Home << 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 >>
List View
 | 
Citations
 | 
Details
   web
Records
Author Paul, S.; Bladt, E.; Richter, A.F.; Döblinger, M.; Tong, Y.; Huang, H.; Dey, A.; Bals, S.; Debnath, T.; Polavarapu, L.; Feldmann, J.
Title Manganese‐Doping‐Induced Quantum Confinement within Host Perovskite Nanocrystals through Ruddlesden–Popper Defects Type A1 Journal article
Year 2020 Publication Angewandte Chemie-International Edition Abbreviated Journal Angew Chem Int Edit
Volume 59 Issue 17 Pages 6794-6799
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The concept of doping Mn2+ ions into II–VI semiconductor nanocrystals (NCs) was recently extended to perovskite NCs. To date, most studies on Mn2+ doped NCs focus on enhancing the emission related to the Mn2+ dopant via an energy transfer mechanism. Herein, we found that the doping of Mn2+ ions into CsPbCl3 NCs not only results in a Mn2+‐related orange emission, but also strongly influences the excitonic properties of the host NCs. We observe for the first time that Mn2+ doping leads to the formation of Ruddlesden–Popper (R.P.) defects and thus induces quantum confinement within the host NCs. We find that a slight doping with Mn2+ ions improves the size distribution of the NCs, which results in a prominent excitonic peak. However, with increasing the Mn2+ concentration, the number of R.P. planes increases leading to smaller single‐crystal domains. The thus enhanced confinement and crystal inhomogeneity cause a gradual blue shift and broadening of the excitonic transition, respectively.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000525279800024 Publication Date 2020-04-20
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1433-7851 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 16.6 Times cited 64 Open Access OpenAccess
Notes Deutsche Forschungsgemeinschaft, EXC 2089/1-390776260 ; H2020 European Research Council, 815128-REALNANO ; Horizon 2020 Framework Programme, 839042 731019 ; Alexander von Humboldt-Stiftung; We acknowledge financial support by the Bavarian State Ministry of Science, Research, and Arts through the grant “Solar Technologies go Hybrid (SolTech)”, the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germanys Excellence Strategy—EXC 2089/1‐390776260 (“e‐conversion”), the Alexander von Humboldt Foundation (A.D. and T.D.), the European Union's Horizon 2020 research and innovation program under the Marie Sklodowska‐Curie grant agreement No. 839042 (H.H.). E.B. acknowledges a postdoctoral grant 12T2719N from the Research Foundation Flanders (FWO, Belgium). E.B. and S.B. acknowledge the financial support from the European Research Council ERC Consolidator Grants #815128‐REALNANO. L.P. thanks the EU Infrastructure Project EUSMI (European Union's Horizon 2020, grant No 731019). We thank local research center “Center for NanoScience (CeNS)” for providing communicative networking structure. We acknowledge the funding of Nanosystems Initiative Munich (NIM) for color figures.; sygma Approved Most recent IF: 16.6; 2020 IF: 11.994
Call Number (up) EMAT @ emat @c:irua:168535 Serial 6399
Permanent link to this record
 
 
Author Marchetti, A.; Saniz, R.; Krishnan, D.; Rabbachin, L.; Nuyts, G.; De Meyer, S.; Verbeeck, J.; Janssens, K.; Pelosi, C.; Lamoen, D.; Partoens, B.; De Wael, K.
Title Unraveling the Role of Lattice Substitutions on the Stabilization of the Intrinsically Unstable Pb2Sb2O7Pyrochlore: Explaining the Lightfastness of Lead Pyroantimonate Artists’ Pigments Type A1 Journal article
Year 2020 Publication Chemistry Of Materials Abbreviated Journal Chem Mater
Volume 32 Issue 7 Pages 2863-2873
Keywords A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT)
Abstract The pyroantimonate pigments Naples yellow and lead tin antimonate yellow are recognized as some of the most stable synthetic yellow pigments in the history of art. However, this exceptional lightfastness is in contrast with experimental evidence suggesting that this class of mixed oxides is of semiconducting nature. In this study the electronic structure and light-induced behavior of the lead pyroantimonate pigments were determined by means of a combined multifaceted analytical and computational approach (photoelectrochemical measurements, UV-vis diffuse reflectance spectroscopy, STEM-EDS, STEM-HAADF, and density functional theory calculations). The results demonstrate both the semiconducting nature and the lightfastness of these pigments. Poor optical absorption and minority carrier mobility are the main properties responsible for the observed stability. In addition, novel fundamental insights into the role played by Na atoms in the stabilization of the otherwise intrinsically unstable Pb2Sb2O7 pyrochlore were obtained.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000526394000016 Publication Date 2020-04-14
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.6 Times cited 8 Open Access OpenAccess
Notes Universiteit Antwerpen; Belgian Federal Science Policy Office; Approved Most recent IF: 8.6; 2020 IF: 9.466
Call Number (up) EMAT @ emat @c:irua:168819 Serial 6363
Permanent link to this record
 
 
Author Albrecht, W.; Bals, S.
Title Fast Electron Tomography for Nanomaterials Type A1 Journal article
Year 2020 Publication Journal Of Physical Chemistry C Abbreviated Journal J Phys Chem C
Volume Issue Pages acs.jpcc.0c08939
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Electron tomography (ET) has become a well-established technique to visualize nanomaterials in three dimensions. A vast richness in information can be gained by ET, but the conventional acquisition of a tomography series is an inherently slow process on the order of 1 h. The slow acquisition limits the applicability of ET for monitoring dynamic processes or visualizing nanoparticles, which are sensitive to the electron beam. In this Perspective, we summarize recent work on the development of emerging experimental and computational schemes to enhance the data acquisition process. We particularly focus on the application of these fast ET techniques for beam-sensitive materials and highlight insight into dynamic transformations of nanoparticles under external stimuli, which could be gained by fast in situ ET. Moreover, we discuss challenges and possible solutions for simultaneously increasing the speed and quality of fast ET.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000608876900003 Publication Date 2020-11-27
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1932-7447 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.7 Times cited 26 Open Access OpenAccess
Notes H2020 Research Infrastructures, 823717 ; H2020 European Research Council, 815128 ; The authors acknowledge funding from the European Research Council under the European Union’s Horizon 2020 research and innovation program (ERC Consolidator Grant No. 815128-REALNANO) and the European Commission (EUSMI). The authors furthermore acknowledge funding from the European Union’s Horizon 2020 research and innovation program, ESTEEM3. The authors also acknowledge contributions from all co-workers that have contributed over the years: J. Batenburg and co-workers, A. Béché, E. Bladt, L. Liz-Marzán and co-workers, H. Pérez Garza and co-workers, A. Skorikov, S. Skrabalak and co-workers, S. Van Aert, A. van Blaaderen and co-workers, H. Vanrompay, and J. Verbeeck.; sygma Approved Most recent IF: 3.7; 2020 IF: 4.536
Call Number (up) EMAT @ emat @c:irua:173965 Serial 6656
Permanent link to this record
 
 
Author Leemans, J.; Singh, S.; Li, C.; Ten Brinck, S.; Bals, S.; Infante, I.; Moreels, I.; Hens, Z.
Title Near-Edge Ligand Stripping and Robust Radiative Exciton Recombination in CdSe/CdS Core/Crown Nanoplatelets Type A1 Journal article
Year 2020 Publication Journal Of Physical Chemistry Letters Abbreviated Journal J Phys Chem Lett
Volume 11 Issue 9 Pages 3339-3344
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract We address the relation between surface chemistry and optoelectronic properties in semiconductor nanocrystals using core/crown CdSe/CdS nanoplatelets passivated by cadmium oleate (Cd(Ol)2) as model systems. We show that addition of butylamine to a nanoplatelet (NPL) dispersion maximally displaces ∼40% of the original Cd(Ol)2 capping. On the basis of density functional theory simulations, we argue that this behavior reflects the preferential displacement of Cd(Ol)2 from (near)-edge surface sites. Opposite from CdSe core NPLs, core/crown NPL dispersions can retain 45% of their initial photoluminescence efficiency after ligand displacement, while radiative exciton recombination keeps dominating the luminescent decay. Using electron microscopy observations, we assign this robust photoluminescence to NPLs with a complete CdS crown, which prevents charge carrier trapping in the near-edge surface sites created by ligand displacement. We conclude that Z-type ligands such as cadmium carboxylates can provide full electronic passivation of (100) facets yet are prone to displacement from (near)-edge surface sites.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000535177500024 Publication Date 2020-05-07
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1948-7185 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 5.7 Times cited 24 Open Access OpenAccess
Notes Universiteit Gent, GOA 01G01019 ; Fonds Wetenschappelijk Onderzoek, 17006602 FWO17/PDO/184 ; H2020 European Research Council, 714876 Phocona 815128 Realnano ; SIM-Flanders, SBO-QDOCCO ; Z.H. and S.B. acknowledge support by SIM-Flanders (SBO-QDOCCO). Z.H. acknowledges support by FWO-Vlaanderen (research project 17006602). Z.H. and I.M. acknowledge support by Ghent University (GOA n◦ 01G01019). J.L. acknowledges FWO-vlaanderen for a fellowship (SB PhD fellow at FWO). Sh.S acknowledges FWO postdoctoral funding (FWO17/PDO/184). This project has further received funding from the European Research Counsil under the European Union’s Horizon 2020 research and innovation programme (ERC Consolidator grant no. 815128 REALNANO and starting grant no. 714876 PHOCONA).; sygma Approved Most recent IF: 5.7; 2020 IF: 9.353
Call Number (up) EMAT @ emat @c:irua:173994 Serial 6657
Permanent link to this record
 
 
Author Imran, M.; Ramade, J.; Di Stasio, F.; De Franco, M.; Buha, J.; Van Aert, S.; Goldoni, L.; Lauciello, S.; Prato, M.; Infante, I.; Bals, S.; Manna, L.
Title Alloy CsCdxPb1–xBr3Perovskite Nanocrystals: The Role of Surface Passivation in Preserving Composition and Blue Emission Type A1 Journal article
Year 2020 Publication Chemistry Of Materials Abbreviated Journal Chem Mater
Volume 32 Issue Pages acs.chemmater.0c03825
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Various strategies have been proposed to engineer the band gap of metal halide perovskite nanocrystals (NCs) while preserving their structure and composition and thus ensuring spectral stability of the emission color. An aspect that has only been marginally investigated is how the type of surface passivation influences the structural/color stability of AMX3 perovskite NCs composed of two different M2+ cations. Here, we report the synthesis of blue-emitting Cs-oleate capped CsCdxPb1–xBr3 NCs, which exhibit a cubic perovskite phase containing Cd-rich domains of Ruddlesden–Popper phases (RP phases). The RP domains spontaneously transform into pure orthorhombic perovskite ones upon NC aging, and the emission color of the NCs shifts from blue to green over days. On the other hand, postsynthesis ligand exchange with various Cs-carboxylate or ammonium bromide salts, right after NC synthesis, provides monocrystalline NCs with cubic phase, highlighting the metastability of RP domains. When NCs are treated with Cs-carboxylates (including Cs-oleate), most of the Cd2+ ions are expelled from NCs upon aging, and the NCs phase evolves from cubic to orthorhombic and their emission color changes from blue to green. Instead, when NCs are coated with ammonium bromides, the loss of Cd2+ ions is suppressed and the NCs tend to retain their blue emission (both in colloidal dispersions and in electroluminescent devices), as well as their cubic phase, over time. The improved compositional and structural stability in the latter cases is ascribed to the saturation of surface vacancies, which may act as channels for the expulsion of Cd2+ ions from NCs.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000603288800034 Publication Date 2020-12-04
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.6 Times cited 44 Open Access OpenAccess
Notes European Commission; Fonds Wetenschappelijk Onderzoek, G.0267.18N ; H2020 European Research Council, 770887 815128 851794 ; We acknowledge funding from the FLAG-ERA JTC2019 project PeroGas. S.B., and S.V.A. acknowledges funding from the European Research Council under the European Union’s Horizon 2020 research and innovation program (ERC Consolidator Grants #815128REALNANO and #770887PICOMETRICS) and from the Research Foundation Flanders (FWO, Belgium) through project funding G.0267.18N. F.D.S. acknowledges the funding from ERC starting grant NANOLED (851794). The computational work was carried out on the Dutch National e-infrastructure with the support of the SURF Cooperative; sygma Approved Most recent IF: 8.6; 2020 IF: 9.466
Call Number (up) EMAT @ emat @c:irua:174004 Serial 6659
Permanent link to this record
 
 
Author Blommaerts, N.; Hoeven, N.; Arenas Esteban, D.; Campos, R.; Mertens, M.; Borah, R.; Glisenti, A.; De Wael, K.; Bals, S.; Lenaerts, S.; Verbruggen, S.W.; Cool, P.
Title Tuning the turnover frequency and selectivity of photocatalytic CO2 reduction to CO and methane using platinum and palladium nanoparticles on Ti-Beta zeolites Type A1 Journal article
Year 2021 Publication Chemical Engineering Journal Abbreviated Journal Chem Eng J
Volume 410 Issue Pages 128234
Keywords A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL); Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Abstract A Ti-Beta zeolite was used in gas phase photocatalytic CO2 reduction to reduce the charge recombination rate and increase the surface area compared to P25 as commercial benchmark, reaching 607 m2 g-1. By adding Pt nanoparticles, the selectivity can be tuned toward CO, reaching a value of 92% and a turnover frequency (TOF) of 96 µmol.gcat-1.h-1, nearly an order of magnitude higher in comparison with P25. By adding Pd nanoparticles the selectivity can be shifted from CO (70% for a bare Ti-Beta zeolite), toward CH4 as the prevalent species (60%). In this way, the selectivity toward CO or CH4 can be tuned by either using Pt or Pd. The TOF values obtained in this work outperform reported state-of-the-art values in similar research. The improved activity by adding the nanoparticles was attributed to an improved charge separation efficiency, together with a plasmonic contribution of the metal nanoparticles under the applied experimental conditions.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000623394200004 Publication Date 2021-01-09
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1385-8947 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.216 Times cited 15 Open Access OpenAccess
Notes N.B., S.L., S.W.V. and P.C. wish to thank the Flemish government and Catalisti for financial support and coordination in terms of a sprint SBO in the context of the moonshot project D2M. N.H. thanks the Flanders Innovation and Entrepreneurship (VLAIO) for the financial support. The Systemic Physiological and Ecotoxicological Research (SPHERE) group, R. Blust, University of Antwerp is acknowledged for the ICP-MS measurements. Approved Most recent IF: 6.216
Call Number (up) EMAT @ emat @c:irua:174591 Serial 6662
Permanent link to this record
 
 
Author Xu, X.; Jones, M.A.; Cassidy, S.J.; Manuel, P.; Orlandi, F.; Batuk, M.; Hadermann, J.; Clarke, S.J.
Title Magnetic Ordering in the Layered Cr(II) Oxide Arsenides Sr2CrO2Cr2As2and Ba2CrO2Cr2As2 Type A1 Journal article
Year 2020 Publication Inorganic Chemistry Abbreviated Journal Inorg Chem
Volume 59 Issue 21 Pages 15898-15912
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Sr2CrO2Cr2As2 and Ba2CrO2Cr2As2 with Cr2+ ions in CrO2 sheets and in CrAs layers crystallize with the Sr2Mn3Sb2O2 structure (space group I4/mmm, Z = 2) and lattice parameters a = 4.00800(2) Å, c = 18.8214(1) Å (Sr2CrO2Cr2As2) and a = 4.05506(2) Å, c = 20.5637(1) Å (Ba2CrO2Cr2As2) at room temperature. Powder neutron diffraction reveals checkerboard-type antiferromagnetic ordering of the Cr2+ ions in the arsenide layers below TN1Sr, of 600(10) K (Sr2CrO2Cr2As2) and TN1Ba 465(5) K (Ba2CrO2Cr2As2) with the moments initially directed perpendicular to the layers in both compounds. Checkerboard-type antiferromagnetic ordering of the Cr2+ ions in the oxide layer below 230(5) K for Ba2CrO2Cr2As2 occurs with these moments also perpendicular to the layers, consistent with the orientation preferences of d4 moments in the two layers. In contrast, below 330(5) K in Sr2CrO2Cr2As2, the oxide layer Cr2+ moments are initially oriented in the CrO2 plane; but on further cooling, these moments rotate to become perpendicular to the CrO2 planes, while the moments in the arsenide layers rotate by 90° with the moments on the two sublattices remaining orthogonal throughout [behavior recently reported independently by Liu et al. [Liu et al. Phys. Rev. B 2018, 98, 134416]]. In Sr2CrO2Cr2As2, electron diffraction and high resolution powder X-ray diffraction data show no evidence for a structural distortion that would allow the two Cr2+ sublattices to couple, but high resolution neutron powder diffraction data suggest a small incommensurability between the magnetic structure and the crystal structure, which may account for the coupling of the two sublattices and the observed spin reorientation. The saturation values of the Cr2+ moments in the CrO2 layers (3.34(1) μB (for Sr2CrO2Cr2As2) and 3.30(1) μB (for Ba2CrO2Cr2As2)) are larger than those in the CrAs layers (2.68(1) μB for Sr2CrO2Cr2As2 and 2.298(8) μB for Ba2CrO2Cr2As2) reflecting greater covalency in the arsenide layers.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000588738100035 Publication Date 2020-11-02
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0020-1669 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.6 Times cited Open Access OpenAccess
Notes We thank the UK EPSRC (EP/M020517/1 and EP/P018874/ 1) and the Leverhulme Trust (RPG-2014-221) for funding and the ISIS pulsed neutron and muon source (RB1610357 and RB1700075) and the Diamond Light Source Ltd. (EE13284 and EE18786) for the award of beam time. We thank Dr. A. Baker and Dr. C. Murray for support on I11. Approved Most recent IF: 4.6; 2020 IF: 4.857
Call Number (up) EMAT @ emat @c:irua:176058 Serial 6704
Permanent link to this record
 
 
Author Chizhov, As.; Rumyantseva, Mn.; Drozdov, Ka.; Krylov, Iv.; Batuk, M.; Hadermann, J.; Filatova, Dg.; Khmelevsky, No.; Kozlovsky, Vf.; Maltseva, Ln.; Gaskov, Am.
Title Photoresistive gas sensor based on nanocrystalline ZnO sensitized with colloidal perovskite CsPbBr3 nanocrystals Type A1 Journal article
Year 2021 Publication Sensors And Actuators B-Chemical Abbreviated Journal Sensor Actuat B-Chem
Volume 329 Issue Pages 129035
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The development of sensor materials of which gas sensitivity activates under light illumination is of great importance for the design of portable gas analyzers with low power consumption. In the present work a ZnO/CsPbBr3 nanocomposite based on nanocrystalline ZnO and colloidal cubic-shaped perovskite CsPbBr3 nanocrystals (NCs) capped by oleic acide and oleylamine was synthesized. The individual materials and obtained nanocomposite are characterized by x-ray diffraction, low-temperature nitrogen adsorption, x-ray photoelectron spectroscopy, high angle annular dark field scanning transmission electron microscopy with energy-dispersive Xray spectroscopy mapping and UV-vis absorption spectroscopy. The spectral dependence of the photoconductivity of the ZnO/CsPbBr3 nanocomposite reveals a well-defined peak that strongly correlates with the its optical absorption spectrum. The nanocomposite ZnO/CsPbBr3 shows enhanced photoresponse under visible light illumination (lambda(max) = 470 nm, 8 mW/cm(2)) in air, oxygen and argone, compared with pure nanocrystalline ZnO. Under periodic illumination in the temperature range of 25-100 degrees C, the ZnO/CsPbBr3 nanocomposite shows a sensor response to 0.5-3.0 ppm NO2, unlike pure nanocrystalline ZnO matrix, which demonstrates sensor sensitivity to NO2 under the same conditions above 100 degrees C. The effects of humidity on the sensor signal and photoresponse are also discussed.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000612060700009 Publication Date 2020-10-25
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0925-4005 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 5.401 Times cited Open Access OpenAccess
Notes The reported study was funded by RFBR according to the research project N◦ 18-33-01004 and in part by a grant from the St. Petersburg State University – Event 3-2018 (id: 46380300). Element mapping for sensors were supported by M.V. Lomonosov Moscow State University Program of Development (X-ray fluorescence spectrometer Tornado M4 plus). Approved Most recent IF: 5.401
Call Number (up) EMAT @ emat @c:irua:176123 Serial 6707
Permanent link to this record
 
 
Author Sanchis-Gual, R.; Susic, I.; Torres-Cavanillas, R.; Arenas-Esteban, D.; Bals, S.; Mallah, T.; Coronado-Puchau, M.; Coronado, E.
Title The design of magneto-plasmonic nanostructures formed by magnetic Prussian Blue-type nanocrystals decorated with Au nanoparticles Type A1 Journal article
Year 2021 Publication Chemical Communications Abbreviated Journal Chem Commun
Volume 57 Issue 15 Pages 1903-1906
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract We have developed a general protocol for the preparation of hybrid nanostructures formed by nanoparticles (NPs) of molecule-based magnets based on Prussian Blue Analogues (PBAs) decorated with plasmonic Au NPs of different shapes. By adjusting the pH, Au NPs can be attached preferentially along the edges of the PBA or randomly on the surface. The protocol allows tuning the plasmonic properties of the hybrids in the whole visible spectrum.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000620719300011 Publication Date 2021-01-18
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1359-7345 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.319 Times cited 5 Open Access OpenAccess
Notes European Commission, COST Action MOLSPIN CA15128 ERC Advanced Grant Mol-2D 788222 ERC Consolidator Grant REALNANO 815128 Grant Agreement No. 731019 (EUSMI) ; Ministry of Education and Science of the Russian Federation, No. 14.W03.31.0001 ; Ministerio de Ciencia, Innovación y Universidades, Maria de Maeztu CEX2019-000919-M Project MAT2017-89993-R ; Generalitat Valenciana, PROMETEO/2017/066 iDiFEDER/2018/061 ; sygma; Approved Most recent IF: 6.319
Call Number (up) EMAT @ emat @c:irua:176542 Serial 6702
Permanent link to this record
 
 
Author Payne, L.M.; Masia, F.; Zilli, A.; Albrecht, W.; Borri, P.; Langbein, W.
Title Quantitative morphometric analysis of single gold nanoparticles by optical extinction microscopy: Material permittivity and surface damping effects Type A1 Journal article
Year 2021 Publication Journal Of Chemical Physics Abbreviated Journal J Chem Phys
Volume 154 Issue 4 Pages 044702
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000630495600001 Publication Date 2021-01-28
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0021-9606 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 2.965 Times cited Open Access OpenAccess
Notes This work was supported by the Welsh Government Life Sciences Bridging Fund (Grant No. LSBF/R6-005), the UK EPSRC (Grant Nos. EP/I005072/1 and EP/M028313/1), and the European Commission (Grant No. EUSMI E191000350). P.B. acknowledges the Royal Society for her Wolfson research merit award (Grant No. WM140077). F.M. acknowledges the Ser Cymru II programme (Case ID 80762-CU-148) which is part-funded by Cardiff University and the European Regional Development Fund through the Welsh Government. W.A. acknowledges an Individual Fellowship from the Marie Skłodowska-Curie actions (MSCA) under the EU’s Horizon 2020 program (Grant No. 797153, SOPMEN) and Sara Bals for supporting the STEM measurements. The brightfield TEM was performed by Thomas Davies at Cardiff University. We acknowledge Iestyn Pope for technical support of the optical equipment. Approved Most recent IF: 2.965
Call Number (up) EMAT @ emat @c:irua:177566 Serial 6748
Permanent link to this record
 
 
Author Albrecht, W.; Van Aert, S.; Bals, S.
Title Three-Dimensional Nanoparticle Transformations Captured by an Electron Microscope Type A1 Journal article
Year 2021 Publication Accounts Of Chemical Research Abbreviated Journal Accounts Chem Res
Volume 54 Issue 5 Pages 1189-1199
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000626269900011 Publication Date 2021-03-02
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 20.268 Times cited 12 Open Access OpenAccess
Notes The authors 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 No. 770887–PICOMETRICS), the Research Foundation Flanders (FWO, G.0267.18N), and the European Commission (EUSMI). The authors furthermore acknowledge funding from the European Union’s Horizon 2020 research and innovation program, ESTEEM3. The authors also acknowledge contributions from all co-workers that have contributed over the years: Thomas Altantzis, Annick De Backer, Joost Batenburg and co-workers, Armand Béché, Eva Bladt, Lewys Jones and co-workers, Luis Liz-Marzán and co-workers, Ivan Lobato, Thais Milagres de Oliveira, Peter Nellist and co-workers, Hugo Pérez Garza and co-workers, Alexander Skorikov, Sara Skrabalak and co-workers, Sandra Van Aert, Alfons van Blaaderen and co-workers, Hans Vanrompay, Staf Van Tendeloo, and Johan Verbeeck.; sygmaSB; Approved Most recent IF: 20.268
Call Number (up) EMAT @ emat @c:irua:177644 Serial 6752
Permanent link to this record
 
 
Author Freund, R.; Canossa, S.; Cohen, S.M.; Yan, W.; Deng, H.; Guillerm, V.; Eddaoudi, M.; Madden, D.G.; Fairen-Jimenez, D.; Lyu, H.; Macreadie, L.K.; Ji, Z.; Zhang, Y.; Wang, B.; Haase, F.; Wöll, C.; Zaremba, O.; Andreo, J.; Wuttke, S.; Diercks, C.S.
Title 25 years of Reticular Chemistry Type A1 Journal article
Year 2021 Publication Angewandte Chemie-International Edition Abbreviated Journal Angew Chem Int Edit
Volume Issue Pages anie.202101644
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract At its core, reticular chemistry has translated the precision and expertise of organic and inorganic synthesis to the solid state. While initial excitement over metal‐organic frameworks (MOFs) and covalent organic frameworks (COFs) was undoubtedly fueled by their unprecedented porosity and surface areas, the most profound scientific innovation of the field has been the elaboration of design strategies for the synthesis of extended crystalline solids through strong directional bonds. In this contribution we highlight the different classes of reticular materials that have been developed, how these frameworks can be functionalized and how complexity can be introduced into their backbones. Finally, we show how the structural control over these materials is being extended from the molecular scale to their crystal morphology and shape on the nanoscale, all the way to their shaping on the bulk scale.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000672037800001 Publication Date 2021-03-29
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1433-7851 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 11.994 Times cited Open Access OpenAccess
Notes Approved Most recent IF: 11.994
Call Number (up) EMAT @ emat @c:irua:177778 Serial 6743
Permanent link to this record
 
 
Author Arenas-Vivo, A.; Rojas, S.; Ocaña, I.; Torres, A.; Liras, M.; Salles, F.; Arenas-Esteban, D.; Bals, S.; Ávila, D.; Horcajada, P.
Title Ultrafast reproducible synthesis of a Ag-nanocluster@MOF composite and its superior visible-photocatalytic activity in batch and in continuous flow Type A1 Journal article
Year 2021 Publication Journal Of Materials Chemistry A Abbreviated Journal J Mater Chem A
Volume 9 Issue 28 Pages 15704-15713
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract The (photo)catalytic properties of metal–organic frameworks (MOFs) can be enhanced by post-synthetic inclusion of metallic species in their porosity. Due to their extraordinarily high surface area and well defined porous structure, MOFs can be used for the stabilization of metal nanoparticles with adjustable size within their porosity. Originally, we present here an optimized ultrafast photoreduction protocol for the<italic>in situ</italic>synthesis of tiny and monodisperse silver nanoclusters (AgNCs) homogeneously supported on a photoactive porous titanium carboxylate MIL-125-NH<sub>2</sub>MOF. The strong metal–framework interaction between –NH<sub>2</sub>and Ag atoms influences the AgNC growth, leading to the surfactant-free efficient catalyst AgNC@MIL-125-NH<sub>2</sub>with improved visible light absorption. The potential use of AgNC@MIL-125-NH<sub>2</sub>was further tested in challenging applications: (i) the photodegradation of the emerging organic contaminants (EOCs) methylene blue (MB-dye) and sulfamethazine (SMT-antibiotic) in water treatment, and (ii) the catalytic hydrogenation of<italic>p</italic>-nitroaniline (4-NA) to<italic>p</italic>-phenylenediamine (PPD) with industrial interest. It is noteworthy that compared with the pristine MIL-125-NH<sub>2</sub>, the composite presents an improved catalytic activity and stability, being able to photodegrade 92% of MB in 60 min and 96% of SMT in 30 min, and transform 100% of 4-NA to PPD in 30 min. Aside from these very good results, this study describes for the first time the use of a MOF in a visible light continuous flow reactor for wastewater treatment. With only 10 mg of AgNC@MIL-125-NH<sub>2</sub>, high SMT removal efficiency over 70% is maintained after >2 h under water flow conditions found in real wastewater treatment plants, signaling a future real application of MOFs in water remediation.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000671839200001 Publication Date 2021-06-21
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2050-7488 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.867 Times cited 18 Open Access OpenAccess
Notes Comunidad de Madrid, CAM PEJD-2016/IND-2828 Talento Modality 2, 2017-T2/IND-5149 ; Secretaría de Estado de Investigación, Desarrollo e Innovación, Raphuel project (ENE2016-79608-C2-1-R) Retos Project MAT2017-84385-R ; Ministerio de Ciencia e Innovación, Juan de la Cierva Incorporación Fellowship (grant agreement no. IJC2019-038894-I) MOFSEIDON project (PID2019-104228RB-I00) Ramón y Cajal, Grant Agreements 2014-15039 and 2015-18677 ; Fundación BBVA, IN[17]CBBQUI_0197 ; H2020 European Research Council, ERC Consolidator Grant REALNANO 815128 Grant Agreement no. 731019 (EUSMI) ; sygmaSB; Approved Most recent IF: 8.867
Call Number (up) EMAT @ emat @c:irua:179791 Serial 6802
Permanent link to this record
 
 
Author Leinders, G.; Baldinozzi, G.; Ritter, C.; Saniz, R.; Arts, I.; Lamoen, D.; Verwerft, M.
Title Charge Localization and Magnetic Correlations in the Refined Structure of U3O7 Type A1 Journal article
Year 2021 Publication Inorganic Chemistry Abbreviated Journal Inorg Chem
Volume 60 Issue 14 Pages 10550-10564
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Atomic arrangements in the mixed-valence oxide U3O7 are refined from high-resolution neutron scattering data. The crystallographic model describes a long-range structural order in a U60O140 primitive cell (space group P42/n) containing distorted cuboctahedral oxygen clusters. By combining experimental data and electronic structure calculations accounting for spin–orbit interactions, we provide robust evidence of an interplay between charge localization and the magnetic moments carried by the uranium atoms. The calculations predict U3O7 to be a semiconducting solid with a band gap of close to 0.32 eV, and a more pronounced charge-transfer insulator behavior as compared to the well-known Mott insulator UO2. Most uranium ions (56 out of 60) occur in 9-fold and 10-fold coordinated environments, surrounding the oxygen clusters, and have a tetravalent (24 out of 60) or pentavalent (32 out of 60) state. The remaining uranium ions (4 out of 60) are not contiguous to the oxygen cuboctahedra and have a very compact, 8-fold coordinated environment with two short (2 × 1.93(3) Å) “oxo-type” bonds. The higher Hirshfeld charge and the diamagnetic character point to a hexavalent state for these four uranium ions. Hence, the valence state distribution corresponds to 24/60 × U(IV) + 32/60 U(V) + 4/60 U(VI). The tetravalent and pentavalent uranium ions are predicted to carry noncollinear magnetic moments (with amplitudes of 1.6 and 0.8 μB, respectively), resulting in canted ferromagnetic order in characteristic layers within the overall fluorite-related structure.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000675430900049 Publication Date 2021-07-19
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0020-1669 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.857 Times cited Open Access OpenAccess
Notes Financial support for this research was partly provided by the Energy Transition Fund of the Belgian FPS Economy (Project SF-CORMOD – Spent Fuel CORrosion MODeling). This work was performed in part using HPC resources from GENCI-IDRIS (Grants 2020-101450 and 2020-101601), and in part by the VSC (Flemish Supercomputer Center) and the HPC infrastructure of the University of Antwerp (CalcUA), both funded by the FWO-Vlaanderen and the Flemish Government-department EWI. GL thanks E. Suard and C. Schreinemachers for assistance during the neutron scattering experiments at the ILL. GB acknowledges V. Petříček for suggestions on using JANA2006. Approved Most recent IF: 4.857
Call Number (up) EMAT @ emat @c:irua:179907 Serial 6801
Permanent link to this record
 
 
Author Renero-Lecuna, C.; Herrero, A.; Jimenez de Aberasturi, D.; Martínez-Flórez, M.; Valiente, R.; Mychinko, M.; Bals, S.; Liz-Marzán, L.M.
Title Nd3+-Doped Lanthanum Oxychloride Nanocrystals as Nanothermometers Type A1 Journal article
Year 2021 Publication Journal Of Physical Chemistry C Abbreviated Journal J Phys Chem C
Volume 125 Issue 36 Pages 19887-19896
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract The development of optical nanothermometers operating in the near-infrared (NIR) is of high relevance toward temperature measurements in biological systems. We propose herein the use of Nd3+-doped lanthanum oxychloride nanocrystals as an efficient system with intense photoluminescence under NIR irradiation in the first biological transparency window and emission in the second biological window with excellent emission stability over time under 808 nm excitation, regardless of Nd3+ concentration, which can be considered as a particular strength of our system. Additionally, surface passivation through overgrowth of an inert LaOCl shell around optically active LaOCl/Nd3+ cores was found to further enhance the photoluminescence intensity and also the lifetime of the 1066 nm, 4F3/2 to 4I11/2 transition, without affecting its (ratiometric) sensitivity toward temperature changes. As required for biological applications, we show that the obtained (initially hydrophobic) nanocrystals can be readily transferred into aqueous solvents with high, long-term stability, through either ligand exchange or encapsulation with an amphiphilic polymer.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000697335100031 Publication Date 2021-09-16
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1932-7447 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.536 Times cited 9 Open Access OpenAccess
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). This work was performed under the Maria de Maeztu Units of Excellence Program from the Spanish State Research Agency−Grant MDM-2017−0720. Realnano; sygmaSB Approved Most recent IF: 4.536
Call Number (up) EMAT @ emat @c:irua:181671 Serial 6831
Permanent link to this record
 
 
Author Feng, X.; Jena, H.S.; Krishnaraj, C.; Arenas-Esteban, D.; Leus, K.; Wang, G.; Sun, J.; Rüscher, M.; Timoshenko, J.; Roldan Cuenya, B.; Bals, S.; Voort, P.V.D.
Title Creation of Exclusive Artificial Cluster Defects by Selective Metal Removal in the (Zn, Zr) Mixed-Metal UiO-66 Type A1 Journal article
Year 2021 Publication Journal Of The American Chemical Society Abbreviated Journal J Am Chem Soc
Volume Issue Pages jacs.1c05357
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract The differentiation between missing linker defects

and missing cluster defects in MOFs is difficult, thereby limiting the

ability to correlate materials properties to a specific type of defects.

Herein, we present a novel and easy synthesis strategy for the

creation of solely “missing cluster defects” by preparing mixed-metal

(Zn, Zr)-UiO-66 followed by a gentle acid wash to remove the Zn

nodes. The resulting material has the reo UiO-66 structure, typical

for well-defined missing cluster defects. The missing clusters are

thoroughly characterized, including low-pressure Ar-sorption, iDPCSTEM

at a low dose (1.5 pA), and XANES/EXAFS analysis. We

show that the missing cluster UiO-66 has a negligible number of missing linkers. We show the performance of the missing cluster

UiO-66 in CO2 sorption and heterogeneous catalysis.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000730569500001 Publication Date 2021-12-07
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0002-7863 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.858 Times cited 29 Open Access OpenAccess
Notes Agentschap Innoveren en Ondernemen, HBC.2019.0110 HBC.2021.0254 ; Universiteit Gent; Fonds Wetenschappelijk Onderzoek, 665501 ; Dalian University of Technology; China Scholarship Council, 201507565009 ; National Natural Science Foundation of China, 22101039 ; H2020 European Research Council, 815128 REALNANO ; sygmaSB Approved Most recent IF: 13.858
Call Number (up) EMAT @ emat @c:irua:183951 Serial 6833
Permanent link to this record
 
 
Author Zhang, Y.; Qin, S.; Claes, N.; Schilling, W.; Sahoo, P.K.; Ching, H.Y.V.; Jaworski, A.; Lemière, F.; Slabon, A.; Van Doorslaer, S.; Bals, S.; Das, S.
Title Direct Solar Energy-Mediated Synthesis of Tertiary Benzylic Alcohols Using a Metal-Free Heterogeneous Photocatalyst Type A1 Journal article
Year 2022 Publication ACS Sustainable Chemistry and Engineering Abbreviated Journal Acs Sustain Chem Eng
Volume 10 Issue 1 Pages 530-540
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Organic synthesis (ORSY)
Abstract Direct hydroxylation via the functionalization of tertiary benzylic C(sp3)-H bond is of great significance for obtaining tertiary alcohols which find wide applications in pharmaceuticals as well as in fine chemical industries. However, current synthetic procedures use toxic reagents and therefore, the development of a sustainable strategy for the synthesis of tertiary benzyl alcohols is highly desirable. To solve this problem, herein, we report a metal-free

heterogeneous photocatalyst to synthesize the hydroxylated products using oxygen as the key reagent. Various benzylic substrates were employed into our mild reaction conditions to afford the desirable products in good to excellent yields. More importantly, gram-scale reaction was achieved via harvesting direct solar energy and exhibited high quantity of the product. The high stability of the catalyst was proved via recycling the catalyst and spectroscopic analyses. Finally, a possible mechanism was proposed based on the EPR and other experimental

evidence.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000736518000001 Publication Date 2022-01-10
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2168-0485 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.4 Times cited 24 Open Access OpenAccess
Notes We thank BOF joint PhD grant (to Y. Z.), Francqui Foundation and FWO research grant (to S.D.), Chinese Scholarship Council (to Y.Z.). A.S. would like to thank the Swedish Energy Agency for financial support (project nr: 5050-1). The SEM microscope was partly funded by the Hercules Fund from the Flemish Government. Approved Most recent IF: 8.4
Call Number (up) EMAT @ emat @c:irua:184744 Serial 6900
Permanent link to this record
 
 
Author Altantzis, T.; Wang, D.; Kadu, A.; van Blaaderen, A.; Bals, S.
Title Optimized 3D Reconstruction of Large, Compact Assemblies of Metallic Nanoparticles Type A1 Journal article
Year 2021 Publication Journal Of Physical Chemistry C Abbreviated Journal J Phys Chem C
Volume 125 Issue 47 Pages 26240-26246
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Abstract 3D characterization of assemblies of nanoparticles is of great importance to determine their structure-property connection. Such investigations become increasingly more challenging when the assemblies become larger and more compact. In this paper, we propose an optimized approach for electron tomography to minimize artefacts related to beam broadening in High Angle Annular Dark-Field Scanning Transmission Electron Microscopy mode. These artefacts are typically present at one side of the reconstructed 3D data set for thick nanoparticle assemblies. To overcome this problem, we propose a procedure in which two tomographic tilt series of the same sample are acquired. After acquiring the first series, the sample is flipped over 180o, and a second tilt series is acquired. By merging the two reconstructions, blurring in the reconstructed volume is minimized. Next, this approach is combined with an advanced three-dimensional reconstruction algorithm yielding quantitative structural information. Here, the approach is applied to a thick and compact assembly of spherical Au nanoparticles, but the methodology can we used to investigate a broad range of samples.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000752810100031 Publication Date 2021-12-02
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1932-7447 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.536 Times cited 4 Open Access OpenAccess
Notes This work was supported by the European Research Council (grant No. 815128−REALNANO to S.B.). T.A. acknowledges the University of Antwerp Research fund (BOF). D.W. and A.v.B. acknowledge partial financial support from the European Research Council under the European Union’s Seventh Framework Program (FP-2007-2013)/ERC Advanced Grant Agreement 291667 HierarSACol. D.W. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (grant 894254 SuprAtom).; sygmaSB Approved Most recent IF: 4.536
Call Number (up) EMAT @ emat @c:irua:185224 Serial 6904
Permanent link to this record
 
 
Author Salzmann, B.B.V.; Wit, J. de; Li, C.; Arenas-Esteban, D.; Bals, S.; Meijerink, A.; Vanmaekelbergh, D.
Title Two-Dimensional CdSe-PbSe Heterostructures and PbSe Nanoplatelets: Formation, Atomic Structure, and Optical Properties Type A1 Journal article
Year 2022 Publication The journal of physical chemistry: C : nanomaterials and interfaces Abbreviated Journal J Phys Chem C
Volume 126 Issue 3 Pages 1513-1522
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000744909200001 Publication Date 2022-01-27
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1932-7447 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.7 Times cited 12 Open Access OpenAccess
Notes H. Meeldijk is kindly acknowledged for helping with electron microscopy at Utrecht University. T. Prins is kindly acknowledged for useful discussions. B.B.V.S. and D.V. acknowledge the Dutch NWO for financial support via the TOP-ECHO Grant No. 715.016.002. D.V. acknowledges financial support from the European ERC Council, ERC Advanced Grant 692691 “First Step”. J.W. and A.M. acknowledge financial support from the project CHEMIE.PGT.2019.004 of TKI/ Topsector Chemie, which is partly financed by the Dutch NWO. S.B, C.L., and D.A.E. acknowledge financial support from the European ERC Council, ERC Consolidator Grant realnano No. 815128. This project has received funding from the European Union’s Horizon 2020 research and innovation program under Grant No. 731019 (EUSMI). sygmaSB Approved Most recent IF: 3.7
Call Number (up) EMAT @ emat @c:irua:185454 Serial 6953
Permanent link to this record
 
 
Author Mallick, S.; Zhang, W.; Batuk, M.; Gibbs, A.S.; Hadermann, J.; Halasyamani, P.S.; Hayward, M.A.
Title The crystal and defect structures of polar KBiNb2O7 Type A1 Journal article
Year 2022 Publication Journal of the Chemical Society : Dalton transactions Abbreviated Journal Dalton T
Volume 51 Issue 5 Pages 1866-1873
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract KBiNb2O7 was prepared from RbBiNb2O7 by a sequence of cation exchange reactions which first convert RbBiNb2O7 to LiBiNb2O7, before KBiNb2O7 is formed by a further K-for-Li cation exchange. A combination of neutron, synchrotron X-ray and electron diffraction data reveal that KBiNb2O7 adopts a polar, layered, perovskite structure (space group A11m) in which the BiNb2O7 layers are stacked in a (0, ½, z) arrangement, with the K+ cations located in half of the available 10-coordinate interlayer cation sites. The inversion symmetry of the phase is broken by a large displacement of the Bi3+ cations parallel to the y-axis. HAADF-STEM images reveal that KBiNb2O7 exhibits frequent stacking faults which convert the (0. ½, z) layer stacking to (½, 0, z) stacking and vice versa, essentially switching the x- and y-axes of the material. By fitting the complex diffraction peak shape of the SXRD data collected from KBiNb2O7 it is estimated that each layer has approximately an ~11% chance of being defective – a high level which is attributed to the lack of cooperative NbO6 tilting in the material, which limits the lattice strain associated with each fault.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000741540300001 Publication Date 2022-01-05
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1477-9226 ISBN Additional Links UA library record; WoS full record
Impact Factor 4 Times cited Open Access OpenAccess
Notes Experiments at the Diamond Light Source were performed as part of the Block Allocation Group award “Oxford/Warwick Solid State Chemistry BAG to probe composition-structure-property relationships in solids” (EE18786). Experiments at the ISIS pulsed neutron facility were supported by a beam time allocation from the STFC (RB 2000148). SM thanks Somerville College for an Oxford Ryniker Lloyd scholarship. PSH and WZ thank the National Science Foundation (DMR-2002319) for support. Approved Most recent IF: 4
Call Number (up) EMAT @ emat @c:irua:185504 Serial 6951
Permanent link to this record
 
 
Author Wang, J.; Zhang, K.; Kavak, S.; Bals, S.; Meynen, V.
Title Modifying the Stöber Process: Is the Organic Solvent Indispensable? Type A1 Journal Article
Year 2022 Publication Chemistry-A European Journal Abbreviated Journal Chem-Eur J
Volume Issue Pages
Keywords A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;
Abstract The Stöber method is one of the most important and fundamental processes for the synthesis of inorganic (nano)materials but has the drawback of using a large amount of organic solvent. Herein, ethanol was used as an example to explore if the organic solvent in a typical Stöber method can be omitted. It was found that ethanol increases the particle size of the obtained silica spheres and aids the formation of uniform silica particles rather than forming a gel. Nevertheless, the results indicated that an organic solvent in the initial synthesis mixture is not indispensable. An initially immiscible synthesis method was discovered, which can replace the organic solvent-based Stöber method to successfully synthesize silica particles with the same size ranges as the original Stöber process without addition of organic solvents. Moreover, this process can be of further value for the extension to synthesis processes of other materials based on the Stöber process.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000898283500001 Publication Date 2022-12-14
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0947-6539 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.3 Times cited 3 Open Access OpenAccess
Notes The authors are grateful to Alexander Vansant and Dr. Steven Mullens of VITO for their contributions to the DLS measurements in this paper. J.W acknowledges the State Scholarship funded by the China Scholarship Council (201806060123). K.Z acknowledges the EASiCHEM project funded by the Flemish Strategic Basic Research Program of the Catalisti cluster and Flanders Innovation & Entrepreneurship (HBC.2018.0484). S.K acknowledges the Flemish Fund for Scientific Research (FWO Flanders) through a PhD research grant (1181122N). Approved Most recent IF: 4.3
Call Number (up) EMAT @ emat @c:irua:191646 Serial 7233
Permanent link to this record
 
 
Author Batuk, M.; Vandemeulebroucke, D.; Ceretti, M.; Paulus, W.; Hadermann, J.
Title Topotactic redox cycling in SrFeO2.5+δ explored by 3D electron diffraction in different gas atmospheres Type A1 Journal article
Year 2022 Publication Journal of materials chemistry A : materials for energy and sustainability Abbreviated Journal J Mater Chem A
Volume Issue Pages
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract For oxygen conducting materials applied in solid oxide fuel cells and chemical-looping processes, the understanding of the oxygen diffusion mechanism and the materials’ crystal structure at different stages of the redox reactions is a key parameter to control their performance. In this paper we report the first ever in situ 3D ED experiment in a gas environment and with it uncover the structure evolution of SrFeO2.5 as notably different from that reported from in situ X-ray and in situ neutron powder diffraction studies in gas environments. Using in situ 3D ED on submicron sized single crystals obtained from a high quality monodomain SrFeO2.5 single crystal , we observe the transformation under O2 flow of SrFeO2.5 with an intra- and interlayer ordering of the left and right twisted (FeO4) tetrahedral chains (space group Pcmb) into consecutively SrFeO2.75 with space group Cmmm (at 350°C, 33% O2) and SrFeO3-δ with space group Pm3 ̅m (at 400°C, 100% O2). Upon reduction in H2 flow, the crystals return to the brownmillerite structure with intralayer order, but without regaining the interlayer order of the pristine crystals. Therefore, redox cycling of SrFeO2.5 crystals in O2 and H2 introduces stacking faults into the structure, resulting in an I2/m(0βγ)0s symmetry with variable β.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000891928400001 Publication Date 0000-00-00
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2050-7488 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 11.9 Times cited Open Access OpenAccess
Notes Financial support is acknowledged from the FWO-Hercules fund I003218N ‘Infrastructure for imaging nanoscale processes in gas/vapor or liquid environments’, from the University of Antwerp through grant BOF TOP 38689. This work was supported by the European Commission Horizon 2020 NanED grant number 956099. Financial support from the French National Research Agency (ANR) through the project “Structural induced Electronic Complexity controlled by low temperature Topotactic Reaction” (SECTOR No. ANR-14-CE36- 0006-01) is gratefully acknowledged. Approved Most recent IF: 11.9
Call Number (up) EMAT @ emat @c:irua:192325 Serial 7229
Permanent link to this record
 
 
Author Daele, K.V.; Arenas‐Esteban, D.; Choukroun, D.; Hoekx, S.; Rossen, A.; Daems, N.; Pant, D.; Bals, S.; Breugelmans, T.
Title Enhanced Pomegranate‐Structured SnO2Electrocatalysts for the Electrochemical CO2Reduction to Formate Type A1 Journal article
Year 2023 Publication ChemElectroChem Abbreviated Journal
Volume Issue Pages
Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Abstract Although most state-of-the-art Sn-based electrocatalysts yield promising results in terms of selectivity and catalyst activity, their stability remains insufficient to date. Here, we demonstrate the successful application of the recently developed pomegranate-structured SnO2 (Pom. SnO2) and SnO2@C (Pom. SnO2@C) nanocomposite electrocatalysts for the efficient electrochemical conversion of CO2 to formate. With an initial selectivity of 83 and 86% towards formate and an operating potential of -0.72 V and -0.64 V vs. RHE, respectively, these pomegranate SnO2 electrocatalysts are able to compete with most of the current state-of-the-art Sn-based electrocatalysts in terms of activity and selectivity. Given the importance of electrocatalyst stability, long-term experiments (24 h) were performed and a temporary loss in selectivity for the Pom. SnO2@C electrocatalyst was largely restored to its initial selectivity upon drying and exposure to air. Of all the used (24 h) electrocatalysts, the pomegranate SnO2@C had the highest selectivity over a time period of one hour, reaching an average recovered FE of 85%, while the commercial SnO2 and bare pomegranate SnO2 electrocatalysts reached an average of 79 and 80% FE towards formate, respectively. Furthermore, the pomegranate structure of Pom. SnO2@C was largely preserved due to the presence of the heterogeneous carbon shell, which acts as a protective layer, physically inhibiting particle segregation/pulverisation and agglomeration.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000936694800001 Publication Date 2023-02-15
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2196-0216 ISBN Additional Links UA library record; WoS full record
Impact Factor 4 Times cited Open Access OpenAccess
Notes European Regional Development Fund, E2C 2S03-019 ; Approved Most recent IF: 4; 2023 IF: 4.136
Call Number (up) EMAT @ emat @c:irua:195228 Serial 7249
Permanent link to this record
 
 
Author de la Encarnación, C.; Jungwirth, F.; Vila-Liarte, D.; Renero-Lecuna, C.; Kavak, S.; Orue, I.; Wilhelm, C.; Bals, S.; Henriksen-Lacey, M.; Jimenez de Aberasturi, D.; Liz-Marzán, L.M.
Title Hybrid core–shell nanoparticles for cell-specific magnetic separation and photothermal heating Type A1 Journal article
Year 2023 Publication Journal of materials chemistry B : materials for biology and medicine Abbreviated Journal
Volume Issue Pages
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Hyperthermia, as the process of heating a malignant site above 42 °C to trigger cell death, has emerged as an effective and selective cancer therapy strategy. Various modalities of hyperthermia have been proposed, among which magnetic and photothermal hyperthermia are known to benefit from the use of nanomaterials. In this context, we introduce herein a hybrid colloidal nanostructure comprising plasmonic gold nanorods (AuNRs) covered by a silica shell, onto which iron oxide nanoparticles (IONPs) are subsequently grown. The resulting hybrid nanostructures are responsive to both external magnetic fields and near-infrared irradiation. As a result, they can be applied for the targeted magnetic separation of selected cell populations – upon targeting by antibody functionalization – as well as for photothermal heating. Through this combined functionality, the therapeutic effect of photothermal heating can be enhanced. We demonstrate both the fabrication of the hybrid system and its application for targeted photothermal hyperthermia of human glioblastoma cells.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000968908400001 Publication Date 2023-04-05
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2050-750X ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 7 Times cited 1 Open Access OpenAccess
Notes Ministerio de Ciencia e Innovación, PID2019-108854RA-I00 ; H2020 European Research Council, ERC AdG 787510, 4DBIOSERS ERC CoG 815128, REALNANO ; Fonds Wetenschappelijk Onderzoek, PhD research grant 1181122N ; Approved Most recent IF: 7; 2023 IF: 4.543
Call Number (up) EMAT @ emat @c:irua:195879 Serial 7261
Permanent link to this record
 
 
Author van der Sluijs, M.M.; Salzmann, B.B.V.; Arenas Esteban, D.; Li, C.; Jannis, D.; Brafine, L.C.; Laning, T.D.; Reinders, J.W.C.; Hijmans, N.S.A.; Moes, J.R.; Verbeeck, J.; Bals, S.; Vanmaekelbergh, D.
Title Study of the Mechanism and Increasing Crystallinity in the Self-Templated Growth of Ultrathin PbS Nanosheets Type A1 Journal article
Year 2023 Publication Chemistry of materials Abbreviated Journal
Volume Issue Pages
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Colloidal 2D semiconductor nanocrystals, the analogue of solid-state quantum wells, have attracted strong interest in material science and physics. Molar quantities of suspended quantum objects with spectrally pure absorption and emission can be synthesized. For the visible region, CdSe nanoplatelets with atomically precise thickness and tailorable emission have been (almost) perfected. For the near-infrared region, PbS nanosheets (NSs) hold strong promise, but the photoluminescence quantum yield is low and many questions on the crystallinity, atomic structure, intriguing rectangular shape, and formation mechanism remain to be answered. Here, we report on a detailed investigation of the PbS NSs prepared with a lead thiocyanate single source precursor. Atomically resolved HAADF-STEM imaging reveals the presence of defects and small cubic domains in the deformed orthorhombic PbS crystal lattice. Moreover, variations in thickness are observed in the NSs, but only in steps of 2 PbS monolayers. To study the reaction mechanism, a synthesis at a lower temperature allowed for the study of reaction intermediates. Specifically, we studied the evolution of pseudo-crystalline templates towards mature, crystalline PbS NSs. We propose a self-induced templating mechanism based on an oleylamine-lead-thiocyanate (OLAM-Pb-SCN) complex with two Pb-SCN units as a building block; the interactions between the long-chain ligands regulate the crystal structure and possibly the lateral dimensions.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000959572100001 Publication Date 2023-03-25
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 8.6 Times cited 2 Open Access OpenAccess
Notes H2020 Research Infrastructures, 731019 ; H2020 European Research Council, 692691 815128 ; Nederlandse Organisatie voor Wetenschappelijk Onderzoek, 715.016.002 ; Approved Most recent IF: 8.6; 2023 IF: 9.466
Call Number (up) EMAT @ emat @c:irua:195894 Serial 7255
Permanent link to this record
 
 
Author Kavak, S.; Kadu, A.A.; Claes, N.; Sánchez-Iglesias, A.; Liz-Marzán, L.M.; Batenburg, K.J.; Bals, S.
Title Quantitative 3D Investigation of Nanoparticle Assemblies by Volumetric Segmentation of Electron Tomography Data Sets Type A1 Journal article
Year 2023 Publication The journal of physical chemistry: C : nanomaterials and interfaces Abbreviated Journal
Volume 127 Issue 20 Pages 9725-9734
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Morphological characterization of nanoparticle assemblies and hybrid nanomaterials is critical in determining their structure-property relationships as well as in the development of structures with desired properties. Electron tomography has become a widely utilized technique for the three-dimensional characterization of nanoparticle assemblies. However, the extraction of quantitative morphological parameters from the reconstructed volume can be a complex and labor-intensive task. In this study, we aim to overcome this challenge by automating the volumetric segmentation process applied to three-dimensional reconstructions of nanoparticle assemblies. The key to enabling automated characterization is to assess the performance of different volumetric segmentation methods in accurately extracting predefined quantitative descriptors for morphological characterization. In our methodology, we compare the quantitative descriptors obtained through manual segmentation with those obtained through automated segmentation methods, to evaluate their accuracy and effectiveness. To show generality, our study focuses on the characterization of assemblies of CdSe/CdS quantum dots, gold nanospheres and CdSe/CdS encapsulated in polymeric micelles, and silica-coated gold nanorods decorated with both CdSe/CdS or PbS quantum dots. We use two unsupervised segmentation algorithms: the watershed transform and the spherical Hough transform. Our results demonstrate that the choice of automated segmentation method is crucial for accurately extracting the predefined quantitative descriptors. Specifically, the spherical Hough transform exhibits superior performance in accurately extracting quantitative descriptors, such as particle size and interparticle distance, thereby allowing for an objective, efficient, and reliable volumetric segmentation of complex nanoparticle assemblies.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000991752700001 Publication Date 2023-05-25
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1932-7447 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.7 Times cited 2 Open Access OpenAccess
Notes Fonds Wetenschappelijk Onderzoek, 1181122N ; Horizon 2020 Framework Programme, 861950 ; H2020 European Research Council, 815128 ; Approved Most recent IF: 3.7; 2023 IF: 4.536
Call Number (up) EMAT @ emat @c:irua:196971 Serial 8793
Permanent link to this record
 
 
Author Sa, J.; Hu, N.; Heyvaert, W.; Van Gordon, K.; Li, H.; Wang, L.; Bals, S.; Liz-Marzán, L.M.; Ni, W.
Title Spontaneous Chirality Evolved at the Au–Ag Interface in Plasmonic Nanorods Type A1 Journal article
Year 2023 Publication Chemistry of materials Abbreviated Journal Chem. Mater.
Volume Issue Pages
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Chiral ligands are considered a required ingredient during the synthesis of dissymmetric plasmonic metal nanocrystals. The mechanism behind the generation of chiral structures involves the formation of high Miller index chiral facets, induced by the adsorption of such chiral ligands. We found however that, chirality can also evolve spontaneously, without the involvement of any chiral ligands, during the co-deposition of Au and Ag on Au nanorods. When using a specific Au/Ag ratio, phase segregation of the two metals leads to an interface within the obtained AuAg shell, which can be exposed by removing the Ag component via oxidative etching. Although a close-to-racemic mixture of chiral Au nanorods with right and left handedness is found in solution, electron tomography analysis evidences left- and righthanded helicities, both at the Au-Ag interface and at the exposed surface of Au NRs after Ag etching. The helicity profile of the NRs indicates dominating inclination angles in a range from 30° to 60°. Single-particle optical characterization also reveals random handedness in the plasmonic response of individual nanorods. We hypothesize that, the origin of chirality is related with symmetry breaking during the co-deposition of Au and Ag, through an initial perturbation in a small region on the Au-Ag interface that eventually leads to chiral segregation throughout the nanocrystal.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001052093300001 Publication Date 2023-08-21
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756 ISBN Additional Links UA library record; WoS full record
Impact Factor 8.6 Times cited Open Access OpenAccess
Notes The authors acknowledge the financial support from the National Natural Science Foundation of China (grant 22074102). LMLM acknowledges funding from 26 MCIN/AEI/10.13039/501100011033 and “ESF Investing in your future” (Grant PID2020- 117779RB-I00). This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 823717 – ESTEEM3.; Ministerio de Ciencia e Innovaci?n, PID2020-117779RB-I00 ; H2020 Research Infrastructures, 823717 ; European Social Fund, PID2020-117779RB-I00 ; National Natural Science Foundation of China, 22074102 ; Approved Most recent IF: 8.6; 2023 IF: 9.466
Call Number (up) EMAT @ emat @c:irua:198151 Serial 8810
Permanent link to this record
 
 
Author Delfino, C.L.; Hao, Y.; Martin, C.; Minoia, A.; Gopi, E.; Mali, K.S.; Van der Auweraer, M.; Geerts, Y.H.; Van Aert, S.; Lazzaroni, R.; De Feyter, S.
Title Conformation-Dependent Monolayer and Bilayer Structures of an Alkylated TTF Derivative Revealed using STM and Molecular Modeling Type A1 Journal Article
Year 2023 Publication The Journal of Physical Chemistry C Abbreviated Journal J. Phys. Chem. C
Volume 127 Issue 47 Pages 23023-23033
Keywords A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;
Abstract In this study, the multi-layer self-assembled molecular network formation of an alkylated tetrathiafulvalene compound is studied at the liquid-solid interface between 1-phenyloctane and graphite. A combined theoretical/experimental approach associating force-field and quantum-chemical calculations with scanning tunnelling microscopy is used to determine the two-dimensional self-assembly beyond the monolayer, but also to further the understanding of the molecular adsorption conformation and its impact on the molecular packing within the assemblies at the monolayer and bilayer level.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 001111637100001 Publication Date 2023-11-30
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 Financial support from the Research Foundation-Flanders (FWO G081518N, G0A3220N) and KU Leuven–Internal Funds (C14/19/079) is acknowledged. This work was in part supported by FWO and F. R. S.-FNRS under the Excellence of Science EOS program (project 30489208 and 40007495). C.M. acknowledges the financial support: Grants PID2021-128761OA-C22 and CNS2022-136052 funded by MCIN/AEI/10.13039/501100011033 by the “European Union” and SBPLY/21/180501/000127 funded by JCCM and by the EU through “Fondo Europeo de Desarollo Regional” (FEDER). Research in Mons is also supported by the Belgian National Fund for Scientific Research (FRS-FNRS) within the Consortium des Équipements de Calcul Intensif – CÉCI, under Grant 2.5020.11, and by the Walloon Region (ZENOBE Tier-1 supercomputer, under grant 1117545). Approved Most recent IF: 3.7; 2023 IF: 4.536
Call Number (up) EMAT @ emat @c:irua:201671 Serial 8974
Permanent link to this record
 
 
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.
Address
Corporate Author Thesis
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 (up) EMAT @ emat @c:irua:202124 Serial 8985
Permanent link to this record
 
 
Author Vandemeulebroucke, D.; Batuk, M.; Hajizadeh, A.; Wastiaux, M.; Roussel, P.; Hadermann, J.
Title Incommensurate Modulations and Perovskite Growth in LaxSr2–xMnO4−δAffecting Solid Oxide Fuel Cell Conductivity Type A1 Journal Article
Year 2024 Publication Chemistry of Materials Abbreviated Journal Chem. Mater.
Volume Issue Pages
Keywords A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;
Abstract Ruddlesden-Popper La????Sr2−????MnO4−???? materials are interesting symmetric solid oxide

fuel cell electrodes due to their good redox stability, mixed ionic and electronic conducting behavior and thermal expansion that matches well with common electrolytes. In reducing environments – as at a solid oxide fuel cell anode – the x = 0.5 member, i.e. La0.5Sr1.5MnO4−????, has a much higher total conductivity than compounds with a different La/Sr ratio, although all those compositions have the same K2NiF4-type I4/mmm structure. The origin for this conductivity difference is not yet known in literature. Now, a combination of in-situ and ex-situ 3D electron diffraction, high-resolution imaging, energy-dispersive X-ray analysis and electron energy-loss spectroscopy uncovered clear differences between x=0.25 and x=0.5 in the pristine structure, as well as in the transformations upon high-temperature reduction. In La0.5Sr1.5MnO4−????, Ruddlesden-Popper n=2 layer defects and an amorphous surface layer are present, but not in La0.25Sr1.75MnO4−????. After annealing at 700°C in 5% H2/Ar, La0.25Sr1.75MnO4−???? transforms to a tetragonal 2D incommensurately modulated structure with modulation vectors ⃗????1 = 0.2848(1) · (⃗????* +⃗????*) and ⃗????2 =0.2848(1) · (⃗????* – ⃗????*), whereas La0.5Sr1.5MnO4−???? only partially transforms to an orthorhombic 1D incommensurately modulated structure,

with ⃗???? = 0.318(2) · ⃗????*. Perovskite domains grow at the crystal edge at 700°C in 5%

H2 or vacuum, due to the higher La concentration on the surface compared to the bulk, which leads to a different thermodynamic equilibrium. Since it is known that a lower degree of oxygen vacancy ordering and a higher amount of perovskite blocks enhance oxygen mobility, those differences in defect structure and structural transformation upon reduction, might all contribute to the higher conductivity of La0.5Sr1.5MnO4−???? in solid oxide fuel cell anode conditions compared to other La/Sr ratios.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language English Wos 001174840900001 Publication Date 2024-02-20
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756 ISBN Additional Links UA library record; WoS full record
Impact Factor 8.6 Times cited Open Access Not_Open_Access
Notes Universiteit Antwerpen, BOF TOP 38689 ; Fonds Wetenschappelijk Onderzoek, I003218N ; European Commission NanED, 956099 ; Approved Most recent IF: 8.6; 2024 IF: 9.466
Call Number (up) EMAT @ emat @c:irua:204354 Serial 8997
Permanent link to this record