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| Author | Cioni, M.; Delle Piane, M.; Polino, D.; Rapetti, D.; Crippa, M.; Arslan Irmak, E.; Van Aert, S.; Bals, S.; Pavan, G.M. | ||||
| Title | Sampling real-time atomic dynamics in metal nanoparticles by combining experiments, simulations, and machine learning | Type | A1 Journal article | ||
| Year | 2024 | Publication | Advanced Science | Abbreviated Journal | |
| Volume | Issue | Pages | 1-13 | ||
| Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Even at low temperatures, metal nanoparticles (NPs) possess atomic dynamics that are key for their properties but challenging to elucidate. Recent experimental advances allow obtaining atomic-resolution snapshots of the NPs in realistic regimes, but data acquisition limitations hinder the experimental reconstruction of the atomic dynamics present within them. Molecular simulations have the advantage that these allow directly tracking the motion of atoms over time. However, these typically start from ideal/perfect NP structures and, suffering from sampling limits, provide results that are often dependent on the initial/putative structure and remain purely indicative. Here, by combining state-of-the-art experimental and computational approaches, how it is possible to tackle the limitations of both approaches and resolve the atomistic dynamics present in metal NPs in realistic conditions is demonstrated. Annular dark-field scanning transmission electron microscopy enables the acquisition of ten high-resolution images of an Au NP at intervals of 0.6 s. These are used to reconstruct atomistic 3D models of the real NP used to run ten independent molecular dynamics simulations. Machine learning analyses of the simulation trajectories allow resolving the real-time atomic dynamics present within the NP. This provides a robust combined experimental/computational approach to characterize the structural dynamics of metal NPs in realistic conditions. Experimental and computational techniques are bridged to unveil atomic dynamics in gold nanoparticles (NPs), using annular dark-field scanning transmission electron microscopy and molecular dynamics simulations informed by machine learning. The approach provides unprecedented insights into the real-time structural behaviors of NPs, merging state-of-the-art techniques to accurately characterize their dynamics under realistic conditions. image | ||||
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| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001206888000001 | Publication Date | 2024-04-24 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 2198-3844 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 15.1 | Times cited | Open Access | ||
| Notes | Approved | Most recent IF: 15.1; 2024 IF: 9.034 | |||
| Call Number | UA @ admin @ c:irua:205442 | Serial  |
9171 | ||
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| Author | Morad, V.; Stelmakh, A.; Svyrydenko, M.; Feld, L.G.; Boehme, S.C.; Aebli, M.; Affolter, J.; Kaul, C.J.; Schrenker, N.J.; Bals, S.; Sahin, Y.; Dirin, D.N.; Cherniukh, I.; Raino, G.; Baumketner, A.; Kovalenko, M.V. | ||||
| Title | Designer phospholipid capping ligands for soft metal halide nanocrystals | Type | A1 Journal article | ||
| Year | 2024 | Publication | Nature | Abbreviated Journal | |
| Volume | 626 | Issue | Pages | 542-548 | |
| Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
| Abstract | The success of colloidal semiconductor nanocrystals (NCs) in science and optoelectronics is inextricable from their surfaces. The functionalization of lead halide perovskite NCs1-5 poses a formidable challenge because of their structural lability, unlike the well-established covalent ligand capping of conventional semiconductor NCs6,7. We posited that the vast and facile molecular engineering of phospholipids as zwitterionic surfactants can deliver highly customized surface chemistries for metal halide NCs. Molecular dynamics simulations implied that ligand-NC surface affinity is primarily governed by the structure of the zwitterionic head group, particularly by the geometric fitness of the anionic and cationic moieties into the surface lattice sites, as corroborated by the nuclear magnetic resonance and Fourier-transform infrared spectroscopy data. Lattice-matched primary-ammonium phospholipids enhance the structural and colloidal integrity of hybrid organic-inorganic lead halide perovskites (FAPbBr3 and MAPbBr3 (FA, formamidinium; MA, methylammonium)) and lead-free metal halide NCs. The molecular structure of the organic ligand tail governs the long-term colloidal stability and compatibility with solvents of diverse polarity, from hydrocarbons to acetone and alcohols. These NCs exhibit photoluminescence quantum yield of more than 96% in solution and solids and minimal photoluminescence intermittency at the single particle level with an average ON fraction as high as 94%, as well as bright and high-purity (about 95%) single-photon emission. Phospholipids enhance the structural and colloidal integrity of hybrid organic-inorganic lead halide perovskites and lead-free metal halide nanocrystals, which then exhibit enhanced robustness and optical properties. | ||||
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| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001176943100001 | Publication Date | 2023-12-18 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 0028-0836; 1476-4687 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 64.8 | Times cited | Open Access | ||
| Notes | Approved | Most recent IF: 64.8; 2024 IF: 40.137 | |||
| Call Number | UA @ admin @ c:irua:204796 | Serial |
9144 | ||
| Permanent link to this record | |||||
| Author | Cioni, M.; Delle Piane, M.; Polino, D.; Rapetti, D.; Crippa, M.; Arslan Irmak, E.; Pavan, G.M.; Van Aert, S.; Bals, S. | ||||
| Title | Data for Sampling Real‐Time Atomic Dynamics in Metal Nanoparticles by Combining Experiments, Simulations, and Machine Learning | Type | Dataset | ||
| Year | 2024 | Publication | Abbreviated Journal | ||
| Volume | Issue | Pages | |||
| Keywords | Dataset; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Even at low temperatures, metal nanoparticles (NPs) possess atomic dynamics that are key for their properties but challenging to elucidate. Recent experimental advances allow obtaining atomic‐resolution snapshots of the NPs in realistic regimes, but data acquisition limitations hinder the experimental reconstruction of the atomic dynamics present within them. Molecular simulations have the advantage that these allow directly tracking the motion of atoms over time. However, these typically start from ideal/perfect NP structures and, suffering from sampling limits, provide results that are often dependent on the initial/putative structure and remain purely indicative. Here, by combining state‐of‐the‐art experimental and computational approaches, how it is possible to tackle the limitations of both approaches and resolve the atomistic dynamics present in metal NPs in realistic conditions is demonstrated. Annular dark‐field scanning transmission electron microscopy enables the acquisition of ten high‐resolution images of an Au NP at intervals of 0.6 s. These are used to reconstruct atomistic 3D models of the real NP used to run ten independent molecular dynamics simulations. Machine learning analyses of the simulation trajectories allows resolving the real‐time atomic dynamics present within the NP. This provides a robust combined experimental/computational approach to characterize the structural dynamics of metal NPs in realistic conditions. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | Publication Date | |||
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | ISBN | Additional Links | UA library record | ||
| Impact Factor | Times cited | Open Access | |||
| Notes | Approved | Most recent IF: NA | |||
| Call Number | UA @ admin @ c:irua:205843 | Serial |
9143 | ||
| Permanent link to this record | |||||
| Author | Lelouche, S.N.K.; Lemir, I.; Biglione, C.; Craig, T.; Bals, S.; Horcajada, P. | ||||
| Title | AuNP/MIL-88B-NH₂ nanocomposite for the valorization of nitroarene by green catalytic hydrogenation | Type | A1 Journal article | ||
| Year | 2024 | Publication | Chemistry: a European journal | Abbreviated Journal | |
| Volume | Issue | Pages | 1-10 | ||
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
| Abstract | The efficiency of a catalytic process is assessed based on conversion, yield, and time effectiveness. However, these parameters are insufficient for evaluating environmentally sustainable research. As the world is urged to shift towards green catalysis, additional factors such as reaction media, raw material availability, sustainability, waste minimization and catalyst biosafety, need to be considered to accurately determine the efficacy and sustainability of the process. By combining the high porosity and versatility of metal organic frameworks (MOFs) and the activity of gold nanoparticles (AuNPs), efficient, cyclable and biosafe composite catalysts can be achieved. Thus, a composite based on AuNPs and the nanometric flexible porous iron(III) aminoterephthalate MIL-88B-NH2 was successfully synthesized and fully characterized. This nanocomposite was tested as catalyst in the reduction of nitroarenes, which were identified as anthropogenic water pollutants, reaching cyclable high conversion rates at short times for different nitroarenes. Both synthesis and catalytic reactions were performed using green conditions, and even further tested in a time-optimizing one-pot synthesis and catalysis experiment. The sustainability and environmental impact of the catalytic conditions were assessed by green metrics. Thus, this study provides an easily implementable synthesis, and efficient catalysis, while minimizing the environmental and health impact of the process. | ||||
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| Language | Wos | 001204094600001 | Publication Date | 2024-03-22 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 0947-6539 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 4.3 | Times cited | Open Access | ||
| Notes | Approved | Most recent IF: 4.3; 2024 IF: 5.317 | |||
| Call Number | UA @ admin @ c:irua:205426 | Serial |
9135 | ||
| Permanent link to this record | |||||
| Author | Gao, Y.-J.; Jin, H.; Esteban, D.A.; Weng, B.; Saha, R.A.; Yang, M.-Q.; Bals, S.; Steele, J.A.; Huang, H.; Roeffaers, M.B.J. | ||||
| Title | 3D-cavity-confined CsPbBr₃ quantum dots for visible-light-driven photocatalytic C(sp³)-H bond activation | Type | A1 Journal article | ||
| Year | 2024 | Publication | Carbon Energy | Abbreviated Journal | |
| Volume | Issue | Pages | e559 | ||
| Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Metal halide perovskite (MHP) quantum dots (QDs) offer immense potential for several areas of photonics research due to their easy and low-cost fabrication and excellent optoelectronic properties. However, practical applications of MHP QDs are limited by their poor stability and, in particular, their tendency to aggregate. Here, we develop a two-step double-solvent strategy to grow and confine CsPbBr3 QDs within the three-dimensional (3D) cavities of a mesoporous SBA-16 silica scaffold (CsPbBr3@SBA-16). Strong confinement and separation of the MHP QDs lead to a relatively uniform size distribution, narrow luminescence, and good ambient stability over 2 months. In addition, the CsPbBr3@SBA-16 presents a high activity and stability for visible-light-driven photocatalytic toluene C(sp(3))-H bond activation to produce benzaldehyde with similar to 730 mu mol g(-1) h(-1) yield rate and near-unity selectivity. Similarly, the structural stability of CsPbBr3@SBA-16 QDs is superior to that of both pure CsPbBr3 QDs and those confined in MCM-41 with 1D channels. | ||||
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| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001223583600001 | Publication Date | 2024-05-16 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 2637-9368 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | Times cited | Open Access | |||
| Notes | Approved | Most recent IF: NA | |||
| Call Number | UA @ admin @ c:irua:206000 | Serial |
9133 | ||
| Permanent link to this record | |||||
| Author | Chakraborty, J.; Chatterjee, A.; Molkens, K.; Nath, I.; Arenas Esteban, D.; Bourda, L.; Watson, G.; Liu, C.; Van Thourhout, D.; Bals, S.; Geiregat, P.; Van der Voort, P. | ||||
| Title | Decoding Excimer Formation in Covalent–Organic Frameworks Induced by Morphology and Ring Torsion | Type | A1 Journal Article | ||
| Year | 2024 | Publication | Advanced Materials | Abbreviated Journal | Advanced Materials |
| Volume | Issue | Pages | |||
| Keywords | A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; | ||||
| Abstract | A thorough and quantitative understanding of the fate of excitons in covalent–organic frameworks (COFs) after photoexcitation is essential for their augmented optoelectronic and photocatalytic applications via precise structure tuning. The synthesis of a library of COFs having identical chemical backbone with impeded conjugation, but varied morphology and surface topography to study the effect of these physical properties on the photophysics of the materials is herein reported. The variation of crystallite size and surface topography substantified different aggregation pattern in the COFs, which leads to disparities in their photoexcitation and relaxation properties. Depending on aggregation, an inverse correlation between bulk luminescence decay time and exciton binding energy of the materials is perceived. Further transient absorption spectroscopic analysis confirms the presence of highly localized, immobile, Frenkel excitons (of diameter 0.3–0.5 nm) via an absence of annihilation at high density, most likely induced by structural torsion of the COF skeletons, which in turn preferentially relaxes via long‐lived (nanosecond to microsecond) excimer formation (in femtosecond scale) over direct emission. These insights underpin the importance of structural and topological design of COFs for their targeted use in photocatalysis. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001206226700001 | Publication Date | 2024-04-22 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 0935-9648 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 29.4 | Times cited | Open Access | ||
| Notes | PVDV, JC, AC, and IN acknowledge the FWO-Vlaanderen for research grant G020521N and the research board of UGent (BOF) through a Concerted Research Action (GOA010-17). JC acknowledges UGent for BOF postdoctoral grant (2022.0032.01). AC acknowledges FWOVlaanderen for postdoctoral grant (12T7521N). KM, DVT and PG acknowledges FWOVlaanderen for research grant G0B2921N. SB and DAE acknowledge financial support from ERC Consolidator Grant Number 815128 REALNANO. CHL acknowledges China Scholarship Council doctoral grant (201908110280). PVDV acknowledges Hercules Project AUGE/17/07 for the UV VIS DRS spectrometer and UGent BASBOF BOF20/BAS/015 for the powder X-Ray Diffractometer. PG thanks UGent for support of the Core Facility NOLIMITS. | Approved | Most recent IF: 29.4; 2024 IF: 19.791 | ||
| Call Number | EMAT @ emat @c:irua:205967 | Serial |
9130 | ||
| Permanent link to this record | |||||
| Author | Van Gordon, K.; Ni, B.; Girod, R.; Mychinko, M.; Bevilacqua, F.; Bals, S.; Liz‐Marzán, L.M. | ||||
| Title | Single Crystal and Pentatwinned Gold Nanorods Result in Chiral Nanocrystals with Reverse Handedness | Type | A1 Journal Article | ||
| Year | 2024 | Publication | Angewandte Chemie International Edition | Abbreviated Journal | Angew Chem Int Ed |
| Volume | Issue | Pages | |||
| Keywords | A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; | ||||
| Abstract | Handedness is an essential attribute of chiral nanocrystals, having a major influence on their properties. During chemical growth, the handedness of nanocrystals is usually tuned by selecting the corresponding enantiomer of chiral molecules involved in asymmetric growth, often known as chiral inducers. We report that, even using the same chiral inducer enantiomer, the handedness of chiral gold nanocrystals can be reversed by using Au nanorod seeds with either single crystalline or pentatwinned structure. This effect holds for chiral growth induced both by amino acids and by chiral micelles. Although it was challenging to discern the morphological handedness for<italic>L</italic>‐cystine‐directed particles, even using electron tomography, both cases showed circular dichroism bands of opposite sign, with nearly mirrored chiroptical signatures for chiral micelle‐directed growth, along with quasi‐helical wrinkles of inverted handedness. These results expand the chiral growth toolbox with an effect that might be exploited to yield a host of interesting morphologies with tunable optical properties. | ||||
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| Publisher | Place of Publication | Editor | |||
| Language | Wos | Publication Date | 2024-05-24 | ||
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 1433-7851 | ISBN | Additional Links | ||
| Impact Factor | 16.6 | Times cited | Open Access | ||
| Notes | Ana Sánchez-Iglesias is acknowledged for support in the synthesis of pentatwinned gold nanorods. The authors acknowledge financial support by the European Research Council (ERC CoG No. 815128 REALNANO to S.B.), from MCIN/AEI/10.13039/501100011033 (Grant PID2020- 117779RB-I00 to L.M.L.-M and FPI Fellowship PRE2021- 097588 to K.V.G.), and by KU Leuven (C14/22/085). This work has been funded by the European Union under Project 101131111—DELIGHT. Funding for open access charge: Universidade de Vigo/ CRUE-CISUG. | Approved | Most recent IF: 16.6; 2024 IF: 11.994 | ||
| Call Number | EMAT @ emat @ | Serial |
9129 | ||
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| Author | Guerrero, R.M.; Lemir, I.D.; Carrasco, S.; Fernández-Ruiz, C.; Kavak, S.; Pizarro, P.; Serrano, D.P.; Bals, S.; Horcajada, P.; Pérez, Y. | ||||
| Title | Scaling-Up Microwave-Assisted Synthesis of Highly Defective Pd@UiO-66-NH2Catalysts for Selective Olefin Hydrogenation under Ambient Conditions | Type | A1 Journal Article | ||
| Year | 2024 | Publication | ACS Applied Materials & Interfaces | Abbreviated Journal | ACS Appl. Mater. Interfaces |
| Volume | Issue | Pages | |||
| Keywords | A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; | ||||
| Abstract | The need to develop green and cost-effective industrial catalytic processes has led to growing interest in preparing more robust, efficient, and selective heterogeneous catalysts at a large scale. In this regard, microwave-assisted synthesis is a fast method for fabricating heterogeneous catalysts (including metal oxides, zeolites, metal–organic frameworks, and supported metal nanoparticles) with enhanced catalytic properties, enabling synthesis scale-up. Herein, the synthesis of nanosized UiO-66-NH2 was optimized via a microwave-assisted hydrothermal method to obtain defective matrices essential for the stabilization of metal nanoparticles, promoting catalytically active sites for hydrogenation reactions (760 kg·m–3·day–1 space time yield, STY). Then, this protocol was scaled up in a multimodal microwave reactor, reaching 86% yield (ca. 1 g, 1450 kg·m–3·day–1 STY) in only 30 min. Afterward, Pd nanoparticles were formed in situ decorating the nanoMOF by an effective and fast microwave-assisted hydrothermal method, resulting in the formation of Pd@UiO-66-NH2 composites. Both the localization and oxidation states of Pd nanoparticles (NPs) in the MOF were achieved using high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and X-ray photoelectron spectroscopy (XPS), respectively. The optimal composite, loaded with 1.7 wt % Pd, exhibited an extraordinary catalytic activity (>95% yield, 100% selectivity) under mild conditions (1 bar H2, 25 °C, 1 h reaction time), not only in the selective hydrogenation of a variety of single alkenes (1-hexene, 1-octene, 1-tridecene, cyclohexene, and tetraphenyl ethylene) but also in the conversion of a complex mixture of alkenes (i.e., 1-hexene, 1-tridecene, and anethole). The results showed a powerful interaction and synergy between the active phase (Pd NPs) and the catalytic porous scaffold (UiO-66-NH2), which are essential for the selectivity and recyclability. | ||||
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| Publisher | Place of Publication | Editor | |||
| Language | Wos | Publication Date | 2024-04-26 | ||
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 1944-8244 | ISBN | Additional Links | ||
| Impact Factor | 9.5 | Times cited | Open Access | ||
| Notes | The authors gratefully acknowledge financial support from “Comunidad de Madrid” and European Regional Development Fund-FEDER through the project HUB MADRID+CIRCULAR; the State Research Agency (MCIN/AEI /10.13039/501100011033) through the grant with reference number CEX2019-000931-M received in the 2019 call for “Severo Ochoa Centres of Excellence” and “María de Maeztu Units of Excellence” of the State Programme for Knowledge Generation and Scientific and Technological Strengthening of the R&D&I System; and MICIU through the project “NAPOLION” (PID2022-139956OB-I00). S.K. acknowledges the Flemish Fund for Scientific Research (FWO Vlaanderen) through a PhD research grant (1181124N). | Approved | Most recent IF: 9.5; 2024 IF: 7.504 | ||
| Call Number | EMAT @ emat @ | Serial |
9126 | ||
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| Author | Vlasov, E.; Heyvaert, W.; Ni, B.; Van Gordon, K.; Girod, R.; Verbeeck, J.; Liz-Marzán, L.M.; Bals, S. | ||||
| Title | High-Throughput Morphological Chirality Quantification of Twisted and Wrinkled Gold Nanorods | Type | A1 Journal Article | ||
| Year | 2024 | Publication | ACS Nano | Abbreviated Journal | ACS Nano |
| Volume | Issue | Pages | |||
| Keywords | A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; | ||||
| Abstract | Chirality in gold nanostructures offers an exciting opportunity to tune their differential optical response to left- and right-handed circularly polarized light, as well as their interactions with biomolecules and living matter. However, tuning and understanding such interactions demands quantification of the structural features that are responsible for the chiral behavior. Electron tomography (ET) enables structural characterization at the single-particle level and has been used to quantify the helicity of complex chiral nanorods. However, the technique is time-consuming and consequently lacks statistical value. To address this issue, we introduce herein a high-throughput methodology that combines images acquired by secondary electron-based electron beam-induced current (SEEBIC) with quantitative image analysis. As a result, the geometric chirality of hundreds of nanoparticles can be quantified in less than 1 h. When combining the drastic gain in data collection efficiency of SEEBIC with a limited number of ET data sets, a better understanding of how the chiral structure of individual chiral nanoparticles translates into the ensemble chiroptical response can be reached. | ||||
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| Publisher | Place of Publication | Editor | |||
| Language | Wos | Publication Date | 2024-04-26 | ||
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 1936-0851 | ISBN | Additional Links | ||
| Impact Factor | 17.1 | Times cited | Open Access | ||
| Notes | The authors acknowledge financial support by the European Research Council (ERC CoG No. 815128 REALNANO to S.B.) and from MCIN/AEI/10.13039/501100011033 (Grant PID2020-117779RB-I00 to L.M.L.-M and FPI Fellowship PRE2021-097588 to K.V.G.). Funded by the European Union under Project 101131111 − DELIGHT, JV acknowledges the eBEAM project supported by the European Union’s Horizon 2020 research and innovation program FETPROACT-EIC-07- 2020: emerging paradigms and communities. | Approved | Most recent IF: 17.1; 2024 IF: 13.942 | ||
| Call Number | EMAT @ emat @ | Serial |
9121 | ||
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| Author | Ignatova, K.; Vlasov, E.; Seddon, S.D.; Gauquelin, N.; Verbeeck, J.; Wermeille, D.; Bals, S.; Hase, T.P.A.; Arnalds, U.B. | ||||
| Title | Phase coexistence induced surface roughness in V2O3/Ni magnetic heterostructures | Type | A1 Journal Article | ||
| Year | 2024 | Publication | APL Materials | Abbreviated Journal | |
| Volume | 12 | Issue | 4 | Pages | |
| Keywords | A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; | ||||
| Abstract | We present an investigation of the microstructure changes in V2O3 as it goes through its inherent structural phase transition. Using V2O3 films with a well-defined crystal structure deposited by reactive magnetron sputtering on r-plane Al2O3 substrates, we study the phase coexistence region and its impact on the surface roughness of the films and the magnetic properties of overlying Ni magnetic layers in V2O3/Ni hybrid magnetic heterostructures. The simultaneous presence of two phases in V2O3 during its structural phase transition was identified with high resolution x-ray diffraction and led to an increase in surface roughness observed using x-ray reflectivity. The roughness reaches its maximum at the midpoint of the transition. In V2O3/Ni hybrid heterostructures, we find a concomitant increase in the coercivity of the magnetic layer correlated with the increased roughness of the V2O3 surface. The chemical homogeneity of the V2O3 is confirmed through transmission electron microscopy analysis. High-angle annular dark field imaging and electron energy loss spectroscopy reveal an atomically flat interface between Al2O3 and V2O3, as well as a sharp interface between V2O3 and Ni. | ||||
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| Language | Wos | 001202661800003 | Publication Date | 2024-04-01 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 2166-532X | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 6.1 | Times cited | Open Access | ||
| Notes | This work was supported by the funding from the University of Iceland Research Fund, the Icelandic Research Fund Grant No. 207111. Instrumentation funding from the Icelandic Infrastructure Fund is acknowledged. This work was based on experiments per- formed at the BM28 (XMaS) beamline at the European Synchrotron Radiation Facility, Grenoble, France. XMaS is a National Research Facility funded by the UK EPSRC and managed by the Universi- ties of Liverpool and Warwick. This project has received funding from the European Union’s Horizon 2020 research and innovation program under Grant Agreement No. 823717—ESTEEM3. | Approved | Most recent IF: 6.1; 2024 IF: 4.335 | ||
| Call Number | EMAT @ emat @c:irua:205569 | Serial |
9120 | ||
| Permanent link to this record | |||||
| Author | Chakraborty, J.; Chatterjee, A.; Molkens, K.; Nath, I.; Arenas Esteban, D.; Bourda, L.; Watson, G.; Liu, C.; Van Thourhout, D.; Bals, S.; Geiregat, P.; Van der Voort, P. | ||||
| Title | Decoding Excimer Formation in Covalent–Organic Frameworks Induced by Morphology and Ring Torsion | Type | A1 Journal Article | ||
| Year | 2024 | Publication | Advanced Materials | Abbreviated Journal | Advanced Materials |
| Volume | Issue | Pages | |||
| Keywords | A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; | ||||
| Abstract | A thorough and quantitative understanding of the fate of excitons in covalent–organic frameworks (COFs) after photoexcitation is essential for their augmented optoelectronic and photocatalytic applications via precise structure tuning. The synthesis of a library of COFs having identical chemical backbone with impeded conjugation, but varied morphology and surface topography to study the effect of these physical properties on the photophysics of the materials is herein reported. The variation of crystallite size and surface topography substantified different aggregation pattern in the COFs, which leads to disparities in their photoexcitation and relaxation properties. Depending on aggregation, an inverse correlation between bulk luminescence decay time and exciton binding energy of the materials is perceived. Further transient absorption spectroscopic analysis confirms the presence of highly localized, immobile, Frenkel excitons (of diameter 0.3–0.5 nm) via an absence of annihilation at high density, most likely induced by structural torsion of the COF skeletons, which in turn preferentially relaxes via long‐lived (nanosecond to microsecond) excimer formation (in femtosecond scale) over direct emission. These insights underpin the importance of structural and topological design of COFs for their targeted use in photocatalysis. | ||||
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| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001206226700001 | Publication Date | 2024-04-22 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 0935-9648 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 29.4 | Times cited | Open Access | ||
| Notes | PVDV, JC, AC, and IN acknowledge the FWO-Vlaanderen for research grant G020521N and the research board of UGent (BOF) through a Concerted Research Action (GOA010-17). JC acknowledges UGent for BOF postdoctoral grant (2022.0032.01). AC acknowledges FWO- Vlaanderen for postdoctoral grant (12T7521N). KM, DVT and PG acknowledges FWO- Vlaanderen for research grant G0B2921N. SB and DAE acknowledge financial support from ERC Consolidator Grant Number 815128 REALNANO. CHL acknowledges China Scholarship Council doctoral grant (201908110280). PVDV acknowledges Hercules Project AUGE/17/07 for the UV VIS DRS spectrometer and UGent BASBOF BOF20/BAS/015 for the powder X-Ray Diffractometer. PG thanks UGent for support of the Core Facility NOLIMITS. | Approved | Most recent IF: 29.4; 2024 IF: 19.791 | ||
| Call Number | EMAT @ emat @c:irua:205967 | Serial |
9118 | ||
| Permanent link to this record | |||||
| Author | De Meyer, R.; Gorbanev, Y.; Ciocarlan, R.-G.; Cool, P.; Bals, S.; Bogaerts, A. | ||||
| Title | Importance of plasma discharge characteristics in plasma catalysis: Dry reforming of methane vs. ammonia synthesis | Type | A1 Journal Article | ||
| Year | 2024 | Publication | Chemical Engineering Journal | Abbreviated Journal | Chemical Engineering Journal |
| Volume | 488 | Issue | Pages | 150838 | |
| Keywords | A1 Journal Article; Gas conversion Dry reforming of methane Ammonia Microdischarges Dielectric barrier discharge; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
| Abstract | Plasma catalysis is a rapidly growing field, often employing a packed-bed dielectric barrier discharge plasma reactor. Such dielectric barrier discharges are complex, especially when a packing material (e.g., a catalyst) is introduced in the discharge volume. Catalysts are known to affect the plasma discharge, though the underlying mechanisms influencing the plasma physics are not fully understood. Moreover, the effect of the catalysts on the plasma discharge and its subsequent effect on the overall performance is often overlooked. In this work, we deliberately design and synthesize catalysts to affect the plasma discharge in different ways. These Ni or Co alumina-based catalysts are used in plasma-catalytic dry reforming of methane and ammonia synthesis. Our work shows that introducing a metal to the dielectric packing can affect the plasma discharge, and that the distribution of the metal is crucial in this regard. Further, the altered discharge can greatly influence the overall performance. In an atmospheric pressure dielectric barrier discharge reactor, this apparently more uniform plasma yields a significantly better performance for ammonia synthesis compared to the more conventional filamentary discharge, while it underperforms in dry reforming of methane. This study stresses the importance of analyzing the plasma discharge in plasma catalysis experiments. We hope this work encourages a more critical view on the plasma discharge characteristics when studying various catalysts in a plasma reactor. | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | Publication Date | 2024-03-30 | ||
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 1385-8947 | ISBN | Additional Links | UA library record | |
| Impact Factor | 15.1 | Times cited | Open Access | ||
| Notes | This research was supported through long-term structural funding (Methusalem FFB15001C) and by the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme with grant agreement No 810182 (SCOPE ERC Synergy project) and with grant agreement No 815128 (REALNANO). We acknowledge the practical contribution of Senne Van Doorslaer. | Approved | Most recent IF: 15.1; 2024 IF: 6.216 | ||
| Call Number | PLASMANT @ plasmant @c:irua:205154 | Serial |
9115 | ||
| Permanent link to this record | |||||
| Author | Grünewald, L.; Chezganov, D.; De Meyer, R.; Orekhov, A.; Van Aert, S.; Bogaerts, A.; Bals, S.; Verbeeck, J. | ||||
| Title | Supplementary Information for “In-situ Plasma Studies using a Direct Current Microplasma in a Scanning Electron Microscope” | Type | Dataset | ||
| Year | 2023 | Publication | Abbreviated Journal | ||
| Volume | Issue | Pages | |||
| Keywords | Dataset; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | Supplementary information for the article “In-situ Plasma Studies using a Direct Current Microplasma in a Scanning Electron Microscope” containing the videos of in-situ SEM imaging (mp4 files), raw data/images, and Jupyter notebooks (ipynb files) for data treatment and plots. Link to the preprint: https://doi.org/10.48550/arXiv.2308.15123 Explanation of the data files can be found in the Information.pdf file. The Videos folder contains the in-situ SEM image series mentioned in the paper. If there are any questions/bugs, feel free to contact me at lukas.grunewaldatuantwerpen.be | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | Publication Date | |||
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | ISBN | Additional Links | UA library record | ||
| Impact Factor | Times cited | Open Access | Not_Open_Access | ||
| Notes | Approved | Most recent IF: NA | |||
| Call Number | UA @ admin @ c:irua:203389 | Serial |
9100 | ||
| Permanent link to this record | |||||
| Author | Johnson, G.; Yang, M.Y.; Liu, C.; Zhou, H.; Zuo, X.; Dickie, D.A.; Wang, S.; Gao, W.; Anaclet, B.; Perras, F.A.; Ma, F.; Zeng, C.; Wang, D.; Bals, S.; Dai, S.; Xu, Z.; Liu, G.; Goddard III, W.A.; Zhang, S. | ||||
| Title | Nanocluster superstructures assembled via surface ligand switching at high temperature | Type | A1 Journal article | ||
| Year | 2023 | Publication | Nature synthesis | Abbreviated Journal | |
| Volume | 2 | Issue | 9 | Pages | 828-837 |
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Superstructures with nanoscale building blocks, when coupled with precise control of the constituent units, open opportunities in rationally designing and manufacturing desired functional materials. Yet, synthetic strategies for the large-scale production of superstructures are scarce. We report a scalable and generalized approach to synthesizing superstructures assembled from atomically precise Ce24O28(OH)8 and other rare-earth metal-oxide nanoclusters alongside a detailed description of the self-assembly mechanism. Combining operando small-angle X-ray scattering, ex situ molecular and structural characterizations, and molecular dynamics simulations indicates that a high-temperature ligand-switching mechanism, from oleate to benzoate, governs the formation of the nanocluster assembly. The chemical tuning of surface ligands controls superstructure disassembly and reassembly, and furthermore, enables the synthesis of multicomponent superstructures. This synthetic approach, and the accurate mechanistic understanding, are promising for the preparation of superstructures for use in electronics, plasmonics, magnetics and catalysis. Synthesizing superstructures with precisely controlled nanoscale building blocks is challenging. Here the assembly of superstructures is reported from atomically precise Ce24O28(OH)8 and other rare-earth metal-oxide nanoclusters and their multicomponent combinations. A high-temperature ligand-switching mechanism controls the self-assembly. | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001124824000001 | Publication Date | 2023-05-01 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | ||
| Impact Factor | Times cited | 2 | Open Access | Not_Open_Access | |
| Notes | Approved | Most recent IF: NA | |||
| Call Number | UA @ admin @ c:irua:202180 | Serial |
9060 | ||
| Permanent link to this record | |||||
| Author | Hugenschmidt, M.; Jannis, D.; Kadu, A.A.; Grünewald, L.; De Marchi, S.; Perez-Juste, J.; Verbeeck, J.; Van Aert, S.; Bals, S. | ||||
| Title | Low-dose 4D-STEM tomography for beam-sensitive nanocomposites | Type | A1 Journal article | ||
| Year | 2023 | Publication | ACS materials letters | Abbreviated Journal | |
| Volume | 6 | Issue | 1 | Pages | 165-173 |
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Electron tomography is essential for investigating the three-dimensional (3D) structure of nanomaterials. However, many of these materials, such as metal-organic frameworks (MOFs), are extremely sensitive to electron radiation, making it difficult to acquire a series of projection images for electron tomography without inducing electron-beam damage. Another significant challenge is the high contrast in high-angle annular dark field scanning transmission electron microscopy that can be expected for nanocomposites composed of a metal nanoparticle and an MOF. This strong contrast leads to so-called metal artifacts in the 3D reconstruction. To overcome these limitations, we here present low-dose electron tomography based on four-dimensional scanning transmission electron microscopy (4D-STEM) data sets, collected using an ultrafast and highly sensitive direct electron detector. As a proof of concept, we demonstrate the applicability of the method for an Au nanostar embedded in a ZIF-8 MOF, which is of great interest for applications in various fields, including drug delivery. | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001141178500001 | Publication Date | 2023-12-11 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 2639-4979 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | Times cited | Open Access | Not_Open_Access | ||
| Notes | This work was supported by the European Research Council (Grant 815128 REALNANO to S.B., Grant 770887 PICOMETRICS to S.V.A.). J.P.-J. and S.M. acknowledge financial support from the MCIN/AEI/10.13039/501100011033 (Grants No. PID2019-108954RB-I00) and EU Horizon 2020 research and innovation program under grant agreement no. 883390 (SERSing). J.V., S.B., S.V.A., and L.G. acknowledge funding from the Flemish government (iBOF-21-085 PERsist). | Approved | Most recent IF: NA | ||
| Call Number | UA @ admin @ c:irua:202771 | Serial |
9053 | ||
| Permanent link to this record | |||||
| Author | Van den Hoek, J.; Daems, N.; Arnouts, S.; Hoekx, S.; Bals, S.; Breugelmans, T. | ||||
| Title | Improving stability of CO₂ electroreduction by incorporating Ag NPs in N-doped ordered mesoporous carbon structures | Type | A1 Journal article | ||
| Year | 2024 | Publication | ACS applied materials and interfaces | Abbreviated Journal | |
| Volume | 16 | Issue | 6 | Pages | 6931-6947 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) | ||||
| Abstract | The electroreduction of carbon dioxide (eCO2RR) to CO using Ag nanoparticles as an electrocatalyst is promising as an industrial carbon capture and utilization (CCU) technique to mitigate CO2 emissions. Nevertheless, the long-term stability of these Ag nanoparticles has been insufficient despite initial high Faradaic efficiencies and/or partial current densities. To improve the stability, we evaluated an up-scalable and easily tunable synthesis route to deposit low-weight percentages of Ag nanoparticles (NPs) on and into the framework of a nitrogen-doped ordered mesoporous carbon (NOMC) structure. By exploiting this so-called nanoparticle confinement strategy, the nanoparticle mobility under operation is strongly reduced. As a result, particle detachment and agglomeration, two of the most pronounced electrocatalytic degradation mechanisms, are (partially) blocked and catalyst durability is improved. Several synthesis parameters, such as the anchoring agent, the weight percentage of Ag NPs, and the type of carbonaceous support material, were modified in a controlled manner to evaluate their respective impact on the overall electrochemical performance, with a strong emphasis on operational stability. The resulting powders were evaluated through electrochemical and physicochemical characterization methods, including X-ray diffraction (XRD), N2-physisorption, Inductively coupled plasma mass spectrometry (ICP-MS), scanning electron microscopy (SEM), SEM-energy-dispersive X-ray spectroscopy (SEM-EDS), high-angle annular dark field scanning transmission electron microscopy (HAADF-STEM), STEM-EDS, electron tomography, and X-ray photoelectron spectroscopy (XPS). The optimized Ag/soft-NOMC catalysts showed both a promising selectivity (∼80%) and stability compared with commercial Ag NPs while decreasing the loading of the transition metal by more than 50%. The stability of both the 5 and 10 wt % Ag/soft-NOMC catalysts showed considerable improvements by anchoring the Ag NPs on and into a NOMC framework, resulting in a 267% improvement in CO selectivity after 72 h (despite initial losses) compared to commercial Ag NPs. These results demonstrate the promising strategy of anchoring Ag NPs to improve the CO selectivity during prolonged experiments due to the reduced mobility of the Ag NPs and thus enhanced stability. | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001158812100001 | Publication Date | 2023-12-21 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 1944-8244 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 9.5 | Times cited | Open Access | Not_Open_Access: Available from 21.06.2024 | |
| Notes | Approved | Most recent IF: 9.5; 2024 IF: 7.504 | |||
| Call Number | UA @ admin @ c:irua:202309 | Serial |
9045 | ||
| Permanent link to this record | |||||
| Author | 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. | ||||
| Title | From multi- to single-hollow trimetallic nanocrystals by ultrafast heating | Type | A1 Journal article | ||
| Year | 2023 | Publication | Chemistry of materials | Abbreviated Journal | |
| Volume | 35 | Issue | 22 | Pages | 9603-9612 |
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
| 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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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001110623500001 | Publication Date | 2023-11-06 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 0897-4756; 1520-5002 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 8.6 | Times cited | 2 | Open Access | OpenAccess |
| Notes | Approved | Most recent IF: 8.6; 2023 IF: 9.466 | |||
| Call Number | UA @ admin @ c:irua:202144 | Serial |
9040 | ||
| Permanent link to this record | |||||
| Author | Jenkinson, K.; Spadaro, M.C.; Golovanova, V.; Andreu, T.; Morante, J.R.; Arbiol, J.; Bals, S. | ||||
| Title | Direct operando visualization of metal support interactions induced by hydrogen spillover during CO₂ hydrogenation | Type | A1 Journal article | ||
| Year | 2023 | Publication | Advanced materials | Abbreviated Journal | |
| Volume | 35 | Issue | 51 | Pages | 2306447-10 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
| 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. | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001106139400001 | Publication Date | 2023-10-22 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 0935-9648 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 29.4 | Times cited | Open Access | OpenAccess | |
| Notes | Approved | Most recent IF: 29.4; 2023 IF: 19.791 | |||
| Call Number | UA @ admin @ c:irua:201143 | Serial |
9022 | ||
| Permanent link to this record | |||||
| Author | Grünewald, L.; Chezganov, D.; De Meyer, R.; Orekhov, A.; Van Aert, S.; Bogaerts, A.; Bals, S.; Verbeeck, J. | ||||
| Title | In Situ Plasma Studies Using a Direct Current Microplasma in a Scanning Electron Microscope | Type | A1 Journal Article | ||
| Year | 2024 | Publication | Advanced Materials Technologies | Abbreviated Journal | Adv Materials Technologies |
| Volume | Issue | Pages | |||
| Keywords | A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; | ||||
| Abstract | Microplasmas can be used for a wide range of technological applications and to improve the understanding of fundamental physics. Scanning electron microscopy, on the other hand, provides insights into the sample morphology and chemistry of materials from the mm‐ down to the nm‐scale. Combining both would provide direct insight into plasma‐sample interactions in real‐time and at high spatial resolution. Up till now, very few attempts in this direction have been made, and significant challenges remain. This work presents a stable direct current glow discharge microplasma setup built inside a scanning electron microscope. The experimental setup is capable of real‐time in situ imaging of the sample evolution during plasma operation and it demonstrates localized sputtering and sample oxidation. Further, the experimental parameters such as varying gas mixtures, electrode polarity, and field strength are explored and experimental<italic>V</italic>–<italic>I</italic>curves under various conditions are provided. These results demonstrate the capabilities of this setup in potential investigations of plasma physics, plasma‐surface interactions, and materials science and its practical applications. The presented setup shows the potential to have several technological applications, for example, to locally modify the sample surface (e.g., local oxidation and ion implantation for nanotechnology applications) on the µm‐scale. | ||||
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| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001168639900001 | Publication Date | 2024-02-25 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 2365-709X | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 6.8 | Times cited | Open Access | OpenAccess | |
| Notes | L.G., S.B., and J.V. acknowledge support from the iBOF-21-085 PERsist research fund. D.C., S.V.A., and J.V. acknowledge funding from a TOPBOF project of the University of Antwerp (FFB 170366). R.D.M., A.B., and J.V. acknowledge funding from the Methusalem project of the University of Antwerp (FFB 15001A, FFB 15001C). A.O. and J.V. acknowledge funding from the Research Foundation Flanders (FWO, Belgium) project SBO S000121N. | Approved | Most recent IF: 6.8; 2024 IF: NA | ||
| Call Number | EMAT @ emat @c:irua:204363 | Serial |
8995 | ||
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| Author | Teunissen, J.L.; Braeckevelt, T.; Skvortsova, I.; Guo, J.; Pradhan, B.; Debroye, E.; Roeffaers, M.B.J.; Hofkens, J.; Van Aert, S.; Bals, S.; Rogge, S.M.J.; Van Speybroeck, V. | ||||
| Title | Additivity of Atomic Strain Fields as a Tool to Strain-Engineering Phase-Stabilized CsPbI3Perovskites | Type | A1 Journal Article | ||
| Year | 2023 | Publication | The Journal of Physical Chemistry C | Abbreviated Journal | J. Phys. Chem. C |
| Volume | 127 | Issue | 48 | Pages | 23400-23411 |
| Keywords | A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; | ||||
| Abstract | CsPbI3 is a promising perovskite material for photovoltaic applications in its photoactive perovskite or black phase. However, the material degrades to a photovoltaically inactive or yellow phase at room temperature. Various mitigation strategies are currently being developed to increase the lifetime of the black phase, many of which rely on inducing strains in the material that hinder the black-to-yellow phase transition. Physical insight into how these strategies exactly induce strain as well as knowledge of the spatial extent over which these strains impact the material is crucial to optimize these approaches but is still lacking. Herein, we combine machine learning potential-based molecular dynamics simulations with our in silico strain engineering approach to accurately quantify strained large-scale atomic structures on a nanosecond time scale. To this end, we first model the strain fields introduced by atomic substitutions as they form the most elementary strain sources. We demonstrate that the magnitude of the induced strain fields decays exponentially with the distance from the strain source, following a decay rate that is largely independent of the specific substitution. Second, we show that the total strain field induced by multiple strain sources can be predicted to an excellent approximation by summing the strain fields of each individual source. Finally, through a case study, we illustrate how this additive character allows us to explain how complex strain fields, induced by spatially extended strain sources, can be predicted by adequately combining the strain fields caused by local strain sources. Hence, the strain additivity proposed here can be adopted to further our insight into the complex strain behavior in perovskites and to design strain from the atomic level onward to enhance their sought-after phase stability. | ||||
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| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001116862000001 | Publication Date | 2023-12-07 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 1932-7447 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 3.7 | Times cited | Open Access | OpenAccess | |
| Notes | This work was supported by iBOF-21-085 PERsist (Special Research Fund of Ghent University, KU Leuven Research Fund, and the Research Fund of the University of Antwerp). S.M.J.R., T.B., and B.P. acknowledge financial support from the Research Foundation-Flanders (FWO) through two postdoctoral fellow- ships [grant nos. 12T3522N (S.M.J.R.) and 1275521N (B.P.)] and an SB-FWO fellowship [grant no. 1SC1319 (T.B.)]. E.D., M.B.J.R., and J.H. acknowledge financial support from the Research Foundation-Flanders (FWO, grant nos. G.0B39.15, G.0B49.15, G098319N, S002019N, S004322N, and ZW15_09- GOH6316). J.H. acknowledges support from the Flemish government through long-term structural funding Methusalem (CASAS2, Meth/15/04) and the MPI as an MPI fellow. S.V.A. and S.B. acknowledge financial support from the Research Foundation-Flanders (FWO, grant no. G0A7723N). S.M.J.R. and V.V.S. acknowledge funding from the Research Board of Ghent University (BOF). The computational resources and services used in this work were provided by the VSC (Flemish Supercomputer Center), funded by the Research Foundation- Flanders (FWO) and the Flemish Government�department EWI.; KU Leuven, iBOF-21-085 PERsist ; Universiteit Antwerpen, iBOF-21-085 PERsist ; Universiteit Gent, iBOF-21-085 PERsist ; Vlaamse regering, CASAS2, Meth/15/04 ; Fonds Wetenschappelijk Onderzoek, G.0B39.15 G098319N G.0B49.15 1SC1319 12T3522N ZW15 09-GOH6316 G0A7723N 1275521N S004322N S002019N ; | Approved | Most recent IF: 3.7; 2023 IF: 4.536 | ||
| Call Number | EMAT @ emat @c:irua:202124 | Serial |
8985 | ||
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| Author | Bhatia, H.; Keshavarz, M.; Martin, C.; Van Gaal, L.; Zhang, Y.; de Coen, B.; Schrenker, N.J.; Valli, D.; Ottesen, M.; Bremholm, M.; Van de Vondel, J.; Bals, S.; Hofkens, J.; Debroye, E. | ||||
| Title | Achieving High Moisture Tolerance in Pseudohalide Perovskite Nanocrystals for Light-Emitting Diode Application | Type | A1 Journal Article | ||
| Year | 2023 | Publication | ACS Applied Optical Materials | Abbreviated Journal | ACS Appl. Opt. Mater. |
| Volume | 1 | Issue | 6 | Pages | 1184-1191 |
| Keywords | A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; | ||||
| Abstract | The addition of potassium thiocyanate (KSCN) to the FAPbBr3 structure and subsequent post-treatment of nanocrystals (NCs) lead to high quantum confinement, resulting in a photoluminescent quantum yield (PLQY) approaching unity and microsecond decay times. This synergistic approach demonstrated exceptional stability under humid conditions, retaining 70% of the PLQY for over a month, while the untreated NCs degrade within 24 h. Additionally, the devices incorporating the post-treated NCs displayed 1.5% external quantum efficiency (EQE), a 5-fold improvement over untreated devices. These results provide promising opportunities for the use of perovskites in moisture-stable optoelectronics. | ||||
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| Publisher | Place of Publication | Editor | |||
| Language | Wos | Publication Date | 2023-06-23 | ||
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 2771-9855 | ISBN | Additional Links | UA library record | |
| Impact Factor | Times cited | Open Access | OpenAccess | ||
| Notes | Hercules Foundation, HER/11/14 ; European Commission; Ministerio de Ciencia e Innovaci?n, PID2021-128761OA-C22 ; European Regional Development Fund; Vlaamse regering, CASAS2 Meth/15/04 ; Fonds Wetenschappelijk Onderzoek, 1238622N 1514220N 1S45223N G.0B39.15 G.0B49.15 G098319N S002019N ZW15_09-GOH6316 ; Onderzoeksraad, KU Leuven, C14/19/079 db/21/006/bm iBOF-21-085 STG/21/010 ; Junta de Comunidades de Castilla-La Mancha, SBPLY/21/180501/000127 ; H2020 European Research Council, 642196 815128 ; | Approved | Most recent IF: NA | ||
| Call Number | EMAT @ emat @c:irua:201011 | Serial |
8975 | ||
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| Author | de la Croix, T.; Claes, N.; Eyley, S.; Thielemans, W.; Bals, S.; De Vos, D. | ||||
| Title | Heterogeneous Pt-catalyzed transfer dehydrogenation of long-chain alkanes with ethylene | Type | A1 Journal Article | ||
| Year | 2023 | Publication | Catalysis Science & Technology | Abbreviated Journal | Catal. Sci. Technol. |
| Volume | Issue | Pages | |||
| Keywords | A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; | ||||
| Abstract | The dehydrogenation of long-chain alkanes to olefins and alkylaromatics is a challenging endothermic reaction, typically requiring harsh conditions which can lead to low selectivity and coking. More favorable thermodynamics can be achieved by using a hydrogen acceptor, such as ethylene. In this work, the potential of heterogeneous platinum catalysts for the transfer dehydrogenation of long-chain alkanes is investigated, using ethylene as a convenient hydrogen acceptor. Pt/C and Pt–Sn/C catalysts were prepared<italic>via</italic>a simple polyol method and characterized with CO pulse chemisorption, HAADF-STEM, and EDX measurements. Conversion of ethylene was monitored<italic>via</italic>gas-phase FTIR, and distribution of liquid products was analyzed<italic>via</italic>GC-FID, GC-MS, and 1H-NMR. Compared to unpromoted Pt/C, Sn-promoted catalysts show lower initial reaction rates, but better resistance to catalyst deactivation, while increasing selectivity towards alkylaromatics. Both reaction products and ethylene were found to inhibit the reaction significantly. At 250 °C for 22 h, TON up to 28 and 86 mol per mol Pt were obtained for Pt/C and PtSn<sub>2</sub>/C, respectively, with olefin selectivities of 94% and 53%. The remaining products were mainly unbranched alkylaromatics. These findings show the potential of simple heterogeneous catalysts in alkane transfer dehydrogenation, for the preparation of valuable olefins and alkylaromatics, or as an essential step in various tandem reactions. | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001104905100001 | Publication Date | 2023-11-09 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 2044-4753 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 5 | Times cited | Open Access | OpenAccess | |
| Notes | T. de la Croix gratefully acknowledges the support of the Flanders Research Foundation (FWO) under project 11F6622N. D. De Vos is grateful to FWO for support of project G0D3721N, and to KU Leuven for the iBOF project 21/016/C3. S. Bals and N. Claes acknowledge funding from the European Research Council under the European Union’s Horizon 2020 research and innovation program (ERC Consolidator Grant No. 815128- REALNANO). W. Thielemans and S. Eyley thank KU Leuven (grant C14/18/061) and FWO (G0A1219N) for financial support. | Approved | Most recent IF: 5; 2023 IF: 5.773 | ||
| Call Number | EMAT @ emat @c:irua:201010 | Serial |
8968 | ||
| Permanent link to this record | |||||
| Author | Van Gordon, K.; Baúlde, S.; Mychinko, M.; Heyvaert, W.; Obelleiro-Liz, M.; Criado, A.; Bals, S.; Liz-Marzán, L.M.; Mosquera, J. | ||||
| Title | Tuning the Growth of Chiral Gold Nanoparticles Through Rational Design of a Chiral Molecular Inducer | Type | A1 Journal Article | ||
| Year | 2023 | Publication | Nano Letters | Abbreviated Journal | Nano Lett. |
| Volume | Issue | Pages | |||
| Keywords | A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; | ||||
| Abstract | The bottom-up production of chiral gold nanomaterials holds great potential for the advancement of biosensing and nano-optics, among other applications. Reproducible preparations of colloidal nanomaterials with chiral morphology have been reported, using cosurfactants or chiral inducers such as thiolated amino acids. However, the underlying growth mechanisms for these nanomaterials remain insufficiently understood. We introduce herein a purposely devised chiral inducer, a cysteine modified with a hydrophobic chain, as a versatile chiral inducer. The amphiphilic and chiral features of this molecule provide control over the chiral morphology and the chiroptical signature of the obtained nanoparticles by simply varying the concentration of chiral inducer. These results are supported by circular dichroism and electromagnetic modeling as well as electron tomography to analyze structural evolution at the facet scale. Our observations suggest complex roles for the factors involved in chiral synthesis: the chemical nature of the chiral inducers and the influence of cosurfactants. | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001092787000001 | Publication Date | 2023-10-25 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 1530-6984 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 10.8 | Times cited | Open Access | OpenAccess | |
| Notes | J.M. Taboada and F. Obelleiro are thanked for support with electromagnetic simulations. The authors acknowledge financial support by the European Research Council (ERC CoG No. 815128 REALNANO to S. Bals; ERC AdG No. 787510, 4DbioSERS to L.M.L.-M.) and from MCIN/AEI/10.13039/501100011033 and “ESF Investing in your future” (Grant PID2020-117779RB-I00 to L.M.L.-M., Grant RYC2020-030183-I to A.C., and Grants RYC2019-027842-I, PID2020-117885GA-I00 to J.M.). | Approved | Most recent IF: 10.8; 2023 IF: 12.712 | ||
| Call Number | EMAT @ emat @c:irua:200590 | Serial |
8963 | ||
| Permanent link to this record | |||||
| Author | Marchetti, A.; Gori, A.; Ferretti, A.M.; Esteban, D.A.; Bals, S.; Pigliacelli, C.; Metrangolo, P. | ||||
| Title | Templated Out‐of‐Equilibrium Self‐Assembly of Branched Au Nanoshells (Small 12/2023) | Type | A1 Journal Article | ||
| Year | 2023 | Publication | Small | Abbreviated Journal | Small |
| Volume | 19 | Issue | 12 | Pages | |
| Keywords | A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ; | ||||
| Abstract | Out-of-equilibrium self-assembly of metal nanoparticles (NPs) has been devised using different types of strategies and fuels, but the achievement of finite 3D structures with a controlled morphology through this assembly mode is still rare. Here we used a spherical peptide-gold superstructure (PAuSS) as a template to control the out-of-equilibrium self-assembly of Au NPs, obtaining a transient 3D branched Au-nanoshell (BAuNS) stabilized by sodium dodecyl sulphate (SDS). The BAuNS dismantled upon concentration gradient equilibration over time in the solution, leading to NPs disassembly. Notably, BAuNS assembly and disassembly favoured temporary interparticle plasmonic coupling, leading to a remarkable oscillation of their optical properties. |
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| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | Publication Date | 2023-03-23 | ||
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 1613-6810 | ISBN | Additional Links | UA library record | |
| Impact Factor | 13.3 | Times cited | Open Access | Not_Open_Access | |
| Notes | P.M. is grateful to the European Research Council (ERC) for the Starting Grant ERC-2012- StG_20111012 FOLDHALO (Grant Agreement no. 307108) and the Proof-of-Concept Grant ERC-2017-PoC MINIRES (Grant Agreement no.789815). A. M. and P. M. are thankful to the project Hydrogex funded by Cariplo Foundation (grant no. 2018-1720). D.A.E. and S.B. acknowledges financial support from ERC Consolidator Grant Number 815128 REALNANO and Grant Agreement No. 731019 (EUSMI). | Approved | Most recent IF: 13.3; 2023 IF: 8.643 | ||
| Call Number | EMAT @ emat @c:irua:200859 | Serial |
8960 | ||
| Permanent link to this record | |||||
| Author | Moggia, G.; Hoekx, S.; Daems, N.; Bals, S.; Breugelmans, T. | ||||
| Title | Synthesis and characterization of a highly electroactive composite based on Au nanoparticles supported on nanoporous activated carbon for electrocatalysis | Type | A1 Journal article | ||
| Year | 2023 | Publication | ChemElectroChem | Abbreviated Journal | |
| Volume | Issue | Pages | 1-11 | ||
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) | ||||
| Abstract | A facile, “one-pot”, chemical approach to synthesize gold-based nanoparticles finely dispersed on porous activated carbon (Norit) was demonstrated in this work. The pH of the synthesis bath played a critical role in determining the optimal gold-carbon interaction, which enabled a successful deposition of the gold nanoparticles onto the carbon matrix with a maximized metal utilization of 93 %. The obtained AuNP/C nanocomposite was characterized using SEM, HAADF-STEM electron tomography and electrochemical techniques. It was found that the Au nanoparticles, with diameters between 5 and 20 nm, were evenly distributed over the carbon matrix, both inside and outside the pores. Electrochemical characterization indicated that the composite had a very large electroactive surface area (EASA), as high as 282.4 m2 gAu-1. By exploiting its very high EASA, the catalyst was intended to boost the productivity of glucaric acid in the electrooxidation of its precursor, gluconic acid. However, cyclic voltammetry experiments revealed a very limited reactivity towards gluconic acid oxidation, due to the spacial hindrance of gluconic acid molecule which prevented diffusion inside the catalyst nanopores. On the other hand, the as-synthesized nanocomposite promises to be effective towards the ORR, and might thus find potential application as anode catalyst for fuel cells as well as for the scalability of all those electrochemical reactions involving small molecules with high diffusivity and catalysed by noble metals (i. e. CO2, CH4, N2, etc..). Electrocatalysis: Gold nanoparticles with diameter between 5 and 20 nm evenly distributed onto porous activated carbon (Norit) were obtained using a facile “one-pot” chemical synthesis technique with very high metal utilization. The AuNP/C nanocomposite was characterized using SEM, HAADF-STEM electron tomography and electrochemical techniques, revealing a very large electroactive surface area (EASA). The figure shows the HAADF-STEM image (a) and the respective EDX elemental distribution (b) for the AuNP/C composite with 9.3 % Au-loading developed in this work (Au is marked in red and C in green).image | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001060398900001 | Publication Date | 2023-09-08 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 2196-0216 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 4 | Times cited | 1 | Open Access | OpenAccess |
| Notes | The research described in this article has not been supported by the Climate, Infrastructure and Environment Executive Agency of the European Commission. The views expressed in this article have not been adopted or in any way approved by the European Commission and do not constitute a statement of the European Commission & apos;s views.r S. Hoekx was supported by Research Foundation Flanders (FWO 1S42623N). The authors would like to thank Prof. Dr. Christophe Vande Velde, University of Antwerp, for the XRD analysis. | Approved | Most recent IF: 4; 2023 IF: 4.136 | ||
| Call Number | UA @ admin @ c:irua:199210 | Serial |
8941 | ||
| Permanent link to this record | |||||
| Author | Mosquera, J.; Wang, D.; Bals, S.; Liz-Marzan, L.M. | ||||
| Title | Surfactant layers on gold nanorods | Type | A1 Journal article | ||
| Year | 2023 | Publication | Accounts of chemical research | Abbreviated Journal | |
| Volume | 56 | Issue | 10 | Pages | 1204-1212 |
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Gold nanorods (Au NRs) are an exceptionally promising tool in nanotechnology due to three key factors: (i) their strong interaction with electromagnetic radiation, stemming from their plasmonic nature, (ii) the ease with which the resonance frequency of their longitudinal plasmon mode can be tuned from the visible to the near-infrared region of the electromagnetic spect r u m based on their aspect ratio, and (iii) their simple and cost-effective preparation through seed-mediated chemical growth. In this synthetic method, surfactants play a critical role in controlling the size, shape, and colloidal stabi l i t y of Au NRs. For example, surfactants can stabilize specific crystallographic facets during the formation of Au NRs, leading to t h e formation of NRs with specific morphologies. The process of surfactant adsorption onto the NR surface may result in various assemblies of surfactant molecules, such as spherical micelles, elongated micelles, or bilayers. Again, the assembly mode is critical toward determining the further availabi l i t y of the Au NR surface to the surrounding medium. Despite its importance and a great deal of research effort, the interaction between Au NPs and surfactants remains insufficiently understood, because the assembly process is influenced by numerous factors, including the chemical nature of the surfactant, the surface morphology of Au NPs, and solution parameters. Therefore, gaining a more comprehensive understanding of these interactions is essential to unlock the full potential of the seed-mediated growth method and the applications of plasmonic NPs. A plethora of characterization techniques have been applied to reach such an understanding , but many open questions remain. In this Account, we review the current knowledge on the interactions between surfactants and Au NRs. We briefly introduce the state-of-the-art methods for synthesizing Au NRs and highlight the crucial role of cationic surfactants during this process. The self-assembly and organization of surfactants on the Au NR surface is then discussed to better understand their role in seed-mediated growth. Subsequently, we provide examples and elucidate how chemical additives can be used to modulate micellar assemblies, in turn allowing for a finer control over the growth of Au NRs, including chiral NRs. Next, we review the main experimental characterization and computational modeling techniques that have been applied to shed light on the arrangement of surfactants on Au NRs and summarize the advantages and disadvantages for each technique. The Account ends with a “Conclusions and Outlook” section, outlining promising future research directions and developments that we consider are sti l l required, mostly related to the application of electron microscopy in liquid and in 3D. Finally, we remark on the potential of exploiting machine learning techniques to predict synthetic routes for NPs with predefined structures and properties. | ||||
| Address | |||||
| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000986447000001 | Publication Date | 2023-05-08 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 0001-4842 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 18.3 | Times cited | 8 | Open Access | OpenAccess |
| Notes | The authors acknowledge financial support by the European Research Council (ERC CoG No. 815128 REALNANO to S.B.; ERC AdG No. 787510, 4DbioSERS to L.M.L.-M.) , from MCIN/AEI/10.13039/501100011033 and “ESF Investing in your future” (Grant PID2020-117779RB-I00 to L.M.L.-M. and Grants RYC2019-027842-I , PID2020-117885GA-I00 to J.M.) , and by Guangdong Provincial Key Laboratory of Optical Information Materials and Technology (No. 2017B030301007) , National Center for International Research on Green Optoelectronics (No. 2016B01018) , MOE Interna-tional Laboratory for Optical Information Technologies, and the 111 projects. | Approved | Most recent IF: 18.3; 2023 IF: 20.268 | ||
| Call Number | UA @ admin @ c:irua:196768 | Serial |
8940 | ||
| Permanent link to this record | |||||
| Author | Filez, M.; Feng, J.-Y.; Minjauw, M.M.; Solano, E.; Poonkottil, N.; Van Daele, M.; Ramachandran, R.K.; Li, C.; Bals, S.; Poelman, H.; Detavernier, C.; Dendooven, J.; Filez, M.; Minjauw, M.; Solano, E.; Poonkottil, N.; Li, C.; Bals, S.; Dendooven, J. | ||||
| Title | Shuffling atomic layer deposition gas sequences to modulate bimetallic thin films and nanoparticle properties | Type | A1 Journal article | ||
| Year | 2022 | Publication | Chemistry of materials | Abbreviated Journal | |
| Volume | Issue | Pages | |||
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT) | ||||
| Abstract | Atomic layer deposition (ALD) typically employs metal precursors and co-reactant pulses to deposit thin films in a layer-by-layer fashion. While conventional ABAB-type ALD sequences implement only two functionalities, namely, a metal source and ligand exchange agent, additional functionalities have emerged, including etching and reduction agents. Herein, we construct gas-phase sequences-coined as ALD+-with complex-ities reaching beyond the classic ABAB-type ALD by freely combining multiple functionalities within irregular pulse schemes, e.g., ABCADC. The possibilities of such combinations are explored as a smart strategy to tailor bimetallic thin films and nanoparticle (NP) properties. By doing so, we demonstrate that bimetallic thin films can be tailored with target thickness and through the full compositional range, while the morphology can be flexibly modulated from thin films to NPs by shuI 1ing the pulse sequence. These complex pulse schemes are expected to be broadly applicable but are here explored for Pd-Ru bimetallic thin films and NPs. | ||||
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| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000823205700001 | Publication Date | 2022-06-29 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 0897-4756; 1520-5002 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | Times cited | 2 | Open Access | OpenAccess | |
| Notes | This research was funded by the Research Foundation, Flanders (FWO) , and the Special Research Fund BOF of Ghent University (GOA 01G01019) . M.F. and M.M.M. acknowledge the FWO for a postdoctoral research fellowship (1280621N) . N.P. acknowledges the European Union's Horizon 2020 research and innovation program under the Marie Skiodowska-Curie grant agreement no. 765378. For the GISAXS measurements, the author s received funding from the European Community's Transnational Access Program CALIPSOplus. E.S. acknowledges the Spanish project RTI2018-093996-B-C32 MICINN/FEDER funds. Air Liquide is acknowledged for supporting this research. The authors acknowledge SOLEIL for the provision of synchrotron radiation facilities and would like to thank Dr. Alessandro Coati for assistance in using beamline SiXS. The GIWAXS experiments were performed at NCD-SWEET beamline at ALBA Synchrotron with the collaboration of ALBA staff . | Approved | no | ||
| Call Number | UA @ admin @ c:irua:189541 | Serial |
8928 | ||
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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. | ||||
| Title | Restructuring of titanium oxide overlayers over nickel nanoparticles during catalysis | Type | A1 Journal article | ||
| Year | 2023 | Publication | Science | Abbreviated Journal | |
| Volume | 380 | Issue | 6645 | Pages | 644-651 |
| Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) | ||||
| 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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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000999020900010 | Publication Date | 2023-05-11 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 0036-8075; 1095-9203 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 56.9 | Times cited | 29 | Open Access | OpenAccess |
| 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 | ||
| Call Number | UA @ admin @ c:irua:197432 | Serial |
8923 | ||
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| Author | Ndayirinde, C.; Gorbanev, Y.; Ciocarlan, R.-G.; De Meyer, R.; Smets, A.; Vlasov, E.; Bals, S.; Cool, P.; Bogaerts, A. | ||||
| Title | Plasma-catalytic ammonia synthesis : packed catalysts act as plasma modifiers | Type | A1 Journal article | ||
| Year | 2023 | Publication | Catalysis today | Abbreviated Journal | |
| Volume | 419 | Issue | Pages | 114156-12 | |
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
| Abstract | We studied the plasma-catalytic production of NH3 from H2 and N2 in a dielectric barrier discharge plasma reactor using five different Co-based catalysts supported on Al2O3, namely Co/Al2O3, CoCe/Al2O3, CoLa/Al2O3, CoCeLa/Al2O3 and CoCeMg/Al2O3. The catalysts were characterized via several techniques, including SEM-EDX, and their performance was compared. The best performing catalyst was found to be CoLa/Al2O3, but the dif-ferences in NH3 concentration, energy consumption and production rate between the different catalysts were limited under the same conditions (i.e. feed gas, flow rate and ratio, and applied power). At the same time, the plasma properties, such as the plasma power and current profile, varied significantly depending on the catalyst. Taken together, these findings suggest that in the production of NH3 by plasma catalysis, our catalysts act as plasma modifiers, i.e., they change the discharge properties and hence the gas phase plasma chemistry. Importantly, this effect dominates over the direct catalytic effect (as e.g. in thermal catalysis) defined by the chemistry on the catalyst surface. | ||||
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| Corporate Author | Thesis | ||||
| Publisher | Place of Publication | Editor | |||
| Language | Wos | 000987221300001 | Publication Date | 2023-04-10 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 0920-5861 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
| Impact Factor | 5.3 | Times cited | 3 | Open Access | OpenAccess |
| Notes | This research was supported by the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation programme (grant agreement No 810182 – SCOPE ERC Synergy project) and the Methusalem project of the University of Antwerp. We also gratefully acknowledge the NH3-TPD analysis performed by Sander Bossier. | Approved | Most recent IF: 5.3; 2023 IF: 4.636 | ||
| Call Number | UA @ admin @ c:irua:197268 | Serial |
8917 | ||
| Permanent link to this record | |||||
| Author | Ramesha, B.M.; Pawlak, B.; Arenas Esteban, D.; Reekmans, G.; Bals, S.; Marchal, W.; Carleer, R.; Adriaensens, P.; Meynen, V. | ||||
| Title | Partial hydrolysis of diphosphonate ester during the formation of hybrid Tio₂ nanoparticles : role of acid concentration | Type | A1 Journal article | ||
| Year | 2023 | Publication | ChemPhysChem : a European journal of chemical physics and physical chemistry | Abbreviated Journal | |
| Volume | Issue | Pages | e202300437-13 | ||
| Keywords | A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA) | ||||
| Abstract | In the present work, a method was utilized to control the in‐situ partial hydrolysis of a diphosphonate ester in presence of a titania precursor and in function of acid content and its impact on the hybrid nanoparticles was assessed. The hydrolysis degree of organodiphosphonate ester linkers during the formation of hybrid organic‐inorganic metal oxide nanoparticles, are relatively underexplored . Quantitative solution NMR spectroscopy revealed that during the synthesis of TiO2 nanoparticles, an increase in acid concentration introduces a higher degree of partial hydrolysis of the TEPD linker into diverse acid/ester derivatives of TEPD. Increasing the HCl/Ti ratio from 1 to 3, resulted in an increase in degree of partial hydrolysis of the TEPD linker in solution from 4% to 18.8% under the here applied conditions. As a result of the difference in partial hydrolysis, the linker‐TiO2 bonding was altered. Upon subsequent drying of the colloidal TiO2 solution, different textures, at nanoscale and macroscopic scale, were obtained dependent on the HCl/Ti ratio and thus the degree of hydrolysis of TEPD. Understanding such linker‐TiO2 nanoparticle surface dynamics is crucial for making hybrid organic‐inorganic materials (i.e. (porous) metal phosphonates) employed in applications such as electronic/photonic devices, separation technology and heterogeneous catalysts. | ||||
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| Publisher | Place of Publication | Editor | |||
| Language | Wos | 001071673900001 | Publication Date | 2023-09-05 | |
| Series Editor | Series Title | Abbreviated Series Title | |||
| Series Volume | Series Issue | Edition | |||
| ISSN | 1439-4235; 1439-7641 | ISBN | Additional Links | UA library record; WoS full record | |
| Impact Factor | 2.9 | Times cited | Open Access | OpenAccess | |
| Notes | This work was supported by the Research Foundation-Flanders (FWO Vlaanderen) Project G.0121.17 N. The work was further supported by Hasselt University and the Research Foundation – Flanders (FWO Vlaanderen) via the Hercules project AUHL/15/2 – GOH3816 N. V. M. acknowledges the Research Foundation Flanders (FWO) for project K801621 N. B. M. R. acknowledges, Prof. Dr. Christophe Detavernier and Dr. Davy Deduystche (COCOON, Ghent University) for PXRD and VT-XRD measurements, Prof. Dr. Christophe Van De Velde (iPRACS, University of Antwerp) and Dr. Radu Ciocarlan (LADCA, University of Antwerp) for helpful discussions on PXRD measurements and Dr. Nick Gys (University of Antwerp and VITO) for ICP-OES measurements. | Approved | Most recent IF: 2.9; 2023 IF: 3.075 | ||
| Call Number | UA @ admin @ c:irua:198934 | Serial |
8911 | ||
| Permanent link to this record | |||||