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Author |
El-Gogary, R.I.; Rubio, N.; Wang, J.T.W.; Al-Jamal, W.T.; Bourgognon, M.; Kafa, H.; Naeem, M.; Klippstein, R.; Abbate, V.; Leroux, F.; Bals, S.; Van Tendeloo, G.; Kamel, A.O.; Awad, G.A.S.; Mortada, N.D.; Al-Jamal, K.T.; |
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Title |
Polyethylene glycol conjugated polymeric nanocapsules for targeted delivery of quercetin to folate-expressing cancer cells in vitro and in vivo |
Type |
A1 Journal article |
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Year |
2014 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
8 |
Issue |
2 |
Pages |
1384-1401 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
In this work we describe the formulation and characterization of chemically modified polymeric nanocapsules incorporating the anticancer drug, quercetin, for the passive and active targeting to tumors. Folic acid was conjugated to poly(lactide-co-glycolide) (PLGA) polymer to facilitate active targeting to cancer cells. Two different methods for the conjugation of PLGA to folic acid were employed utilizing polyethylene glycol (PEG) as a spacer. Characterization of the conjugates was performed using FTIR and H-1 NMR studies. The PEG and folk acid content was independent of the conjugation methodology employed. PEGylation has shown to reduce the size of the nanocapsule; moreover, zeta-potential was shown to be polymer-type dependent. Comparative studies on the cytotoxicity and cellular uptake of the different formulations by He La cells, in the presence and absence of excess folic acid, were carried out using MTT assay and Confocal Laser Scanning Microscopy, respectively. Both results confirmed the selective uptake and cytotoxicity of the folic acid targeted nanocapsules to the folate enriched cancer cells in a folate-dependent manner. Finally, the passive tumor accumulation and the active targeting of the nanocapsules to folate-expressing cells were confirmed upon intravenous administration in He La or IGROV-1 tumor-bearing mice. The developed nanocapsules provide a system for targeted delivery of a range of hydrophobic anticancer drugs in vivo. |
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Wos |
000332059200032 |
Publication Date |
2014-01-07 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851;1936-086X; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor  |
13.942 |
Times cited |
144 |
Open Access |
Not_Open_Access |
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Notes |
290023 Raddel; 262348 Esmi; Iap-Pai |
Approved |
Most recent IF: 13.942; 2014 IF: 12.881 |
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Call Number |
UA @ lucian @ c:irua:115862 |
Serial |
2670 |
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Author |
Galván-Moya, J.E.; Altantzis, T.; Nelissen, K.; Peeters, F.M.; Grzelczak, M.; Liz-Marán, L.M.; Bals, S.; Van Tendeloo, G. |
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Title |
Self-organization of highly symmetric nanoassemblies : a matter of competition |
Type |
A1 Journal article |
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Year |
2014 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
8 |
Issue |
4 |
Pages |
3869-3875 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT) |
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Abstract |
The properties and applications of metallic nanoparticles are inseparably connected not only to their detailed morphology and composition but also to their structural configuration and mutual interactions. As a result, the assemblies often have superior properties as compared to individual nanoparticles. Although it has been reported that nanoparticles can form highly symmetric clusters, if the configuration can be predicted as a function of the synthesis parameters, more targeted and accurate synthesis will be possible. We present here a theoretical model that accurately predicts the structure and configuration of self-assembled gold nanoclusters. The validity of the model is verified using quantitative experimental data extracted from electron tomography 3D reconstructions of different assemblies. The present theoretical model is generic and can in principle be used for different types of nanoparticles, providing a very wide window of potential applications. |
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Wos |
000334990600084 |
Publication Date |
2014-03-13 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851;1936-086X; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
34 |
Open Access |
OpenAccess |
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Notes |
FWO; Methusalem; 246791 COUNTATOMS; 335078 COLOURATOM; 262348 ESMI; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 13.942; 2014 IF: 12.881 |
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Call Number |
UA @ lucian @ c:irua:116955 |
Serial |
2977 |
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Author |
Groeneveld, E.; Witteman, L.; Lefferts, M.; Ke, X.; Bals, S.; Van Tendeloo, G.; de Mello Donega, C. |
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Title |
Tailoring ZnSe-CdSe colloidal quantum dots via cation exchange : from core/shell to alloy nanocrystals |
Type |
A1 Journal article |
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Year |
2013 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
7 |
Issue |
9 |
Pages |
7913-7930 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
We report a study of Zn2+ by Cd2+ cation exchange (CE) in colloidal ZnSe nanocrystals (NCs). Our results reveal that CE in ZnSe NCs is a thermally activated isotropic process. The CE efficiency (i.e., fraction of Cd2+ ions originally in solution, Cdsol, that is incorporated in the ZnSe NC) increases with temperature and depends also on the Cdsol/ZnSe ratio. Interestingly, the reaction temperature can be used as a sensitive parameter to tailor both the composition and the elemental distribution profile of the product (Zn,Cd)Se NCs. At 150 °C ZnSe/CdSe core/shell hetero-NCs (HNCs) are obtained, while higher temperatures (200 and 220 °C) produce (Zn1xCdx)Se gradient alloy NCs, with increasingly smoother gradients as the temperature increases, until homogeneous alloy NCs are obtained at T ≥ 240 °C. Remarkably, sequential heating (150 °C followed by 220 °C) leads to ZnSe/CdSe core/shell HNCs with thicker shells, rather than (Zn1xCdx)Se gradient alloy NCs. Thermal treatment at 250 °C converts the ZnSe/CdSe core/shell HNCs into (Zn1xCdx)Se homogeneous alloy NCs, while preserving the NC shape. A mechanism for the cation exchange in ZnSe NCs is proposed, in which fast CE takes place at the NC surface, and is followed by relatively slower thermally activated solid-state cation diffusion, which is mediated by Frenkel defects. The findings presented here demonstrate that cation exchange in colloidal ZnSe NCs provides a very sensitive tool to tailor the nature and localization regime of the electron and hole wave functions and the optoelectronic properties of colloidal ZnSeCdSe NCs. |
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Corporate Author |
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Place of Publication |
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Wos |
000330016900051 |
Publication Date |
2013-08-13 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851;1936-086X; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
153 |
Open Access |
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Notes |
262348 Esmi; 246791 Countatoms |
Approved |
Most recent IF: 13.942; 2013 IF: 12.033 |
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Call Number |
UA @ lucian @ c:irua:110038 |
Serial |
3469 |
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Author |
Goris, B.; Turner, S.; Bals, S.; Van Tendeloo, G. |
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Title |
Three-dimensional valency mapping in ceria nanocrystals |
Type |
A1 Journal article |
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Year |
2014 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
8 |
Issue |
10 |
Pages |
10878-10884 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Using electron tomography combined with electron energy loss spectroscopy (EELS), we are able to map the valency of the Ce ions in CeO2-x nanocrystals in three dimensions. Our results show a clear facet-dependent reduction shell at the surface of ceria nanoparticles; {111} surface facets show a low surface reduction, whereas at {001} surface facets, the cerium ions are more likely to be reduced over a larger surface shell. Our generic tomographic technique allows a full 3D data cube to be reconstructed, containing an EELS spectrum in each voxel. This possibility enables a three-dimensional investigation of a plethora of material-specific physical properties such as valency, chemical composition, oxygen coordination, or bond lengths, triggering the synthesis of nanomaterials with improved properties. |
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Corporate Author |
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Place of Publication |
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Editor |
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Language |
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Wos |
000343952600126 |
Publication Date |
2014-10-06 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851;1936-086X; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
85 |
Open Access |
OpenAccess |
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Notes |
335078 Colouratom; 246791 Countatoms; Fwo; 312483 Esteem2; esteem2jra4; ECASSara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 13.942; 2014 IF: 12.881 |
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Call Number |
UA @ lucian @ c:irua:121219 |
Serial |
3656 |
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Author |
van der Stam, W.; Bladt, E.; Rabouw, F.T.; Bals, S.; de Mello Donega, C. |
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Title |
Near-Infrared Emitting CuInSe/CuInS Dot Core/Rod Shell Heteronanorods by Sequential Cation Exchange |
Type |
A1 Journal article |
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Year |
2015 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
9 |
Issue |
9 |
Pages |
11430-11438 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
The direct synthesis of heteronanocrystals (HNCs) combining different ternary semiconductors is challenging and has not yet been successful. Here, we report a sequential topotactic cation exchange (CE) pathway that yields CuInSe2/CuInS2 dot core/rod shell nanorods with near-infrared luminescence. In our approach, the Cu+ extraction rate is coupled to the In3+ incorporation rate by the use of a stoichiometric trioctylphosphine-InCl3 complex, which fulfills the roles of both In-source and Cu-extracting agent. In this way, Cu+ ions can be extracted by trioctylphosphine ligands only when the In-P bond is broken. This results in readily available In3+ ions at the same surface site from which the Cu+ is extracted, making the process a direct place exchange reaction and shifting the overall energy balance in favor of the CE. Consequently, controlled cation exchange can occur even in large and anisotropic heterostructured nanocrystals with preservation of the size, shape, and heterostructuring of the template NCs into the product NCs. The cation exchange is self-limited, stopping when the ternary core/shell CuInSe2/CuInS2 composition is reached. The method is very versatile, successfully yielding a variety of luminescent CuInX2 (X = S, Se, and Te) quantum dots, nanorods, and HNCs, by using Cd-chalcogenide NCs and HNCs as templates. The approach reported here thus opens up routes toward materials with unprecedented properties, which would otherwise remain inaccessible. |
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Address |
Debye Institute for Nanomaterials Science, Utrecht University , P.O. Box 80000, 3508 TA Utrecht, The Netherlands |
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Corporate Author |
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English |
Wos |
000365464800094 |
Publication Date |
2015-10-09 |
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Series Editor |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851;1936-086X; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
88 |
Open Access |
OpenAccess |
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Notes |
The authors thank Gang Wang for XRD measurements and Eline Hutter for providing CdSe/CdS NRs. 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. This work was supported by the European Research Council (ERC Starting Grant #335078 Colouratom). E.B. gratefully acknowledges financial support by the Flemish Fund for Scientific Research (FWO Vlaanderen).; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 13.942; 2015 IF: 12.881 |
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Call Number |
c:irua:129184 |
Serial |
3948 |
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Author |
Altantzis, T.; Coutino-Gonzalez, E.; Baekelant, W.; Martinez, G.T.; Abakumov, A.M.; Van Tendeloo, G.; Roeffaers, M.B.J.; Bals, S.; Hofkens, J. |
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Title |
Direct Observation of Luminescent Silver Clusters Confined in Faujasite Zeolites |
Type |
A1 Journal article |
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Year |
2016 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
10 |
Issue |
10 |
Pages |
7604-7611 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
One of the ultimate goals in the study of metal clusters is the correlation between the atomic-scale organization and their physicochemical properties. However, direct observation of the atomic organization of such minuscule metal clusters is heavily hindered by radiation damage imposed by the different characterization techniques. We present direct evidence of the structural arrangement, at an atomic level, of luminescent silver species stabilized in faujasite (FAU) zeolites using aberration-corrected scanning transmission electron microscopy. Two different silver clusters were identified in Ag-FAU zeolites, a trinuclear silver species associated with green emission and a tetranuclear silver species related to yellow emission. By combining direct imaging with complementary information obtained from X-ray powder diffraction and Rietveld analysis, we were able to elucidate the main differences at an atomic scale between luminescent (heat-treated) and nonluminescent (cation-exchanged) Ag-FAU zeolites. It is expected that such insights will trigger the directed synthesis of functional metal nanocluster-zeolite composites with tailored luminescent properties. |
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Address |
RIES, Hokkaido University , N20W10, Kita-Ward Sapporo 001-0020, Japan |
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Place of Publication |
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Language |
English |
Wos |
000381959100043 |
Publication Date |
2016-07-08 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
57 |
Open Access |
OpenAccess |
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Notes |
The authors gratefully acknowledge financial support from the Belgian Federal government (Belspo through the IAP-VI/27 and IAP-VII/05 programs), the European Union’s Seventh Framework Programme (FP7/2007-2013 under grant agreement no. 310651 SACS and no. 312483-ESTEEM2), the Flemish government in the form of long-term structural funding “Methusalem” grant METH/15/04 CASAS2, the Hercules foundation (HER/11/14), the “Strategisch Initiatief Materialen” SoPPoM program, and the Fund for Scientific Research Flanders (FWO) grants G.0349.12 and G.0B39.15. S.B. acknowledges funding from ERC Starting Grant COLOURATOMS (335078). The authors thank Prof. S. Van Aert for helpful discussions, Dr. T. De Baerdemaeker for XRD measurements, Mr. B. Dieu for the preparation of graphical material, and UOP Antwerp for the kind donation of zeolite samples.; esteem2jra4; ECASSara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 13.942 |
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Call Number |
c:irua:134576 c:irua:134576 |
Serial |
4102 |
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Author |
Montanarella, F.; Altantzis, T.; Zanaga, D.; Rabouw, F.T.; Bals, S.; Baesjou, P.; Vanmaekelbergh, D.; van Blaaderen, A. |
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Title |
Composite Supraparticles with Tunable Light Emission |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
11 |
Issue |
11 |
Pages |
9136-9142 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Robust luminophores emitting light with broadly tunable colors are desirable in many applications such as light-emitting diode (LED)-based lighting, displays, integrated optoelectronics and biology. Nanocrystalline quantum dots with multicolor emission, from core- and shell-localized excitons, as well as solid layers of mixed quantum dots that emit different colors have been proposed. Here, we report on colloidal supraparticles that are composed of three types of Cd(Se,ZnS) core/(Cd,Zn)S shell nanocrystals with emission in the red, green, and blue. The emission of the supraparticles can be varied from pure to composite colors over the entire visible region and finetuned into variable shades of white light by mixing the nanocrystals in controlled proportions. Our approach results in supraparticles with sizes spanning the colloidal domain and beyond that combine versatility and processability with a broad, stable, and tunable emission, promising applications in lighting devices and biological research. |
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Wos |
000411918200062 |
Publication Date |
2017-09-26 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
36 |
Open Access |
OpenAccess |
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Notes |
We thank J. J. Geuchies for help with the optical analysis, W. Vlug for providing silica particles filled with RITC, J. D. Meeldijk for his assistance with SE-STEM measurements, E. B. van der Wee for help with the calculation of the radial distribution functions, and M. van Huis and S. Dussi for very fruitful discussions. This work was supported by the European Comission via the Marie-Sklodowska Curie action Phonsi (H2020-MSCA-ITN-642656). D.V. wishes to thank the Dutch FOM (program DDC13), NWO−CW (Toppunt 718.015.002), and the European Research Council under HORIZON 2020 (grant 692691 FIRSTSTEP) for financial support. A.v.B. and F.M. acknowledge partial funding from the European Research Council under the European Union’s Seventh Framework Programme (FP-2007-2013)/ERC advanced grant agreement 291667: HierarSACol. S.B. and D.Z. acknowledge financial support from the European Research Council (starting grant no. COLOURATOM 335078), and T.A. acknowledges funding from the Research Foundation Flanders (FWO, Belgium) through a postdoctoral grant. ECAS_Sara (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 13.942 |
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Call Number |
EMAT @ emat @c:irua:146095UA @ admin @ c:irua:146095 |
Serial |
4732 |
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Author |
Feld, A.; Weimer, A.; Kornowski, A.; Winckelmans, N.; Merkl, J.-P.; Kloust, H.; Zierold, R.; Schmidtke, C.; Schotten, T.; Riedner, M.; Bals, S.; Weller, P.D., Horst |
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Title |
Chemistry of Shape-Controlled Iron Oxide Nanocrystal Formation |
Type |
A1 Journal article |
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Year |
2018 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
13 |
Issue |
13 |
Pages |
152-162 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Herein we demonstrate that meticulous and in-depth analysis of the reaction mechanisms of nanoparticle formation is rewarded by full control of size, shape and crystal structure of superparamagnetic iron oxide nanocrystals during synthesis. Starting from two iron sources – iron(II)- and iron(III) carbonate -a strict separation of oleate formation from the generation of reactive pyrolysis products and concomitant nucleation of iron oxide nanoparticles was achieved. This protocol enabled us to analyze each step of nanoparticle formation independently in depth. Progress of the entire reaction was monitored via matrix-assisted laser desorption ionization time-of-flight mass spectrometry (MALDI-TOF MS) and gas chromatography (GC) gaining insight into the formation of various iron oleate species prior to nucleation. Interestingly, due to the intrinsic strongly reductive pyrolysis conditions of the oleate intermediates and redox process in early stages of the synthesis, pristine iron oxide nuclei were composed exclusively from wustite, irrespective of the oxidation state of the iron source. Controlling the reaction conditions provided a very broad range of size- and shape defined monodisperse iron oxide nanoparticles. Curiously, after nucleation star shaped nanocrystals were obtained, which underwent metamorphism towards cubic shaped particles. EELS tomography revealed ex post oxidation of the primary wustite nanocrystal providing a full 3D image of Fe2+ and Fe3+ distribution within. Overall, we developed a highly flexible synthesis, yielding multigram amounts of well-defined iron oxide nanocrystals of different sizes and morphologies. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000456749900017 |
Publication Date |
2018-12-12 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
54 |
Open Access |
OpenAccess |
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Notes |
The authors gratefully acknowledge financial support from the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) – Projektnummer 192346071 – SFB 986 and the excellence cluster ‘The Hamburg Centre for Ultrafast Imaging – Structure, Dynamics and Control of Matter at the Atomic Scale’ (by grant EXC 1074) S.B. and N.W. acknowledge financial support from European Research Council (ERC Starting Grant #335078-COLOURATOMS) and from the Research Foundation Flanders (FWO, Belgium) through Project fundings G038116N. Dr. Volker Sauerland for his support in calibrating the MALDI-TOF spectra. Almut Bark for measuring XRD (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); ecas_sara |
Approved |
Most recent IF: 13.942 |
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Call Number |
EMAT @ emat @c:irua:155716UA @ admin @ c:irua:155716 |
Serial |
5073 |
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| Permanent link to this record |
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Author |
Gonzalez-Rubio, G.; Kumar, V.; Llombart, P.; Diaz-Nunez, P.; Bladt, E.; Altantzis, T.; Bals, S.; Pena-Rodriguez, O.; Noya, E.G.; MacDowell, L.G.; Guerrero-Martinez, A.; Liz-Marzan, L.M. |
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Title |
Disconnecting Symmetry Breaking from Seeded Growth for the Reproducible Synthesis of High Quality Gold Nanorods |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
13 |
Issue |
13 |
Pages |
4424-4435 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
One of the major difficulties hindering the widespread application of colloidal anisotropic plasmonic nanoparticles is the limited robustness and reproducibility of multistep synthetic methods. We demonstrate herein that the reproducibility and reliability of colloidal gold nanorod (AuNR) synthesis can be greatly improved by disconnecting the symmetry-breaking event from the seeded growth process. We have used a modified silver-assisted seeded growth method in the presence of the surfactant hexadecyltrimethylammonium bromide and n-decanol as a co-surfactant to prepare small AuNRs in high yield, which were then used as seeds for the growth of high quality AuNR colloids. Whereas the use of n-decanol provides a more-rigid micellar system, the growth on anisotropic seeds avoids sources of irreproducibility during the symmetry breaking step, yielding uniform AuNR colloids with narrow plasmon bands, ranging from 600 to 1270 nm, and allowing the fine-tuning of the final dimensions. This method provides a robust route for the preparation of high quality AuNR colloids with tunable morphology, size, and optical response in a reproducible and scalable manner. |
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Thesis |
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Place of Publication |
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Editor |
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Language |
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Wos |
000466052900067 |
Publication Date |
2019-04-02 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
100 |
Open Access |
OpenAccess |
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Notes |
; This work has been funded by the Spanish MINECO (grant nos. FIS2017-89361-C3-2-P and MAT2017-86659-R), the Madrid Regional Government (grant no. P2018/NMT-4389) and the Complutense University of Madrid (grant no. PR75/18-21616). Funding is acknowledged from the European Commission (grant no. EUSMI 731019). G.G.-R. acknowledges receipt of FPI Fellowship from the Spanish MINECO. E.B. and T.A. acknowledge postdoctoral grants from the Research Foundation Flanders (FWO). The authors are indebted to Profs. Justin Gooding, Watson Loh, Nicholas Kotov, Deqing Zhang, Mihaela Delcea, Maurizio Prato, and Krishna Ganesh, for providing milli-Q water samples. ; |
Approved |
Most recent IF: 13.942 |
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| |
Call Number |
UA @ admin @ c:irua:160417 |
Serial |
5246 |
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| Permanent link to this record |
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Author |
Albrecht, W.; Bladt, E.; Vanrompay, H.; Smith, J.D.; Skrabalak, S.E.; Bals, S. |
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Title |
Thermal Stability of Gold/Palladium Octopods Studied in Situ in 3D: Understanding Design Rules for Thermally Stable Metal Nanoparticles |
Type |
A1 Journal article |
| |
Year |
2019 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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| |
Volume |
13 |
Issue |
13 |
Pages |
6522-6530 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Multifunctional metal nanoparticles (NPs) such as anisotropic multimetallic NPs are crucial for boosting nanomaterial based applications. Advanced synthetic protocols exist to make a large variety of such nanostructures. However, a major limiting factor for the usability of them in real life applications is their stability. Here, we show that Au/Pd octopods, 8-branched nanocrystals with Oh symmetry, with only a low amount of Pd exhibited a high thermal stability and maintained strong plasmon resonances up to 600 ◦C. Furthermore, we study the influence of the composition, morphology and environment on the thermal stability and define key parameters for the design of thermally stable multifunctional NPs. |
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Corporate Author |
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Place of Publication |
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Editor |
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Language |
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Wos |
000473248300038 |
Publication Date |
2019-06-25 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
46 |
Open Access |
OpenAccess |
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Notes |
W. A. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020. H. V. acknowledges financial support by the Research Foundation Flanders (FWO grant 1S32617N). E. B. acknowledges a post-doctoral grant from the Research Foundation Flanders (FWO, Belgium). J. D. S. and S.E.S acknowledge funding from the US National Science Foundation (award number: CHE-1602476). The authors acknowledge funding from the European Commission Grant (EUSMI E180600101 to S. B. and S. E. S.) and European Research Council (ERC Starting Grant #335078-COLOURATOMS). Realnano 815128; sygma |
Approved |
Most recent IF: 13.942 |
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| |
Call Number |
EMAT @ emat @c:irua:161356 |
Serial |
5285 |
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| Permanent link to this record |
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Author |
Skorikov, A.; Albrecht, W.; Bladt, E.; Xie, X.; van der Hoeven, J.E.S.; van Blaaderen, A.; Van Aert, S.; Bals, S. |
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Title |
Quantitative 3D Characterization of Elemental Diffusion Dynamics in Individual Ag@Au Nanoparticles with Different Shapes |
Type |
A1 Journal article |
| |
Year |
2019 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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| |
Volume |
13 |
Issue |
13 |
Pages |
13421-13429 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Anisotropic bimetallic nanoparticles are promising candidates for plasmonic and catalytic applications. Their catalytic performance and plasmonic properties are closely linked to the distribution of the two metals, which can change during applications in which the particles are exposed to heat. Due to this fact, correlating the thermal stability of complex heterogeneous nanoparticles to their microstructural properties is of high interest for the practical applications of such materials. Here, we employ quantitative electron tomography in high-angle annular dark-field scanning transmission electron microscopy (HAADFSTEM) mode to measure the 3D elemental diffusion dynamics in individual anisotropic Au−Ag nanoparticles upon heating in situ. This approach allows us to study the elemental redistribution in complex, asymmetric nanoparticles on a single particle level, which has been inaccessible to other techniques so far. In this work, we apply the proposed method to compare the alloying dynamics of Au−Ag nanoparticles with different shapes and compositions and find that the shape of the nanoparticle does not exhibit a significant effect on the alloying speed whereas the composition does. Finally, comparing the experimental results to diffusion simulations allows us to estimate the diffusion coefficients of the metals for individual nanoparticles. |
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Thesis |
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Place of Publication |
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Language |
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Wos |
000500650000115 |
Publication Date |
2019-10-25 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
29 |
Open Access |
OpenAccess |
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Notes |
This project has received funding from the European Commission (grant 731019, EUSMI) and European Research Council (ERC Consolidator Grants 815128, REALNANO; 770887, PICOMETRICS; 648991, 3MC; and ERC Advanced Grant 291667, HierarSACol). This project has also received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement 823717, ESTEEM3. W.A. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (grant 797153, SOPMEN). E.B. acknowledges a postdoctoral grant 12T2719N from the Research Foundation Flanders (FWO, Belgium). X.X. acknowledges financial support from the EU H2020-MSCAITN-2015 project 676045, MULTIMAT. The authors also acknowledge financial support by the Research Foundation Flanders (FWO grants G038116N, G026718N, and G036915N).; sygma; esteem3JRA; esteem3reported |
Approved |
Most recent IF: 13.942 |
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Call Number |
EMAT @ emat @c:irua:164061 |
Serial |
5379 |
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Author |
Hinterding, S.O.M.; Berends, A.C.; Kurttepeli, M.; Moret, M.-E.; Meeldijk, J.D.; Bals, S.; van der Stam, W.; de Donega, C.M. |
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Title |
Tailoring Cu+ for Ga3+ cation exchange in Cu2-xS and CuInS2 nanocrystals by controlling the Ga precursor chemistry |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
ACS nano |
Abbreviated Journal |
Acs Nano |
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Volume |
13 |
Issue |
13 |
Pages |
12880-12893 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Nanoscale cation exchange (CE) has resulted in colloidal nanomaterials that are unattainable by direct synthesis methods. Aliovalent CE is complex and synthetically challenging because the exchange of an unequal number of host and guest cations is required to maintain charge balance. An approach to control aliovalent CE reactions is the use of a single reactant to both supply the guest cation and extract the host cation. Here, we study the application of GaCl3-L complexes [L = trioctylphosphine (TOP), triphenylphosphite (TPP), diphenylphosphine (DPP)] as reactants in the exchange of Cu+ for Ga3+ in Cu2-xS nanocrystals. We find that noncomplexed GaCl3 etches the nanocrystals by S2- extraction, whereas GaCl3-TOP is unreactive. Successful exchange of Cu+ for Ga3+ is only possible when GaCl3 is complexed with either TPP or DPP. This is attributed to the pivotal role of the Cu2-xS-GaCl3-L activated complex that forms at the surface of the nanocrystal at the onset of the CE reaction, which must be such that simultaneous Ga3+ insertion and Cu+ extraction can occur. This requisite is only met if GaCl3 is bound to a phosphine ligand, with a moderate bond strength, to allow facile dissociation of the complex at the nanocrystal surface. The general validity of this mechanism is demonstrated by using GaCl3-DPP to convert CuInS2 into (Cu,Ga,In)S-2 nanocrystals, which increases the photoluminescence quantum yield 10 -fold, while blue -shifting the photoluminescence into the NIR biological window. This highlights the general applicability of the mechanistic insights provided by our work. |
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Place of Publication |
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Language |
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Wos |
000500650000061 |
Publication Date |
2019-10-16 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
27 |
Open Access |
OpenAccess |
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Notes |
; S.O.M.H., W.v.d.S., A.C.B., and C.d.M.D. acknowledge financial support from the division of Chemical Sciences (CW) of The Netherlands Organization for Scientific Research (NWO) under Grant Nos. ECHO.712.012.0001 and ECHO.712.014.001. S.B. acknowledges financial support from the European Research Council (ERC Consolidator Grant No. 815128-REALNANO). S.O.M.H. is supported by The Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation Programme funded by the Ministry of Education, Culture and Science of the government of The Netherlands. DFT calculations were carried out on the Dutch national e-infrastructure with the support of SURF Cooperative. This work was sponsored by NWO Physical Sciences for the use of supercomputer facilities. The authors thank Jessi van der Hoeven for EDS and TEM measurements. ; sygma |
Approved |
Most recent IF: 13.942 |
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Call Number |
UA @ admin @ c:irua:165149 |
Serial |
6324 |
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Author |
Bagiński, M.; Pedrazo-Tardajos, A.; Altantzis, T.; Tupikowska, M.; Vetter, A.; Tomczyk, E.; Suryadharma, R.N.S.; Pawlak, M.; Andruszkiewicz, A.; Górecka, E.; Pociecha, D.; Rockstuhl, C.; Bals, S.; Lewandowski, W. |
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Title |
Understanding and Controlling the Crystallization Process in Reconfigurable Plasmonic Superlattices |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Acs Nano |
Abbreviated Journal |
Acs Nano |
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Volume |
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Issue |
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Pages |
acsnano.0c09746 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
The crystallization of nanomaterials is a primary source of solid-state, photonic structures. Thus, a detailed understanding of this process is of paramount importance for the successful application of photonic nanomaterials in emerging optoelectronic technologies. While colloidal crystallization has been thoroughly studied, for example, with advanced in situ electron microscopy methods, the noncolloidal crystallization (freezing) of nanoparticles (NPs) remains so far unexplored. To fill this gap, in this work, we present proof-of principle experiments decoding a crystallization of reconfigurable assemblies of NPs at a solid state. The chosen material corresponds to an excellent testing bed, as it enables both in situ and ex situ investigation using X-ray diffraction (XRD), transmission electron microscopy (TEM), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), atomic force microscopy (AFM), and optical spectroscopy in visible and ultraviolet range (UV−vis) techniques. In particular, ensemble measurements with small-angle XRD highlighted the dependence of the correlation length in the NPs assemblies on the number of heating/cooling cycles and the rate of cooling. Ex situ TEM imaging further supported these results by revealing a dependence of domain size and structure on the sample preparation route and by showing we can control the domain size over 2 orders of magnitude. The application of HAADF-STEM tomography, combined with in situ thermal control, provided three-dimensional single-particle level information on the positional order evolution within assemblies. This combination of real and reciprocal space provides insightful information on the anisotropic, reversibly reconfigurable assemblies of NPs. TEM measurements also highlighted the importance of interfaces in the polydomain structure of nanoparticle solids, allowing us to understand experimentally observed differences in UV−vis extinction spectra of the differently prepared crystallites. Overall, the obtained results show that the combination of in situ heating HAADF-STEM tomography with XRD and ex situ TEM techniques is a powerful approach to study nanoparticle freezing processes and to reveal the crucial impact of disorder in the solid-state aggregates of NPs on their plasmonic properties. |
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Place of Publication |
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Wos |
000634569100101 |
Publication Date |
2021-02-23 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
10 |
Open Access |
OpenAccess |
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Notes |
Ministerstwo Nauki i Szkolnictwa Wyzszego, 0112/DIA/2019/48 ; European Commission, 731019 E171000009 (EUSMI) ; Narodowe Centrum Nauki, 2016/21/N/ST5/03356 ; Deutsche Forschungsgemeinschaft, RO 3640/12-1 ; Fundacja na rzecz Nauki Polskiej, First TEAM2016–2/15 ; European Research Council, 815128 (REALNANO) ; sygma; |
Approved |
Most recent IF: 13.942 |
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Call Number |
EMAT @ emat @c:irua:175872 |
Serial |
6673 |
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Author |
Walters, A.A.; Santacana-Font, G.; Li, J.; Routabi, N.; Qin, Y.; Claes, N.; Bals, S.; Tzu-Wen Wang, J.; Al-Jamal, K.T. |
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Title |
Nanoparticle-MediatedIn SituMolecular Reprogramming of Immune Checkpoint Interactions for Cancer Immunotherapy |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Acs Nano |
Abbreviated Journal |
Acs Nano |
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| |
Volume |
15 |
Issue |
11 |
Pages |
17549-17564 |
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Keywords |
A1 Journal article; Pharmacology. Therapy; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Immune checkpoint blockade involves targeting immune
regulatory molecules with antibodies. Preclinically, complex multiantibody
regimes of both inhibitory and stimulatory targets are a promising
candidate for the next generation of immunotherapy. However, in this
setting, the antibody platform may be limited due to excessive toxicity
caused by off target effects as a result of systemic administration. RNA
can be used as an alternate to antibodies as it can both downregulate
immunosuppressive checkpoints (siRNA) or induce expression of
immunostimulatory checkpoints (mRNA). In this study, we demonstrate
that the combination of both siRNA and mRNA in a single
formulation can simultaneously knockdown and induce expression of
immune checkpoint targets, thereby reprogramming the tumor
microenvironment from immunosuppressive to immunostimulatory
phenotype. To achieve this, RNA constructs were synthesized and
formulated into stable nucleic acid lipid nanoparticles (SNALPs); the SNALPs produced were 140−150 nm in size with >80%
loading efficiency. SNALPs could transfect macrophages and B16F10 cells in vitro resulting in 75% knockdown of inhibitory
checkpoint (PDL1) expression and simultaneously express high levels of stimulatory checkpoint (OX40L) with minimal
toxicity. Intratumoral treatment with the proposed formulation resulted in statistically reduced tumor growth, a greater
density of CD4+ and CD8+ infiltrates in the tumor, and immune activation within tumor-draining lymph nodes. These data
suggest that a single RNA-based formulation can successfully reprogram multiple immune checkpoint interactions on a
cellular level. Such a candidate may be able to replace future immune checkpoint therapeutic regimes composed of both
stimulatory- and inhibitory-receptor-targeting antibodies. |
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Place of Publication |
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Wos |
000747115200039 |
Publication Date |
2021-11-23 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
11 |
Open Access |
OpenAccess |
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Notes |
A.A.W. is the grateful recipient of a Maplethorpe Fellowship. K.A.J. acknowledges funding from the British Council (Newton Fund, 337313), Wellcome Trust (WT103913), and the Cancer Research UK King’s Health Partners Centre at King’s College London. Financial support is acknowledged from the European Commission under the Horizon 2020 Programme, by means of Grant Agreement No. 731019 (EUSMI). Images were drawn on BioRender.com. |
Approved |
Most recent IF: 13.942 |
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Call Number |
EMAT @ emat @c:irua:183950 |
Serial |
6829 |
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Author |
Choukroun, D.; Pacquets, L.; Li, C.; Hoekx, S.; Arnouts, S.; Baert, K.; Hauffman, T.; Bals, S.; Breugelmans, T. |
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Title |
Mapping composition–selectivity relationships of supported sub-10 nm Cu–Ag nanocrystals for high-rate CO₂ electroreduction |
Type |
A1 Journal article |
| |
Year |
2021 |
Publication |
Acs Nano |
Abbreviated Journal |
Acs Nano |
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Volume |
15 |
Issue |
9 |
Pages |
14858-14872 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
Colloidal Cu–Ag nanocrystals measuring less than 10 nm across are promising candidates for integration in hybrid CO2 reduction reaction (CO2RR) interfaces, especially in the context of tandem catalysis and selective multicarbon (C2–C3) product formation. In this work, we vary the synthetic-ligand/copper molar ratio from 0.1 to 1.0 and the silver/copper atomic ratio from 0 to 0.7 and study the variations in the nanocrystals’ size distribution, morphology and reactivity at rates of ≥100 mA cm–2 in a gas-fed recycle electrolyzer operating under neutral to mildly basic conditions (0.1–1.0 M KHCO3). High-resolution electron microscopy and spectroscopy are used in order to characterize the morphology of sub-10 nm Cu–Ag nanodimers and core–shells and to elucidate trends in Ag coverage and surface composition. It is shown that Cu–Ag nanocrystals can be densely dispersed onto a carbon black support without the need for immediate ligand removal or binder addition, which considerably facilitates their application. Although CO2RR product distribution remains an intricate function of time, (kinetic) overpotential and processing conditions, we nevertheless conclude that the ratio of oxygenates to hydrocarbons (which depends primarily on the initial dispersion of the nanocrystals and their composition) rises 3-fold at moderate Ag atom % relative to Cu NCs-based electrodes. Finally, the merits of this particular Cu–Ag/C system and the recycling reactor employed are utilized to obtain maximum C2–C3 partial current densities of 92–140 mA cm–2 at −1.15 VRHE and liquid product concentrations in excess of 0.05 wt % in 1 M KHCO3 after short electrolysis periods. |
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Corporate Author |
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Publisher |
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Place of Publication |
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Wos |
000703553600082 |
Publication Date |
2021-08-24 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
25 |
Open Access |
OpenAccess |
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Notes |
D.C. acknowledges Thomas Kenis for configuring the analytical instrumentation (HPLC/GC-FID/ICP-MS), Hannelore Andries for assistance with ICP-MS measurements, and Dr. Saeid Pourbabak and Dr. Tine Derez for assistance with Cu sputtering. L.P. was supported by Research Foundation of Flanders (FWO 1S56920N). S.B. acknowledges financial support from ERC Consolidator grant number 815128 REALNANO. S.B. and T.B. acknowledge financial support from the university research fund (BOF-GOA-PS ID no. 33928).; sygmaSB |
Approved |
Most recent IF: 13.942 |
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Call Number |
UA @ admin @ c:irua:180305 |
Serial |
6844 |
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Author |
Dey, A.; Ye, J.; De, A.; Debroye, E.; Ha, S.K.; Bladt, E.; Kshirsagar, A.S.; Wang, Z.; Yin, J.; Wang, Y.; Quan, L.N.; Yan, F.; Gao, M.; Li, X.; Shamsi, J.; Debnath, T.; Cao, M.; Scheel, M.A.; Kumar, S.; Steele, J.A.; Gerhard, M.; Chouhan, L.; Xu, K.; Wu, X.-gang; Li, Y.; Zhang, Y.; Dutta, A.; Han, C.; Vincon, I.; Rogach, A.L.; Nag, A.; Samanta, A.; Korgel, B.A.; Shih, C.-J.; Gamelin, D.R.; Son, D.H.; Zeng, H.; Zhong, H.; Sun, H.; Demir, H.V.; Scheblykin, I.G.; Mora-Sero, I.; Stolarczyk, J.K.; Zhang, J.Z.; Feldmann, J.; Hofkens, J.; Luther, J.M.; Perez-Prieto, J.; Li, L.; Manna, L.; Bodnarchuk, M., I; Kovalenko, M., V; Roeffaers, M.B.J.; Pradhan, N.; Mohammed, O.F.; Bakr, O.M.; Yang, P.; Muller-Buschbaum, P.; Kamat, P., V; Bao, Q.; Zhang, Q.; Krahne, R.; Galian, R.E.; Stranks, S.D.; Bals, S.; Biju, V.; Tisdale, W.A.; Yan, Y.; Hoye, R.L.Z.; Polavarapu, L. |
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Title |
State of the art and prospects for Halide Perovskite Nanocrystals |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Acs Nano |
Abbreviated Journal |
Acs Nano |
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Volume |
15 |
Issue |
7 |
Pages |
10775-10981 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Metal-halide perovskites have rapidly emerged as one of the most promising materials of the 21st century, with many exciting properties and great potential for a broad range of applications, from photovoltaics to optoelectronics and photocatalysis. The ease with which metal-halide perovskites can be synthesized in the form of brightly luminescent colloidal nanocrystals, as well as their tunable and intriguing optical and electronic properties, has attracted researchers from different disciplines of science and technology. In the last few years, there has been a significant progress in the shape-controlled synthesis of perovskite nanocrystals and understanding of their properties and applications. In this comprehensive review, researchers having expertise in different fields (chemistry, physics, and device engineering) of metal-halide perovskite nanocrystals have joined together to provide a state of the art overview and future prospects of metal-halide perovskite nanocrystal research. |
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Wos |
000679406500006 |
Publication Date |
2021-06-17 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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| |
ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
538 |
Open Access |
OpenAccess |
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Notes |
E.D. and J.H. acknowledge financial support from the Research FoundationFlanders (FWO Grant Nos. S002019N, G.0B39.15, G.0B49.15, G.0962.13, G098319N, and ZW15_09-GOH6316), the Research Foundation Flanders postdoctoral fellowships to J.A.S. and E.D. (FWO Grant Nos. 12Y7218N and 12O3719N, respectively), |
Approved |
Most recent IF: 13.942 |
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Call Number |
UA @ admin @ c:irua:180553 |
Serial |
6846 |
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| Permanent link to this record |
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Author |
Locardi, F.; Samoli, M.; Martinelli, A.; Erdem, O.; Vale Magalhaes, D.; Bals, S.; Hens, Z. |
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Title |
Cyan emission in two-dimensional colloidal Cs2CdCl4:SB3+ Ruddlesden-Popper phase nanoplatelets |
Type |
A1 Journal article |
| |
Year |
2021 |
Publication |
Acs Nano |
Abbreviated Journal |
Acs Nano |
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| |
Volume |
15 |
Issue |
11 |
Pages |
17729-17737 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Metal halide perovskites are one of the most investigated materials in optoelectronics, with their lead-based counterparts being renowned for their enhanced optoelectronic performance. The 3D CsPbX3 structure has set the standard with many studies currently attempting to substitute lead with other metals while retaining the properties of this material. This effort has led to the fabrication of metal halides with lower dimensionality, wherein particular 2D layered perovskite structures have captured attention as inspiration for the next generation of colloidal semiconductors. Here we report the synthesis of the Ruddlesden-Popper Cs2CdCl4:Sb3+ phase as colloidal nanoplatelets (NPs) using a facile hot injection approach under atmospheric conditions. Through strict adjustment of the synthesis parameters with emphasis on the ligand ratio, we obtained NPs with a relatively uniform size and good morphological control. The particles were characterized through transmission electron microscopy, synchrotron X-ray diffraction, and pair distribution function analysis. The spectroscopic characterization revealed most strikingly an intense cyan emission under UV excitation with a measured PLQY of similar to 20%. The emission was attributed to the Sb3+-doping within the structure. |
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Place of Publication |
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Wos |
000747115200053 |
Publication Date |
0000-00-00 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
13.942 |
Times cited |
34 |
Open Access |
OpenAccess |
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Notes |
The authors acknowledge the European Synchrotron Radiation Facility for provision of synchrotron radiation facilities and they would like to thank Andrew Fitch for assistance in using beamline ID22 (proposal HC-4098). Z.H. and S.B acknowledge funding from the Research Foundation − Flanders (FWO-Vlaanderen under the SBO − PROCEED project (No: S0002019N). Z.H. acknowledges Ghent University for funding (BOF-GOA 01G01019). S.B. is grateful to the European Research Council (ERC Consolidator Grant 815128, REALNANO). F.L. thanks Emanuela Sartori and Stefano Toso for the fruitful discussions. M.S. would like to thank Olivier Janssens for collecting XRPD data and Gabriele Pippia for helpful insights and discussions. |
Approved |
Most recent IF: 13.942 |
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| |
Call Number |
UA @ admin @ c:irua:186465 |
Serial |
7059 |
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| Permanent link to this record |
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Author |
Toso, S.; Akkerman, Q.A.; Martin-Garcia, B.; Prato, M.; Zito, J.; Infante, I.; Dang, Z.; Moliterni, A.; Giannini, C.; Bladt, E.; Lobato, I.; Ramade, J.; Bals, S.; Buha, J.; Spirito, D.; Mugnaioli, E.; Gemmi, M.; Manna, L. |
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Title |
Nanocrystals of lead chalcohalides : a series of kinetically trapped metastable nanostructures |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Journal Of The American Chemical Society |
Abbreviated Journal |
J Am Chem Soc |
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| |
Volume |
142 |
Issue |
22 |
Pages |
10198-10211 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
We report the colloidal synthesis of a series of surfactant-stabilized lead chalcohalide nanocrystals. Our work is mainly focused on Pb4S3Br2, a chalcohalide phase unknown to date that does not belong to the ambient-pressure PbS-PbBr2 phase diagram. The Pb4S3Br2 nanocrystals herein feature a remarkably narrow size distribution (with a size dispersion as low as 5%), a good size tunability (from 7 to similar to 30 nm), an indirect bandgap, photoconductivity (responsivity = 4 +/- 1 mA/W), and stability for months in air. A crystal structure is proposed for this new material by combining the information from 3D electron diffraction and electron tomography of a single nanocrystal, X-ray powder diffraction, and density functional theory calculations. Such a structure is closely related to that of the recently discovered high-pressure chalcohalide Pb4S3I2 phase, and indeed we were able to extend our synthesis scheme to Pb4S3I2 colloidal nanocrystals, whose structure matches the one that has been published for the bulk. Finally, we could also prepare nanocrystals of Pb3S2Cl2, which proved to be a structural analogue of the recently reported bulk Pb3Se2Br2 phase. It is remarkable that one high-pressure structure (for Pb4S3I2) and two metastable structures that had not yet been reported (for Pb4S3Br2 and Pb3S2Cl2) can be prepared on the nanoscale by wet-chemical approaches. This highlights the important role of colloidal chemistry in the discovery of new materials and motivates further exploration into metal chalcohalide nanocrystals. |
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Corporate Author |
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Thesis |
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Place of Publication |
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Language |
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Wos |
000538526500035 |
Publication Date |
2020-05-06 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0002-7863 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15 |
Times cited |
32 |
Open Access |
OpenAccess |
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Notes |
; We would like to thank Dr. A. Toma for the access to the IIT clean room facilities' SEM/FIB and evaporators, the Smart Materials group (IIT) for the access to the ATR-FTIR equipment, S. Marras for the support during XRPD measurements, G. Pugliese for help with the TGA measurements, M. Campolucci for help with the experiments on NC growth kinetics, S. Lauciello for help with the SEM-EDX analyses, and D. Baranov and R. Brescia for the helpful discussions. We also acknowledge funding from the Programme for Research and Innovation Horizon 2020 (2014-2020) under the Marie Sklodowska-Curie Grant Agreement COMPASS No. 691185. I.I. acknowledges the Dutch NWO for financial support under the Vidi scheme (Grant No. 723.013.002). S.B. acknowledges support by means of the ERC Consolidator Grant No. 815128 REALNANO. E. M. and M.G acknowledge the Regione Toscana for funding the purchase of the Timepix detector through the FELIX project (Por CREO FESR 2014-2020 action). ; sygma |
Approved |
Most recent IF: 15; 2020 IF: 13.858 |
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Call Number |
UA @ admin @ c:irua:170218 |
Serial |
6566 |
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Author |
Ren, P.; Zhang, T.; Jain, N.; Ching, H.Y.V.; Jaworski, A.; Barcaro, G.; Monti, S.; Silvestre-Albero, J.; Celorrio, V.; Chouhan, L.; Rokicinska, A.; Debroye, E.; Kustrowski, P.; Van Doorslaer, S.; Van Aert, S.; Bals, S.; Das, S. |
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Title |
An atomically dispersed Mn-photocatalyst for generating hydrogen peroxide from seawater via the Water Oxidation Reaction (WOR) |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Journal of the American Chemical Society |
Abbreviated Journal |
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Volume |
145 |
Issue |
30 |
Pages |
16584-16596 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Organic synthesis (ORSY); Theory and Spectroscopy of Molecules and Materials (TSM²) |
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Abstract |
In this work, we have fabricatedan aryl amino-substitutedgraphiticcarbon nitride (g-C3N4) catalyst with atomicallydispersed Mn capable of generating hydrogen peroxide (H2O2) directly from seawater. This new catalyst exhibitedexcellent reactivity, obtaining up to 2230 & mu;M H2O2 in 7 h from alkaline water and up to 1800 & mu;Mfrom seawater under identical conditions. More importantly, the catalystwas quickly recovered for subsequent reuse without appreciable lossin performance. Interestingly, unlike the usual two-electron oxygenreduction reaction pathway, the generation of H2O2 was through a less common two-electron water oxidation reaction(WOR) process in which both the direct and indirect WOR processesoccurred; namely, photoinduced h(+) directly oxidized H2O to H2O2 via a one-step 2e(-) WOR, and photoinduced h(+) first oxidized a hydroxide (OH-) ion to generate a hydroxy radical ((OH)-O-& BULL;), and H2O2 was formed indirectly by thecombination of two (OH)-O-& BULL;. We have characterized thematerial, at the catalytic sites, at the atomic level using electronparamagnetic resonance, X-ray absorption near edge structure, extendedX-ray absorption fine structure, high-resolution transmission electronmicroscopy, X-ray photoelectron spectroscopy, magic-angle spinningsolid-state NMR spectroscopy, and multiscale molecular modeling, combiningclassical reactive molecular dynamics simulations and quantum chemistrycalculations. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Wos |
001034983300001 |
Publication Date |
2023-07-24 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0002-7863 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
15 |
Times cited |
21 |
Open Access |
Not_Open_Access |
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Notes |
S.D. thanks the IOF grant and Francqui start up grant from the University of Antwerp, Belgium, for the financial support. P.R. thanks CSC and T.Z. thanks FWO for their financial assistance to finish this work. E.D. would like to thank the KU Leuven Research Fund for financial support through STG/21/010. J.S.A. acknowledges financial support from MCIN/AEI/10.13039/501100011033 and EU NextGeneration/PRTR (Project PCI2020-111968/3D-Photocat) and Diamond Synchrotron (rapid access proposal SP32609). This work was supported by the European Research Council (grant 770887-PICOMETRICS to S.V.A. and Grant 815128-REALNANO to S.B.). S.B. and S.V.A. acknowledge financial support from the Research Foundation Flanders (FWO, Belgium, project G.0346.21 N). We also thank Mr. Jian Zhu and Mr. Shahid Ullah Khan from the University of Antwerp, Belgium, for helpful discussions. |
Approved |
Most recent IF: 15; 2023 IF: 13.858 |
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Call Number |
UA @ admin @ c:irua:198426 |
Serial |
8831 |
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Author |
Smith, J.D.; Bladt, E.; Burkhart, J.A.C.; Winckelmans, N.; Koczkur, K.M.; Ashberry, H.M.; Bals, S.; Skrabalak, S.E. |
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Title |
Defect-directed growth of symmetrically branched metal nanocrystals |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Angewandte Chemie-International Edition |
Abbreviated Journal |
Angew Chem Int Edit |
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Volume |
59 |
Issue |
59 |
Pages |
943-950 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Branched plasmonic nanocrystals (NCs) have attracted much attention due to electric field enhancements at their tips. Seeded growth provides routes to NCs with defined branching patterns and, in turn, near-field distributions with defined symmetries. Here, a systematic analysis was undertaken in which seeds containing different distributions of planar defects were used to grow branched NCs in order to understand how their distributions direct the branching. Characterization of the products by multimode electron tomography and analysis of the NC morphologies at different overgrowth stages indicate that the branching patterns are directed by the seed defects, with the emergence of branches from the seed faces consistent with minimizing volumetric strain energy at the expense of surface energy. These results contrast with growth of branched NCs from single-crystalline seeds and provide a new platform for the synthesis of symmetrically branched plasmonic NCs. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000498760200001 |
Publication Date |
2019-11-13 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1433-7851; 0570-0833 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
16.6 |
Times cited |
23 |
Open Access |
OpenAccess |
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Notes |
; The authors thank Samantha Harvey for her initial observations of branched structures, Alexander Chen for his help with SAED, the staff of the Nanoscale Characterization Facility (Dr. Yi Yi), Electron Microscopy Center (Dr. David Morgan and Dr. Barry Stein), and Molecular Structure Center at Indiana University. J.S. recognizes a fellowship provided by the Indiana Space Grant Consortium. E.B. acknowledges a post-doctoral grant from the Research Foundation Flanders (FWO, Belgium). This project has received funding to S.E.S. from the U.S. National Science Foundation (award numbers: 1602476 and 1904499) and Research Corporation for Scientific Advancement (2017 Frontiers in Research Excellence and Discovery Award) as well as to S.B. from the European Union's Horizon 2020 research and innovation program under grant agreement No 731019 (EUSMI) and No 815128 (REALNANO). ; sygma |
Approved |
Most recent IF: 16.6; 2020 IF: 11.994 |
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Call Number |
UA @ admin @ c:irua:165124 |
Serial |
6293 |
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Author |
Paul, S.; Bladt, E.; Richter, A.F.; Döblinger, M.; Tong, Y.; Huang, H.; Dey, A.; Bals, S.; Debnath, T.; Polavarapu, L.; Feldmann, J. |
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Title |
Manganese‐Doping‐Induced Quantum Confinement within Host Perovskite Nanocrystals through Ruddlesden–Popper Defects |
Type |
A1 Journal article |
| |
Year |
2020 |
Publication |
Angewandte Chemie-International Edition |
Abbreviated Journal |
Angew Chem Int Edit |
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Volume |
59 |
Issue |
17 |
Pages |
6794-6799 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
The concept of doping Mn2+ ions into II–VI semiconductor nanocrystals (NCs) was recently extended to perovskite NCs. To date, most studies on Mn2+ doped NCs focus on enhancing the emission related to the Mn2+ dopant via an energy transfer mechanism. Herein, we found that the doping of Mn2+ ions into CsPbCl3 NCs not only results in a Mn2+‐related orange emission, but also strongly influences the excitonic properties of the host NCs. We observe for the first time that Mn2+ doping leads to the formation of Ruddlesden–Popper (R.P.) defects and thus induces quantum confinement within the host NCs. We find that a slight doping with Mn2+ ions improves the size distribution of the NCs, which results in a prominent excitonic peak. However, with increasing the Mn2+ concentration, the number of R.P. planes increases leading to smaller single‐crystal domains. The thus enhanced confinement and crystal inhomogeneity cause a gradual blue shift and broadening of the excitonic transition, respectively. |
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Place of Publication |
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Language |
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Wos |
000525279800024 |
Publication Date |
2020-04-20 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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| |
ISSN |
1433-7851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
16.6 |
Times cited |
64 |
Open Access |
OpenAccess |
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Notes |
Deutsche Forschungsgemeinschaft, EXC 2089/1-390776260 ; H2020 European Research Council, 815128-REALNANO ; Horizon 2020 Framework Programme, 839042 731019 ; Alexander von Humboldt-Stiftung; We acknowledge financial support by the Bavarian State Ministry of Science, Research, and Arts through the grant “Solar Technologies go Hybrid (SolTech)”, the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germanys Excellence Strategy—EXC 2089/1‐390776260 (“e‐conversion”), the Alexander von Humboldt Foundation (A.D. and T.D.), the European Union's Horizon 2020 research and innovation program under the Marie Sklodowska‐Curie grant agreement No. 839042 (H.H.). E.B. acknowledges a postdoctoral grant 12T2719N from the Research Foundation Flanders (FWO, Belgium). E.B. and S.B. acknowledge the financial support from the European Research Council ERC Consolidator Grants #815128‐REALNANO. L.P. thanks the EU Infrastructure Project EUSMI (European Union's Horizon 2020, grant No 731019). We thank local research center “Center for NanoScience (CeNS)” for providing communicative networking structure. We acknowledge the funding of Nanosystems Initiative Munich (NIM) for color figures.; sygma |
Approved |
Most recent IF: 16.6; 2020 IF: 11.994 |
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Call Number |
EMAT @ emat @c:irua:168535 |
Serial |
6399 |
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Author |
Quan, L.N.; Ma, D.; Zhao, Y.; Voznyy, O.; Yuan, H.; Bladt, E.; Pan, J.; de Arquer, F.P.G.; Sabatini, R.; Piontkowski, Z.; Emwas, A.-H.; Todorovic, P.; Quintero-Bermudez, R.; Walters, G.; Fan, J.Z.; Liu, M.; Tan, H.; Saidaminov, M., I; Gao, L.; Li, Y.; Anjum, D.H.; Wei, N.; Tang, J.; McCamant, D.W.; Roeffaers, M.B.J.; Bals, S.; Hofkens, J.; Bakr, O.M.; Lu, Z.-H.; Sargent, E.H. |
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Title |
Edge stabilization in reduced-dimensional perovskites |
Type |
A1 Journal article |
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Year |
2020 |
Publication |
Nature Communications |
Abbreviated Journal |
Nat Commun |
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Volume |
11 |
Issue |
1 |
Pages |
170 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Reduced-dimensional perovskites are attractive light-emitting materials due to their efficient luminescence, color purity, tunable bandgap, and structural diversity. A major limitation in perovskite light-emitting diodes is their limited operational stability. Here we demonstrate that rapid photodegradation arises from edge-initiated photooxidation, wherein oxidative attack is powered by photogenerated and electrically-injected carriers that diffuse to the nanoplatelet edges and produce superoxide. We report an edge-stabilization strategy wherein phosphine oxides passivate unsaturated lead sites during perovskite crystallization. With this approach, we synthesize reduced-dimensional perovskites that exhibit 97 +/- 3% photoluminescence quantum yields and stabilities that exceed 300 h upon continuous illumination in an air ambient. We achieve green-emitting devices with a peak external quantum efficiency (EQE) of 14% at 1000 cd m(-2); their maximum luminance is 4.5 x 10(4) cd m(-2) (corresponding to an EQE of 5%); and, at 4000 cd m(-2), they achieve an operational half-lifetime of 3.5 h. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000551458200001 |
Publication Date |
2020-01-10 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2041-1723 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
16.6 |
Times cited |
147 |
Open Access |
OpenAccess |
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Notes |
; This publication is based in part on work supported by an award (KUS-11-009-21) from the King Abdullah University of Science and Technology (KAUST), by the Ontario Research Fund Research Excellence Program, by the Ontario Research Fund (ORF), by the Natural Sciences and Engineering Research Council (NSERC) of Canada, and by the US Department of Navy, Office of Naval Research (Grant Award No. N00014-17-12524). H.Y. acknowledges the Research Foundation-Flanders (FWO Vlaanderen) for a postdoctoral fellowship. E.B. gratefully acknowledges financial support by the Research Foundation-Flanders (FWO Vlaanderen). S.B. acknowledges financial support from European Research Council (ERC Starting Grant #815128-REALNANO). M.B.J.R. and J.H. acknowledge the Research Foundation-Flanders (FWO, Grants G.0962.13, G.0B39.15, AKUL/11/14 and G0H6316N), KU Leuven Research Fund (C14/15/053) and the European Research Council under the European Union's Seventh Framework Programme (FP/2007-2013)/ ERC Grant Agreement No. [307523], ERC-Stg LIGHT to M.B.J.R. DFT calculations were performed on the IBM BlueGene Q supercomputer with support from the Southern Ontario Smart Computing Innovation Platform (SOSCIP). M.I.S. acknowledges the Banting Postdoctoral Fellowship program from the Natural Sciences and Engineering Research Council of Canada (NSERC). H.T. acknowledges the Netherlands Organisation for Scientific Research (NWO) for a Rubicon grant (680-50-1511). ; sygma |
Approved |
Most recent IF: 16.6; 2020 IF: 12.124 |
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Call Number |
UA @ admin @ c:irua:171327 |
Serial |
6496 |
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Author |
Otero-Martinez, C.; Imran, M.; Schrenker, N.J.; Ye, J.; Ji, K.; Rao, A.; Stranks, S.D.; Hoye, R.L.Z.; Bals, S.; Manna, L.; Perez-Juste, J.; Polavarapu, L. |
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Title |
Fast A-site cation cross-exchange at room temperature : single-to double- and triple-cation halide perovskite nanocrystals |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
Angewandte Chemie: international edition in English |
Abbreviated Journal |
Angew Chem Int Edit |
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Volume |
61 |
Issue |
34 |
Pages |
e202205617-11 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
We report here fast A-site cation cross-exchange between APbX(3) perovskite nanocrystals (NCs) made of different A-cations (Cs (cesium), FA (formamidinium), and MA (methylammonium)) at room temperature. Surprisingly, the A-cation cross-exchange proceeds as fast as the halide (X=Cl, Br, or I) exchange with the help of free A-oleate complexes present in the freshly prepared colloidal perovskite NC solutions. This enabled the preparation of double (MACs, MAFA, CsFA)- and triple (MACsFA)-cation perovskite NCs with an optical band gap that is finely tunable by their A-site composition. The optical spectroscopy together with structural analysis using XRD and atomically resolved high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and integrated differential phase contrast (iDPC) STEM indicates the homogeneous distribution of different cations in the mixed perovskite NC lattice. Unlike halide ions, the A-cations do not phase-segregate under light illumination. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000823857300001 |
Publication Date |
2022-06-24 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1433-7851; 0570-0833 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
16.6 |
Times cited |
28 |
Open Access |
OpenAccess |
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| |
Notes |
L.P. acknowledges the support from the Spanish Ministerio de Ciencia e Innovacion through Ramon y Cajal grant (RYC2018-026103-I) and the Spanish State Research Agency (Grant No. PID2020-117371RA-I00), the grant from the Xunta de Galicia (ED431F2021/05). N.J.S. acknowledges financial support from the Research Foundation-Flanders via a postdoctoral fellowship (FWO Grant No. 1238622N). S.B. thanks the financial support of the European Research Council (ERC-CoG-2019815128) and of the European Commission (EUSMI, Grant 731019). R.L.Z.H. thanks the Royal Academy of Engineering through the Research Fellowships scheme (No.: RF\201718\1701). S.D.S. and K.J. acknowledge the Royal Society for funding. S.D.S. acknowledges the Royal Society and Tata Group (UF150033). The work has received funding from the European Research Council under the European Union's Horizon 2020 research and innovation programme (HYPERION -grant agreement no. 756962). The authors acknowledge the Engineering and Physical Sciences Research Council (EPSRC) for funding (EP/R023980/1). M.I. and L.M. acknowledge financial support from the Italian Ministry of University and Research (MIUR) through the Flag-Era JTC2019 project “Solution-Processed Perovskite/Graphene Nanocomposites for Self-Powered Gas Sensors” (PeroGaS). The authors acknowledge the Universidade de Vigo/CISUG for open access funding. |
Approved |
Most recent IF: 16.6 |
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| |
Call Number |
UA @ admin @ c:irua:189675 |
Serial |
7083 |
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| Permanent link to this record |
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| |
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Author |
Toso, S.; Imran, M.; Mugnaioli, E.; Moliterni, A.; Caliandro, R.; Schrenker, N.J.; Pianetti, A.; Zito, J.; Zaccaria, F.; Wu, Y.; Gemmi, M.; Giannini, C.; Brovelli, S.; Infante, I.; Bals, S.; Manna, L. |
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| |
Title |
Halide perovskites as disposable epitaxial templates for the phase-selective synthesis of lead sulfochloride nanocrystals |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
Nature communications |
Abbreviated Journal |
Nat Commun |
|
| |
Volume |
13 |
Issue |
1 |
Pages |
3976-10 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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| |
Abstract |
Colloidal chemistry grants access to a wealth of materials through simple and mild reactions. However, even few elements can combine in a variety of stoichiometries and structures, potentially resulting in impurities or even wrong products. Similar issues have been long addressed in organic chemistry by using reaction-directing groups, that are added to a substrate to promote a specific product and are later removed. Inspired by such approach, we demonstrate the use of CsPbCl3 perovskite nanocrystals to drive the phase-selective synthesis of two yet unexplored lead sulfochlorides: Pb3S2Cl2 and Pb4S3Cl2. When homogeneously nucleated in solution, lead sulfochlorides form Pb3S2Cl2 nanocrystals. Conversely, the presence of CsPbCl3 triggers the formation of Pb4S3Cl2/CsPbCl3 epitaxial heterostructures. The phase selectivity is guaranteed by the continuity of the cationic subnetwork across the interface, a condition not met in a hypothetical Pb3S2Cl2/CsPbCl3 heterostructure. The perovskite domain is then etched, delivering phase-pure Pb4S3Cl2 nanocrystals that could not be synthesized directly. Phase-selective approaches, such using reaction-directing groups, are often seen in traditional organic chemistry and catalysis. Here authors use perovskite nanocrystals as disposable templates to drive the phase-selective synthesis of two colloidal nanomaterials, the lead sulfohalides Pb3S2Cl2 and Pb4S3Cl2. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000825867200003 |
Publication Date |
2022-07-08 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
|
Edition |
|
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| |
ISSN |
2041-1723 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
16.6 |
Times cited |
15 |
Open Access |
OpenAccess |
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| |
Notes |
The authors would like to acknowledge Dr. Joka Buha for the help with preliminary tests preceding this project, and Dr. B. M. Aresta and Dr. L. Cassano for their administrative support. The authors acknowledge financial support from the Research Foundation Flanders (FWO) through a postdoctoral fellowship to N.J.S. (FWO Grant No. 1238622N, N.J.S). S.B. acknowledges financial support from the European Commission by ERC Consolidator grant REALNANO (No. 815128, S.B.). L.M. acknowledges financial support from the Italian Ministry of University and Research (MIUR) through the Flag-Era JTC2019 project “Solution-Processed Perovskite/Graphene Nanocomposites for SelfPowered Gas Sensors” (PeroGaS, L.M.). The access to the National Synchrotron Light Source, Brookhaven National Laboratory, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC0298CH10886 (NSLS-II Proposal Number 307441). |
Approved |
Most recent IF: 16.6 |
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| |
Call Number |
UA @ admin @ c:irua:189684 |
Serial |
7085 |
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| Permanent link to this record |
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| |
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Author |
Wang, D.; Hermes, M.; Najmr, S.; Tasios, N.; Grau-Carbonell, A.; Liu, Y.; Bals, S.; Dijkstra, M.; Murray, C.B.; van Blaaderen, A. |
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Title |
Structural diversity in three-dimensional self-assembly of nanoplatelets by spherical confinement |
Type |
A1 Journal article |
| |
Year |
2022 |
Publication |
Nature communications |
Abbreviated Journal |
Nat Commun |
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| |
Volume |
13 |
Issue |
1 |
Pages |
6001-6012 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Nanoplatelets offer many possibilities to construct advanced materials due to new properties associated with their (semi)two-dimensional shapes. However, precise control of both positional and orientational order of the nanoplatelets in three dimensions, which is required to achieve emerging and collective properties, is challenging to realize. Here, we combine experiments, advanced electron tomography and computer simulations to explore the structure of supraparticles self-assembled from nanoplatelets in slowly drying emulsion droplets. We demonstrate that the rich phase behaviour of nanoplatelets, and its sensitivity to subtle changes in shape and interaction potential can be used to guide the self-assembly into a wide range of different structures, offering precise control over both orientation and position order of the nanoplatelets. Our research is expected to shed light on the design of hierarchically structured metamaterials with distinct shape- and orientation- dependent properties. Nanoplatelets can be used as anisotropic building blocks for constructing novel optoelectronic materials. Here, Wang et al. show a route of assembling nanoplatelets with controllable positional and orientational order in three dimensions facilitated by the surface tension of drying emulsion droplets. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000867312100031 |
Publication Date |
2022-10-12 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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| |
ISSN |
2041-1723 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
16.6 |
Times cited |
7 |
Open Access |
OpenAccess |
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Notes |
We thank A. Kadu, M. Chiappini, F. Rabouw, S. Paliwal, X. Xie, C. Xia and Z. Wang for fruitful discussions. D.W. and A.v.B. acknowledge partial financial support from the European Research Council under the European Union's Seventh Framework Programme (FP-2007-2013)/ERC Advanced Grant Agreement 291667 HierarSACol. M.H. was supported by the Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC). D.W. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (grant 894254 SuprAtom). Y.L. acknowledges the Sustainability project between the faculties of Science and Geosciences of Utrecht University. M.D. acknowledges financial support from European Research Council (Grant No. ERC-2019-ADV-H2020 884902 SoftML). S.B. acknowledges financial support from ERC Consolidator Grant No. 815128 REALNANO. C.B.M. acknowledges support for materials synthesis from the Office of Naval Research Multidisciplinary University Research Initiative Award ONR N00014-18-1-2497. The authors acknowledge the EM square center at Utrecht University for the access to the microscopes. |
Approved |
Most recent IF: 16.6 |
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| |
Call Number |
UA @ admin @ c:irua:191387 |
Serial |
7214 |
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| Permanent link to this record |
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Author |
Chen, H.; Xiong, Y.; Li, J.; Abed, J.; Wang, D.; Pedrazo-Tardajos, A.; Cao, Y.; Zhang, Y.; Wang, Y.; Shakouri, M.; Xiao, Q.; Hu, Y.; Bals, S.; Sargent, E.H.H.; Su, C.-Y.; Yang, Z. |
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Title |
Epitaxially grown silicon-based single-atom catalyst for visible-light-driven syngas production |
Type |
A1 Journal article |
| |
Year |
2023 |
Publication |
Nature communications |
Abbreviated Journal |
Nat Commun |
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| |
Volume |
14 |
Issue |
1 |
Pages |
1719-11 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Despite the natural abundance and promising properties of Si, there are few examples of crystalline Si-based catalysts. Here, the authors report an epitaxial growth method to construct Co single atoms on Si for light driven CO2 reduction to syngas. Improving the dispersion of active sites simultaneous with the efficient harvest of photons is a key priority for photocatalysis. Crystalline silicon is abundant on Earth and has a suitable bandgap. However, silicon-based photocatalysts combined with metal elements has proved challenging due to silicon's rigid crystal structure and high formation energy. Here we report a solid-state chemistry that produces crystalline silicon with well-dispersed Co atoms. Isolated Co sites in silicon are obtained through the in-situ formation of CoSi2 intermediate nanodomains that function as seeds, leading to the production of Co-incorporating silicon nanocrystals at the CoSi2/Si epitaxial interface. As a result, cobalt-on-silicon single-atom catalysts achieve an external quantum efficiency of 10% for CO2-to-syngas conversion, with CO and H-2 yields of 4.7 mol g((Co))(-1) and 4.4 mol g((Co))(-1), respectively. Moreover, the H-2/CO ratio is tunable between 0.8 and 2. This photocatalyst also achieves a corresponding turnover number of 2 x 10(4) for visible-light-driven CO2 reduction over 6 h, which is over ten times higher than previously reported single-atom photocatalysts. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000962607600018 |
Publication Date |
2023-03-28 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
|
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| |
ISSN |
2041-1723 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
16.6 |
Times cited |
6 |
Open Access |
OpenAccess |
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| |
Notes |
This work was supported by the National Natural Science Foundation of China (21821003, 21890380, 21905316), Guangdong Natural Science Foundation (2019A1515011748), the Science and Technology Planning Project of Guangdong Province (2019A050510018), Pearl River Recruitment Program of Talent (2019QN01C108), the EU Infrastructure Project EUSMI (Grant No. E190700310), and Sun Yat-sen University. D.W. acknowledges an Individual Fellowship funded by the Marie-Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (grant 894254 SuprAtom). S.B. and A.P.-T. acknowledge financial support from the European Commission under the Horizon 2020 Programme by grant no. 731019 (EUSMI) and ERC Consolidator grant no. 815128 (REALNANO). This project has received funding from the European Commission Grant (EUSMI E190700310). Synchrotron XAS data described in this paper was performed at the Canadian Light Source, a national research facility of the University of Saskatchewan, which is supported by the Canada Foundation for Innovation (CFI), the Natural Sciences and Engineering Research Council (NSERC), the National Research Council (NRC), the Canadian Institutes of Health Research (CIHR), the Government of Saskatchewan, and the University of Saskatchewan. |
Approved |
Most recent IF: 16.6; 2023 IF: 12.124 |
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| |
Call Number |
UA @ admin @ c:irua:196062 |
Serial |
7932 |
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| Permanent link to this record |
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Author |
Arteaga Cardona, F.; Jain, N.; Popescu, R.; Busko, D.; Madirov, E.; Arús, B.A.; Gerthsen, D.; De Backer, A.; Bals, S.; Bruns, O.T.; Chmyrov, A.; Van Aert, S.; Richards, B.S.; Hudry, D. |
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Title |
Preventing cation intermixing enables 50% quantum yield in sub-15 nm short-wave infrared-emitting rare-earth based core-shell nanocrystals |
Type |
A1 Journal Article |
| |
Year |
2023 |
Publication |
Nature communications |
Abbreviated Journal |
Nat Commun |
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| |
Volume |
14 |
Issue |
1 |
Pages |
4462 |
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| |
Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Short-wave infrared (SWIR) fluorescence could become the new gold standard in optical imaging for biomedical applications due to important advantages such as lack of autofluorescence, weak photon absorption by blood and tissues, and reduced photon scattering coefficient. Therefore, contrary to the visible and NIR regions, tissues become translucent in the SWIR region. Nevertheless, the lack of bright and biocompatible probes is a key challenge that must be overcome to unlock the full potential of SWIR fluorescence. Although rare-earth-based core-shell nanocrystals appeared as promising SWIR probes, they suffer from limited photoluminescence quantum yield (PLQY). The lack of control over the atomic scale organization of such complex materials is one of the main barriers limiting their optical performance. Here, the growth of either homogeneous (α-NaYF<sub>4</sub>) or heterogeneous (CaF<sub>2</sub>) shell domains on optically-active α-NaYF<sub>4</sub>:Yb:Er (with and without Ce<sup>3+</sup>co-doping) core nanocrystals is reported. The atomic scale organization can be controlled by preventing cation intermixing only in heterogeneous core-shell nanocrystals with a dramatic impact on the PLQY. The latter reached 50% at 60 mW/cm<sup>2</sup>; one of the highest reported PLQY values for sub-15 nm nanocrystals. The most efficient nanocrystals were utilized for in vivo imaging above 1450 nm. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
001037058500022 |
Publication Date |
2023-07-25 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
|
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| |
ISSN |
2041-1723 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
16.6 |
Times cited |
1 |
Open Access |
OpenAccess |
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| |
Notes |
D.H. would like to thank Dominique Ectors (Bruker AXS GmbH, Karlsruhe, Germany) for assistance and discussion on the PXRD data and TOPAS evaluations. The authors would like to acknowledge the financial support provided by the Helmholtz Association via: i) the Professorial Recruitment Initiative Funding (B.S.R.); ii) the Research Field Energy – Program Materials and Technologies for the Energy Transition – Topic 1 Photovoltaics (F.A.C., D.B., E.M., B.S.R., D.H.). This project received funding from the European Union’s Horizon 2020 innovation programme under grant agreement 823717. This work was supported by the European Research Council (grant 770887-PICOMETRICS to S.V.A. and Grant 815128-REALNANO to S.B.). The authors acknowledge financial support from the ResearchFoundation Flanders (FWO, Belgium) through project fundings (G.0346.21 N to S.V.A. and S.B.) and a postdoctoral grant (A.D.B.). The authors (B.A.A., O.T.B. and A.C.) acknowledge funding from the Helmholtz Zentrum München, the DFG-Emmy Noether program (BR 5355/2-1) and from the CZI Deep Tissue Imaging (DTI-0000000248). The authors (O.T.B. and D.H.) would like to thank the Helmholtz Imaging (ZT-I-PF-4-038-BENIGN). |
Approved |
Most recent IF: 16.6; 2023 IF: 12.124 |
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Call Number |
EMAT @ emat @c:irua:198158 |
Serial |
8808 |
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| Permanent link to this record |
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Author |
Guerrero, A.; Heidari, H.; Ripolles, T.S.; Kovalenko, A.; Pfannmöller, M.; Bals, S.; Kauffmann, L.-D.; Bisquert, J.; Garcia-Belmonte, G. |
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Title |
Shelf life degradation of bulk heterojunction solar cells : intrinsic evolution of charge transfer complex |
Type |
A1 Journal article |
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Year |
2015 |
Publication |
Laser physics review |
Abbreviated Journal |
Adv Energy Mater |
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| |
Volume |
5 |
Issue |
5 |
Pages |
1401997 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Achievement of long-term stability of organic photovoltaics is currently one of the major topics for this technology to reach maturity. Most of the techniques used to reveal degradation pathways are destructive and/or do not allow for real-time measurements in operating devices. Here, three different, nondestructive techniques able to provide real-time information, namely, film absorbance, capacitance-voltage (C-V), and impedance spectroscopy (IS), are combined over a period of 1 year using non-accelerated intrinsic degradation conditions. It is discerned between chemical modifications in the active layer, physical processes taking place in the bulk of the blend from those at the active layer/contact interfaces. In particular, it is observed that during the ageing experiment, the main source for device performance degradation is the formation of donor-acceptor charge-transfer complex (P3HT(center dot+)-PCBM center dot-) that acts as an exciton quencher. Generation of these radical species diminishes photocurrent and reduces open-circuit voltage by the creation of electronic defect states. Conclusions extracted from absorption, C-V, and IS measurements will be further supported by a range of other techniques such as atomic force microscopy, X-ray diffraction, and dark-field imaging of scanning transmission electron microscopy on ultrathin cross-sections. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
S.l. |
Editor |
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Language |
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Wos |
000352708600013 |
Publication Date |
2014-12-12 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1614-6832; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
16.721 |
Times cited |
30 |
Open Access |
OpenAccess |
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Notes |
287594 Sunflower; 335078 Colouratom; ECAS_Sara; (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:cannot); |
Approved |
Most recent IF: 16.721; 2015 IF: 16.146 |
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Call Number |
c:irua:126000 |
Serial |
2994 |
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| Permanent link to this record |
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Author |
Ben Dkhil, S.; Pfannmöller, M.; Bals, S.; Koganezawa, T.; Yoshimoto, N.; Hannani, D.; Gaceur, M.; Videlot-Ackermann, C.; Margeat, O.; Ackermann, J. |
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Title |
Square-centimeter-sized high-efficiency polymer solar cells : how the processing atmosphere and film quality influence performance at large scale |
Type |
A1 Journal article |
| |
Year |
2016 |
Publication |
Laser physics review |
Abbreviated Journal |
Adv Energy Mater |
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Volume |
6 |
Issue |
6 |
Pages |
1600290 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Organic solar cells based on two benzodithiophene-based polymers (PTB7 and PTB7-Th) processed at square centimeter-size under inert atmosphere and ambient air, respectively, are investigated. It is demonstrated that the performance of solar cells processed under inert atmosphere is not limited by the upscaling of photoactive layer and the interfacial layers. Thorough morphological and electrical characterizations of optimized layers and corresponding devices reveal that performance losses due to area enlargement are only caused by the sheet resistance of the transparent electrode reducing the effi ciency from 9.3% of 7.8% for PTB7-Th in the condition that both photoactive layer and the interfacial layers are of high layer quality. Air processing of photoactive layer and the interfacial layers into centimeter-sized solar cells lead to additional, but only slight, losses (< 10%) in all photovoltaic parameters, which can be addressed to changes in the electronic properties of both active layer and ZnO layers rather than changes in layer morphology. The demonstrated compatibility of polymer solar cells using solution-processed photoactive layer and interfacial layers with large area indicates that the introduction of a standard active area of 1 cm(2) for measuring effi ciency of organic record solar cells is feasible. However electric standards for indium tin oxides (ITO) or alternative transparent electrodes need to be developed so that performance of new photovoltaic materials can be compared at square centimeter-size. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
Place of publication unknown |
Editor |
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Language |
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Wos |
000379314700010 |
Publication Date |
2016-05-04 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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| |
ISSN |
1614-6832 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
16.721 |
Times cited |
6 |
Open Access |
Not_Open_Access |
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Notes |
; The authors acknowledge financial support by the French Fond Unique Intermisteriel (FUI) under the project “SFUMATO” (Grant number: F1110019V/ 201308815) as well as by the European Commission under the Project “SUNFLOWER” (FP7-ICT-2011-7-contract no. 287594). Generalitat Valenciana (ISIC/2012/008 Institute of Nanotechnologies for Clean Energies) is also acknowledged for providing financial support. The synchrotron radiation experiments were performed at BL46XU and BL19B2 in SPring-8 with the approval of Japan Synchrotron Radiation Research Institute (JASRI) (Proposal Nos. 2014B1916 and 2015A1984). The authors further acknowledge financial support from the European Research Council (ERC Starting Grant #335078-COLOURATOMS). ; |
Approved |
Most recent IF: 16.721 |
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| |
Call Number |
UA @ lucian @ c:irua:134951 |
Serial |
4249 |
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| Permanent link to this record |
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Author |
Ben Dkhil, S.; Pfannmöller, M.; Saba, M.I.; Gaceur, M.; Heidari, H.; Videlot-Ackermann, C.; Margeat, O.; Guerrero, A.; Bisquert, J.; Garcia-Belmonte, G.; Mattoni, A.; Bals, S.; Ackermann, J. |
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Title |
Toward high-temperature stability of PTB7-based bulk heterojunction solar cells : impact of fullerene size and solvent additive |
Type |
A1 Journal article |
| |
Year |
2017 |
Publication |
Laser physics review |
Abbreviated Journal |
Adv Energy Mater |
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| |
Volume |
7 |
Issue |
7 |
Pages |
1601486 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
The use of fullerene as acceptor limits the thermal stability of organic solar cells at high temperatures as their diffusion inside the donor leads to phase separation via Ostwald ripening. Here it is reported that fullerene diffusion is fully suppressed at temperatures up to 140 degrees C in bulk heterojunctions based on the benzodithiophene-based polymer (the poly[[4,8-bis[(2-ethylhexyl)oxy]benzo[1,2-b: 4,5-b']dithiophene-2,6-diyl][3-fluoro-2-[(2-ethylhexyl) carbonyl]thieno[3,4-b]thiophenediyl]], (PTB7) in combination with the fullerene derivative [6,6]-phenyl-C71-butyric acid methyl ester (PC70BM). The blend stability is found independently of the presence of diiodooctane (DIO) used to optimize nanostructuration and in contrast to PTB7 blends using the smaller fullerene derivative PC70BM. The unprecedented thermal stability of PTB7: PC70BM layers is addressed to local minima in the mixing enthalpy of the blend forming stable phases that inhibit fullerene diffusion. Importantly, although the nanoscale morphology of DIO processed blends is thermally stable, corresponding devices show strong performance losses under thermal stress. Only by the use of a high temperature annealing step removing residual DIO from the device, remarkably stable high efficiency solar cells with performance losses less than 10% after a continuous annealing at 140 degrees C over 3 days are obtained. These results pave the way toward high temperature stable polymer solar cells using fullerene acceptors. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
Place of publication unknown |
Editor |
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Language |
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Wos |
000396328500009 |
Publication Date |
2016-11-07 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
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| |
ISSN |
1614-6832; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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| |
Impact Factor |
16.721 |
Times cited |
27 |
Open Access |
Not_Open_Access |
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Notes |
; The authors 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). Generalitat Valenciana (ISIC/2012/008 Institute of Nanotechnologies for Clean Energies) is also acknowledged for providing financial support. The authors further acknowledge financial support via ERC Starting Grant Colouratoms (335078). ; |
Approved |
Most recent IF: 16.721 |
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Call Number |
UA @ lucian @ c:irua:141991UA @ admin @ c:irua:141991 |
Serial |
4697 |
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| Permanent link to this record |
