co-deposition of Au and Ag on Au nanorods. When using a specific Au/Ag ratio, phase segregation of the two metals leads to an interface within the obtained AuAg shell, which can be exposed by removing the Ag component via oxidative etching. Although a close-to-racemic mixture of chiral Au nanorods with right and left handedness is found in solution, electron tomography analysis evidences left- and righthanded helicities, both at the Au-Ag interface and at the exposed surface of Au NRs after Ag etching. The helicity profile of the NRs indicates dominating inclination angles in a range from 30° to 60°. Single-particle optical characterization also reveals random handedness in the plasmonic response of individual nanorods. We hypothesize that, the origin of chirality is related with symmetry breaking during the co-deposition of Au and Ag, through an initial perturbation in a small region on the Au-Ag interface that eventually leads to chiral segregation throughout the nanocrystal. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
001052093300001 |
Publication Date |
2023-08-21 |
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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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|
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ISSN |
0897-4756 |
ISBN |
|
Additional Links |
UA library record; WoS full record |
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Impact Factor |
8.6 |
Times cited |
|
Open Access |
OpenAccess |
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Notes |
The authors acknowledge the financial support from the National Natural Science Foundation of China (grant 22074102). LMLM acknowledges funding from 26 MCIN/AEI/10.13039/501100011033 and “ESF Investing in your future” (Grant PID2020- 117779RB-I00). This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 823717 – ESTEEM3.; Ministerio de Ciencia e Innovaci?n, PID2020-117779RB-I00 ; H2020 Research Infrastructures, 823717 ; European Social Fund, PID2020-117779RB-I00 ; National Natural Science Foundation of China, 22074102 ; |
Approved |
Most recent IF: 8.6; 2023 IF: 9.466 |
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Call Number |
EMAT @ emat @c:irua:198151 |
Serial |
8810 |
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Permanent link to this record |
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Author |
Zhuo, X.; Mychinko, M.; Heyvaert, W.; Larios, D.; Obelleiro-Liz, M.; Taboada, J.M.; Bals, S.; Liz-Marzán, L.M. |
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Title |
Morphological and Optical Transitions during Micelle-Seeded Chiral Growth on Gold Nanorods |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
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Issue |
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Pages |
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|
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Chiral plasmonics is a rapidly developing field where breakthroughs and unsolved problems coexist. We have recently reported binary surfactant-assisted seeded growth of chiral gold nanorods (Au NRs) with high chiroptical activity. Such a seeded-growth process involves the use of a chiral cosurfactant that induces micellar helicity, in turn driving the transition from achiral to chiral Au NRs, from both the morphological and the optical points of view. We report herein a detailed study on both transitions, which reveals intermediate states that were hidden so far. The correlation between structure and optical response is carefully analyzed, including the (linear and CD) spectral evolution over time, electron tomography, the impact of NR dimensions on their optical response, the variation of the absorption-to-scattering ratio during the evolution from achiral to chiral Au NRs, and the near-field enhancement related to chiral plasmon modes. Our findings provide further understanding of the growth process of chiral Au NRs and the associated optical changes, which will facilitate further study and applications of chiral nanomaterials. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000878324400001 |
Publication Date |
2022-10-26 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
|
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
17.1 |
Times cited |
17 |
Open Access |
OpenAccess |
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Notes |
This work was supported by the European Research Council (ERC-AdG-4DbioSERS-787510 to L.M.L.-M. and ERC-CoG-REALNANO-815128 to S.B.) and the MCIN/AEI/10.13039/501100011033 (Grant PID2020-117779RB-I00). X.Z. acknowledges funding from the Juan de la Cierva fellowship (FJC2018-036104-I) and the University Development Fund (UDF01002665, CUHK-Shenzhen). D.L., M.O.-L., and J.M.T. acknowledge funding from the European Regional Development Fund (ERDF) and the Spanish Ministerio de Ciencia, Innovación y Universidades, under Projects PID2020-116627RB-C21 and PID2020-116627RB-C22, as well as from the ERDF/Galician Regional Government as part of the agreement for funding the Atlantic Research Center for Information and Communication Technologies (atlanTTic) and ERDF/Extremadura Regional Government under Projects IB18073 and GR18055. This work was performed in the framework of the Maria de Maeztu Units of Excellence Program from the Spanish State Research Agency (Grant No. MDM-2017-0720). The authors acknowledge Dr. Guillermo González-Rubio for providing suggestions for synthesis and Dr. Irantzu Llarena for assisting with the CD measurements. |
Approved |
Most recent IF: 17.1 |
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Call Number |
EMAT @ emat @c:irua:191815 |
Serial |
7116 |
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Permanent link to this record |
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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 |
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Year |
2022 |
Publication |
ACS materials letters |
Abbreviated Journal |
ACS Materials Lett. |
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Volume |
4 |
Issue |
|
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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Permanent link to this record |
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Author |
Yao, Y.; Ugras, T.J.; Meyer, T.; Dykes, M.; Wang, D.; Arbe, A.; Bals, S.; Kahr, B.; Robinson, R.D. |
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Title |
Extracting pure circular dichroism from hierarchically structured CdS magic cluster films |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
16 |
Issue |
12 |
Pages |
20457-20469 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Chiroptically active, hierarchically structured materials are difficult to accurately characterize due to linear anisotropic contributions (i.e., linear dichroism (LD) and linear birefringence (LB)) and parasitic ellipticities that produce artifactual circular dichroism (CD) signals, in addition to chiral analyte contributions ranging from molecular-scale clusters to micron-sized assemblies. Recently, we have shown that CdS magic-sized clusters (MSC) can self-assemble into ordered films that have a hierarchical structure spanning seven orders of length-scale. These films have a strong CD response, but the chiral origins are obfuscated by the hierarchical architecture and LDLB contributions. Here, we derive and demonstrate a method for extracting the “pure” CD signal (CD generated by structural dissymmetry) from hierarchical MSC films and identified the chiral origin. The theory behind the method is derived using Mueller matrix and Stokes vector conventions and verified experimentally before being applied to hierarchical MSC and nanoparticle films with varying macroscopic orderings. Each film's extracted “true CD” shares a bisignate profile aligned with the exciton peak, indicating the assemblies adopt a chiral arrangement and form an exciton coupled system. Interestingly, the linearly aligned MSC film possesses one of the highest g-factors (0.05) among semiconducting nanostructures reported. Additionally, we find that films with similar electronic transition dipole alignment can possess greatly different g-factors, indicating chirality change rather than anisotropy is the cause of the difference in the CD signal. The difference in g-factor is controllable via film evaporation geometry. This study provides a simple means to measure “true” CD and presents an example of experimentally understanding chiroptic interactions in hierarchical nanostructures. |
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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 |
000888219600001 |
Publication Date |
2022-11-17 |
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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 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
17.1 |
Times cited |
8 |
Open Access |
Not_Open_Access |
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Notes |
This work was supported in part by the National Science Foundation (NSF) under Award Nos. DMR-2003431 and CHE-2003586. This work made use of the Cornell Center for Materials Research Shared Facilities, which are supported through the NSF MRSEC program (DMR-1719875). This work is partly supported by Grant PID2021-123438NB-I00 (MCIN/AEI/10.13039/501100011033 and “ERDF vA way of making Europe”) and Grant IT1566-22 (Eusko Jaurlaritza). D.W. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in the Horizon 2020 program (Grant 894254 SuprAtom). S.B. acknowledges financial support from ERC Consolidator Grant No. 815128 REALNANO. B.K. acknowledges NSF award DMR-2003968. We would like to thank Dr. Mark August Pfeifer for help with circular dichroism measurements. Additionally, we would like to thank Professor Luis M. Liz-Marzan for invaluable discussions on chirality. |
Approved |
Most recent IF: 17.1 |
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Call Number |
UA @ admin @ c:irua:192070 |
Serial |
7305 |
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Permanent link to this record |
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Author |
Parzyszek, S.; Tessarolo, J.; Pedrazo-Tardajos, A.; Ortuno, A.M.; Baginski, M.; Bals, S.; Clever, G.H.; Lewandowski, W. |
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Title |
Tunable circularly polarized luminescence via chirality induction and energy transfer from organic films to semiconductor nanocrystals |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
16 |
Issue |
11 |
Pages |
18472-18482 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Circularly polarized luminescent (CPL) films with high dissymmetry factors hold great potential for optoelectronic applications. Herei n , we propose a strategy for achieving strongly dissymetric CPL in nanocomposite films based on chira l i t y induction and energy transfer to semiconductor nanocrystals. First, focusing on a purely organic system, aggregation-induced emission (AIE) and CPL activity of organic liquid crystals (LCs) forming helical nanofilaments was detected, featuring green emission with high dissymmetry factors g(lum) similar to 10(-2). The handedness of helical filaments, and thus the sign of CPL, was controlled via minute amounts of a small chiral organic dopant. Second, nanocomposite films were fabricated by incorporating InP/ZnS semi-conductor quantum dots (QDs) into the LC matri x , which induced the chiral assembly of QDs and endowed them with chiroptical properties. Due to the spectral matching of the components, energy transfer (ET) from LC to QDs was possible enabling a convenient way of tuning CPL wavelengths by varying the LC/QD ratio. As obtained, composite films exhibited absolute glum values up to similar to 10(-2) and thermally on/off switchable luminescence. Overall, we demonstrate the induction of chiroptical properties by the assembly of nonchiral building QDs on the chiral organic template and energy transfer from organic films to QDs, representing a simple and versatile approach to tune the CPL activity of organic materials. |
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Corporate Author |
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Thesis |
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Place of Publication |
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Language |
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Wos |
000883943600001 |
Publication Date |
2022-11-07 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
17.1 |
Times cited |
10 |
Open Access |
OpenAccess |
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Notes |
W.L., S.P., and M.B. acknowledge support from the National Science Center Poland under the OPUS Grant UMO-2019/35/B/ST5/04488. J.T. and G.H.C. acknowledge the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany's Excellence Strategy, Grant EXC 2033-390677874-RESOLV. W.L. acknowledges financial support from the European Commission under the Horizon 2020 Programme by Grant E210400529. S.B. and A.P.-T. acknowledge financial support from the European Commission under the Horizon 2020 Programme by Grant 731019 (EUSMI) and ERC Consolidator Grant 815128 (REALNANO). We thank Elie Benchimol for his help with the CPL measurements. We thank Damian Pociecha for his help in the determination of phase sequences of organic compounds. |
Approved |
Most recent IF: 17.1 |
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Call Number |
UA @ admin @ c:irua:192101 |
Serial |
7345 |
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Permanent link to this record |
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Author |
Hill, E.H.; Claes, N.; Bals, S.; Liz-Marzán, L.M. |
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Title |
Layered Silicate Clays as Templates for Anisotropic Gold Nanoparticle Growth |
Type |
A1 Journal article |
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Year |
2016 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
28 |
Issue |
28 |
Pages |
5131-5139 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Clay minerals are abundant natural materials arising in the presence of water and are composed of small particles of different sizes and shapes. The interlamellar space between layered silicate clays can also be used to host a variety of different organic and inorganic guest molecules or particles. Recent studies of clay−metal hybrids formed by impregnation of nanoparticles into the interlayer spaces of the clays have not demonstrated the ability for templated growth following the shape of the particles. Following this line of interest, a method for the synthesis of gold nanoparticles on the synthetic layered silicate clay laponite was developed. This approach can be used to make metal−clay nanoparticles with a variety of morphologies while retaining the molecular adsorption properties of the clay. The surface enhanced Raman scattering enhancement of these particles was also found to be greater than that obtained from other metal nanoparticles of a similar morphology, likely due to increased dye adsorption by the presence of the clay. The hybrid particles presented herein will contribute to further study of plasmonic
sensing, catalysis, dye aggregation, and novel composite materials. |
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Corporate Author |
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Place of Publication |
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Wos |
000380576700031 |
Publication Date |
2016-07-02 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
13 |
Open Access |
OpenAccess |
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Notes |
This work has been supported by the European Research Council (ERC Advanced Grant No. 267867, PLASMAQUO). E.H.H. thanks the Spanish Ministry of Economy and Competitiveness for providing a Juan de la Cierva Fellowship (FJCI-2014-22598). N.C. and S.B. acknowledge financial support from European Research Council (ERC Starting Grant #335078-COLOURATOM). We gratefully acknowledge A. B. Serrano-Montes for providing the seed-mediated Au nanostars.; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 9.466 |
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Call Number |
c:irua:135178 c:irua:135178 |
Serial |
4117 |
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Permanent link to this record |
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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 |
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Year |
2015 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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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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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 |
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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 |
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 |
van der Sluijs, M.M.; Salzmann, B.B.V.; Arenas Esteban, D.; Li, C.; Jannis, D.; Brafine, L.C.; Laning, T.D.; Reinders, J.W.C.; Hijmans, N.S.A.; Moes, J.R.; Verbeeck, J.; Bals, S.; Vanmaekelbergh, D. |
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Title |
Study of the Mechanism and Increasing Crystallinity in the Self-Templated Growth of Ultrathin PbS Nanosheets |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Chemistry of materials |
Abbreviated Journal |
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Volume |
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Issue |
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Pages |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Colloidal 2D semiconductor nanocrystals, the analogue of solid-state quantum wells, have attracted strong interest in material science and physics. Molar quantities of suspended quantum objects with spectrally pure absorption and emission can be synthesized. For the visible region, CdSe nanoplatelets with atomically precise thickness and tailorable emission have been (almost) perfected. For the near-infrared region, PbS nanosheets (NSs) hold strong promise, but the photoluminescence quantum yield is low and many questions on the crystallinity, atomic structure, intriguing rectangular shape, and formation mechanism remain to be answered. Here, we report on a detailed investigation of the PbS NSs prepared with a lead thiocyanate single source precursor. Atomically resolved HAADF-STEM imaging reveals the presence of defects and small cubic domains in the deformed orthorhombic PbS crystal lattice. Moreover, variations in thickness are observed in the NSs, but only in steps of 2 PbS monolayers. To study the reaction mechanism, a synthesis at a lower temperature allowed for the study of reaction intermediates. Specifically, we studied the evolution of pseudo-crystalline templates towards mature, crystalline PbS NSs. We propose a self-induced templating mechanism based on an oleylamine-lead-thiocyanate (OLAM-Pb-SCN) complex with two Pb-SCN units as a building block; the interactions between the long-chain ligands regulate the crystal structure and possibly the lateral dimensions. |
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Corporate Author |
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Thesis |
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Place of Publication |
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Language |
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Wos |
000959572100001 |
Publication Date |
2023-03-25 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
8.6 |
Times cited |
2 |
Open Access |
OpenAccess |
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Notes |
H2020 Research Infrastructures, 731019 ; H2020 European Research Council, 692691 815128 ; Nederlandse Organisatie voor Wetenschappelijk Onderzoek, 715.016.002 ; |
Approved |
Most recent IF: 8.6; 2023 IF: 9.466 |
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Call Number |
EMAT @ emat @c:irua:195894 |
Serial |
7255 |
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Permanent link to this record |
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Author |
Toso, S.; Imran, M.; Mugnaioli, E.; Moliterni, A.; Caliandro, R.; Schrenker, N.J.; Pianetti, A.; Zito, J.; Zaccaria, F.; Wu, Y.; Gemmi, M.; Giannini, C.; Brovelli, S.; Infante, I.; Bals, S.; Manna, L. |
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Title |
Halide perovskites as disposable epitaxial templates for the phase-selective synthesis of lead sulfochloride nanocrystals |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Nature communications |
Abbreviated Journal |
Nat Commun |
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Volume |
13 |
Issue |
1 |
Pages |
3976-10 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Colloidal chemistry grants access to a wealth of materials through simple and mild reactions. However, even few elements can combine in a variety of stoichiometries and structures, potentially resulting in impurities or even wrong products. Similar issues have been long addressed in organic chemistry by using reaction-directing groups, that are added to a substrate to promote a specific product and are later removed. Inspired by such approach, we demonstrate the use of CsPbCl3 perovskite nanocrystals to drive the phase-selective synthesis of two yet unexplored lead sulfochlorides: Pb3S2Cl2 and Pb4S3Cl2. When homogeneously nucleated in solution, lead sulfochlorides form Pb3S2Cl2 nanocrystals. Conversely, the presence of CsPbCl3 triggers the formation of Pb4S3Cl2/CsPbCl3 epitaxial heterostructures. The phase selectivity is guaranteed by the continuity of the cationic subnetwork across the interface, a condition not met in a hypothetical Pb3S2Cl2/CsPbCl3 heterostructure. The perovskite domain is then etched, delivering phase-pure Pb4S3Cl2 nanocrystals that could not be synthesized directly. Phase-selective approaches, such using reaction-directing groups, are often seen in traditional organic chemistry and catalysis. Here authors use perovskite nanocrystals as disposable templates to drive the phase-selective synthesis of two colloidal nanomaterials, the lead sulfohalides Pb3S2Cl2 and Pb4S3Cl2. |
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Wos |
000825867200003 |
Publication Date |
2022-07-08 |
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ISSN |
2041-1723 |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
16.6 |
Times cited |
15 |
Open Access |
OpenAccess |
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Notes |
The authors would like to acknowledge Dr. Joka Buha for the help with preliminary tests preceding this project, and Dr. B. M. Aresta and Dr. L. Cassano for their administrative support. The authors acknowledge financial support from the Research Foundation Flanders (FWO) through a postdoctoral fellowship to N.J.S. (FWO Grant No. 1238622N, N.J.S). S.B. acknowledges financial support from the European Commission by ERC Consolidator grant REALNANO (No. 815128, S.B.). L.M. acknowledges financial support from the Italian Ministry of University and Research (MIUR) through the Flag-Era JTC2019 project “Solution-Processed Perovskite/Graphene Nanocomposites for SelfPowered Gas Sensors” (PeroGaS, L.M.). The access to the National Synchrotron Light Source, Brookhaven National Laboratory, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC0298CH10886 (NSLS-II Proposal Number 307441). |
Approved |
Most recent IF: 16.6 |
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Call Number |
UA @ admin @ c:irua:189684 |
Serial |
7085 |
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Permanent link to this record |
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Author |
Xia, C.; Pedrazo-Tardajos, A.; Wang, D.; Meeldijk, J.D.; Gerritsen, H.C.; Bals, S.; de Donega, C.M. |
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Title |
Seeded growth combined with cation exchange for the synthesis of anisotropic Cu2-xS/ZnS, Cu2-xS, and CuInS2 nanorods |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Chemistry of materials |
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Volume |
33 |
Issue |
1 |
Pages |
102-116 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Colloidal copper(I) sulfide (Cu2-xS) nanocrystals (NCs) have attracted much attention for a wide range of applications because of their unique optoelectronic properties, driving scientists to explore the potential of using Cu2-xS NCs as seeds in the synthesis of heteronanocrystals to achieve new multifunctional materials. Herein, we developed a multistep synthesis strategy toward Cu2-xS/ZnS heteronanorods. The Janus-type Cu2-xS/ZnS heteronanorods are obtained by the injection of hexagonal high-chalcocite Cu2-xS seed NCs in a hot zinc oleate solution in the presence of suitable surfactants, 20 s after the injection of sulfur precursors. The Cu2-xS seed NCs undergo rapid aggregation and coalescence in the first few seconds after the injection, forming larger NCs that act as the effective seeds for heteronucleation and growth of ZnS. The ZnS heteronucleation occurs on a single (100) facet of the Cu2-xS seed NCs and is followed by fast anisotropic growth along a direction that is perpendicular to the c-axis, thus leading to Cu2-xS/ZnS Janus-type heteronanorods with a sharp heterointerface. Interestingly, the high-chalcocite crystal structure of the injected Cu2-xS seed NCs is preserved in the Cu2-xS segments of the heteronanorods because of the highthermodynamic stability of this Cu2-xS phase. The Cu2-xS/ZnS heteronanorods are subsequently converted into single-component Cu2-xS and CuInS2 nanorods by postsynthetic topotactic cation exchange. This work expands the possibilities for the rational synthesis of colloidal multicomponent heteronanorods by allowing the design principles of postsynthetic heteroepitaxial seeded growth and nanoscale cation exchange to be combined, yielding access to a plethora of multicomponent heteronanorods with diameters in the quantum confinement regime. |
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Wos |
000610984700009 |
Publication Date |
2020-12-28 |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Times cited |
10 |
Open Access |
OpenAccess |
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Notes |
C.X. acknowledges China Scholarship Council (CSC) for the financial support (grant number 201406330055). C.d.M.D. acknowledges funding from the European Commission for access to the EMAT facilities (grant number EUSMI E180900184). D.W. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (grant 894254 SuprAtom). S.B. acknowledges support by means of the ERC Consolidator grant no. 815128 REALNANO. The authors thank Donglong Fu for XRD measurements.; sygma |
Approved |
Most recent IF: NA |
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Call Number |
UA @ admin @ c:irua:176587 |
Serial |
6732 |
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Author |
Bals, S.; Casavola, M.; van Huis, M.A.; Van Aert, S.; Batenburg, K.J.; Van Tendeloo, G.; Vanmaekelbergh, D. |
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Title |
Three-dimensional atomic imaging of colloidal core-shell nanocrystals |
Type |
A1 Journal article |
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Year |
2011 |
Publication |
Nano letters |
Abbreviated Journal |
Nano Lett |
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Volume |
11 |
Issue |
8 |
Pages |
3420-3424 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Vision lab |
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Abstract |
Colloidal coreshell semiconductor nanocrystals form an important class of optoelectronic materials, in which the exciton wave functions can be tailored by the atomic configuration of the core, the interfacial layers, and the shell. Here, we provide a trustful 3D characterization at the atomic scale of a free-standing PbSe(core)CdSe(shell) nanocrystal by combining electron microscopy and discrete tomography. Our results yield unique insights for understanding the process of cation exchange, which is widely employed in the synthesis of coreshell nanocrystals. The study that we present is generally applicable to the broad range of colloidal heteronanocrystals that currently emerge as a new class of materials with technological importance. |
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Place of Publication |
Washington |
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Wos |
000293665600062 |
Publication Date |
2011-07-25 |
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ISSN |
1530-6984;1530-6992; |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
12.712 |
Times cited |
121 |
Open Access |
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Notes |
Esteem 026019; Fwo |
Approved |
Most recent IF: 12.712; 2011 IF: 13.198 |
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Call Number |
UA @ lucian @ c:irua:91263 |
Serial |
3643 |
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Author |
van der Burgt, J.S.; Geuchies, J.J.; van der Meer, B.; Vanrompay, H.; Zanaga, D.; Zhang, Y.; Albrecht, W.; Petukhov, A.V.; Filion, L.; Bals, S.; Swart, I.; Vanmaekelbergh, D. |
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Title |
Cuboidal supraparticles self-assembled from cubic CsPbBr3 perovskite nanocrystals |
Type |
A1 Journal article |
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Year |
2018 |
Publication |
The journal of physical chemistry: C : nanomaterials and interfaces |
Abbreviated Journal |
J Phys Chem C |
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122 |
Issue |
122 |
Pages |
15706-15712 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Colloidal CsPbBr3 nanocrystals (NCs) have emerged as promising candidates for various opto-electronic applications, such as light-emitting diodes, photodetectors, and solar cells. Here, we report on the self-assembly of cubic NCs from an organic suspension into ordered cuboidal supraparticles (SPs) and their structural and optical properties. Upon increasing the NC concentration or by addition of a nonsolvent, the formation of the SPs occurs homogeneously in the suspension, as monitored by in situ X-ray scattering measurements. The three-dimensional structure of the SPs was resolved through high-angle annular dark-field scanning transmission electron microscopy and electron tomography. The NCs are atomically aligned but not connected. We characterize NC vacancies on superlattice positions both in the bulk and on the surface of the SPs. The occurrence of localized atomic-type NC vacancies-instead of delocalized ones-indicates that NC-NC attractions are important in the assembly, as we verify with Monte Carlo simulations. Even when assembled in SPs, the NCs show bright emission, with a red shift of about 30 meV compared to NCs in suspension. |
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Washington, D.C. |
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Wos |
000439003600071 |
Publication Date |
2018-06-14 |
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ISSN |
1932-7447; 1932-7455 |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.536 |
Times cited |
60 |
Open Access |
OpenAccess |
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Notes |
; The authors thank Dr. Rajeev Dattani and Jacques Gorini from the ID02 beamline of the ESRF for their excellent assistance during the X-ray scattering experiments. We also thank Carlo van Overbeek, P. Tim Prins, and Federico Montanarella for their support during the synchrotron experiments. The authors gratefully acknowledge Prof. Dr. Alfons van Blaaderen for fruitful discussions. D.V. acknowledges funding from NWO-CW TOPPUNT “Superficial superstructures.” J.J.G. acknowledges the joint Debye and ESRF graduate programs for the financial support. H.V. gratefully acknowledges the financial support by the Flemish Fund for Scientific Research (FWO grant 1S32617NN). S.B. acknowledges the financial support from the European Research Council (ERC Starting grant # 335078-COLOURATOMS). Y.Z. acknowledges the financial support from the European Union's Horizon 2020 research and innovation program, under the Marie Sklodowska-Curie grant agreement #665501 through a FWO [PEGASUS]2 Marie Sklodowska-Curie fellowship (12U4917N). W.A. acknowledges the financial support from the European Research Council under the European Unions Seventh Framework Program (FP-2007-2013)/ERC Advanced grant agreement 291667 HierarSACol. ; ecas_Sara |
Approved |
Most recent IF: 4.536 |
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Call Number |
UA @ lucian @ c:irua:153161UA @ admin @ c:irua:153161 |
Serial |
5087 |
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