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Manzaneda-Gonzalez, V.; Jenkinson, K.; Pena-Rodriguez, O.; Borrell-Grueiro, O.; Trivino-Sanchez, S.; Banares, L.; Junquera, E.; Espinosa, A.; Gonzalez-Rubio, G.; Bals, S.; Guerrero-Martinez, A. |
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Title |
From multi- to single-hollow trimetallic nanocrystals by ultrafast heating |
Type |
A1 Journal article |
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Year  |
2023 |
Publication |
Chemistry of materials |
Abbreviated Journal |
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Volume |
35 |
Issue |
22 |
Pages |
9603-9612 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Metal nanocrystals (NCs) display unique physicochemical features that are highly dependent on nanoparticle dimensions, anisotropy, structure, and composition. The development of synthesis methodologies that allow us to tune such parameters finely emerges as crucial for the application of metal NCs in catalysis, optical materials, or biomedicine. Here, we describe a synthetic methodology to fabricate hollow multimetallic heterostructures using a combination of seed-mediated growth routes and femtosecond-pulsed laser irradiation. The envisaged methodology relies on the coreduction of Ag and Pd ions on gold nanorods (Au NRs) to form Au@PdAg core-shell nanostructures containing small cavities at the Au-PdAg interface. The excitation of Au@PdAg NRs with low fluence femtosecond pulses was employed to induce the coalescence and growth of large cavities, forming multihollow anisotropic Au@PdAg nanostructures. Moreover, single-hollow alloy AuPdAg could be achieved in high yield by increasing the irradiation energy. Advanced electron microscopy techniques, energy-dispersive X-ray spectroscopy (EDX) tomography, X-ray absorption near-edge structure (XANES) spectroscopy, and finite differences in the time domain (FDTD) simulations allowed us to characterize the morphology, structure, and elemental distribution of the irradiated NCs in detail. The ability of the reported synthesis route to fabricate multimetallic NCs with unprecedented hollow nanostructures offers attractive prospects for the fabrication of tailored high-entropy alloy nanoparticles. |
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Wos |
001110623500001 |
Publication Date |
2023-11-06 |
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Edition |
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ISSN |
0897-4756; 1520-5002 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
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Times cited |
2 |
Open Access |
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no |
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Call Number |
UA @ admin @ c:irua:202144 |
Serial |
9040 |
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Author |
Jenkinson, K.; Spadaro, M.C.; Golovanova, V.; Andreu, T.; Morante, J.R.; Arbiol, J.; Bals, S. |
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Title |
Direct operando visualization of metal support interactions induced by hydrogen spillover during CO₂ hydrogenation |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Advanced materials |
Abbreviated Journal |
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Volume |
35 |
Issue |
51 |
Pages |
2306447-10 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
The understanding of catalyst active sites is a fundamental challenge for the future rational design of optimized and bespoke catalysts. For instance, the partial reduction of Ce4+ surface sites to Ce3+ and the formation of oxygen vacancies are critical for CO2 hydrogenation, CO oxidation, and the water gas shift reaction. Furthermore, metal nanoparticles, the reducible support, and metal support interactions are prone to evolve under reaction conditions; therefore a catalyst structure must be characterized under operando conditions to identify active states and deduce structure-activity relationships. In the present work, temperature-induced morphological and chemical changes in Ni nanoparticle-decorated mesoporous CeO2 by means of in situ quantitative multimode electron tomography and in situ heating electron energy loss spectroscopy, respectively, are investigated. Moreover, operando electron energy loss spectroscopy is employed using a windowed gas cell and reveals the role of Ni-induced hydrogen spillover on active Ce3+ site formation and enhancement of the overall catalytic performance. |
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Wos |
001106139400001 |
Publication Date |
2023-10-22 |
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Edition |
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ISSN |
0935-9648 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
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Times cited |
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Open Access |
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no |
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Call Number |
UA @ admin @ c:irua:201143 |
Serial |
9022 |
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Author |
Mulder, J.T.T.; Jenkinson, K.; Toso, S.; Prato, M.; Evers, W.H.H.; Bals, S.; Manna, L.; Houtepen, A.J.J. |
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Title |
Nucleation and growth of bipyramidal Yb:LiYF₄ nanocrystals : growing up in a hot environment |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Chemistry of materials |
Abbreviated Journal |
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Volume |
35 |
Issue |
14 |
Pages |
5311-5321 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Lanthanide-doped LiYF4 (Ln:YLF) is commonlyused fora broad variety of optical applications, such as lasing, photon upconversionand optical refrigeration. When synthesized as nanocrystals (NCs),this material is also of interest for biological applications andfundamental physical studies. Until now, it was unclear how Ln:YLFNCs grow from their ionic precursors into tetragonal NCs with a well-defined,bipyramidal shape and uniform dopant distribution. Here, we studythe nucleation and growth of ytterbium-doped LiYF4 (Yb:YLF),as a template for general Ln:YLF NC syntheses. We show that the formationof bipyramidal Yb:YLF NCs is a multistep process starting with theformation of amorphous Yb:YLF spheres. Over time, these spheres growvia Ostwald ripening and crystallize, resulting in bipyramidal Yb:YLFNCs. We further show that prolonged heating of the NCs results inthe degradation of the NCs, observed by the presence of large LiFcubes and small, irregular Yb:YLF NCs. Due to the similarity in chemicalnature of all lanthanide ions our work sheds light on the formationstages of Ln:YLF NCs in general. |
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Wos |
001021474500001 |
Publication Date |
2023-07-03 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756; 1520-5002 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
8.6 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
This project has received funding from the European Union's Horizon 2020 research and innovation program under Grant Agreement No. 766900 (Testing the large-scale limit of quantum mechanics). The authors thank Niranjan Saikumar for proof reading the manuscript. |
Approved |
Most recent IF: 8.6; 2023 IF: 9.466 |
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Call Number |
UA @ admin @ c:irua:197787 |
Serial |
8907 |
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Author |
Monai, M.; Jenkinson, K.; Melcherts, A.E.M.; Louwen, J.N.; Irmak, E.A.; Van Aert, S.; Altantzis, T.; Vogt, C.; van der Stam, W.; Duchon, T.; Smid, B.; Groeneveld, E.; Berben, P.; Bals, S.; Weckhuysen, B.M. |
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Title |
Restructuring of titanium oxide overlayers over nickel nanoparticles during catalysis |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Science |
Abbreviated Journal |
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Volume |
380 |
Issue |
6645 |
Pages |
644-651 |
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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 |
Reducible supports can affect the performance of metal catalysts by the formation of suboxide overlayers upon reduction, a process referred to as the strong metal-support interaction (SMSI). A combination of operando electron microscopy and vibrational spectroscopy revealed that thin TiOx overlayers formed on nickel/titanium dioxide catalysts during 400 degrees C reduction were completely removed under carbon dioxide hydrogenation conditions. Conversely, after 600 degrees C reduction, exposure to carbon dioxide hydrogenation reaction conditions led to only partial reexposure of nickel, forming interfacial sites in contact with TiOx and favoring carbon-carbon coupling by providing a carbon species reservoir. Our findings challenge the conventional understanding of SMSIs and call for more-detailed operando investigations of nanocatalysts at the single-particle level to revisit static models of structure-activity relationships. |
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Wos |
000999020900010 |
Publication Date |
2023-05-11 |
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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 |
0036-8075; 1095-9203 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
56.9 |
Times cited |
29 |
Open Access |
Not_Open_Access |
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Notes |
This work was supported by BASF and NWO CHIPP (research grant to B.M.W.); the MCEC NWO Gravitation Program (B.M.W.); the ARC-CBBC NWO Program (B.M.W.); the European Research Council (grant 770887 PICOMETRICS to S.V.A.); and the European Research Council (grant 815128 REALNANO to S.B.). |
Approved |
Most recent IF: 56.9; 2023 IF: 37.205 |
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Call Number |
UA @ admin @ c:irua:197432 |
Serial |
8923 |
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Author |
Mulder, J.T.; Meijer, M.S.; van Blaaderen, J.J.; du Fosse, I.; Jenkinson, K.; Bals, S.; Manna, L.; Houtepen, A.J. |
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Title |
Understanding and preventing photoluminescence quenching to achieve unity photoluminescence quantum yield in Yb:YLF nanocrystals |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
ACS applied materials and interfaces |
Abbreviated Journal |
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Volume |
15 |
Issue |
2 |
Pages |
3274-3286 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Ytterbium-doped LiYF4 (Yb:YLF) is a commonly used material for laser applications, as a photon upconversion medium, and for optical refrigeration. As nanocrystals (NCs), the material is also of interest for biological and physical applications. Unfortunately, as with most phosphors, with the reduction in size comes a large reduction of the photoluminescence quantum yield (PLQY), which is typically associated with an increase in surface-related PL quenching. Here, we report the synthesis of bipyramidal Yb:YLF NCs with a short axis of similar to 60 nm. We systematically study and remove all sources of PL quenching in these NCs. By chemically removing all traces of water from the reaction mixture, we obtain NCs that exhibit a near-unity PLQY for an Yb3+ concentration below 20%. At higher Yb3+ concentrations, efficient concentration quenching occurs. The surface PL quenching is mitigated by growing an undoped YLF shell around the NC core, resulting in near-unity PLQY values even for fully Yb3+-based LiYbF4 cores. This unambiguously shows that the only remaining quenching sites in core-only Yb:YLF NCs reside on the surface and that concentration quenching is due to energy transfer to the surface. Monte Carlo simulations can reproduce the concentration dependence of the PLQY. Surprisingly, Fo''rster resonance energy transfer does not give satisfactory agreement with the experimental data, whereas nearest-neighbor energy transfer does. This work demonstrates that Yb3+-based nanophosphors can be synthesized with a quality close to that of bulk single crystals. The high Yb3+ concentration in the LiYbF4/LiYF4 core/shell nanocrystals increases the weak Yb3+ absorption, making these materials highly promising for fundamental studies and increasing their effectiveness in bioapplications and optical refrigeration. |
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Wos |
000912997300001 |
Publication Date |
2023-01-06 |
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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 |
1944-8244 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.5 |
Times cited |
3 |
Open Access |
OpenAccess |
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Notes |
This project has received funding from the European Union's Horizon 2020 research and innovation program under Grant Agreement No. 766900 (Testing the Large-Scale Limit of Quantum Mechanics). A.J.H. and I.d.F. further acknowledge the European Research Council Horizon 2020 ERC Grant Agreement No. 678004 (Doping on Demand) for financial support. The authors thank Freddy Rabouw and Andries Meijerink (Utrecht University) for very fruitful discussions and extremely useful advice. The author s thank Jos Thieme for his help with the laser setups used . The authors furthermore thank Niranjan Saikumar for proofreading the manuscript. |
Approved |
Most recent IF: 9.5; 2023 IF: 7.504 |
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Call Number |
UA @ admin @ c:irua:194317 |
Serial |
7348 |
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Author |
dela Encarnacion, C.; Lenzi, E.; Henriksen-Lacey, M.; Molina, B.; Jenkinson, K.; Herrero, A.; Colas, L.; Ramos-Cabrer, P.; Toro-Mendoza, J.; Orue, I.; Langer, J.; Bals, S.; Jimenez de Aberasturi, D.; Liz-Marzan, L.M. |
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Title |
Hybrid magnetic-plasmonic nanoparticle probes for multimodal bioimaging |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
The journal of physical chemistry: C : nanomaterials and interfaces |
Abbreviated Journal |
J Phys Chem C |
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Volume |
126 |
Issue |
45 |
Pages |
19519-19531 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Multimodal contrast agents, which take advantage of different imaging modalities, have emerged as an interesting approach to overcome the technical limitations of individual techniques. We developed hybrid nanoparticles comprising an iron oxide core and an outer gold spiky layer, stabilized by a biocompatible polymeric shell. The combined magnetic and optical properties of the different components provide the required functionalities for magnetic resonance imaging (MRI), surface-enhanced Raman scattering (SERS), and fluorescence imaging. The fabrication of such hybrid nanoprobes comprised the adsorption of small gold nanoparticles onto premade iron oxide cores, followed by controlled growth of spiky gold shells. The gold layer thickness and branching degree (tip sharpness) can be controlled by modifying both the density of Au nanoparticle seeds on the iron oxide cores and the subsequent nanostar growth conditions. We additionally demonstrated the performance of these hybrid multifunctional nanoparticles as multimodal contrast agents for correlative imaging of in vitro cell models and ex vivo tissues. |
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Wos |
000883021700001 |
Publication Date |
2022-11-04 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1932-7447; 1932-7455 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.7 |
Times cited |
10 |
Open Access |
Not_Open_Access |
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Notes |
The authors acknowledge financial support from the European Research Council (ERC-AdG-2017, 787510) and MCIN/AEI/10.13039/501100011033 through grants PID2019-108854RA-I00 and Maria de Maeztu Unit of Excellence No. MDM-2017-0720. S.B. and K.J. acknowledge financial support from the European Commission under the Horizon 2020Programme by Grant No. 823717 (ESTEEM3) and ERC Consolidator Grant No. 815128 (REALNANO) . |
Approved |
Most recent IF: 3.7 |
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Call Number |
UA @ admin @ c:irua:192104 |
Serial |
7311 |
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Author |
Jenkinson, K.; Liz-Marzan, L.M.; Bals, S. |
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Title |
Multimode electron tomography sheds light on synthesis, structure, and properties of complex metal-based nanoparticles |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Advanced materials |
Abbreviated Journal |
Adv Mater |
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Volume |
34 |
Issue |
36 |
Pages |
2110394-19 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Electron tomography has become a cornerstone technique for the visualization of nanoparticle morphology in three dimensions. However, to obtain in-depth information about a nanoparticle beyond surface faceting and morphology, different electron microscopy signals must be combined. The most notable examples of these combined signals include annular dark-field scanning transmission electron microscopy (ADF-STEM) with different collection angles and the combination of ADF-STEM with energy-dispersive X-ray or electron energy loss spectroscopies. Here, the experimental and computational development of various multimode tomography techniques in connection to the fundamental materials science challenges that multimode tomography has been instrumental to overcoming are summarized. Although the techniques can be applied to a wide variety of compositions, the study is restricted to metal and metal oxide nanoparticles for the sake of simplicity. Current challenges and future directions of multimode tomography are additionally discussed. |
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Wos |
000831332200001 |
Publication Date |
2022-04-19 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0935-9648 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
29.4 |
Times cited |
10 |
Open Access |
OpenAccess |
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Notes |
The authors thank the financial support of the European Research Council (ERC-AdG-2017 787510, ERC-CoG-2019 815128) and of the European Commission (EUSMI, Grant 731019 and ESTEEM3, Grant 823717). |
Approved |
Most recent IF: 29.4 |
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Call Number |
UA @ admin @ c:irua:189616 |
Serial |
7087 |
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Author |
Sanchez-Iglesias, A.; Jenkinson, K.; Bals, S.; Liz-Marzan, L.M. |
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Title |
Kinetic regulation of the synthesis of pentatwinned gold nanorods below room temperature |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Journal Of Physical Chemistry C |
Abbreviated Journal |
J Phys Chem C |
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Volume |
125 |
Issue |
43 |
Pages |
23937-23944 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
The synthesis of gold nanorods requires the presence of symmetry-breaking and shape-directing additives, among which bromide ions and quaternary ammonium surfactants have been reported as essential. As a result, hexadecyltrimethylammonium bromide (CTAB) has been selected as the most efficient surfactant to direct anisotropic growth. One of the difficulties arising from this selection is the low solubility of CTAB in water at room temperature, and therefore the seeded growth of gold nanorods is usually performed at 25 degrees C or above, which has restricted so far the analysis of kinetic effects derived from lower temperatures. We report a systematic study of the synthesis of gold nanorods from pentatwinned seeds using hexadecyltrimethylammonium chloride (CTAC) as the principal surfactant and a low concentration of bromide as shape-directing agent. Under these conditions, the synthesis can be performed at temperatures as low as 8 degrees C, and the corresponding kinetic effects can be studied, resulting in temperature-controlled aspect ratio tunability. |
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Wos |
000716453300038 |
Publication Date |
2021-10-23 |
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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 |
1932-7447; 1932-7455 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.536 |
Times cited |
6 |
Open Access |
OpenAccess |
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Notes |
realnano; sygmaSB; This work was supported by the National Science Foundation (NSF) under award NSF CHE-1808502 (P.C. and I.J.). This work made use of the EPIC facility of Northwestern University's NUANCE Center, which has received support from the SHyNE Resource (NSF ECCS-2025633), the IIN, and Northwestern's MRSEC program (NSF DMR-1720139). D.A E. and S.B. acknowledge funding from the European Research Council under the European Union's Horizon 2020 research and innovation program (ERC Consolidator Grants No. 815128 REALNANO and Grant Agreement No. 731019 EUSMI). |
Approved |
Most recent IF: 4.536 |
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Call Number |
UA @ admin @ c:irua:184104 |
Serial |
6868 |
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