| |
Records |
Links |
|
Author |
Pietra, F.; van Dijk-Moes, R.J.A.; Ke, X.; Bals, S.; Van Tendeloo, G.; de Mello Donega, C.; Vanmaekelbergh, D. |
|
| |
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 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
|
| |
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. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
Washington, D.C. |
Editor |
|
|
| |
Language |
|
Wos |
000330097900004 |
Publication Date |
2013-08-13 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
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 |
46 |
Open Access |
|
|
| |
Notes |
262348 ESMI; 246791 COUNTATOMS; Hercules |
Approved |
Most recent IF: 9.466; 2013 IF: 8.535 |
|
| |
Call Number |
UA @ lucian @ c:irua:110037 |
Serial |
3456 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Dendooven, J.; Goris, B.; Devloo-Casier, K.; Levrau, E.; Biermans, E.; Baklanov, M.R.; Ludwig, K.F.; van der Voort, P.; Bals, S.; Detavernier, C. |
|
| |
Title |
Tuning the pore size of ink-bottle mesopores by atomic layer deposition |
Type |
A1 Journal article |
| |
Year |
2012 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
|
| |
Volume |
24 |
Issue |
11 |
Pages |
1992-1994 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
|
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
Washington, D.C. |
Editor |
|
|
| |
Language |
|
Wos |
000305092600002 |
Publication Date |
2012-05-03 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
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 |
52 |
Open Access |
|
|
| |
Notes |
Fwo |
Approved |
Most recent IF: 9.466; 2012 IF: 8.238 |
|
| |
Call Number |
UA @ lucian @ c:irua:99078 |
Serial |
3760 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Altantzis, T.; Yang, Z.; Bals, S.; Van Tendeloo, G.; Pileni, M.-P. |
|
| |
Title |
Thermal Stability of CoAu13Binary Nanoparticle Superlattices under the Electron Beam |
Type |
A1 Journal article |
| |
Year |
2016 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
|
| |
Volume |
28 |
Issue |
28 |
Pages |
716-719 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
One primary goal of self-assembly in nanoscale regime is to implement multifunctional binary nanoparticle superlattices into practical use. In the last decade, considerable effort has been put into the fabrication of binary nanoparticle superlattices with controllable structure and stoichiometry. However, limited effort has been made in order to improve the stability of these binary nanoparticle superlattices, which is a prerequisite for their potential application. In this work, we demonstrate that the carbon deposition from specimen contamination can play an auxiliary role during the heat treatment of binary nanoparticle superlattices. With the in-situ carbon matrix formation, the thermal stability of CoAu 13 binary nanoparticle superlattices is unambiguously enhanced. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000370112200007 |
Publication Date |
2016-01-20 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
0897-4756 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
9.466 |
Times cited |
10 |
Open Access |
OpenAccess |
|
| |
Notes |
The research leading to these results has been supported by an Advanced Grant of the European Research Council under Grant 267129. The authors appreciate financial support by theEuropean Union under the Framework 7 program under a contract for an Integrated Infrastructure Initiative (Reference No. 262348 ESMI). S.B. acknowledges funding from ERC Starting Grant COLOURATOMS (335078).; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 9.466 |
|
| |
Call Number |
c:irua:131908 |
Serial |
4040 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Hill, E.H.; Claes, N.; Bals, S.; Liz-Marzán, L.M. |
|
| |
Title |
Layered Silicate Clays as Templates for Anisotropic Gold Nanoparticle Growth |
Type |
A1 Journal article |
| |
Year |
2016 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
|
| |
Volume |
28 |
Issue |
28 |
Pages |
5131-5139 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
|
| |
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. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000380576700031 |
Publication Date |
2016-07-02 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
0897-4756 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
9.466 |
Times cited |
13 |
Open Access |
OpenAccess |
|
| |
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 |
|
| |
Call Number |
c:irua:135178 c:irua:135178 |
Serial |
4117 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
van der Stam, W.; Gradmann, S.; Altantzis, T.; Ke, X.; Baldus, M.; Bals, S.; de Mello Donega, C. |
|
| |
Title |
Shape Control of Colloidal Cu2-x S Polyhedral Nanocrystals by Tuning the Nucleation Rates |
Type |
A1 Journal article |
| |
Year |
2016 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
|
| |
Volume |
28 |
Issue |
28 |
Pages |
6705-6715 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
Synthesis protocols for colloidal nanocrystals (NCs) with narrow size and shape distributions are of particular interest for the successful implementation of these nanocrystals into devices. Moreover, the preparation of NCs with well-defined crystal phases is of key importance. In this work, we show that Sn(IV)-thiolate complexes formed in situ strongly influence the nucleation and growth rates of colloidal Cu2-x S polyhedral NCs, thereby dictating their final size, shape, and crystal structure. This allowed us to successfully synthesize hexagonal bifrustums and hexagonal bipyramid NCs with low-chalcocite crystal structure, and hexagonal nanoplatelets with various thicknesses and aspect ratios with the djurleite crystal structure, by solely varying the concentration of Sn(IV)-additives (namely, SnBr4) in the reaction medium. Solution and solid-state 119Sn NMR measurements show that SnBr4 is converted in situ to Sn(IV)-thiolate complexes, which increase the Cu2-x S nucleation barrier without affecting the precursor conversion rates. This influences both the nucleation and growth rates in a concentration-dependent fashion and leads to a better separation between nucleation and growth. Our approach of tuning the nucleation and growth rates with in situ-generated Sn-thiolate complexes might have a more general impact due to the availability of various metal-thiolate complexes, possibly resulting in polyhedral NCs of a wide variety of metal-sulfide compositions. |
|
| |
Address |
Condensed Matter and Interfaces, Debye Institute for Nanomaterials Science, Utrecht University , P.O. Box 80000, 3508 TA Utrecht, The Netherlands |
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
English |
Wos |
000384399000037 |
Publication Date |
2016-09-02 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
0897-4756 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
9.466 |
Times cited |
27 |
Open Access |
OpenAccess |
|
| |
Notes |
W.v.d.S. and C.d.M.D. acknowledge financial support from the division of Chemical Sciences (CW) of The Netherlands Organization for Scientific Research (NWO) under grant number ECHO.712.012.001. M.B. also gratefully acknowledges NWO for funding the NMR infrastructure (Middle Groot program, grant number 700.58.102). S.B. acknowledges financial support from the European Research Council (ERC Starting Grant # 335078-COLOURATOMS).; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 9.466 |
|
| |
Call Number |
EMAT @ emat @ c:irua:135928 |
Serial |
4285 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Rodal-Cedeira, S.; Montes-García, V.; Polavarapu, L.; Solís, D.M.; Heidari, H.; La Porta, A.; Angiola, M.; Martucci, A.; Taboada, J.M.; Obelleiro, F.; Bals, S.; Pérez-Juste, J.; Pastoriza-Santos, I. |
|
| |
Title |
Plasmonic Au@Pd Nanorods with Boosted Refractive Index Susceptibility and SERS Efficiency: A Multifunctional Platform for Hydrogen Sensing and Monitoring of Catalytic Reactions |
Type |
A1 Journal article |
| |
Year |
2016 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
|
| |
Volume |
28 |
Issue |
28 |
Pages |
9169-9180 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
Palladium nanoparticles (NPs) have received tremendous attention over the years due to their high catalytic activity for various chemical reactions. However, unlike other noble metal nanoparticles such as Au and Ag NPs, they exhibit poor plasmonic properties with broad extinction spectra and less scattering efficiency, and thus limiting their applications in the field of plasmonics. Therefore, it has been challenging to integrate tunable and strong plasmonic properties into catalytic Pd nanoparticles. Here we show that plasmonic Au@Pd nanorods (NRs) with relatively narrow and remarkably tunable optical responses in the NIR region can be obtained by directional growth of Pd on penta-twinned Au NR seeds. We found the presence of bromide ions facilitates the stabilization of facets for the directional growth of Pd shell to obtain Au@Pd nanorods (NR) with controlled length scales. Interestingly, it turns out the Au NR supported Pd NRs exhibit much narrow extinction compared to pure Pd NRs, which makes them suitable for plasmonic sensing applications. Moreover, these nanostructures display, to the best of our knowledge, one of the highest ensemble refractive index sensitivity values reported to date (1067 nm per refractive index unit, RIU). Additionally, we showed the application of such plasmonic Au@Pd NRs for localized surface plasmon resonance (LSPR)-based sensing of hydrogen both in solution as well as on substrate. Finally, we demonstrate the integration of excellent plasmonic properties in catalytic palladium enables the in situ monitoring of a reaction progress by surface-enhanced Raman scattering. We postulate the proposed approach to boost the plasmonic properties of Pd nanoparticles will ignite the design of complex shaped plasmonic Pd NPs to be used in various plasmonic applications such as sensing and in situ monitoring of various chemical reactions. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000391080900036 |
Publication Date |
2016-12-27 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
0897-4756 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
9.466 |
Times cited |
80 |
Open Access |
OpenAccess |
|
| |
Notes |
Funding from Spanish Ministerio de Economía y Competitividad (Grants MAT2013-45168-R and MAT2016-77809-R) is gratefully acknowledge. A.L.P. and S.B. acknowledge support by the European Research Council through an ERC Starting Grant (#335078-COLOURATOMS). L. P. acknowledges the financial support from by the Alexander von Humboldt-Stiftung. V. M.-G. acknowledges the financial support from FPU scholarship from the Spanish MINECO. (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); ECAS_Sara |
Approved |
Most recent IF: 9.466 |
|
| |
Call Number |
EMAT @ emat @ c:irua:139513 |
Serial |
4344 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Peters, J.L.; van den Bos, K.H.W.; Van Aert, S.; Goris, B.; Bals, S.; Vanmaekelbergh, D. |
|
| |
Title |
Ligand-Induced Shape Transformation of PbSe Nanocrystals |
Type |
A1 Journal article |
| |
Year |
2017 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
|
| |
Volume |
29 |
Issue |
29 |
Pages |
4122-4128 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
We present a study of the relation between the surface chemistry and nanocrystal shape of PbSe nanocrystals with a variable Pb-to-Se stoichiometry and density of oleate ligands. The oleate ligand density and binding configuration are monitored by nuclear magnetic resonance and Fourier transform infrared absorbance spectroscopy, allowing us to quantify the number of surface-attached ligands per NC and the nature of the surface−Pb−oleate configuration. The three-dimensional shape of the PbSe nanocrystals is obtained from high-angle annular dark field scanning transmission electron microscopy combined with an atom counting method. We show that the enhanced oleate capping results in a stabilization and extension of the {111} facets, and a crystal shape transformation from a truncated nanocube to a truncated octahedron. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000401221700034 |
Publication Date |
2017-05-09 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
0897-4756 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
9.466 |
Times cited |
45 |
Open Access |
OpenAccess |
|
| |
Notes |
D.V. acknowledges the European Research Council, ERC advanced grant, Project 692691-First Step, for financial support. We also acknowledge the Dutch FOM programme “Designing Dirac carriers in honeycomb semiconductor superlattices” (FOM Program 152) for financial support. The authors gratefully acknowledge funding from the Research Foundation Flanders (G.036915, G.037413, and funding of a Ph.D. research grant to K.H.W.v.d.B. and a postdoctoral grant to B.G.). S.B. acknowledges the European Research Council, ERC Grant 335078-Colouratom. (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); ECAS_Sara |
Approved |
Most recent IF: 9.466 |
|
| |
Call Number |
EMAT @ emat @ c:irua:143750 c:irua:142983UA @ admin @ c:irua:143750 |
Serial |
4571 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Arias-Duque, C.; Bladt, E.; Munoz, M.A.; Hernandez-Garrido, J.C.; Cauqui, M.A.; Rodriguez-Izquierdo, J.M.; Blanco, G.; Bals, S.; Calvino, J.J.; Perez-Omil, J.A.; Yeste, M.P. |
|
| |
Title |
Improving the redox response stability of ceria-zirconia nanocatalysts under harsh temperature conditions |
Type |
A1 Journal article |
| |
Year |
2017 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
|
| |
Volume |
29 |
Issue |
29 |
Pages |
9340-9350 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
<script type='text/javascript'>document.write(unpmarked('By depositing ceria on the surface of yttrium stabilized zirconia (YSZ) nanocrystals and further activation under high-temperature reducing conditions, a 13% mol. CeO2/YSZ catalyst structured as subnanometer thick, pyrochlore-type, ceria-zirconia islands has been prepared. This nanostructured catalyst depicts not only high oxygen storage capacity (OSC) values but, more importantly, an outstandingly stable redox response upon oxidation and reduction treatments at very high temperatures, above 1000 degrees C. This behavior largely improves that observed on conventional ceria-zirconia solid solutions, not only of the same composition but also of those with much higher molar cerium contents. Advanced scanning transmission electron microscopy (STEM-XEDS) studies have revealed as key not only to detect the actual state of the lanthanide in this novel nanocatalyst but also to rationalize its unusual resistance to redox deactivation at very high temperatures. In particular, high-resolution X-ray dispersive energy studies have revealed the presence of unique bilayer ceria islands on top of the surface of YSZ nanocrystals, which remain at surface positions upon oxidation and reduction treatments up to 1000 degrees C. Diffusion of ceria into the bulk of these crystallites upon oxidation at 1100 degrees C irreversibly deteriorates both the reducibility and OSC of this nanostructured catalyst.')); |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
American Chemical Society |
Place of Publication |
Washington, D.C |
Editor |
|
|
| |
Language |
|
Wos |
000415911600047 |
Publication Date |
2017-10-10 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
0897-4756 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
9.466 |
Times cited |
20 |
Open Access |
OpenAccess |
|
| |
Notes |
; Financial support from MINECO/FEDER (Project ref: MAT2013-40823-R), Junta de Andalucia (FQM334 and FQM110), and EU FP7 (ESTEEM2) are acknowledged. E.B. and S.B. acknowledges financial support from European Research Council (ERC- Starting Grant #33S078-COLOURA-TOM). J.C.H.-G. acknowledges support from the Ramon y Cajal Fellowships Program of MINECO (RYC-2012-10004). ; |
Approved |
Most recent IF: 9.466 |
|
| |
Call Number |
UA @ lucian @ c:irua:147706UA @ admin @ c:irua:147706 |
Serial |
4880 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Berends, A.C.; van der Stam, W.; Hofmann, J.P.; Bladt, E.; Meeldijk, J.D.; Bals, S.; de Donega, C.M. |
|
| |
Title |
Interplay between surface chemistry, precursor reactivity, and temperature determines outcome of ZnS shelling reactions on CuInS2 nanocrystals |
Type |
A1 Journal article |
| |
Year |
2018 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
|
| |
Volume |
30 |
Issue |
30 |
Pages |
2400-2413 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
ZnS shelling of I-III-VI(2 )nanocrystals (NCs) invariably leads to blue-shifts in both the absorption and photoluminescence spectra. These observations imply that the outcome of ZnS shelling reactions on I-III-VI2 colloidal NCs results from a complex interplay between several processes taking place in solution, at the surface of, and within the seed NC. However, a fundamental understanding of the factors determining the balance between these different processes is still lacking. In this work, we address this need by investigating the impact of precursor reactivity, reaction temperature, and surface chemistry (due to the washing procedure) on the outcome of ZnS shelling reactions on CuInS2 NCs using a seeded growth approach. We demonstrate that low reaction temperatures (150 degrees C) favor etching, cation exchange, and alloying regardless of the precursors used. Heteroepitaxial shell overgrowth becomes the dominant process only if reactive S- and Zn-precursors (S-ODE/OLAM and ZnI2 ) and high reaction temperatures (210 degrees C) are used, although a certain degree of heterointerfacial alloying still occurs. Remarkably, the presence of residual acetate at the surface of CIS seed NCs washed with ethanol is shown to facilitate heteroepitaxial shell overgrowth, yielding for the first time CIS/ZnS core/shell NCs displaying red-shifted absorption spectra, in agreement with the spectral shifts expected for a type-I band alignment. The insights provided by this work pave the way toward the design of improved synthesis strategies to CIS/ZnS core/shell and alloy NCs with tailored elemental distribution profiles, allowing precise tuning of the optoelectronic properties of the resulting materials. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
American Chemical Society |
Place of Publication |
Washington, D.C |
Editor |
|
|
| |
Language |
|
Wos |
000430023700027 |
Publication Date |
2018-03-25 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
0897-4756 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
9.466 |
Times cited |
85 |
Open Access |
OpenAccess |
|
| |
Notes |
; Annelies van der Bok is gratefully acknowledged for performing the ICP measurements. A.C.B. and C.d.M.D. acknowledge financial support from the division of Chemical Sciences (CW) of The Netherlands Organization for Scientific Research (NWO) under Grant No. ECHO.712.014.001. S.B. and E.B. acknowledge financial support from European Research Council (ERC Starting Grant No. 335078-COLOURATOMS). ; Ecas_Sara |
Approved |
Most recent IF: 9.466 |
|
| |
Call Number |
UA @ lucian @ c:irua:150772UA @ admin @ c:irua:150772 |
Serial |
4972 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Peters, J.L.; Altantzis, T.; Lobato, I.; Jazi, M.A.; van Overbeek, C.; Bals, S.; Vanmaekelbergh, D.; Sinai, S.B. |
|
| |
Title |
Mono- and Multilayer Silicene-Type Honeycomb Lattices by Oriented Attachment of PbSe Nanocrystals: Synthesis, Structural Characterization, and Analysis of the Disorder |
Type |
A1 Journal article |
| |
Year |
2018 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
|
| |
Volume |
30 |
Issue |
30 |
Pages |
4831-4837 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
Nanocrystal (NC) solids are commonly prepared from nonpolar organic NC suspensions. In many cases, the capping on the NC surface is preserved and forms a barrier between the NCs. More recently, superstructures with crystalline connections between the NCs, implying the removal of the capping, have been reported, too. Here, we present large-scale uniform superstructures of attached PbSe NCs with a silicene-type honeycomb geometry, resulting from solvent evaporation under nearly reversible conditions. We also prepared multilayered silicene honeycomb structures by using larger amounts of PbSe NCs. We show that the two-dimensional silicene superstructures can be seen as a crystallographic slice from a 3-D simple cubic structure. We describe the disorder in the silicene lattices in terms of the nanocrystals position and their atomic alignment. The silicene honeycomb sheets are large enough to be used in transistors and optoelectronic devices. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000440105500042 |
Publication Date |
2018-07-24 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
0897-4756 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
9.466 |
Times cited |
33 |
Open Access |
OpenAccess |
|
| |
Notes |
The authors acknowledge funding from the European Commission (Grant EUSMI 731019). S.B. acknowledges funding from the European Research Council (Grant 335078 COLOURATOM). T.A. acknowledges a postdoctoral grant from the Research Foundation Flanders (FWO). The authors acknowledge financial support from the European Commission under the Horizon 2020 Programme by means of the Grant Agreement No. 731019 EUSMI. (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); ecas_sara |
Approved |
Most recent IF: 9.466 |
|
| |
Call Number |
EMAT @ emat @c:irua:152997UA @ admin @ c:irua:152997 |
Serial |
5011 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Van Tendeloo, L.; Wangermez, W.; Vandekerkhove, A.; Willhammar, T.; Bals, S.; Maes, A.; Martens, J.A.; Kirschhock, C.E.A.; Breynaert, E. |
|
| |
Title |
Postsynthetic high-alumina zeolite crystal engineering in organic free hyper-alkaline media |
Type |
A1 Journal article |
| |
Year |
2017 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
|
| |
Volume |
29 |
Issue |
29 |
Pages |
629-638 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
Postsynthetic modification of high -alumina zeolites in hyper alkaline media can be tailored toward alteration of framework topology, crystal size and morphology, or desired Si/A1 ratio. FAU, EMT, MAZ, KFI, HEU, and LTA starting materials were treated with 1.2 M MOH (M = Na, K, RE, or Cs), leading to systematic ordered porosity or fully transformed frameworks with new topology and adjustable Si/Al ratio. In addition to the versatility of this tool for zeolite crystal engineering, these alterations improve understanding of the crystal chemistry. Such knowledge can guide further development in zeolite crystal engineering. Postsynthetic alteration also provides insight on the long-term stability of aluminosilicate zeolites that are used as a sorption sink in concrete -based waste disposal facilities in harsh alkaline conditions. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
American Chemical Society |
Place of Publication |
Washington, D.C |
Editor |
|
|
| |
Language |
|
Wos |
000392891700021 |
Publication Date |
2016-12-20 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
0897-4756 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
9.466 |
Times cited |
16 |
Open Access |
OpenAccess |
|
| |
Notes |
; This work was supported by long-term structural funding by the Flemish Government (Methusalem grant of Prof. J. Martens) and by ONDRAF/NIRAS, the Belgian Agency for Radioactive Waste and Fissile Materials, as part of the program on surface disposal of Belgian Category A waste. The Belgian government is acknowledged for financing the interuniversity poles of attraction (IAP-PAI). S.B. acknowledges financial support from European Research Council (ERC Advanced Grant No. 24691-COUNTATOMS, ERC Starting Grant No. 335078-COLOURATOMS). ; Ecas_Sara |
Approved |
Most recent IF: 9.466 |
|
| |
Call Number |
UA @ lucian @ c:irua:152674UA @ admin @ c:irua:152674 |
Serial |
5145 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Tessier, M.D.; Baquero, E.A.; Dupont, D.; Grigel, V.; Bladt, E.; Bals, S.; Coppel, Y.; Hens, Z.; Nayral, C.; Delpech, F. |
|
| |
Title |
Interfacial oxidation and photoluminescence of InP-Based core/shell quantum dots |
Type |
A1 Journal article |
| |
Year |
2018 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
|
| |
Volume |
30 |
Issue |
30 |
Pages |
6877-6883 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
Indium phosphide colloidal quantum dots (QDs) are emerging as an efficient cadmium-free alternative for optoelectronic applications. Recently, syntheses based on easy-to-implement aminophosphine precursors have been developed. We show by solid-state nuclear magnetic resonance spectroscopy that this new approach allows oxide-free indium phosphide core or core/shell quantum dots to be made. Importantly, the oxide-free core/shell interface does not help in achieving higher luminescence efficiencies. We demonstrate that in the case of InP/ZnS and InP/ZnSe QDs, a more pronounced oxidation concurs with a higher photoluminescence efficiency. This study suggests that a II-VI shell on a III-V core generates an interface prone to defects. The most efficient InP/ZnS or InP/ZnSe QDs are therefore made with an oxide buffer layer between the core and the shell: it passivates these interface defects but also results in a somewhat broader emission line width. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
American Chemical Society |
Place of Publication |
Washington, D.C |
Editor |
|
|
| |
Language |
|
Wos |
000447237800031 |
Publication Date |
2018-09-12 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
0897-4756 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
9.466 |
Times cited |
74 |
Open Access |
OpenAccess |
|
| |
Notes |
; The authors thank L. Biadala and C. Delerue for fruitful discussion. Z.H. acknowledges support by the European Commission via the Marie-Sklodowska Curie action Phonsi (H2020-MSCA-ITN-642656), by Research Foundation Flanders (Project 17006602), and by Ghent University (GOA No. 01G01513). Z.H., M.D.T., and D.D. acknowledge the Strategisch Initiatief Materialen in Vlaanderen of Agentschap Innoveren en Ondernemen (SIM VLAIO), vzw (SBO-QDOCCO, ICON-QUALIDI). This work was supported by the Universite Paul Sabatier, the Region Midi-Pyrenees, the CNRS, the Institut National des Sciences Appliquees of Toulouse, and the Agence Nationale pour la Recherche (Project ANR-13-IS10-0004-01). E.A.B. is grateful to Marie Curie Actions and Campus France for a PRESTIGE postdoc fellowship (FP7 /2007-2013) under REA Grant Agreement PCOFUND-GA-2013-609102. E.B. acknowledges financial support from Research Foundation Flanders (FWO). ; |
Approved |
Most recent IF: 9.466 |
|
| |
Call Number |
UA @ lucian @ c:irua:154732UA @ admin @ c:irua:154732 |
Serial |
5109 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Akkerman, Q.A.; Bladt, E.; Petralanda, U.; Dang, Z.; Sartori, E.; Baranov, D.; Abdelhady, A.L.; Infante, I.; Bals, S.; Manna, L. |
|
| |
Title |
Fully inorganic Ruddlesden-Popper double CI-I and triple CI-Br-I lead halide perovskite nanocrystals |
Type |
A1 Journal article |
| |
Year |
2019 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
|
| |
Volume |
31 |
Issue |
31 |
Pages |
2182-2190 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
The vast majority of lead halide perovskite (LHP) nanocrystals (NCs) are currently based on either a single halide composition (CsPbCl3, CsPbBr3, and CsPbI3) or an alloyed mixture of bromide with either Cl- or I- [i.e., CsPb(Br:Cl)(3) or CsPb(Br:I)(3)]. In this work, we present the synthesis as well as a detailed optical and structural study of two halide alloying cases that have not previously been reported for LHP NCs: Cs2PbI2Cl2 NCs and triple halide CsPb(Cl:Br:I)(3) NCs. In the case of Cs2PbI2Cl2, we observe for the first time NCs with a fully inorganic Ruddlesden-Popper phase (RPP) crystal structure. Unlike the well-explored organic-inorganic RPP, here, the RPP formation is triggered by the size difference between the halide ions. These NCs exhibit a strong excitonic absorption, albeit with a weak photoluminescence quantum yield (PLQY). In the case of the triple halide CsPb(Cl:Br:I)(3) composition, the NCs comprise a CsPbBr2Cl perovskite crystal lattice with only a small amount of incorporated iodide, which segregates at RPP planes' interfaces within the CsPb(Cl:Br:I)(3) NCs. Supported by density functional theory calculations and postsynthetic surface treatments to enhance the PLQY, we show that the combination of iodide segregation and defective RPP interfaces are most likely linked to the strong PL quenching observed in these nanostructures. In summary, this work demonstrates the limits of halide alloying in LHP NCs because a mixture that contains halide ions of very different sizes leads to the formation of defective RPP interfaces and a severe quenching of LHP NC's optical properties. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000462950400038 |
Publication Date |
2019-03-04 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
0897-4756 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
9.466 |
Times cited |
58 |
Open Access |
OpenAccess |
|
| |
Notes |
; Q.A.A. and L.M. acknowledge funding from the European Union Seventh Framework Programme under grant agreement no. 614897 (ERC Consolidator Grant “TRANS-NANO”). The work of D.B. was supported by the European Union's Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie grant agreement no. 794560. E.B. and S.B. acknowledge funding from the Research Foundation Flanders (G.038116N, G.03691, and funding of a postdoctoral grant to E.B.). I.I. acknowledges The Netherlands Organization of Scientific Research (NWO) for financial support through the Innovational Research Incentive (Vidi) Scheme (grant no. 723.013.002). The computational work was carried out on the Dutch national e-infrastructure with the support of the SURF Cooperative. ; |
Approved |
Most recent IF: 9.466 |
|
| |
Call Number |
UA @ admin @ c:irua:159414 |
Serial |
5250 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Ramachandran, R.K.; Filez, M.; Solano, E.; Poelman, H.; Minjauw, M.M.; Van Daele, M.; Feng, J.-Y.; La Porta, A.; Altantzis, T.; Fonda, E.; Coati, A.; Garreau, Y.; Bals, S.; Marin, G.B.; Detavernier, C.; Dendooven, J. |
|
| |
Title |
Chemical and Structural Configuration of Pt Doped Metal Oxide Thin Films Prepared by Atomic Layer Deposition |
Type |
A1 Journal article |
| |
Year |
2019 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
|
| |
Volume |
31 |
Issue |
31 |
Pages |
9673-9683 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
|
| |
Abstract |
Pt doped semiconducting metal oxides and Pt metal clusters embedded in an oxide matrix are of interest for applications such as catalysis and gas sensing, energy storage and memory devices. Accurate tuning of the dopant level is crucial for adjusting the properties of these materials. Here, a novel atomic layer deposition (ALD) based method for doping Pt into In2O3 in specific, and metals in metal oxides in general, is demonstrated. This approach combines alternating exposures of Pt and In2O3 ALD processes in a single ‘supercycle’, followed by supercycle repetition leading to multilayered nanocomposites. The atomic level control of ALD and its conformal nature make the method suitable for accurate dopant control even on high surface area supports. Oxidation state, local structural environment and crystalline phase of the embedded Pt dopants were obtained by means of X-ray characterization methods and high angle annular dark-field scanning transmission electron microscopy (HAADF-STEM). In addition, this approach allows characterization of the nucleation stages of metal ALD processes, by stacking those states multiple times in an oxide matrix. Regardless of experimental conditions, a few Pt ALD cycles leads to the formation of oxidized Pt species due to their highly dispersed nature, as proven by X-ray absorption spectroscopy (XAS). Grazing-incidence small-angle X-ray scattering (GISAXS) and highresolution scanning transmission electron microscopy, combined with energy dispersive X-ray spectroscopy (HR-STEM/EDXS) show that Pt is evenly distributed in the In2O3 metal oxide matrix without the formation of clusters. For a larger number of Pt ALD
cycles, typ. > 10, the oxidation state gradually evolves towards fully metallic, and metallic Pt clusters are obtained within the In2O3 metal oxide matrix. This work reveals how tuning of the ALD supercycle approach for Pt doping allows controlled engineering of the Pt compositional and structural configuration within a metal oxide matrix. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000502418000010 |
Publication Date |
2019-11-11 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
0897-4756 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
9.466 |
Times cited |
6 |
Open Access |
OpenAccess |
|
| |
Notes |
This research was supported by the Flemish Research Foundation (FWO-Vlaanderen), the Flemish Government (Long term structural funding – Methusalem funding and Medium scale research infrastructure funding-Hercules funding), the Special Research Fund BOF of Ghent University (GOA 01G01513) and the CALIPSO Trans National Access Program funded by the European Commission in supplying financing of travel costs. We are grateful to the SIXS and SAMBA-SOLEIL staff for smoothly running the beamline facilities. J.D. and R.K.R. are postdoctoral fellows of the FWO. |
Approved |
Most recent IF: 9.466 |
|
| |
Call Number |
EMAT @ emat @c:irua:164056 |
Serial |
5380 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Kirkwood, N.; De Backer, A.; Altantzis, T.; Winckelmans, N.; Longo, A.; Antolinez, F.V.; Rabouw, F.T.; De Trizio, L.; Geuchies, J.J.; Mulder, J.T.; Renaud, N.; Bals, S.; Manna, L.; Houtepen, A.J. |
|
| |
Title |
Locating and controlling the Zn content in In(Zn)P quantum dots |
Type |
A1 Journal article |
| |
Year |
2019 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
|
| |
Volume |
32 |
Issue |
32 |
Pages |
557-565 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
Zinc is routinely employed in the synthesis of InP quantum dots (QDs) to improve the photoluminescence efficiency and carrier mobility of the resulting In(Zn)P alloy nanostructures. The exact location of Zn in the final structures and the mechanism by which it enhances the optoelectronic properties of the QDs is debated. We use synchrotron X-ray absorbance spectroscopy to show that the majority of Zn in In(Zn)P QDs is located at their surface as Zn-carboxylates. However, a small amount of Zn is present inside the bulk of the QDs with the consequent contraction of their lattice, as confirmed by combining high resolution high-angle annular dark-field imaging scanning transmission electron microscopy (HAADF-STEM) with statistical parameter estimation theory. We further demonstrate that the Zn content and its incorporation into the QDs can be tuned by the ligation of commonly employed Zn carboxylate precursors: the use of highly reactive Zn-acetate leads to the formation of undesired Zn3P2 and the final nanostructures being characterized by broad optical features, whereas Zn-carboxylates with longer carbon chains lead to InP crystals with much lower zinc content and narrow optical features. These results can explain the differences between structural and optical properties of In(Zn)P samples reported across the literature, and provide a rational method to tune the amount of Zn in InP nanocrystals and to drive the incorporation of Zn either as surface Zn-carboxylate, as a substitutional dopant inside the InP crystal lattice, or even predominantly as Zn3P2. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000507721600056 |
Publication Date |
2019-12-13 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
0897-4756 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
9.466 |
Times cited |
39 |
Open Access |
OpenAccess |
|
| |
Notes |
A.J.H. acknowledges support from the European Research Council Horizon 2020 ERC Grant Agreement No. 678004 (Doping on Demand). This research is supported by the Dutch Technology Foundation TTW, which is part of The Netherlands Organization for Scientific Research (NWO), and which is partly funded by Ministry of Economic Affairs. SB acknowledges funding from the European Research Council (grant 815128 REALNANO). The authors gratefully acknowledge funding from the Research Foundation Flanders (FWO, Belgium) through project funding G.0381.16N and a postdoctoral grant to A.D.B. AJH, LM and JM acknowledge support from the H2020 Collaborative Project TEQ (Grant No. 766900).; sygma |
Approved |
Most recent IF: 9.466 |
|
| |
Call Number |
EMAT @ emat @c:irua:165234 |
Serial |
5438 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Salzmann, B.B.V.; Vliem, J.F.; Maaskant, D.N.; Post, L.C.; Li, C.; Bals, S.; Vanmaekelbergh, D. |
|
| |
Title |
From CdSe nanoplatelets to quantum rings by thermochemical edge reconfiguration |
Type |
A1 Journal article |
| |
Year |
2021 |
Publication |
Chemistry Of Materials |
Abbreviated Journal |
Chem Mater |
|
| |
Volume |
33 |
Issue |
17 |
Pages |
6853-6859 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
The variation in the shape of colloidal semiconductor nanocrystals (NCs) remains intriguing. This interest goes beyond crystallography as the shape of the NC determines its energy levels and optoelectronic properties. While thermodynamic arguments point to a few or just a single shape(s), terminated by the most stable crystal facets, a remarkable variation in NC shape has been reported for many different compounds. For instance, for the well-studied case of CdSe, close-to-spherical quantum dots, rods, two-dimensional nanoplatelets, and quantum rings have been reported. Here, we report how two-dimensional CdSe nanoplatelets reshape into quantum rings. We monitor the reshaping in real time by combining atomically resolved structural characterization with optical absorption and photoluminescence spectroscopy. We observe that CdSe units leave the vertical sides of the edges and recrystallize on the top and bottom edges of the nanoplatelets, resulting in a thickening of the rims. The formation of a central hole, rendering the shape into a ring, only occurs at a more elevated temperature. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000696553600024 |
Publication Date |
2021-08-24 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
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 |
7 |
Open Access |
OpenAccess |
|
| |
Notes |
Hans Meeldijk is kindly acknowledged for helping with electron microscopy at Utrecht University. B.B.V.S. and D.V. acknowledge the Dutch NWO for financial support via the TOP-ECHO grant no. 715.016.002. D.V. acknowledges financial support from the European ERC Council, ERC Advanced grant 692691 “First Step”. D.V. and L.C.P. acknowledge the Dutch NWO for financial support via the TOP-ECHO grant nr. 718.015.002. S.B acknowledges financial support from the European ERC Council, ERC Consolidator grant 815128. This project has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement no. 731019 (EUSMI). Realnano; sygmaSB |
Approved |
Most recent IF: 9.466 |
|
| |
Call Number |
UA @ admin @ c:irua:181550 |
Serial |
6839 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Li, W.; Tong, W.; Yadav, A.; Bladt, E.; Bals, S.; Funston, A.M.; Etheridge, J. |
|
| |
Title |
Shape control beyond the seeds in gold nanoparticles |
Type |
A1 Journal article |
| |
Year |
2021 |
Publication |
Chemistry Of Materials |
Abbreviated Journal |
Chem Mater |
|
| |
Volume |
33 |
Issue |
23 |
Pages |
9152-9164 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
In typical seed-mediated syntheses of metal nanocrystals, the shape of the nanocrystal is determined largely by the seed nucleation environment and subsequent growth environment (where “environment” refers to the chemical environment, including the surfactant and additives). In this approach, crystallinity is typically determined by the seeds, and surfaces are controlled by the environment(s). However, surface energies, and crystallinity, are both influenced by the choice of environment(s). This limits the permutations of crystallinity and surface facets that can be mixed and matched to generate new nanocrystal morphologies. Here, we control post-seed growth to deliberately incorporate twin planes during the growth stage to deliver new final morphologies, including twinned cubes and bipyramids from single-crystal seeds. The nature and number of twin planes, together with surfactant control of facet growth, define the final nanoparticle morphology. Moreover, by breaking symmetry, the twin planes introduce new facet orientations. This additional mechanism opens new routes for the synthesis of different morphologies and facet orientations. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000753956100012 |
Publication Date |
0000-00-00 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
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 |
3 |
Open Access |
Not_Open_Access |
|
| |
Notes |
This work was supported by the Australian Research Council (ARC) Grants DP160104679 and CE170100026 and used microscopes at the Monash Centre for Electron Microscopy funded by ARC Grants LE0454166, LE110100223, and LE140100104. W.L. thanks the support of the Australian Government Research Training Program (RTP) scholarship. W.T. thanks the Australian Department of Education and Monash University for the IPRS and APA scholarships. E.B. acknowledges financial support and a post-doctoral grant from the Research Foundation Flanders (FWO, Belgium). The authors thank Dr. Matthew Weyland and Dr. Tim Peterson for helpful discussions. A.Y. thanks the support from Post Graduation Publication Award (PPA) scholarship from Monash University. |
Approved |
Most recent IF: 9.466 |
|
| |
Call Number |
UA @ admin @ c:irua:187229 |
Serial |
7065 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Ben Dkhil, S.; Perkhun, P.; Luo, C.; Mueller, D.; Alkarsifi, R.; Barulina, E.; Quiroz, Y.A.A.; Margeat, O.; Dubas, S.T.; Koganezawa, T.; Kuzuhara, D.; Yoshimoto, N.; Caddeo, C.; Mattoni, A.; Zimmermann, B.; Wuerfel, U.; Pfannmöller, M.; Bals, S.; Ackermann, J.; Videlot-Ackermann, C. |
|
| |
Title |
Direct correlation of nanoscale morphology and device performance to study photocurrent generation in donor-enriched phases of polymer solar cells |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Acs Applied Materials & Interfaces |
Abbreviated Journal |
Acs Appl Mater Inter |
|
| |
Volume |
12 |
Issue |
25 |
Pages |
28404-28415 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
The nanoscale morphology of polymer blends is a key parameter to reach high efficiency in bulk heterojunction solar cells. Thereby, research typically focusing on optimal blend morphologies while studying nonoptimized blends may give insight into blend designs that can prove more robust against morphology defects. Here, we focus on the direct correlation of morphology and device performance of thieno[3,4-b]-thiophene-alt-benzodithiophene (PTB7):[6,6]phenyl C-71 butyric acid methyl ester (PC71BM) bulk heterojunction (BHJ) blends processed without additives in different donor/acceptor weight ratios. We show that while blends of a 1:1.5 ratio are composed of large donor-enriched and fullerene domains beyond the exciton diffusion length, reducing the ratio below 1:0.5 leads to blends composed purely of polymer-enriched domains. Importantly, the photocurrent density in such blends can reach values between 45 and 60% of those reached for fully optimized blends using additives. We provide here direct visual evidence that fullerenes in the donor-enriched domains are not distributed homogeneously but fluctuate locally. To this end, we performed compositional nanoscale morphology analysis of the blend using spectroscopic imaging of low-energy-loss electrons using a transmission electron microscope. Charge transport measurement in combination with molecular dynamics simulations shows that the fullerene substructures inside the polymer phase generate efficient electron transport in the polymer-enriched phase. Furthermore, we show that the formation of densely packed regions of fullerene inside the polymer phase is driven by the PTB7:PC71BM enthalpy of mixing. The occurrence of such a nanoscale network of fullerene clusters leads to a reduction of electron trap states and thus efficient extraction of photocurrent inside the polymer domain. Suitable tuning of the polymer-acceptor interaction can thus introduce acceptor subnetworks in polymer-enriched phases, improving the tolerance for high-efficiency BHJ toward morphological defects such as donor-enriched domains exceeding the exciton diffusion length. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000543780900058 |
Publication Date |
2020-06-01 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
1944-8244 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
9.5 |
Times cited |
7 |
Open Access |
OpenAccess |
|
| |
Notes |
; J.A., O.M., and C.V.-A. acknowledge financial support by the French Fond Unique Interministeriel (FUI) under the project “SFUMATO” (Grant Number: F1110019V/ 201308815) as well as by the European Commission under the Project “SUNFLOWER” (FP7-ICT-2011-7, Grant Number: 287594). J.A., C.V.-A., and E.B. acknowledge the Association Nationale de la Recherche et de la Technologie (ANRT) and the Ministere de l'Enseignement Superieur, de la Recherche et de l'Innovation, awarded through the company Dracula Technologies (Valence, France), for framework of a CIFRE Ph.D. grant 2017/0529. J.A. and P.P. received funding from the European Union's Horizon 2020 research and innovation program under the Marie Sklodowska-Curie Grant agreement no. 713750. They further acknowledge support of the Regional Council of Provence-Alpes-Cote d'Azur, A*MIDEX (no. ANR-11-IDEX-0001-02), and the Investissements d'Avenir project funded by the French Government, managed by the French National Research Agency (ANR). J.A. and Y.A.A.Q. acknowledge the French Research Agency for funding through the project NFA-15 (ANR-17-CE05-0020-01). N.Y. acknowledges that the synchrotron radiation experiments were performed at BL19B2 in SPring-8 with the approval of Japan Synchrotron Radiation Research Institute (JASRI) (proposal nos. 2017B1629 and 2018B1791). S.B. acknowledges financial support from the European Research Council (ERC Consolidator Grant 815128-REALNANO) and from FWO (G.0381.16N). M.P. gratefully acknowledges funding by the Ministerium fur Wissenschaft, Forschung und Kunst Baden-Wurttemberg through the HEiKA materials research centre FunTECH-3D (MWK, 33-753-30-20/3/3) and the Large-Scale-Data-Facility (LSDF) sds@hd through grant INST 35/1314-1 FUGG. A.M. acknowledges Italian MIUR for funding through the project PON04a2 00490 M2M Netergit, PRACE, for awarding access to Marconi KNL at CINECA, Italy, through projects DECONVOLVES (2018184466) and PROVING-IL (2019204911). C.C. acknowledges the CINECA award under the ISCRA initiative for the availability of high-performance computing resources and support (project MITOMASC). ; sygma |
Approved |
Most recent IF: 9.5; 2020 IF: 7.504 |
|
| |
Call Number |
UA @ admin @ c:irua:170703 |
Serial |
6484 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Kertik, A.; Wee, L.H.; Şentosun, K.; Navarro, J.A.R.; Bals, S.; Martens, J.A.; Vankelecom, I.F.J. |
|
| |
Title |
High-performance CO2-selective hybrid membranes by exploiting MOF-breathing effects |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Acs Applied Materials & Interfaces |
Abbreviated Journal |
Acs Appl Mater Inter |
|
| |
Volume |
12 |
Issue |
2 |
Pages |
2952-2961 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
Conventional CO2 separation in the petrochemical industry via cryogenic distillation or amine-based absorber-stripper units is energy-intensive and environmentally unfriendly. Membrane-based gas separation technology, in contrast, has contributed significantly to the development of energy-efficient systems for processes such as natural gas purification. The implementation of commercial polymeric membranes in gas separation processes is restricted by their permeability-selectivity trade-off and by their insufficient thermal and chemical stability. Herein, we present the fabrication of a Matrimid-based membrane loaded with a breathing metal-organic framework (MOF) (NH2-MIL-53(Al)) which is capable of separating binary CO2/CH4 gas mixtures with high selectivities without sacrificing much of its CO2 permeabilities. NH2-MIL-53(Al) crystals were embedded in a polyimide (PI) matrix, and the mixed-matrix membranes (MMMs) were treated at elevated temperatures (up to 350 degrees C) in air to trigger PI cross-linking and to create PI-MOF bonds at the interface to effectively seal the grain boundary. Most importantly, the MOF transitions from its narrow-pore form to its large-pore form during this treatment, which allows the PI chains to partly penetrate the pores and cross-link with the amino functions at the pore mouth of the NH2-MIL-53(Al) and stabilizes the open-pore form of NH2-MIL-53(Al). This cross-linked MMM, with MOF pore entrances was made more selective by the anchored PI-chains and achieves outstanding CO2/CH4 selectivities. This approach provides significant advancement toward the design of selective MMMs with enhanced thermal and chemical stabilities which could also be applicable for other potential applications, such as separation of hydrocarbons (olefin/paraffin or isomers), pervaporation, and solvent-resistant nanofiltration. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000508464500108 |
Publication Date |
2019-12-20 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
1944-8244 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
9.5 |
Times cited |
26 |
Open Access |
OpenAccess |
|
| |
Notes |
; A.K. is grateful to the Erasmus Mundus Doctorate in Membrane Engineering (EUDIME) programme. L.H.W. thanks the FWO-Vlaanderen for a postdoctoral research fellowships under contract number 12M1418N. We thank Methusalem and IAP-PAI for research funding. S.B. acknowledges financial support from European Research Council (ERC) (ERC Starting Grant No. 335078-COLOURATOM). We are also grateful to Frank Mathijs (KU Leuven) for the mechanical tests, Bart Goderis and Olivier Verkinderen for the DSC measurements, and Huntsman (Switzerland) for providing the Matrimid polymer. ; |
Approved |
Most recent IF: 9.5; 2020 IF: 7.504 |
|
| |
Call Number |
UA @ admin @ c:irua:166576 |
Serial |
6534 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Bhatia, H.; Martin, C.; Keshavarz, M.; Dovgaliuk, I.; Schrenker, N.J.; Ottesen, M.; Qiu, W.; Fron, E.; Bremholm, M.; Van de Vondel, J.; Bals, S.; Roeffaers, M.B.J.; Hofkens, J.; Debroye, E. |
|
| |
Title |
Deciphering the role of water in promoting the optoelectronic performance of surface-engineered lead halide perovskite nanocrystals |
Type |
A1 Journal article |
| |
Year |
2023 |
Publication |
ACS applied materials and interfaces |
Abbreviated Journal |
|
|
| |
Volume |
15 |
Issue |
5 |
Pages |
7294-7307 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
Lead halide perovskites are promising candidates for applicability is limited by their structural instability toward moisture. Although a deliberate addition of water to the precursor solution has recently been shown to improve the crystallinity and optical properties of perovskites, the corresponding thin films still do not exhibit a near-unity quantum yield. Herein, we report that the direct addition of a minute amount of water to post-treated substantially enhances the stability while achieving a 95% photoluminescence quantum yield in a NC thin film. We unveil the mechanism of how moisture assists in the formation of an additional NH4Br component. Alongside, we demonstrate the crucial role of moisture in assisting localized etching of the perovskite crystal, facilitating the partial incorporation of NH4+, which is key for improved performance under ambient conditions. Finally, as a proof-of-concept, the application of post-treated and watertreated perovskites is tested in LEDs, with the latter exhibiting a superior performance, offering opportunities toward commercial application in moisture-stable optoelectronics. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000931729400001 |
Publication Date |
2023-01-27 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
1944-8244 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
9.5 |
Times cited |
3 |
Open Access |
Not_Open_Access |
|
| |
Notes |
H.B. would like to express her sincere gratitude to Dr. Peter Erk (formerly BASF SE, Germany) for very insightful discussions. The authors acknowledge financial support from the Research Foundation-Flanders (FWO grant numbers S002019N, 1514220N, G.0B39.15, G.0B49.15, G098319N, and ZW15_09-GOH6316) , the KU Leuven Research Fund (C14/19/079, iBOF-21-085 PERSIST, and STG/21/010) , the Flemish government through long-term structural funding Methusalem (CASAS2, Meth/15/04) , the Hercules Founda-tion (HER/11/14) , and the ERC through the Marie Curie ITN iSwitch Ph.D. fellowship to H.B. (grant number 642196) . C.M. acknowledges the financial support from grants PID2021-128761OA-C22 funded by MCIN/AEI/10.13039/501100011033 by the ?European Union? and SBPLY/21/180501/000127 funded by JCCM and by the EU through Fondo Europeo de Desarollo Regional? (FEDER) . Martin Bremholm and Martin Ottesen acknowledge funding from the Danish Council for Independent Research, Natural Sciences, under the Sapere Aude program (grant no. 7027-00077B) and VILLUM FONDEN through the Centre of Excellence for Dirac Materials (grant no. 11744) . Affiliation with the Center for Integrated Materials Research (iMAT) at Aarhus University is gratefully acknowledged.-N.J.S. acknowledges financial support from the research foundation Flanders (FWO) through a postdoctoral fellowship (FWO grant no. 1238622N) . S.B. acknowledges financial support from the European Commission by the ERC Consolidator grant REALNANO (no. 815128) . |
Approved |
Most recent IF: 9.5; 2023 IF: 7.504 |
|
| |
Call Number |
UA @ admin @ c:irua:195375 |
Serial |
7293 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Mulder, J.T.; Meijer, M.S.; van Blaaderen, J.J.; du Fosse, I.; Jenkinson, K.; Bals, S.; Manna, L.; Houtepen, A.J. |
|
| |
Title |
Understanding and preventing photoluminescence quenching to achieve unity photoluminescence quantum yield in Yb:YLF nanocrystals |
Type |
A1 Journal article |
| |
Year |
2023 |
Publication |
ACS applied materials and interfaces |
Abbreviated Journal |
|
|
| |
Volume |
15 |
Issue |
2 |
Pages |
3274-3286 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
Ytterbium-doped LiYF4 (Yb:YLF) is a commonly used material for laser applications, as a photon upconversion medium, and for optical refrigeration. As nanocrystals (NCs), the material is also of interest for biological and physical applications. Unfortunately, as with most phosphors, with the reduction in size comes a large reduction of the photoluminescence quantum yield (PLQY), which is typically associated with an increase in surface-related PL quenching. Here, we report the synthesis of bipyramidal Yb:YLF NCs with a short axis of similar to 60 nm. We systematically study and remove all sources of PL quenching in these NCs. By chemically removing all traces of water from the reaction mixture, we obtain NCs that exhibit a near-unity PLQY for an Yb3+ concentration below 20%. At higher Yb3+ concentrations, efficient concentration quenching occurs. The surface PL quenching is mitigated by growing an undoped YLF shell around the NC core, resulting in near-unity PLQY values even for fully Yb3+-based LiYbF4 cores. This unambiguously shows that the only remaining quenching sites in core-only Yb:YLF NCs reside on the surface and that concentration quenching is due to energy transfer to the surface. Monte Carlo simulations can reproduce the concentration dependence of the PLQY. Surprisingly, Fo''rster resonance energy transfer does not give satisfactory agreement with the experimental data, whereas nearest-neighbor energy transfer does. This work demonstrates that Yb3+-based nanophosphors can be synthesized with a quality close to that of bulk single crystals. The high Yb3+ concentration in the LiYbF4/LiYF4 core/shell nanocrystals increases the weak Yb3+ absorption, making these materials highly promising for fundamental studies and increasing their effectiveness in bioapplications and optical refrigeration. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000912997300001 |
Publication Date |
2023-01-06 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
1944-8244 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
9.5 |
Times cited |
3 |
Open Access |
OpenAccess |
|
| |
Notes |
This project has received funding from the European Union's Horizon 2020 research and innovation program under Grant Agreement No. 766900 (Testing the Large-Scale Limit of Quantum Mechanics). A.J.H. and I.d.F. further acknowledge the European Research Council Horizon 2020 ERC Grant Agreement No. 678004 (Doping on Demand) for financial support. The authors thank Freddy Rabouw and Andries Meijerink (Utrecht University) for very fruitful discussions and extremely useful advice. The author s thank Jos Thieme for his help with the laser setups used . The authors furthermore thank Niranjan Saikumar for proofreading the manuscript. |
Approved |
Most recent IF: 9.5; 2023 IF: 7.504 |
|
| |
Call Number |
UA @ admin @ c:irua:194317 |
Serial |
7348 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Van den Hoek, J.; Daems, N.; Arnouts, S.; Hoekx, S.; Bals, S.; Breugelmans, T. |
|
| |
Title |
Improving stability of CO₂ electroreduction by incorporating Ag NPs in N-doped ordered mesoporous carbon structures |
Type |
A1 Journal article |
| |
Year |
2024 |
Publication |
ACS applied materials and interfaces |
Abbreviated Journal |
|
|
| |
Volume |
16 |
Issue |
6 |
Pages |
6931-6947 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
|
| |
Abstract |
The electroreduction of carbon dioxide (eCO2RR) to CO using Ag nanoparticles as an electrocatalyst is promising as an industrial carbon capture and utilization (CCU) technique to mitigate CO2 emissions. Nevertheless, the long-term stability of these Ag nanoparticles has been insufficient despite initial high Faradaic efficiencies and/or partial current densities. To improve the stability, we evaluated an up-scalable and easily tunable synthesis route to deposit low-weight percentages of Ag nanoparticles (NPs) on and into the framework of a nitrogen-doped ordered mesoporous carbon (NOMC) structure. By exploiting this so-called nanoparticle confinement strategy, the nanoparticle mobility under operation is strongly reduced. As a result, particle detachment and agglomeration, two of the most pronounced electrocatalytic degradation mechanisms, are (partially) blocked and catalyst durability is improved. Several synthesis parameters, such as the anchoring agent, the weight percentage of Ag NPs, and the type of carbonaceous support material, were modified in a controlled manner to evaluate their respective impact on the overall electrochemical performance, with a strong emphasis on operational stability. The resulting powders were evaluated through electrochemical and physicochemical characterization methods, including X-ray diffraction (XRD), N2-physisorption, Inductively coupled plasma mass spectrometry (ICP-MS), scanning electron microscopy (SEM), SEM-energy-dispersive X-ray spectroscopy (SEM-EDS), high-angle annular dark field scanning transmission electron microscopy (HAADF-STEM), STEM-EDS, electron tomography, and X-ray photoelectron spectroscopy (XPS). The optimized Ag/soft-NOMC catalysts showed both a promising selectivity (∼80%) and stability compared with commercial Ag NPs while decreasing the loading of the transition metal by more than 50%. The stability of both the 5 and 10 wt % Ag/soft-NOMC catalysts showed considerable improvements by anchoring the Ag NPs on and into a NOMC framework, resulting in a 267% improvement in CO selectivity after 72 h (despite initial losses) compared to commercial Ag NPs. These results demonstrate the promising strategy of anchoring Ag NPs to improve the CO selectivity during prolonged experiments due to the reduced mobility of the Ag NPs and thus enhanced stability. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
001158812100001 |
Publication Date |
2023-12-21 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
1944-8244 |
ISBN |
|
Additional Links |
UA library record; WoS full record |
|
| |
Impact Factor |
9.5 |
Times cited |
|
Open Access |
Not_Open_Access: Available from 21.06.2024 |
|
| |
Notes |
|
Approved |
Most recent IF: 9.5; 2024 IF: 7.504 |
|
| |
Call Number |
UA @ admin @ c:irua:202309 |
Serial |
9045 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Guerrero, R.M.; Lemir, I.D.; Carrasco, S.; Fernández-Ruiz, C.; Kavak, S.; Pizarro, P.; Serrano, D.P.; Bals, S.; Horcajada, P.; Pérez, Y. |
|
| |
Title |
Scaling-Up Microwave-Assisted Synthesis of Highly Defective Pd@UiO-66-NH2Catalysts for Selective Olefin Hydrogenation under Ambient Conditions |
Type |
A1 Journal Article |
| |
Year |
2024 |
Publication |
ACS Applied Materials & Interfaces |
Abbreviated Journal |
ACS Appl. Mater. Interfaces |
|
| |
Volume |
|
Issue |
|
Pages |
|
|
| |
Keywords |
A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; |
|
| |
Abstract |
The need to develop green and cost-effective industrial catalytic processes has led to growing interest in preparing more robust, efficient, and selective heterogeneous catalysts at a large scale. In this regard, microwave-assisted synthesis is a fast method for fabricating heterogeneous catalysts (including metal oxides, zeolites, metal–organic frameworks, and supported metal nanoparticles) with enhanced catalytic properties, enabling synthesis scale-up. Herein, the synthesis of nanosized UiO-66-NH2 was optimized via a microwave-assisted hydrothermal method to obtain defective matrices essential for the stabilization of metal nanoparticles, promoting catalytically active sites for hydrogenation reactions (760 kg·m–3·day–1 space time yield, STY). Then, this protocol was scaled up in a multimodal microwave reactor, reaching 86% yield (ca. 1 g, 1450 kg·m–3·day–1 STY) in only 30 min. Afterward, Pd nanoparticles were formed in situ decorating the nanoMOF by an effective and fast microwave-assisted hydrothermal method, resulting in the formation of Pd@UiO-66-NH2 composites. Both the localization and oxidation states of Pd nanoparticles (NPs) in the MOF were achieved using high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and X-ray photoelectron spectroscopy (XPS), respectively. The optimal composite, loaded with 1.7 wt % Pd, exhibited an extraordinary catalytic activity (>95% yield, 100% selectivity) under mild conditions (1 bar H2, 25 °C, 1 h reaction time), not only in the selective hydrogenation of a variety of single alkenes (1-hexene, 1-octene, 1-tridecene, cyclohexene, and tetraphenyl ethylene) but also in the conversion of a complex mixture of alkenes (i.e., 1-hexene, 1-tridecene, and anethole). The results showed a powerful interaction and synergy between the active phase (Pd NPs) and the catalytic porous scaffold (UiO-66-NH2), which are essential for the selectivity and recyclability. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
|
Publication Date |
2024-04-26 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
1944-8244 |
ISBN |
|
Additional Links |
|
|
| |
Impact Factor |
9.5 |
Times cited |
|
Open Access |
|
|
| |
Notes |
The authors gratefully acknowledge financial support from “Comunidad de Madrid” and European Regional Development Fund-FEDER through the project HUB MADRID+CIRCULAR; the State Research Agency (MCIN/AEI /10.13039/501100011033) through the grant with reference number CEX2019-000931-M received in the 2019 call for “Severo Ochoa Centres of Excellence” and “María de Maeztu Units of Excellence” of the State Programme for Knowledge Generation and Scientific and Technological Strengthening of the R&D&I System; and MICIU through the project “NAPOLION” (PID2022-139956OB-I00). S.K. acknowledges the Flemish Fund for Scientific Research (FWO Vlaanderen) through a PhD research grant (1181124N). |
Approved |
Most recent IF: 9.5; 2024 IF: 7.504 |
|
| |
Call Number |
EMAT @ emat @ |
Serial |
9126 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Kumar, J.; Eraña, H.; López-Martínez, E.; Claes, N.; Martín, V.F.; Solís, D.M.; Bals, S.; Cortajarena, A.L.; Castilla, J.; Liz-Marzán, L.M. |
|
| |
Title |
Detection of amyloid fibrils in Parkinson’s disease using plasmonic chirality |
Type |
A1 Journal article |
| |
Year |
2018 |
Publication |
Proceedings of the National Academy of Sciences of the United States of America |
Abbreviated Journal |
P Natl Acad Sci Usa |
|
| |
Volume |
115 |
Issue |
115 |
Pages |
3225-3230 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
Amyloid fibrils, which are closely associated with various neurodegenerative
diseases, are the final products in many protein aggregation pathways. The identification of fibrils at low concentration is, therefore, pivotal in disease diagnosis and development of therapeutic strategies. We report a methodology for the specific identification of amyloid fibrils using chiroptical effects in plasmonic nanoparticles. The formation of amyloid fibrils based on α-synuclein was probed using gold nanorods, which showed no
apparent interaction with monomeric proteins but effective adsorption onto fibril structures via noncovalent interactions. The amyloid structure drives a helical nanorod arrangement, resulting in intense optical activity at the surface plasmon resonance wavelengths. This sensing technique was successfully applied to human brain homogenates of patients affected by Parkinson’s disease,
wherein protein fibrils related to the disease were identified through chiral signals from Au nanorods in the visible and near IR, whereas healthy brain samples did not exhibit any meaningful optical activity. The technique was additionally extended to the specific detection of infectious amyloids formed by prion proteins, thereby confirming the wide potential of the technique. The intense chiral response driven by strong dipolar coupling in helical Au nanorod arrangements allowed us to detect amyloid fibrils down to nanomolar concentrations. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000428382400032 |
Publication Date |
2018-03-12 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
0027-8424 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
9.661 |
Times cited |
187 |
Open Access |
OpenAccess |
|
| |
Notes |
We thank Prof. Dr. J.-P. Timmermans and the Antwerp Centre of Advanced Microscopy for providing access to the Tecnai G2 Spirit BioTWIN TEM. We also thank the Basque Biobank (Basque Foundation for Health Innovation and Research, BIOEF) for providing us with Parkinson’s disease-affected brain samples. J.K. acknowledges financial support from the European Commission under Marie Sklodowska-Curie Program H2020- MSCA-IF-2015708321. S.B. and A.L.C. acknowledge European Research Council Grants 335078 COLOURATOM and 648071 ProNANO. S.B. and L.M.L.-M. acknowledge funding from European Commission Grant EUSMI 731019. A.L.C., J.C., and L.M.L.-M. acknowledge funding from Spanish Ministry of Economy and Competitiveness (MINECO) Grants MAT2013-46101- R, AGL2015-65046-C2-1-R, and BIO2016-77367-C2-1-R. (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:restricted); saraecas; ECASSara; |
Approved |
Most recent IF: 9.661 |
|
| |
Call Number |
EMAT @ emat @c:irua:150355UA @ admin @ c:irua:150355 |
Serial |
4918 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Windels, S.; Diefenhardt, T.; Jain, N.; Marquez, C.; Bals, S.; Schlummer, M.; De Vos, D.E. |
|
| |
Title |
Catalytic upcycling of PVC waste-derived phthalate esters into safe, hydrogenated plasticizers |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
Green chemistry : cutting-edge research for a greener sustainable future |
Abbreviated Journal |
Green Chem |
|
| |
Volume |
24 |
Issue |
2 |
Pages |
754-766 |
|
| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
Recycling of end-of-life polyvinyl chloride (PVC) calls for solutions to deal with the vast amounts of harmful phthalate plasticizers that have historically been incorporated in PVC. Here, we report on the upcycling of such waste-extracted phthalate esters into analogues of the much safer diisononyl 1,2-cyclohexanedicarboxylate plasticizer (DINCH), via a catalytic one-pot (trans)esterification-hydrogenation process. For most of the virgin phthalates, Ru/Al2O3 is a highly effective hydrogenation catalyst, yielding >99% ring-hydrogenated products under mild reaction conditions (0.1 mol% Ru, 80 degrees C, 50 bar H-2). However, applying this reaction to PVC-extracted phthalates proved problematic, (1) as benzyl phthalates are hydrogenolyzed to benzoic acids that inhibit the Ru-catalyst, and (2) because impurities in the plasticizer extract (PVC, sulfur) further retard the hydrogenation. These complications were solved by coupling the hydrogenation to an in situ (trans)esterification with a higher alcohol, and by pretreating the extract with an activated carbon adsorbent. In this way, a real phthalate extract obtained from post-consumer PVC waste was eventually completely (>99%) hydrogenated to phthalate-free, cycloaliphatic plasticizers. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000726865200001 |
Publication Date |
2021-11-30 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
1463-9262; 1463-9270 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
9.8 |
Times cited |
8 |
Open Access |
Not_Open_Access |
|
| |
Notes |
This project has received funding from the European Union’s Horizon 2020 Research and Innovation Programme under grant agreement no. 821366 (programma acronym: Circular Flooring). D. E. D. V. thanks FWO for project funding (SBO project S001819N Triple Cycle); N. J. and S. B. acknowledge the financial support from FWO and FNRS (EOS 30489208). Finally, the authors also thank S. Smolders for assistance with the TGA-MS experiments and D. Paredaens for his experimental contribution |
Approved |
Most recent IF: 9.8 |
|
| |
Call Number |
UA @ admin @ c:irua:184746 |
Serial |
6958 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Carrasco, S.; Orcajo, G.; Martínez, F.; Imaz, I.; Kavak, S.; Arenas-Esteban, D.; Maspoch, D.; Bals, S.; Calleja, G.; Horcajada, P. |
|
| |
Title |
Hf/porphyrin-based metal-organic framework PCN-224 for CO2 cycloaddition with epoxides |
Type |
A1 Journal article |
| |
Year |
2023 |
Publication |
Materials Today Advances |
Abbreviated Journal |
|
|
| |
Volume |
19 |
Issue |
|
Pages |
100390 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
Herein, we describe for the first time the synthesis of the highly porous Hf-tetracarboxylate porphyrin-based metal-organic framework (MOF) (Hf)PCN-224(M) (M = H2, Co2+). (Hf)PCN-224(H2) was easily and efficiently prepared following a simple microwave-assisted procedure with good yields (56–67%; space-time yields: 1100–1270 kg m−3·day−1), high crystallinity and phase purity by using trifluoromethanesulfonic acid and benzoic acid as modulators in less than 30 min. By simply introducing a preliminary step (10 min), 5,10,15,20-(tetra-4-carboxyphenyl)porphyrin linker (TCPP) was quantitatively metalated with Co2+ without additional purification and/or time consuming protection/deprotection steps to further obtain (Hf)PCN-224(Co). (Hf)PCN-224(Co) was then tested as catalyst in CO2 cycloaddition reaction with different epoxides to yield cyclic carbonates, showing the best catalytic performance described to date compared to other PCNs, under mild conditions (1 bar CO2, room temperature, 18–24 h). Twelve epoxides were tested, obtaining from moderate to excellent conversions (35–96%). Moreover, this reaction was gram scaled-up (x50) without significant loss of yield to cyclic carbonates. (Hf)PCN-224(Co) maintained its integrity and crystallinity even after 8 consecutive runs, and poisoning was efficiently reverted by a simple thermal treatment (175 °C, 6 h), fully recovering the initial catalytic activity. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
001025764000001 |
Publication Date |
2023-06-19 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
2590-0498 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
10 |
Times cited |
1 |
Open Access |
OpenAccess |
|
| |
Notes |
S.C. acknowledges the European Union's Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie (MSCA-COFUND) grant agreement No 754382 (GOT Energy Talent). S.C. and P.H. acknowledge “Comunidad de Madrid” and European Regional Development Fund-FEDER 2014-2020-OE REACT-UE 1 for their financial support to VIRMOF-CM project associated to R&D projects in response to COVID-19. The authors acknowledge H2020-MSCA-ITN-2019 HeatNMof (ref. 860942), the M-ERA-NET C-MOF-cell (grant PCI2020-111998 funded by MCIN/AEI /10.13039/501100011033 and European Union NextGenerationEU/PRTR) project, and Retos Investigación MOFSEIDON (grant PID2019-104228RB-I00 funded by MCIN/AEI/10.13039/501100011033) project. This work has been also supported by the Regional Government of Madrid (Project ACES2030-CM, S2018/EMT-4319) and the Universidad Rey Juan Carlos IMPULSO Project (grant MATER M − 3000). S.K acknowledges the Flemish Fund for Scientific Research (FWO Vlaanderen) through a PhD research grant (1181122 N). |
Approved |
Most recent IF: 10; 2023 IF: NA |
|
| |
Call Number |
EMAT @ emat @c:irua:197198 |
Serial |
8800 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Ennaert, T.; Geboers, J.; Gobechiya, E.; Courtin, C.M.; Kurttepeli, M.; Houthoofd, K.; Kirschhock, C.E.A.; Magusin, P.C.M.M.; Bals, S.; Jacobs, P.A.; Sels, B.F. |
|
| |
Title |
Conceptual frame rationalizing the self-stabilization of H-USY zeolites in hot liquid water |
Type |
A1 Journal article |
| |
Year |
2015 |
Publication |
ACS catalysis |
Abbreviated Journal |
Acs Catal |
|
| |
Volume |
5 |
Issue |
5 |
Pages |
754-768 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
The wide range of liquid-phase reactions required for the catalytic conversion of biomass compounds into new bioplatform molecules defines a new set of challenges for the development of active, selective, and stable catalysts. The potential of bifunctional Ru/H-USY catalysts for conversions in hot liquid water (HLW) is assessed in terms of physicochemical stability and long-term catalytic performance of acid sites and noble metal functionality, as probed by hydrolytic hydrogenation of cellulose. It is shown that zeolite desilication is the main zeolite degradation mechanism in HLW. USY zeolite stability depends on two main parameters, viz., framework and extra-framework aluminum content. The former protects the zeolite lattice by counteracting hydrolysis of framework bonds, and the latter, when located at the external crystal surface, prevents solubilization of the zeolite framework which is the result of its low water-solubility. Hence, the hot liquid water stability of commercial H-USY zeolites, in contrast to their steam stability, increased with decreasing Si/AI ratio. As a result, mildly steamed USY zeolites containing a high amount of both Al species exhibit the highest resistance to HLW. During an initial period of transformations, Al-rich zeolites form additional protective extra-framework Al species at the outer surface, self-stabilizing the framework. A critical bulk Si/AI ratio of 3 was determined whereby USY zeolites with a lower Si/AI ratio will self-stabilize over time. Besides, due to the initial transformation period, the accessibility of the catalytic active sites is extensively enhanced resulting in a material that is more stable and drastically more accessible to large substrates than the original zeolite. When these findings are applied in the hydrolytic hydrogenation of cellulose, unprecedented nearly quantitative hexitol yields were obtained with a stable catalytic system. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000349275300031 |
Publication Date |
2014-12-09 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
2155-5435;2155-5435; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
10.614 |
Times cited |
65 |
Open Access |
OpenAccess |
|
| |
Notes |
335078 Colouratom; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 10.614; 2015 IF: 9.312 |
|
| |
Call Number |
c:irua:125288 |
Serial |
474 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Geboes, B.; Ustarroz, J.; Sentosun, K.; Vanrompay, H.; Hubin, A.; Bals, S.; Breugelmans, T. |
|
| |
Title |
Electrochemical behavior of electrodeposited nanoporous Pt catalysts for the oxygen reduction reaction |
Type |
A1 Journal article |
| |
Year |
2016 |
Publication |
ACS catalysis |
Abbreviated Journal |
Acs Catal |
|
| |
Volume |
6 |
Issue |
6 |
Pages |
5856-5864 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
|
| |
Abstract |
Nanoporous Pt based nanoparticles (NP's) are promising fuel cell catalysts due to their high surface area and increased electrocatalytic activity toward the ORR In this work a direct double-pulse electrodeposition procedure at room temperature is applied to obtain dendritic Pt structures (89 nm diameter) with a high level of porosity (ca. 25%) and nanopores of 2 nm protruding until the center of the NP's. The particle morphology is characterized using aberration corrected high angle annular dark field scanning transmission electron microscopy (HAADF-STEM) and electron tomography (ET) combined with field emission scanning electron microscopy (FESEM) and macroscopic electrochemical measurements to assess their activity and stability toward the ORR. Macroscopic determination of the active surface area through hydrogen UPD measurements in combination with FESEM and ET showed that a considerable amount of the active sites inside the pores of the low overpotential NP's were accessible to oxygen species. As a result of this accessibility, up to a 9-fold enhancement of the Pt mass corrected ORR activity at 0.85 V vs RHE was observed at the highly porous structures. After successive potential cycling upward to 1.5 V vs RHE in a deaerated HClO4 solution a negative shift of 71 mV in half-wave potential occurred. This decrease in ORR activity could be correlated to the partial collapse of the nanopores, visible in both the EASA values and 3D ET reconstructions. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000382714000025 |
Publication Date |
2016-07-18 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
2155-5435 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
10.614 |
Times cited |
48 |
Open Access |
OpenAccess |
|
| |
Notes |
; The Quanta 250 FEG microscope of the Electron Microscopy for Material Science group at the University of Antwerp was funded by the Hercules foundation of the Flemish Government. The authors acknowledge financial support from the Fonds Wetenschappelijk Onderzoek in Flanders (FWOAL708). S.B. acknowledges financial support from the European Research Council (ERC Starting Grant # 335078-COLOURATOMS). J.U. acknowledges funding from the Fonds Wetenschappelijk Onderzoek in Flanders (FWO, postdoctoral grant 12I7816N). ; ecas_Sara |
Approved |
Most recent IF: 10.614 |
|
| |
Call Number |
UA @ lucian @ c:irua:135703 |
Serial |
4302 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Verduyckt, J.; Van Hoof, M.; De Schouwer, F.; Wolberg, M.; Kurttepeli, M.; Eloy, P.; Gaigneaux, E.M.; Bals, S.; Kirschhock, C.E.A.; De Vos, D.E. |
|
| |
Title |
PdPb-catalyzed decarboxylation of proline to pyrrolidine : highly selective formation of a biobased amine in water |
Type |
A1 Journal article |
| |
Year |
2016 |
Publication |
ACS catalysis |
Abbreviated Journal |
Acs Catal |
|
| |
Volume |
6 |
Issue |
6 |
Pages |
7303-7310 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
Amino acids have huge potential as platform chemicals in the biobased industry. Pd-catalyzed decarboxylation is a very promising route for the valorization of these natural compounds derived from protein waste or fermentation. We report that the highly abundant and nonessential amino acid L-proline is very reactive in the Pd-catalyzed decarboxylation. Full conversions are obtained with Pd/C and different Pd/MeOx catalysts; this allowed the identification of the different side reactions and the mapping of the reaction network. Due to the high reactivity of pyrrolidine, the selectivity for pyrrolidine was initially low. By carefully modifying Pd/ZrO2 with Pb in a controlled manner-via two incipient wetness impregnation steps-the selectivity increased remarkably. Finally, a thorough investigation of the reaction parameters resulted in an increased activity of this modified catalyst and an even further enhanced selectivity under a low H-2 pressure of 4 bar at 235 degrees C in water. This results in a very selective and sustainable production route for the highly interesting pyrrolidine. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000387306100005 |
Publication Date |
2016-09-16 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
2155-5435 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
10.614 |
Times cited |
27 |
Open Access |
OpenAccess |
|
| |
Notes |
; J.V. and F.D.S. thank Fonds Wetenschappelijk Onderzoek (FWO) and Agency for Innovation by Science and Technology (IWT) for doctoral fellowships. D.D.V. acknowledges IWT and FWO for research project funding. D.D.V. and C.E.A.K. acknowledge the Flemish government for long-term structural funding through Methusalem. D.D.V. and S.B. acknowledge Belspo (IAP-PAI 7/05) for financial support. S.B. is grateful for funding by the European Research Council (ERC starting grant no. 335078-COLOURATOMS). The authors also thank the Department of Chemistry, University of Cologne, Germany for use of their XRD equipment. Finally, the assistance of Karel Duerinckx, Werner Wouters, Walter Vermandel, Ivo Stassen, Dries Jonckheere, Sabina Accardo and Bart Bueken with 11-1 NMR, pressure reactors, CO chemisorption, N<INF>2</INF> physisorption, SEM, gas phase FTIR and high-throughput XRD, respectively, is very much appreciated. ; ecas_Sara |
Approved |
Most recent IF: 10.614 |
|
| |
Call Number |
UA @ lucian @ c:irua:139171 |
Serial |
4445 |
|
| Permanent link to this record |
| |
|
| |
|
Author |
Tang, Z.; Liu, P.; Cao, H.; Bals, S.; Heeres, H.J.; Pescarmona, P.P. |
|
| |
Title |
Pr/ZrO2 prepared by atomic trapping : an efficient catalyst for the conversion of glycerol to lactic acid with concomitant transfer hydrogenation of cyclohexene |
Type |
A1 Journal article |
| |
Year |
2019 |
Publication |
ACS catalysis |
Abbreviated Journal |
Acs Catal |
|
| |
Volume |
9 |
Issue |
9 |
Pages |
9953-9963 |
|
| |
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
|
| |
Abstract |
A series of heterogeneous catalysts consisting of highly dispersed Pt nanoparticles supported on nanosized ZrO2 (20 to 60 nm) was synthesized and investigated for the one-pot transfer hydrogenation between glycerol and cyclohexene to produce lactic acid and cyclohexane, without any additional H-2. Different preparation methods were screened, by varying the calcination and reduction procedures with the purpose of optimizing the dispersion of Pt species (i.e., as single-atom sites or extra-fine Pt nanoparticles) on the ZrO2 support. The Pt/ZrO2 catalysts were characterized by means of transmission electron microscopy techniques (HAADF-STEM, TEM), elemental analysis (ICP-OES, EDX mapping), N-2-physisorption, H-2 temperature-programmed-reduction (H-2-TPR), X-ray photoelectron spectroscopy (XPS), and X-ray diffraction (XRD). Based on this combination of techniques it was possible to correlate the temperature of the calcination and reduction treatments with the nature of the Pt species. The best catalyst consisted of subnanometer Pt clusters (<1 nm) and atomically dispersed Pt (as Pt2+ and Pt4+) on the ZrO2 support, which were converted into extra-fine Pt nanoparticles (average size = 1.4 nm) upon reduction. These nanoparticles acted as catalytic species for the transfer hydrogenation of glycerol with cyclohexene, which gave an unsurpassed 95% yield of lactic acid salt at 96% glycerol conversion (aqueous glycerol solution, NaOH as promoter, 160 degrees C, 4.5 h, at 20 bar N-2). This is the highest yield and selectivity of lactic acid (salt) reported in the literature so far. Reusability experiments showed a partial and gradual loss of activity of the Pt/ZrO2 catalyst, which was attributed to the experimentally observed aggregation of Pt nanoparticles. |
|
| |
Address |
|
|
| |
Corporate Author |
|
Thesis |
|
|
| |
Publisher |
|
Place of Publication |
|
Editor |
|
|
| |
Language |
|
Wos |
000494549700025 |
Publication Date |
2019-09-16 |
|
| |
Series Editor |
|
Series Title |
|
Abbreviated Series Title |
|
|
| |
Series Volume |
|
Series Issue |
|
Edition |
|
|
| |
ISSN |
2155-5435 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
| |
Impact Factor |
10.614 |
Times cited |
46 |
Open Access |
OpenAccess |
|
| |
Notes |
Zhenchen Tang acknowledges the financial support from the China Scholarship Council for his Ph.D. grant. All the authors are grateful for the technical support from Erwin Wilbers, Anne Appeldoorn, and Marcel de Vries, the TEM support from Dr. Marc Stuart, and the ICP-OES support from Johannes van der Velde. Pei Liu and Sara Bals acknowledge financial support from the European Commission under the Horizon 2020 Programme by means of grant agreement No. 731019 EUSMI. |
Approved |
Most recent IF: 10.614 |
|
| |
Call Number |
UA @ admin @ c:irua:164643 |
Serial |
6326 |
|
| Permanent link to this record |
