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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 (up) 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
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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 (up) 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
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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.
Address
Corporate Author Thesis
Publisher (up) 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 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 (up) 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 EMAT @ emat @c:irua:201671 Serial 8974
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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.
Address
Corporate Author Thesis
Publisher (up) 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 Şentürk, D.G.; De Backer, A.; Van Aert, S.
Title Element specific atom counting for heterogeneous nanostructures: Combining multiple ADF STEM images for simultaneous thickness and composition determination Type A1 Journal Article
Year 2024 Publication Ultramicroscopy Abbreviated Journal Ultramicroscopy
Volume 259 Issue Pages 113941
Keywords A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;
Abstract In this paper, a methodology is presented to count the number of atoms in heterogeneous nanoparticles based on the combination of multiple annular dark field scanning transmission electron microscopy (ADF STEM) images. The different non-overlapping annular detector collection regions are selected based on the principles of optimal statistical experiment design for the atom-counting problem. To count the number of atoms, the total intensities of scattered electrons for each atomic column, the so-called scattering cross-sections, are simultaneously compared with simulated library values for the different detector regions by minimising the squared differences. The performance of the method is evaluated for simulated Ni@Pt and Au@Ag core-shell nanoparticles. Our approach turns out to be a dose efficient alternative for the investigation of beam-sensitive heterogeneous materials as compared to the combination of ADF STEM and energy dispersive X-ray spectroscopy.
Address
Corporate Author Thesis
Publisher (up) Place of Publication Editor
Language Wos Publication Date 2024-02-19
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0304-3991 ISBN Additional Links UA library record
Impact Factor 2.2 Times cited Open Access OpenAccess
Notes This work was supported by the European Research Council (Grant 770887 PICOMETRICS to S. Van Aert). The authors acknowledge financial support from the Research Foundation Flanders (FWO, Belgium) through project fundings (G.0346.21N, GOA7723N, and EOS 40007495) and a postdoctoral grant to A. De Backer. S. Van Aert acknowledges funding from the University of Antwerp Research fund (BOF). Approved Most recent IF: 2.2; 2024 IF: 2.843
Call Number EMAT @ emat @c:irua:204353 Serial 8996
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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 (up) 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 EMAT @ emat @c:irua:204354 Serial 8997
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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 (up) 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
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Author Esteban, D.A.; Chamocho, E.G.; Carretero González, J.; Urones Garrote, E.; Otero Díaz, L.C.; Brande, D.Á.
Title Enhancing Electrochemical Properties of Walnut Shell Activated Carbon with Embedded MnO Clusters for Supercapacitor Applications Type A1 Journal Article
Year 2024 Publication Batteries & Supercaps Abbreviated Journal Batteries &amp; Supercaps
Volume Issue Pages
Keywords A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;
Abstract Activated carbon (AC) materials from renewable sources are widely used in electrochemical applications due to their well‐known high surface area. However, their application as electrode material in double‐layer electrochemical devices may be limited due to their relatively low electrical conductivity and lightweight. To overcome these limitations, the incorporation of pseudocapacitance metal oxide nanoparticles is an optimum approach. These nanoparticles can provide a second energy storage mechanism to the composite, mitigating the loss of surface area associated with their incorporation. As a result, the composite material is endowed with increased conductivity and higher density, making it more suitable for practical implementation in real devices. In this study, we have incorporated a fine dispersion of 1 % of MnO clusters into a highly porous activated carbon synthesized from walnut shells (WAC). The high‐resolution electron microscopy studies, combined with their related analytical techniques, allow us to determine the presence of the cluster within the matrix carbon precisely. The resulting MnO@WAC composite demonstrated significantly improved capacitive behavior compared with the WAC material, with increased volumetric capacitance and higher charge retention at higher current densities. The composite‘s electrochemical performance suggests its potential as a promising electrode material for supercapacitors, addressing drawbacks associated with traditional AC materials.
Address
Corporate Author Thesis
Publisher (up) Place of Publication Editor
Language Wos 001198179300001 Publication Date 2024-04-08
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2566-6223 ISBN Additional Links UA library record; WoS full record
Impact Factor Times cited Open Access
Notes Grants PID2020-112848RB-C21 funded by MCIN/AEI/ 10.13039/501100011033 and by the European Union PRTR funding through projects are acknowledged. Access to the ICTS- CNME for TEM is also acknowledged. Approved Most recent IF: NA
Call Number EMAT @ emat @c:irua:205463 Serial 9119
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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.
Address
Corporate Author Thesis
Publisher (up) Place of Publication Editor
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
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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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Corporate Author Thesis
Publisher (up) 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 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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Corporate Author Thesis
Publisher (up) 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 Leinders, G.; Grendal, O.G.; Arts, I.; Bes, R.; Prozheev, I.; Orlat, S.; Fitch, A.; Kvashnina, K.; Verwerft, M.
Title Refinement of the uranium dispersion corrections from anomalous diffraction Type A1 Journal Article
Year 2024 Publication Journal of Applied Crystallography Abbreviated Journal J Appl Cryst
Volume 57 Issue 2 Pages 284-295
Keywords A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;
Abstract The evolution of the uranium chemical state in uranium compounds, principally in the oxides, is of concern in the context of nuclear fuel degradation under storage and repository conditions, and in accident scenarios. The U–O system shows complicated phase relations between single-valence uranium dioxide (UO<sub>2</sub>) and different mixed-valence compounds (<italic>e.g.</italic>U<sub>4</sub>O<sub>9</sub>, U<sub>3</sub>O<sub>7</sub>and U<sub>3</sub>O<sub>8</sub>). To try resolving the electronic structure associated with unique atomic positions, a combined application of diffraction and spectroscopic techniques, such as diffraction anomalous fine structure (DAFS), can be considered. Reported here is the application of two newly developed routines for assessing a DAFS data set, with the aim of refining the uranium X-ray dispersion corrections. High-resolution anomalous diffraction data were acquired from polycrystalline powder samples of UO<sub>2</sub>(containing tetravalent uranium) and potassium uranate (KUO<sub>3</sub>, containing pentavalent uranium) using synchrotron radiation in the vicinity of the U<italic>L</italic><sub>3</sub>edge (17.17 keV). Both routines are based on an iterative refinement of the dispersion corrections, but they differ in either using the intensity of a selection of reflections or doing a full-pattern (Rietveld method) refinement. The uranium dispersion corrections obtained using either method are in excellent agreement with each other, and they show in great detail the chemical shifts and differences in fine structure expected for tetravalent and pentavalent uranium. This approach may open new possibilities for the assessment of other, more complicated, materials such as mixed-valence compounds. Additionally, the DAFS methodology can offer a significant resource optimization because each data set contains both structural (diffraction) and chemical (spectroscopy) information, which can avoid the requirement to use multiple experimental stations at synchrotron sources.
Address
Corporate Author Thesis
Publisher (up) Place of Publication Editor
Language Wos 001208800100008 Publication Date 2024-04-01
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1600-5767 ISBN Additional Links UA library record; WoS full record
Impact Factor 6.1 Times cited Open Access
Notes FPS Economy, SF-CORMOD; Approved Most recent IF: 6.1; 2024 IF: 2.495
Call Number EMAT @ emat @c:irua:206011 Serial 9127
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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.
Address
Corporate Author Thesis
Publisher (up) 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
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.
Address
Corporate Author Thesis
Publisher (up) 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
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Author Cziraki, A.; Gerocs, I.; Fogarassy, B.; Van Tendeloo, G.; Sommer, F.; Bakonyi, I.
Title Study of the thermal decomposition of melt-quenched Ni-rich metastable bcc and amorphous Ni-Zr alloys Type A1 Journal article
Year 1998 Publication International journal of non-equilibrium processing Abbreviated Journal Int J Non-Equilib Pr
Volume 10 Issue 3-4 Pages 265-282
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract The phase transformation sequences during thermal decomposition are investigated for Ni-rich melt-quenched body-centred cubic (bcc) and amorphous Ni-Zr alloys. Transmission electron microscopy (TEM) and X-ray diffraction (XRD) are used to determine the structure of crystallization products occurring after heating the melt-spun ribbon samples to various degrees of the phase transformation process monitored by differential scanning calorimetry (DSC). A single DSC peak is observed for both the bcc and amorphous Ni(91)Zr(9) alloys and a two-step process is indicated by DSC for the amorphous Ni(90)Zr(10) alloy. In the bcc-Ni(91)Zr(9) alloy which is actually a Ni(Zr) solid solution phase, the phase transformation starts with the precipitation of Ni(5)Zr crystallites followed, after a sufficient depletion of the matrix in Zr, by the subsequent transformation of the bcc-Ni(Zr) lattice to face-centred cubic (fcc) Ni. In the amorphous alloy of the same composition, the final products are fcc-Ni and Ni(5)Zr but at intermediate stages of the phase transformation, bcc-Ni(Zr) crystallites also appear. In the a-Ni(90)Zr(10) alloy the first DSC peak corresponds to the formation of the bcc-Ni(Zr) phase which then decomposes (second DSC peak) to the equilibrium phases fcc-Ni and Ni(5)Zr. Thus, in addition to the previous observation of the formation of the metastable bcc-Ni(Zr) phase by rapid quenching from the melt, here we present evidence that this phase can form also after partial crystallization of metallic glasses of appropriate chemical compositions.
Address
Corporate Author Thesis
Publisher (up) AB Academic Publishers Place of Publication Bicester Editor
Language Wos 000075187300004 Publication Date 0000-00-00
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1368-9290 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor Times cited 2 Open Access
Notes Approved Most recent IF: NA
Call Number UA @ lucian @ c:irua:104005 Serial 3341
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Author Van Aert, S.; den Dekker, A.J.; van den Bos, A.; van Dyck, D.
Title Statistical experimental design for quantitative atomic resolution transmission electron microscopy Type H1 Book chapter
Year 2004 Publication Abbreviated Journal Adv Imag Elect Phys
Volume Issue Pages 1-164
Keywords H1 Book chapter; Electron microscopy for materials research (EMAT); Vision lab
Abstract
Address
Corporate Author Thesis
Publisher (up) Academic Press Place of Publication San Diego, Calif. Editor
Language Wos 000223226700001 Publication Date 2011-01-05
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1076-5670; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor Times cited 13 Open Access
Notes Approved Most recent IF: NA
Call Number UA @ lucian @ c:irua:47513 Serial 3156
Permanent link to this record
 
 
Author Biró, L.P.; Khanh, N.Q.; Horváth, Z.E.; Vértesy, Z.; Kocsonya, A.; Konya, Z.; Osváth, Z.; Koós, A.; Guylai, J.; Zhang, X.B.; Van Tendeloo, G.; Fonseca, A.; Nagy, J.B.
Title Catalyst traces after chemical purification in CVD grown carbon nanotubes Type P3 Proceeding
Year 2001 Publication Abbreviated Journal
Volume Issue Pages 183-186
Keywords P3 Proceeding; Electron microscopy for materials research (EMAT)
Abstract
Address
Corporate Author Thesis
Publisher (up) AIP Conference Proceedings Place of Publication s.l. Editor
Language Wos Publication Date 0000-00-00
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 Open Access
Notes Approved Most recent IF: NA
Call Number UA @ lucian @ c:irua:54778 Serial 288
Permanent link to this record
 
 
Author Nagy, J.B.; Fonseca, A.; Pierard, N.; Willems, I.; Bister, G.; Pirlot, C.; Demortier, A.; Delhalle, J.; Mekhalif, Z.; Niesz, K.; Bossuot, C.; Pirard, J.-P.; Biró, L.P.; Konya, Z.; Colomer, J.-F.; Van Tendeloo, G.; Kiricsi, I.
Title Large scale synthesis of carbon nanotubes and their composite materials Type P3 Proceeding
Year 2001 Publication Abbreviated Journal
Volume Issue Pages
Keywords P3 Proceeding; Electron microscopy for materials research (EMAT)
Abstract
Address
Corporate Author Thesis
Publisher (up) AIP Conference Proceedings Place of Publication s.l. Editor
Language Wos Publication Date 0000-00-00
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 @ lucian @ c:irua:54839 Serial 1781
Permanent link to this record
 
 
Author Vishwakarma, M.; Thota, N.; Karakulina, O.; Hadermann, J.; Mehta, B.R.
Title Role of graphene inter layer on the formation of the MoS2 – CZTS interface during growth Type P1 Proceeding
Year 2018 Publication (icc-2017) Abbreviated Journal
Volume Issue Pages
Keywords P1 Proceeding; Electron microscopy for materials research (EMAT)
Abstract The growth of MoS2 layer near the Mo/CZTS interface during sulphurization process can have an impact on back contact cell parameters (series resistance and fill factor) depending upon the thickness or quality of MoS2. This study reports the dependence of the thickness of interfacial MoS2 layer on the growth of graphene at the interface between molybdenum back contact and deposited CZTS layer. The graphene layer reduces the accumulation of Zn/ZnS, Sn/SnO2 and formation of pores near the MoS2-CZTS interface. The use of graphene as interface layer can be potentially useful for improving the quality of Mo/MoS2/CZTS interface.
Address
Corporate Author Thesis
Publisher (up) Amer inst physics Place of Publication Melville Editor
Language Wos 000436313003046 Publication Date 2018-05-09
Series Editor Series Title Abbreviated Series Title
Series Volume 1953 Series Issue Edition
ISSN 978-0-7354-1648-2; 0094-243x; 0094-243x ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor Times cited 1 Open Access OpenAccess
Notes ; The authors acknowledge support provided by DST project. M.V. acknowledges IIT Delhi for MHRD fellowship. Prof. B. R. Mehta acknowledges the support of the Schlumberger chair professorship. ; Approved Most recent IF: NA
Call Number UA @ lucian @ c:irua:153203 Serial 5126
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Author Gómez-Graña, S.; Goris, B.; Altantzis, T.; Fernández-López, C.; Carbó-Argibay, E.; Guerrero-Martínez, A.; Almora-Barrios, N.; López, N.; Pastoriza-Santos, I.; Pérez-Juste, J.; Bals, S.; Van Tendeloo, G.; Liz-Marzán, L.M.;
Title Au@Ag nanoparticles : halides stabilize {100} facets Type A1 Journal article
Year 2013 Publication The journal of physical chemistry letters Abbreviated Journal J Phys Chem Lett
Volume 4 Issue 13 Pages 2209-2216
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Seed-mediated growth is the most efficient methodology to control the size and shape of colloidal metal nanoparticles. In this process, the final nanocrystal shape is defined by the crystalline structure of the initial seed as well as by the presence of ligands and other additives that help to stabilize certain crystallographic facets. We analyze here the growth mechanism in aqueous solution of silver shells on presynthesized gold nanoparticles displaying various well-defined crystalline structures and morphologies. A thorough three-dimensional electron microscopy characterization of the morphology and internal structure of the resulting core-shell nanocrystals indicates that {100} facets are preferred for the outer silver shell, regardless of the morphology and crystallinity of the gold cores. These results are in agreement with theoretical analysis based on the relative surface energies of the exposed facets in the presence of halide ions.
Address
Corporate Author Thesis
Publisher (up) American Chemical Society Place of Publication Washington, D.C Editor
Language Wos 000321809500018 Publication Date 2013-06-20
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 9.353 Times cited 131 Open Access
Notes 267867 Plasmaquo; 246791 COUNTATOMS; 262348 ESMI; FWO Approved Most recent IF: 9.353; 2013 IF: 6.687
Call Number UA @ lucian @ c:irua:109811 Serial 204
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Author Berends, A.C.; Rabouw, F.T.; Spoor, F.C.M.; Bladt, E.; Grozema, F.C.; Houtepen, A.J.; Siebbeles, L.D.A.; de Donega, C.M.
Title Radiative and nonradiative recombination in CuInS2 nanocrystals and CuInS2-based core/shell nanocrystals Type A1 Journal article
Year 2016 Publication The journal of physical chemistry letters Abbreviated Journal J Phys Chem Lett
Volume 7 Issue 7 Pages 3503-3509
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Luminescent copper indium sulfide (CIS) nanocrystals are a potential solution to the toxicity issues associated with Cd- and Pb-based nanocrystals. However, the development of high-quality CIS nanocrystals has been complicated by insufficient knowledge of the electronic structure and of the factors that lead to luminescence quenching. Here we investigate the exciton decay pathways in CIS nanocrystals using time resolved photoluminescence and transient absorption spectroscopy. Core-only CIS nanocrystals with low quantum yield are compared to core/shell nanocrystals (CIS/ZnS and CIS/CdS) with higher quantum yield. Our measurements support the model of photoluminescence by radiative recombination of a conduction band electron with a localized hole. Moreover, we find that photoluminescence quenching in low-quantum-yield nanocrystals involves initially uncoupled decay pathways for the electron and hole. The electron decay pathway determines whether the exciton recombines radiatively or nonradiatively. The development of high-quality CIS nanocrystals should therefore focus on the elimination of electron traps.
Address
Corporate Author Thesis
Publisher (up) American Chemical Society Place of Publication Washington, D.C Editor
Language Wos 000382603300037 Publication Date 2016-08-23
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 9.353 Times cited 67 Open Access
Notes Approved Most recent IF: 9.353
Call Number UA @ lucian @ c:irua:135715 Serial 4308
Permanent link to this record
 
 
Author Sathiya, M.; Thomas, J.; Batuk, D.; Pimenta, V.; Gopalan, R.; Tarascon, J.-M.
Title Dual stabilization and sacrificial effect of Na2CO3 for increasing capacities of Na-Ion cells based on P2-NaxMO2 electrodes Type A1 Journal article
Year 2017 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 29 Issue 14 Pages 5948-5956
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Sodium ion battery technology is gradually advancing and can be viewed as a viable alternative to lithium ion batteries in niche applications. One of the promising positive electrode candidates is P2 type layered sodium transition metal oxide, which offers attractive sodium ion conductivity. However, the reversible capacity of P2 phases is limited by the inability to directly synthesize stoichiometric compounds with a sodium to transition metal ratio equal to 1. To alleviate this issue, we report herein the in situ synthesis of P2-NaxO2 (x <= 0.7, M = transition metal ions)-Na2CO3 composites. We find that sodium carbonate acts as a sacrificial salt, providing Na+ ion to increase the reversible capacity of the P2 phase in sodium ion full cells, and also as a useful additive that stabilizes the formation of P2 over competing P3 phases. We offer a new phase diagram for tuning the synthesis of the P2 phase under various experimental conditions and demonstrate, by in situ XRD analysis, the role of Na2CO3 as a sodium reservoir in full sodium ion cells. These results provide insights into the practical use of P2 layered materials and can be extended to a variety of other layered phases.
Address
Corporate Author Thesis
Publisher (up) American Chemical Society Place of Publication Washington, D.C Editor
Language Wos 000406573200026 Publication Date 2017-07-03
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.466 Times cited 26 Open Access Not_Open_Access
Notes ; M.S., J.T., and R.G. acknowledge the financial support received from the Department of Science and Technology (DST-SERC), Government of India under the funding from the TRC Grant Agreement No. AI/1/65/ARCI/2014. The authors are thankful to Dr. Sundararajan, Chairman, TRC and Dr. G. Padmanabham, Director, ARCI for helpful discussions. Initial microscopy analysis by Dr. M. B. Sahana, Dr. Prabu, and Mr. Ravi Gautham of ARCI are greatly acknowledged. The elemental analysis by Dr. Domitille Giaume, IRCP – ENSCP, Chimie Paris Tech, Paris is greatly acknowledged. ; Approved Most recent IF: 9.466
Call Number UA @ lucian @ c:irua:145759 Serial 4740
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Author Yang, C.; Laberty-Robert, C.; Batuk, D.; Cibin, G.; Chadwick, A.V.; Pimenta, V.; Yin, W.; Zhang, L.; Tarascon, J.-M.; Grimaud, A.
Title Phosphate ion functionalization of perovskite surfaces for enhanced oxygen evolution reaction Type A1 Journal article
Year 2017 Publication The journal of physical chemistry letters Abbreviated Journal J Phys Chem Lett
Volume 8 Issue 15 Pages 3466-3472
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Recent findings revealed that surface oxygen can participate in the oxygen evolution reaction (OER) for the most active catalysts, which eventually triggers a new mechanism for which the deprotonation of surface intermediates limits the OER activity. We propose in this work a “dual strategy” in which tuning the electronic properties of the oxide, such as La1-xSrxCoO3-delta, can be dissociated from the use of surface functionalization with phosphate ion groups (P-i) that enhances the interfacial proton transfer. Results show that the P-i functionalized La0.5Sr0.5CoO3-delta gives rise to a significant enhancement of the OER activity when compared to La0.5Sr0.5Co3-delta and LaCoO3. We further demonstrate that the P-i surface functionalization selectivity enhances the activity when the OER kinetics is limited by the proton transfer. Finally, this work suggests that tuning the catalytic activity by such a “dual approach” may be a new and largely unexplored avenue for the design of novel high-performance catalysts.
Address
Corporate Author Thesis
Publisher (up) American Chemical Society Place of Publication Washington, D.C Editor
Language Wos 000407191300003 Publication Date 2017-07-07
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 9.353 Times cited 31 Open Access OpenAccess
Notes ; C.Y., J.-M.T., D.B., and A.G. acknowledge funding from the European Research Council (ERC) (FP/2014)/ERC Grant-Project 670116-ARPEMA. We acknowledge Diamond Light Source for time awarded to the Energy Materials BAG on Beamline B18, under Proposal sp12559. ; Approved Most recent IF: 9.353
Call Number UA @ lucian @ c:irua:145730 Serial 4747
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Author Verchenko, V.Y.; Wei, Z.; Tsirlin, A.A.; Callaert, C.; Jesche, A.; Hadermann, J.; Dikarev, E.V.; Shevelkov, A.V.
Title Crystal growth of the Nowotny chimney ladder phase Fe2Ge3 : exploring new Fe-based narrow-gap semiconductor with promising thermoelectric performance Type A1 Journal article
Year 2017 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 29 Issue 23 Pages 9954-9963
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract <script type='text/javascript'>document.write(unpmarked('A new synthetic approach based on chemical transport reactions has been introduced to obtain the Nowotny chimney ladder phase Fe2Ge3 in the form of single crystals and polycrystalline powders. The single crystals possess the stoichiometric composition and the commensurate chimney ladder structure of the Ru2Sn3 type in contrast to the polycrystalline samples that are characterized by a complex microstructure. In compliance with the 18-n electron counting rule formulated for T-E intermetallics, electronic structure calculations reveal a narrow-gap semiconducting behavior of Fe2Ge3 favorable for high thermoelectric performance. Measurements of transport and thermoelectric properties performed on the polycrystalline samples confirm the formation of a narrow band gap of similar to 30 meV and reveal high absolute values of the Seebeck coefficient at elevated temperatures. Low glass-like thermal conductivity is observed in a wide temperature range that might be caused by the underlying complex microstructure.'));
Address
Corporate Author Thesis
Publisher (up) American Chemical Society Place of Publication Washington, D.C Editor
Language Wos 000418206600013 Publication Date 2017-11-14
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 9.466 Times cited 11 Open Access OpenAccess
Notes ; The authors thank Dr. Sergey Kazakov and Oleg Tyablikov for their help with the PXRD experiments. V.Y.V. appreciates the help of Dr. Sergey Dorofeev in provision and handling of the Mo(CO)<INF>6</INF> reagent. The work is supported by the Russian Science Foundation, Grant No. 17-13-01033. V.Y.V. appreciates the support from the European Regional Development Fund, Project No. TK134. A.A.T. acknowledges financial support by the Federal Ministry for Education and Research under the Sofia Kovalevskaya Award of the Alexander von Humboldt Foundation. E.V.D. thanks the National Science Foundation, Grant No. CHE-1152441. C.C. acknowledges the support from the University of Antwerp through the BOF Grant No. 31445. ; Approved Most recent IF: 9.466
Call Number UA @ lucian @ c:irua:148531 Serial 4869
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Author Arias-Duque, C.; Bladt, E.; Munoz, M.A.; Hernandez-Garrido, J.C.; Cauqui, M.A.; Rodriguez-Izquierdo, J.M.; Blanco, G.; Bals, S.; Calvino, J.J.; Perez-Omil, J.A.; Yeste, M.P.
Title Improving the redox response stability of ceria-zirconia nanocatalysts under harsh temperature conditions Type A1 Journal article
Year 2017 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 29 Issue 29 Pages 9340-9350
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract <script type='text/javascript'>document.write(unpmarked('By depositing ceria on the surface of yttrium stabilized zirconia (YSZ) nanocrystals and further activation under high-temperature reducing conditions, a 13% mol. CeO2/YSZ catalyst structured as subnanometer thick, pyrochlore-type, ceria-zirconia islands has been prepared. This nanostructured catalyst depicts not only high oxygen storage capacity (OSC) values but, more importantly, an outstandingly stable redox response upon oxidation and reduction treatments at very high temperatures, above 1000 degrees C. This behavior largely improves that observed on conventional ceria-zirconia solid solutions, not only of the same composition but also of those with much higher molar cerium contents. Advanced scanning transmission electron microscopy (STEM-XEDS) studies have revealed as key not only to detect the actual state of the lanthanide in this novel nanocatalyst but also to rationalize its unusual resistance to redox deactivation at very high temperatures. In particular, high-resolution X-ray dispersive energy studies have revealed the presence of unique bilayer ceria islands on top of the surface of YSZ nanocrystals, which remain at surface positions upon oxidation and reduction treatments up to 1000 degrees C. Diffusion of ceria into the bulk of these crystallites upon oxidation at 1100 degrees C irreversibly deteriorates both the reducibility and OSC of this nanostructured catalyst.'));
Address
Corporate Author Thesis
Publisher (up) American Chemical Society Place of Publication Washington, D.C Editor
Language Wos 000415911600047 Publication Date 2017-10-10
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.466 Times cited 20 Open Access OpenAccess
Notes ; Financial support from MINECO/FEDER (Project ref: MAT2013-40823-R), Junta de Andalucia (FQM334 and FQM110), and EU FP7 (ESTEEM2) are acknowledged. E.B. and S.B. acknowledges financial support from European Research Council (ERC- Starting Grant #33S078-COLOURA-TOM). J.C.H.-G. acknowledges support from the Ramon y Cajal Fellowships Program of MINECO (RYC-2012-10004). ; Approved Most recent IF: 9.466
Call Number UA @ lucian @ c:irua:147706UA @ admin @ c:irua:147706 Serial 4880
Permanent link to this record
 
 
Author Savina, A.A.; Morozov, V.A.; Buzlukov, A.L.; Arapova, I.Y.; Stefanovich, S.Y.; Baklanova, Y.V.; Denisova, T.A.; Medvedeva, N.I.; Bardet, M.; Hadermann, J.; Lazoryak, B.I.; Khaikina, E.G.
Title New solid electrolyte Na9Al(MoO4)6 : structure and Na+ ion conductivity Type A1 Journal article
Year 2017 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 29 Issue 20 Pages 8901-8913
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract <script type='text/javascript'>document.write(unpmarked('Solid electrolytes are important materials with a wide range of technological applications. This work reports the crystal structure and electrical properties of a new solid electrolyte Na9Al(MoO4)(6). The monoclinic Na9Al(MoO4)(6) consists of isolated polyhedral, [Al(MoO4)(6)](9-) clusters composed of a central AlO6 octahedron sharing vertices with six MoO4 tetrahedra to form a three-dimensional framework. The AlO6 octahedron also shares edges with one NalO(6) octahedron and two Na2O(6) octahedra. Na3-Na5 atoms are located in the framework cavities. The structure is related to that of sodium ion conductor II-Na3Fe2(AsO4)(3). High-temperature conductivity measurements revealed that the conductivity (sigma) of Na9Al(MoO4)(6) at 803 K equals 1.63 X 10(-2) S cm(-1). The temperature behavior of the Na-23 and Al-27 nuclear magnetic resonance spectra and the spin-lattice relaxation rates of the Na-23 nuclei indicate the presence of fast Na+ ion diffusion in the studied compound. At T\u003C490 K, diffusion occurs by means of Na+ ion jumps exclusively through the sublattice of Na3-Na5 positions, whereas Na1 and Na2 become involved in the diffusion processes (through chemical exchange with the Na3-Na5 sublattice) only at higher temperatures.'));
Address
Corporate Author Thesis
Publisher (up) American Chemical Society Place of Publication Washington, D.C Editor
Language Wos 000413884900037 Publication Date 2017-09-26
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.466 Times cited 13 Open Access OpenAccess
Notes ; The research was performed within the state assignment of FASO of Russia (Themes 01201463330, A16-116122810214-9, and 0339-2016-0007), supported in part by the Russian Foundation for Basic Research (Projects 16-03-00510, 16-03-00164, and 17-03-00333). ; Approved Most recent IF: 9.466
Call Number UA @ lucian @ c:irua:147432 Serial 4886
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Author Pimenta, V.; Sathiya, M.; Batuk, D.; Abakumov, A.M.; Giaume, D.; Cassaignon, S.; Larcher, D.; Tarascon, J.-M.
Title Synthesis of Li-Rich NMC : a comprehensive study Type A1 Journal article
Year 2017 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 29 Issue 23 Pages 9923-9936
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract <script type='text/javascript'>document.write(unpmarked('Li-rich NMC are considered nowadays as one of the most promising candidates for high energy density cathodes. One significant challenge is nested in adjusting their synthesis conditions to reach optimum electrochemical performance, but no consensus has been reached yet on the ideal synthesis protocol. Herein, we revisited the elaboration of Li-rich NMC electrodes by focusing on the science involved through each synthesis steps using carbonate Ni0.1625Mn0.675Co0.1625CO3 precursor coprecipitation combined with solid state synthesis. We demonstrated the effect of precursors concentration on the kinetics of the precipitation reaction and provided clues to obtain spherically agglomerated NMC carbonates of different sizes. Moreover, we highlighted the strong impact of the Li2CO3/NMC carbonate ratio on the morphology and particles size of Li-rich NMC and subsequently on their electrochemical performance. Ratio of 1.35 was found to reproducibly give the best performance with namely a first discharge capacity of 269 mAh g(-1) and capacity retention of 89.6% after 100 cycles. We hope that our results, which reveal how particle size, morphology, and phase composition affect the materials electrochemical performance, will help in reconciling literature data while providing valuable fundamental information for up scaling approaches.'));
Address
Corporate Author Thesis
Publisher (up) American Chemical Society Place of Publication Washington, D.C Editor
Language Wos 000418206600010 Publication Date 2017-11-08
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.466 Times cited 23 Open Access Not_Open_Access
Notes ; The authors acknowledge the French Research Network on Electrochemical Energy Storage (RS2E). V.P and J.-M.T. acknowledges funding from the European Research Council (ERC) (FP/2014)/ERC Grant-Project 670116-ARPEMA. The authors are thankful to Dr. G. Rousse for the help on Rietveld refinements. ; Approved Most recent IF: 9.466
Call Number UA @ lucian @ c:irua:148530 Serial 4899
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Author Berends, A.C.; van der Stam, W.; Hofmann, J.P.; Bladt, E.; Meeldijk, J.D.; Bals, S.; de Donega, C.M.
Title Interplay between surface chemistry, precursor reactivity, and temperature determines outcome of ZnS shelling reactions on CuInS2 nanocrystals Type A1 Journal article
Year 2018 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 30 Issue 30 Pages 2400-2413
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract ZnS shelling of I-III-VI(2 )nanocrystals (NCs) invariably leads to blue-shifts in both the absorption and photoluminescence spectra. These observations imply that the outcome of ZnS shelling reactions on I-III-VI2 colloidal NCs results from a complex interplay between several processes taking place in solution, at the surface of, and within the seed NC. However, a fundamental understanding of the factors determining the balance between these different processes is still lacking. In this work, we address this need by investigating the impact of precursor reactivity, reaction temperature, and surface chemistry (due to the washing procedure) on the outcome of ZnS shelling reactions on CuInS2 NCs using a seeded growth approach. We demonstrate that low reaction temperatures (150 degrees C) favor etching, cation exchange, and alloying regardless of the precursors used. Heteroepitaxial shell overgrowth becomes the dominant process only if reactive S- and Zn-precursors (S-ODE/OLAM and ZnI2 ) and high reaction temperatures (210 degrees C) are used, although a certain degree of heterointerfacial alloying still occurs. Remarkably, the presence of residual acetate at the surface of CIS seed NCs washed with ethanol is shown to facilitate heteroepitaxial shell overgrowth, yielding for the first time CIS/ZnS core/shell NCs displaying red-shifted absorption spectra, in agreement with the spectral shifts expected for a type-I band alignment. The insights provided by this work pave the way toward the design of improved synthesis strategies to CIS/ZnS core/shell and alloy NCs with tailored elemental distribution profiles, allowing precise tuning of the optoelectronic properties of the resulting materials.
Address
Corporate Author Thesis
Publisher (up) American Chemical Society Place of Publication Washington, D.C Editor
Language Wos 000430023700027 Publication Date 2018-03-25
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.466 Times cited 85 Open Access OpenAccess
Notes ; Annelies van der Bok is gratefully acknowledged for performing the ICP measurements. A.C.B. and C.d.M.D. acknowledge financial support from the division of Chemical Sciences (CW) of The Netherlands Organization for Scientific Research (NWO) under Grant No. ECHO.712.014.001. S.B. and E.B. acknowledge financial support from European Research Council (ERC Starting Grant No. 335078-COLOURATOMS). ; Ecas_Sara Approved Most recent IF: 9.466
Call Number UA @ lucian @ c:irua:150772UA @ admin @ c:irua:150772 Serial 4972
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Author Grimaud, A.; Iadecola, A.; Batuk, D.; Saubanere, M.; Abakumov, A.M.; Freeland, J.W.; Cabana, J.; Li, H.; Doublet, M.-L.; Rousse, G.; Tarascon, J.-M.
Title Chemical activity of the peroxide/oxide redox couple : case study of Ba5Ru2O11 in aqueous and organic solvents Type A1 Journal article
Year 2018 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 30 Issue 11 Pages 3882-3893
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The finding that triggering the redox activity of oxygen ions within the lattice of transition metal oxides can boost the performances of materials used in energy storage and conversion devices such as Li-ion batteries or oxygen evolution electrocatalysts has recently spurred intensive and innovative research in the field of energy. While experimental and theoretical efforts have been critical in understanding the role of oxygen nonbonding states in the redox activity of oxygen ions, a clear picture of the redox chemistry of the oxygen species formed upon this oxidation process is still missing. This can be, in part, explained by the complexity in stabilizing and studying these species once electrochemically formed. In this work, we alleviate this difficulty by studying the phase Ba5Ru2O11, which contains peroxide O-2(2-) groups, as oxygen evolution reaction electrocatalyst and Li-ion battery material. Combining physical characterization and electrochemical measurements, we demonstrate that peroxide groups can easily be oxidized at relatively low potential, leading to the formation of gaseous dioxygen and to the instability of the oxide. Furthermore, we demonstrate that, owing to the stabilization at high energy of peroxide, the high-lying energy of the empty sigma* antibonding O-O states limits the reversibility of the electrochemical reactions when the O-2(2-)/O2- redox couple is used as redox center for Li-ion battery materials or as OER redox active sites. Overall, this work suggests that the formation of true peroxide O-2(2-) states are detrimental for transition metal oxides used as OER catalysts and Li-ion battery materials. Rather, oxygen species with O-O bond order lower than 1 would be preferred for these applications.
Address
Corporate Author Thesis
Publisher (up) American Chemical Society Place of Publication Washington, D.C Editor
Language Wos 000435416600038 Publication Date 2018-05-21
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.466 Times cited 2 Open Access Not_Open_Access
Notes ; We thank S. Belin of the ROCK beamline (financed by the French National Research Agency (ANR) as a part of the “Investissements d'Avenir” program, reference: ANR-10-EQPX-45; proposal no. 20160095) of synchrotron SOLEIL for her assistance during XAS measurements. Authors would also like to thank V. Nassif for her assistance on the D1B beamline. A.G, G.R, and J.-M.T. acknowledge funding from the European Research Council (ERC) (FP/2014)/ERC Grant Project 670116-ARPEMA. ; Approved Most recent IF: 9.466
Call Number UA @ lucian @ c:irua:151980 Serial 5016
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