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Author |
Zankowski, S.P.; Van Hoecke, L.; Mattelaer, F.; de Raedt, M.; Richard, O.; Detavernier, C.; Vereecken, P.M. |
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Title |
Redox layer deposition of thin films of MnO2 on nanostructured substrates from aqueous solutions |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
Chemistry of materials |
Abbreviated Journal |
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Volume |
31 |
Issue |
13 |
Pages |
4805-4816 |
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Keywords |
A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL) |
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Abstract |
In this work, we report a new method for depositing thin films of MnO2 on planar and complex nanostructured surfaces, with high precision and conformality. The method is based on repeating cycles of adsorption of an unsaturated alcohol on a surface, followed by its oxidation with aqueous KMnO4 and formation of thin, solid MnO2. The amount of manganese oxide formed in each cycle is limited by the quantity of the adsorbed alcohol; thus, the growth exhibits the self-limiting characteristics of atomic layer deposition (ALD). Contrary to the typical ALD, however, the new redox layer deposition is performed in air, at room temperature, using common chemicals and simple laboratory glassware, which greatly reduces its cost and complexity. We also demonstrate application of the method for the fabrication of a nanostructured MnO2/Ni electrode, which was not possible with thermal ALD because of the rapid decomposition of the gaseous precursor on the high surface-area substrate. Thanks to its simplicity, the conformal deposition of MnO2 can be easily upscaled and thus exploited for its numerous (electro)chemical applications. |
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Wos |
000475408400021 |
Publication Date |
2019-06-12 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756; 1520-5002 |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
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Times cited |
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Open Access |
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Approved |
no |
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Call Number |
UA @ admin @ c:irua:161225 |
Serial |
8465 |
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Permanent link to this record |
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Author |
Zaikina, J.V.; Kovnir, K.A.; Sobolev, A.N.; Presniakov, I.A.; Kytin, V.G.; Kulbachinskii, V.A.; Olenev, A.V.; Lebedev, O.I.; Van Tendeloo, G.; Dikarev, E.V.; Shevelkov, A.V. |
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Title |
Highly disordered crystal structure and thermoelectric properties of Sn3P4 |
Type |
A1 Journal article |
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Year |
2008 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
20 |
Issue |
7 |
Pages |
2476-2483 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Place of Publication |
Washington, D.C. |
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Wos |
000254605000011 |
Publication Date |
2008-03-07 |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756;1520-5002; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
33 |
Open Access |
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Notes |
Fwo |
Approved |
Most recent IF: 9.466; 2008 IF: 5.046 |
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Call Number |
UA @ lucian @ c:irua:69999 |
Serial |
1470 |
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Permanent link to this record |
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Author |
Xia, C.; Pedrazo-Tardajos, A.; Wang, D.; Meeldijk, J.D.; Gerritsen, H.C.; Bals, S.; de Donega, C.M. |
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Title |
Seeded growth combined with cation exchange for the synthesis of anisotropic Cu2-xS/ZnS, Cu2-xS, and CuInS2 nanorods |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Chemistry of materials |
Abbreviated Journal |
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Volume |
33 |
Issue |
1 |
Pages |
102-116 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Colloidal copper(I) sulfide (Cu2-xS) nanocrystals (NCs) have attracted much attention for a wide range of applications because of their unique optoelectronic properties, driving scientists to explore the potential of using Cu2-xS NCs as seeds in the synthesis of heteronanocrystals to achieve new multifunctional materials. Herein, we developed a multistep synthesis strategy toward Cu2-xS/ZnS heteronanorods. The Janus-type Cu2-xS/ZnS heteronanorods are obtained by the injection of hexagonal high-chalcocite Cu2-xS seed NCs in a hot zinc oleate solution in the presence of suitable surfactants, 20 s after the injection of sulfur precursors. The Cu2-xS seed NCs undergo rapid aggregation and coalescence in the first few seconds after the injection, forming larger NCs that act as the effective seeds for heteronucleation and growth of ZnS. The ZnS heteronucleation occurs on a single (100) facet of the Cu2-xS seed NCs and is followed by fast anisotropic growth along a direction that is perpendicular to the c-axis, thus leading to Cu2-xS/ZnS Janus-type heteronanorods with a sharp heterointerface. Interestingly, the high-chalcocite crystal structure of the injected Cu2-xS seed NCs is preserved in the Cu2-xS segments of the heteronanorods because of the highthermodynamic stability of this Cu2-xS phase. The Cu2-xS/ZnS heteronanorods are subsequently converted into single-component Cu2-xS and CuInS2 nanorods by postsynthetic topotactic cation exchange. This work expands the possibilities for the rational synthesis of colloidal multicomponent heteronanorods by allowing the design principles of postsynthetic heteroepitaxial seeded growth and nanoscale cation exchange to be combined, yielding access to a plethora of multicomponent heteronanorods with diameters in the quantum confinement regime. |
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Wos |
000610984700009 |
Publication Date |
2020-12-28 |
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Abbreviated Series Title |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
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Times cited |
10 |
Open Access |
OpenAccess |
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Notes |
C.X. acknowledges China Scholarship Council (CSC) for the financial support (grant number 201406330055). C.d.M.D. acknowledges funding from the European Commission for access to the EMAT facilities (grant number EUSMI E180900184). D.W. acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (grant 894254 SuprAtom). S.B. acknowledges support by means of the ERC Consolidator grant no. 815128 REALNANO. The authors thank Donglong Fu for XRD measurements.; sygma |
Approved |
Most recent IF: NA |
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Call Number |
UA @ admin @ c:irua:176587 |
Serial |
6732 |
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Permanent link to this record |
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Author |
Wolf, D.; Rodriguez, L.A.; Béché, A.; Javon, E.; Serrano, L.; Magen, C.; Gatel, C.; Lubk, A.; Lichte, H.; Bals, S.; Van Tendeloo, G.; Fernández-Pacheco, A.; De Teresa, J.M.; Snoeck, E. |
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Title |
3D Magnetic Induction Maps of Nanoscale Materials Revealed by Electron Holographic Tomography |
Type |
A1 Journal article |
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Year |
2015 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
27 |
Issue |
27 |
Pages |
6771-6778 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
The investigation of three-dimensional (3D) ferromagnetic nanoscale materials constitutes one of the key research areas of the current magnetism roadmap, and carries great potential to impact areas such as data storage, sensing and biomagnetism. The properties of such nanostructures are closely connected with their 3D magnetic nanostructure, making their determination highly valuable. Up to now, quantitative 3D maps providing both the internal magnetic and electric configuration of the same specimen with high spatial resolution are missing. Here, we demonstrate the quantitative 3D reconstruction of the dominant axial component of the magnetic induction and electrostatic potential within a cobalt nanowire (NW) of 100 nm in diameter with spatial resolution below 10 nanometers by applying electron holographic tomography. The tomogram was obtained using a dedicated TEM sample holder for acquisition, in combination with advanced alignment and tomographic reconstruction routines. The powerful approach presented here is widely applicable to a broad range of 3D magnetic nanostructures and may trigger the progress of novel spintronic non-planar nanodevices. |
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Wos |
000362920700037 |
Publication Date |
2015-09-08 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756;1520-5002; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
50 |
Open Access |
OpenAccess |
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Notes |
This work was supported by the European Union under the Seventh Framework Program under a contract for an Inte-grated Infrastructure Initiative Reference 312483-ESTEEM2. S.B. and A.B. gratefully acknowledge funding by ERC Starting grants number 335078 COLOURATOMS and number 278510 VORTEX. AF-P acknowledges an EPSRC Early Career fellowship and support from the Winton Foundation. E.S., C.G. and L.A. R. acknowledge the French ANR program for support though the project EMMA.; esteem2jra4; ECASJO;; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 9.466; 2015 IF: 8.354 |
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Call Number |
c:irua:129180 c:irua:129180 c:irua:129180 |
Serial |
3950 |
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Permanent link to this record |
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Author |
Wang, Y.; Sentosun, K.; Li, A.; Coronado-Puchau, M.; Sánchez-Iglesias, A.; Li, S.; Su, X.; Bals, S.; Liz-Marzán, L.M. |
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Title |
Engineering Structural Diversity in Gold Nanocrystals by Ligand-Mediated Interface Control |
Type |
A1 Journal article |
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Year |
2015 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
27 |
Issue |
27 |
Pages |
8032-8040 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Surface and interface control is fundamentally important for crystal growth engineering, catalysis, surface enhanced spectroscopies, and self-assembly, among other processes and applications. Understanding the role of ligands in regulating surface properties of plasmonic metal nanocrystals during growth has received considerable attention. However, the underlying mechanisms and the diverse functionalities of ligands are yet to be fully addressed. In this contribution,
we report a systematic study of ligand-mediated interface control in seeded growth of gold nanocrystals, leading to diverse and exotic nanostructures with an improved surface enhanced Raman scattering (SERS) activity. Three dimensional transmission electron microscopy (3D TEM) revealed an intriguing gold shell growth process mediated by the bifunctional ligand 1,4-benzenedithiol (BDT), which leads to a unique crystal growth mechanism as compared to other ligands, and subsequently to the concept of interfacial energy control mechanism. Volmer-Weber growth mode was proposed to be responsible for BDT-mediated seeded growth, favoring the strongest interfacial energy and generating an asymmetric island growth pathway with internal crevices/gaps. This additionally favors incorporation of BDT at the plasmonic nanogaps, thereby generating strong SERS activity with a maximum efficiency for a core-semishell configuration obtained along seeded growth. Numerical modeling was used to explain this observation. Interestingly, the same strategy can be used to engineer the structural diversity of this system, by using gold nanoparticle seeds with various sizes and shapes, and varying the [Au3+]/[Au0] ratio. This rendered a series of diverse and exotic plasmonic nanohybrids such as semishell-coated gold nanorods, with embedded Raman-active tags and Janus surface with distinct surface functionalities.
These would greatly enrich the plasmonic nanostructure toolbox for various studies and applications such as anisotropic nanocrystal engineering, SERS, and high-resolution Raman bioimaging or nanoantenna devices. |
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Wos |
000366223200023 |
Publication Date |
2015-10-09 |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756;1520-5002; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
18 |
Open Access |
OpenAccess |
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Notes |
The authors thank Bart Goris for his help with electron tomography. This work was funded by the European Commission (Grant #310445-2, SAVVY). The authors acknowledge financial support from European Research Council (ERC Advanced Grant # 267867- PLASMAQUO, ERC Starting Grant #335078-COLOURATOMS). The authors also appreciate financial support from the European Union under the Seventh Framework Program (Integrated Infrastructure Initiative N. 262348 European Soft Matter Infrastructure, ESMI). Wang Y. and Su X. would like to acknowledge the Agency for Science, Technology and Research (A*STAR), Singapore, for the financial support under the Grant JCO 14302FG096. M. C.-P. acknowledges an FPU scholarship from the Spanish Ministry of Education, Culture and Sports.; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 9.466; 2015 IF: 8.354 |
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Call Number |
c:irua:129598 c:irua:129598 |
Serial |
3972 |
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Permanent link to this record |
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Author |
Volkova, N.E.; Lebedev, O.I.; Gavrilova, L.Y.; Turner, S.; Gauquelin, N.; Seikh, M.M.; Caignaert, V.; Cherepanov, V.A.; Raveau, B.; Van Tendeloo, G. |
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Title |
Nanoscale ordering in oxygen deficient quintuple perovskite Sm2-\epsilonBa3+\epsilonFe5O15-\delta : implication for magnetism and oxygen stoichiometry |
Type |
A1 Journal article |
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Year |
2014 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
26 |
Issue |
21 |
Pages |
6303-6310 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
The investigation of the system SmBaFe-O in air has allowed an oxygen deficient perovskite Sm2-epsilon Ba3+epsilon Fe5O15-delta (delta = 0.75, epsilon = 0.125) to be synthesized. In contrast to the XRPD pattern which gives a cubic symmetry (a(p) = 3.934 angstrom), the combined HREM/EELS study shows that this phase is nanoscale ordered with a quintuple tetragonal cell, a(p) X a(p) X 5(ap). The nanodomains exhibit a unique stacking sequence of the A-site cationic layers along the crystallographic c-axis, namely SmBaBa/SmBa/SmBaSm, and are chemically twinned in the three crystallographic directions. The nanoscale ordering of this perovskite explains its peculiar magnetic properties on the basis of antiferromagnetic interactions with spin blockade at the boundary between the nanodomains. The variation of electrical conductivity and oxygen content of this oxide versus temperature suggest potential SOFC applications. They may be related to the particular distribution of oxygen vacancies in the lattice and to the 3d(5)(L) under bar configuration of iron. |
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Wos |
000344905600029 |
Publication Date |
2014-10-07 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756;1520-5002; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
16 |
Open Access |
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Notes |
The UrFU authors were financially supported by the Ministry of Education and Science of Russian Federation (project N 4.1039.2014/K) and by UrFU under the Framework Program of development of UrFU through the «Young scientists UrFU» competition. The CRISMAT authors gratefully acknowledge the EC, the CNRS and the French Minister of Education and Research for financial support through their Research, Strategic and Scholarship programs. This work was supported by funding from the European Research Council under the Seventh Framework Program (FP7), ERC grant N°246791 – COUNTATOMS. S.T. gratefully acknowledges the fund for scientific research Flanders for a post-doctoral fellowship and for financial support under contract number G004413N. N.G. acknowledges funding from the European Research Council under the 7th Framework Program (FP7), ERC starting grant number 278510 – VORTEX; ECASJO_; |
Approved |
Most recent IF: 9.466; 2014 IF: 8.354 |
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Call Number |
UA @ lucian @ c:irua:122137 |
Serial |
2269 |
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Permanent link to this record |
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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. |
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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 |
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Year |
2017 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
29 |
Issue |
23 |
Pages |
9954-9963 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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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.')); |
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Publisher |
American Chemical Society |
Place of Publication |
Washington, D.C |
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Wos |
000418206600013 |
Publication Date |
2017-11-14 |
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Series Editor |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
11 |
Open Access |
OpenAccess |
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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 |
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Call Number |
UA @ lucian @ c:irua:148531 |
Serial |
4869 |
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Permanent link to this record |
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Author |
Vandemeulebroucke, D.; Batuk, M.; Hajizadeh, A.; Wastiaux, M.; Roussel, P.; Hadermann, J. |
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Title |
Incommensurate Modulations and Perovskite Growth in LaxSr2–xMnO4−δAffecting Solid Oxide Fuel Cell Conductivity |
Type |
A1 Journal article |
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Year |
2024 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem. Mater. |
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Volume |
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Issue |
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Pages |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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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. |
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Language |
English |
Wos |
001174840900001 |
Publication Date |
2024-02-20 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
8.6 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
Universiteit Antwerpen, BOF TOP 38689 ; Fonds Wetenschappelijk Onderzoek, I003218N ; European Commission NanED, 956099 ; |
Approved |
Most recent IF: 8.6; 2024 IF: 9.466 |
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Call Number |
EMAT @ emat @c:irua:204354 |
Serial |
8997 |
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Permanent link to this record |
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Author |
Van Tendeloo, L.; Wangermez, W.; Vandekerkhove, A.; Willhammar, T.; Bals, S.; Maes, A.; Martens, J.A.; Kirschhock, C.E.A.; Breynaert, E. |
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Title |
Postsynthetic high-alumina zeolite crystal engineering in organic free hyper-alkaline media |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
29 |
Issue |
29 |
Pages |
629-638 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Postsynthetic modification of high -alumina zeolites in hyper alkaline media can be tailored toward alteration of framework topology, crystal size and morphology, or desired Si/A1 ratio. FAU, EMT, MAZ, KFI, HEU, and LTA starting materials were treated with 1.2 M MOH (M = Na, K, RE, or Cs), leading to systematic ordered porosity or fully transformed frameworks with new topology and adjustable Si/Al ratio. In addition to the versatility of this tool for zeolite crystal engineering, these alterations improve understanding of the crystal chemistry. Such knowledge can guide further development in zeolite crystal engineering. Postsynthetic alteration also provides insight on the long-term stability of aluminosilicate zeolites that are used as a sorption sink in concrete -based waste disposal facilities in harsh alkaline conditions. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
American Chemical Society |
Place of Publication |
Washington, D.C |
Editor |
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Language |
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Wos |
000392891700021 |
Publication Date |
2016-12-20 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
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Edition |
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|
|
ISSN |
0897-4756 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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|
Impact Factor |
9.466 |
Times cited |
16 |
Open Access |
OpenAccess |
|
|
Notes |
; This work was supported by long-term structural funding by the Flemish Government (Methusalem grant of Prof. J. Martens) and by ONDRAF/NIRAS, the Belgian Agency for Radioactive Waste and Fissile Materials, as part of the program on surface disposal of Belgian Category A waste. The Belgian government is acknowledged for financing the interuniversity poles of attraction (IAP-PAI). S.B. acknowledges financial support from European Research Council (ERC Advanced Grant No. 24691-COUNTATOMS, ERC Starting Grant No. 335078-COLOURATOMS). ; Ecas_Sara |
Approved |
Most recent IF: 9.466 |
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|
Call Number |
UA @ lucian @ c:irua:152674UA @ admin @ c:irua:152674 |
Serial |
5145 |
|
Permanent link to this record |
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Author |
van der Stam, W.; Gradmann, S.; Altantzis, T.; Ke, X.; Baldus, M.; Bals, S.; de Mello Donega, C. |
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|
Title |
Shape Control of Colloidal Cu2-x S Polyhedral Nanocrystals by Tuning the Nucleation Rates |
Type |
A1 Journal article |
|
Year |
2016 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
|
|
Volume |
28 |
Issue |
28 |
Pages |
6705-6715 |
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|
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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|
Abstract |
Synthesis protocols for colloidal nanocrystals (NCs) with narrow size and shape distributions are of particular interest for the successful implementation of these nanocrystals into devices. Moreover, the preparation of NCs with well-defined crystal phases is of key importance. In this work, we show that Sn(IV)-thiolate complexes formed in situ strongly influence the nucleation and growth rates of colloidal Cu2-x S polyhedral NCs, thereby dictating their final size, shape, and crystal structure. This allowed us to successfully synthesize hexagonal bifrustums and hexagonal bipyramid NCs with low-chalcocite crystal structure, and hexagonal nanoplatelets with various thicknesses and aspect ratios with the djurleite crystal structure, by solely varying the concentration of Sn(IV)-additives (namely, SnBr4) in the reaction medium. Solution and solid-state 119Sn NMR measurements show that SnBr4 is converted in situ to Sn(IV)-thiolate complexes, which increase the Cu2-x S nucleation barrier without affecting the precursor conversion rates. This influences both the nucleation and growth rates in a concentration-dependent fashion and leads to a better separation between nucleation and growth. Our approach of tuning the nucleation and growth rates with in situ-generated Sn-thiolate complexes might have a more general impact due to the availability of various metal-thiolate complexes, possibly resulting in polyhedral NCs of a wide variety of metal-sulfide compositions. |
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Address |
Condensed Matter and Interfaces, Debye Institute for Nanomaterials Science, Utrecht University , P.O. Box 80000, 3508 TA Utrecht, The Netherlands |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
English |
Wos |
000384399000037 |
Publication Date |
2016-09-02 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
|
|
ISSN |
0897-4756 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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|
Impact Factor |
9.466 |
Times cited |
27 |
Open Access |
OpenAccess |
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|
Notes |
W.v.d.S. and C.d.M.D. acknowledge financial support from the division of Chemical Sciences (CW) of The Netherlands Organization for Scientific Research (NWO) under grant number ECHO.712.012.001. M.B. also gratefully acknowledges NWO for funding the NMR infrastructure (Middle Groot program, grant number 700.58.102). S.B. acknowledges financial support from the European Research Council (ERC Starting Grant # 335078-COLOURATOMS).; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 9.466 |
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|
Call Number |
EMAT @ emat @ c:irua:135928 |
Serial |
4285 |
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Permanent link to this record |
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Author |
van der Stam, W.; Berends, A.C.; Rabouw, F.T.; Willhammar, T.; Ke, X.; Meeldijk, J.D.; Bals, S.; de Donega, C.M. |
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Title |
Luminescent CuInS2 quantum dots by partial cation exchange in Cu2-xS nanocrystals |
Type |
A1 Journal article |
|
Year |
2015 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
|
|
Volume |
27 |
Issue |
27 |
Pages |
621-628 |
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|
Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Here, we show successful partial cation exchange reactions in Cu2-xS nanocrystals (NCs) yielding luminescent CuInS2 (CIS) NCs. Our approach of mild reaction conditions ensures slow Cu extraction rates, which results in a balance with the slow In incorporation rate. With this method, we obtain CIS NCs with photoluminescence (PL) far in the near-infrared (NIR), which cannot be directly synthesized by currently available synthesis protocols. We discuss the factors that favor partial, self-limited cation exchange from Cu2-xS to CIS NCs, rather than complete cation exchange to In2S3. The product CIS NCs have the wurtzite crystal structure, which is understood in terms of conservation of the hexagonal close packing of the anionic sublattice of the parent NCs into the product NCs. These results are an important step toward the design of CIS NCs with sizes and shapes that are not attainable by direct synthesis protocols and may thus impact a number of potential applications. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000348618400028 |
Publication Date |
2014-12-29 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
|
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ISSN |
0897-4756;1520-5002; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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|
Impact Factor |
9.466 |
Times cited |
119 |
Open Access |
OpenAccess |
|
|
Notes |
335078 Colouratom; 262348 Esmi; ECAS_Sara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 9.466; 2015 IF: 8.354 |
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Call Number |
c:irua:125291 |
Serial |
1858 |
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Permanent link to this record |
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Author |
van der Stam, W.; Akkerman, Q.A.; Ke, X.; van Huis, M.A.; Bals, S.; de Donega, C.M. |
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Title |
Solution-processable ultrathin size- and shape-controlled colloidal Cu2-xS nanosheets |
Type |
A1 Journal article |
|
Year |
2015 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
|
|
Volume |
27 |
Issue |
27 |
Pages |
283-291 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Ultrathin two-dimensional (2D) nanosheets (NSs) possess extraordinary properties that are attractive for both fundamental studies and technological devices. Solution-based bottom-up methods are emerging as promising routes to produce free-standing NSs, but the synthesis of colloidal NSs with well-defined size and shape has remained a major challenge. In this work, we report a novel method that yields 2 nm thick colloidal Cu2-xS NSs with well-defined shape (triangular or hexagonal) and size (100 nm to 3 mu m). The key feature of our approach is the use of a synergistic interaction between halides (Br or Cl) and copper-thiolate metal-organic frameworks to create a template that imposes 2D constraints on the Cu-catalyzed C-S thermolysis, resulting in nucleation and growth of colloidal 2D Cu2-xS NSs. Moreover, the NS composition can be postsynthetically tailored by exploiting topotactic cation exchange reactions. This is illustrated by converting the Cu2-xS NSs into ZnS and CdS NSs while preserving their size and shape. The method presented here thus holds great promise as a route to solution-processable compositionally diverse ultrathin colloidal NSs with well-defined shape and size. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000348085300036 |
Publication Date |
2014-12-04 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
|
Edition |
|
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ISSN |
0897-4756;1520-5002; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
9.466 |
Times cited |
68 |
Open Access |
OpenAccess |
|
|
Notes |
335078 Colouratom; 246791 Countatoms; 312483 Esteem2; esteem2ta; ECASSara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); |
Approved |
Most recent IF: 9.466; 2015 IF: 8.354 |
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Call Number |
c:irua:123865 c:irua:123865 |
Serial |
3052 |
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Permanent link to this record |
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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. |
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Title |
Study of the Mechanism and Increasing Crystallinity in the Self-Templated Growth of Ultrathin PbS Nanosheets |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Chemistry of materials |
Abbreviated Journal |
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Volume |
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Issue |
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Pages |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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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. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000959572100001 |
Publication Date |
2023-03-25 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
8.6 |
Times cited |
2 |
Open Access |
OpenAccess |
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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 |
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Call Number |
EMAT @ emat @c:irua:195894 |
Serial |
7255 |
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Permanent link to this record |
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Author |
Ustarroz, J.; Altantzis, T.; Hammons, J.A.; Hubin, A.; Bals, S.; Terryn, H. |
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Title |
The role of nanocluster aggregation, coalescence, and recrystallization in the electrochemical deposition of platinum nanostructures |
Type |
A1 Journal article |
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Year |
2014 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
26 |
Issue |
7 |
Pages |
2396-2406 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
By using an optimized characterization approach that combines aberration-corrected transmission electron microscopy, electron tomography, and in situ ultrasmall angle X-ray scattering (USAXS), we show that the early stages of Pt electrochemical growth on carbon substrates may be affected by the aggregation, self-alignment, and partial coalescence of nanoclusters of d ≈ 2 nm. The morphology of the resulting nanostructures depends on the degree of coalescence and recrystallization of nanocluster aggregates, which in turn depends on the electrodeposition potential. At low overpotentials, a self-limiting growth mechanism may block the epitaxial growth of primary nanoclusters and results in loose dendritic aggregates. At more negative potentials, the extent of nanocluster coalescence and recrystallization is larger and further growth by atomic incorporation may be allowed. On one hand, this suggests a revision of the VolmerWeber island growth mechanism. Whereas this theory has traditionally assumed direct attachment as the only growth mechanism, it is suggested that nanocluster self-limiting growth, aggregation, and coalescence should also be taken into account during the early stages of nanoscale electrodeposition. On the other hand, depending on the deposition potential, ultrahigh porosities can be achieved, turning electrodeposition in an ideal process for highly active electrocatalyst production without the need of using high surface area carbon supports. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
Washington, D.C. |
Editor |
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Language |
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Wos |
000334572300026 |
Publication Date |
2014-03-10 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
|
Edition |
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ISSN |
0897-4756;1520-5002; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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|
Impact Factor |
9.466 |
Times cited |
55 |
Open Access |
Not_Open_Access |
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|
Notes |
FWO; contract no. FWOAL527 |
Approved |
Most recent IF: 9.466; 2014 IF: 8.354 |
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Call Number |
UA @ lucian @ c:irua:116956 |
Serial |
2916 |
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Permanent link to this record |
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Author |
Turner, S.; Verbeeck, J.; Ramezanipour, F.; Greedan, J.E.; Van Tendeloo, G.; Botton, G.A. |
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Title |
Atomic resolution coordination mapping in Ca2FeCoO5 brownmillerite by spatially resolved electron energy-loss spectroscopy |
Type |
A1 Journal article |
|
Year |
2012 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
24 |
Issue |
10 |
Pages |
1904-1909 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Using a combination of high-angle annular dark field scanning transmission electron microscopy and atomically resolved electron energy-loss spectroscopy at high energy resolution in an aberration-corrected electron microscope, we demonstrate the capability of coordination mapping in complex oxides. Brownmillerite compound Ca2FeCoO5, consisting of repetitive octahedral and tetrahedral coordination layers with Fe and Co in a fixed 3+ valency, is selected to demonstrate the principle of atomic resolution coordination mapping. Analysis of the Co-L2,3 and the Fe-L2,3 edges shows small variations in the fine structure that can be specifically attributed to Co/Fe in tetrahedral or in octahedral coordination. Using internal reference spectra, we show that the coordination of the Fe and Co atoms in the compound can be mapped at atomic resolution. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
Washington, D.C. |
Editor |
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Language |
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Wos |
000304237500024 |
Publication Date |
2012-04-25 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756;1520-5002; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
9.466 |
Times cited |
33 |
Open Access |
|
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|
Notes |
A.M. Abakumov is thanked for fruitful discussions. S.T. gratefully acknowledges the Fund for Scientific Research Flanders (FWO). J.E.G. and GAB. acknowledge the support of the NSERC of Canada through Discovery Grants. The Canadian Centre for Electron Microscopy is a National Facility supported by NSERC and McMaster University and was funded by the Canada Foundation for Innovation and the Ontario Government. Part of this work was supported by funding from the European Research Council under the FP7, ERC Grant N 246791 COUNTATOMS and ERC Starting Grant N 278510 VORTEX. The EMAT microscope is partially funded by the Hercules fund of the Flemish Government. ECASJO_; |
Approved |
Most recent IF: 9.466; 2012 IF: 8.238 |
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Call Number |
UA @ lucian @ c:irua:98379UA @ admin @ c:irua:98379 |
Serial |
175 |
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Permanent link to this record |
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Author |
Turner, S.; Lebedev, O.I.; Schroeder, F.; Fischer, R.A.; Van Tendeloo, G. |
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Title |
Direct imaging of loaded metal-organic framework materials (metal@MOF-5) |
Type |
A1 Journal article |
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Year |
2008 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
20 |
Issue |
17 |
Pages |
5622-5627 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
We illustrate the potential of advanced transmission electron microscopy for the characterization of a new class of soft porous materials: metal@Zn4O(bdc)3 (metal@MOF-5; bdc = 1,4-benzenedicarboxylate). By combining several electron microscopy techniques (transmission electron microscopy (TEM), high-resolution transmission electron microscopy (HRTEM), electron diffraction (ED), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), and electron tomography) and by carefully reducing the electron dose to avoid beam damage, it is possible to simultaneously characterize the MOF-5 framework material and the loaded metal nanoparticles. We also demonstrate that electron tomography can be used to accurately determine the position and distribution of the particles within the MOF-5 framework. To demonstrate the implementation of these microscopy techniques and what kind of results can be expected, measurements on gas-phase-loaded metal−organic framework materials Ru@MOF-5 and Pd@MOF-5 are presented. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
Washington, D.C. |
Editor |
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Language |
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Wos |
000258941400021 |
Publication Date |
2008-08-07 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756;1520-5002; |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
9.466 |
Times cited |
112 |
Open Access |
|
|
|
Notes |
Esteem 026019 |
Approved |
Most recent IF: 9.466; 2008 IF: 5.046 |
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Call Number |
UA @ lucian @ c:irua:76595 |
Serial |
714 |
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Permanent link to this record |
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Author |
Tessier, M.D.; Baquero, E.A.; Dupont, D.; Grigel, V.; Bladt, E.; Bals, S.; Coppel, Y.; Hens, Z.; Nayral, C.; Delpech, F. |
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Title |
Interfacial oxidation and photoluminescence of InP-Based core/shell quantum dots |
Type |
A1 Journal article |
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Year |
2018 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
30 |
Issue |
30 |
Pages |
6877-6883 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Indium phosphide colloidal quantum dots (QDs) are emerging as an efficient cadmium-free alternative for optoelectronic applications. Recently, syntheses based on easy-to-implement aminophosphine precursors have been developed. We show by solid-state nuclear magnetic resonance spectroscopy that this new approach allows oxide-free indium phosphide core or core/shell quantum dots to be made. Importantly, the oxide-free core/shell interface does not help in achieving higher luminescence efficiencies. We demonstrate that in the case of InP/ZnS and InP/ZnSe QDs, a more pronounced oxidation concurs with a higher photoluminescence efficiency. This study suggests that a II-VI shell on a III-V core generates an interface prone to defects. The most efficient InP/ZnS or InP/ZnSe QDs are therefore made with an oxide buffer layer between the core and the shell: it passivates these interface defects but also results in a somewhat broader emission line width. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
American Chemical Society |
Place of Publication |
Washington, D.C |
Editor |
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Language |
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Wos |
000447237800031 |
Publication Date |
2018-09-12 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
|
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ISSN |
0897-4756 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
|
|
Impact Factor |
9.466 |
Times cited |
74 |
Open Access |
OpenAccess |
|
|
Notes |
; The authors thank L. Biadala and C. Delerue for fruitful discussion. Z.H. acknowledges support by the European Commission via the Marie-Sklodowska Curie action Phonsi (H2020-MSCA-ITN-642656), by Research Foundation Flanders (Project 17006602), and by Ghent University (GOA No. 01G01513). Z.H., M.D.T., and D.D. acknowledge the Strategisch Initiatief Materialen in Vlaanderen of Agentschap Innoveren en Ondernemen (SIM VLAIO), vzw (SBO-QDOCCO, ICON-QUALIDI). This work was supported by the Universite Paul Sabatier, the Region Midi-Pyrenees, the CNRS, the Institut National des Sciences Appliquees of Toulouse, and the Agence Nationale pour la Recherche (Project ANR-13-IS10-0004-01). E.A.B. is grateful to Marie Curie Actions and Campus France for a PRESTIGE postdoc fellowship (FP7 /2007-2013) under REA Grant Agreement PCOFUND-GA-2013-609102. E.B. acknowledges financial support from Research Foundation Flanders (FWO). ; |
Approved |
Most recent IF: 9.466 |
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|
Call Number |
UA @ lucian @ c:irua:154732UA @ admin @ c:irua:154732 |
Serial |
5109 |
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Permanent link to this record |
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Author |
Tan, X.; Stephens, P.W.; Hendrickx, M.; Hadermann, J.; Segre, C.U.; Croft, M.; Kang, C.-J.; Deng, Z.; Lapidus, S.H.; Kim, S.W.; Jin, C.; Kotliar, G.; Greenblatt, M. |
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Title |
Tetragonal Cs1.17In0.81Cl3 : a charge-ordered indium halide perovskite derivative |
Type |
A1 Journal article |
|
Year |
2019 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
|
|
Volume |
31 |
Issue |
6 |
Pages |
1981-1989 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Polycrystalline samples of Cs1.17In0.81Cl3 were prepared by annealing a mixture of CsCl, InCl, and InCl3, stoichiometric for the targeted CsInCl3. Synchrotron powder X-ray diffraction refinement and chemical analysis by energy dispersive X-ray indicated that Cs1.17In0.81Cl3, a tetragonal distorted perovskite derivative (I4/m), is the thermodynamically stable product. The refined unit cell parameters and space group were confirmed by electron diffraction. In the tetragonal structure, In+ and In3+ are located in four different crystallographic sites, consistent with their corresponding bond lengths. In1, In2, and In3 are octahedrally coordinated, whereas In4 is at the center of a pentagonal bipyramid of Cl because of the noncooperative octahedral tilting of In4Cl6. The charged-ordered In+ and In3+ were also confirmed by X-ray absorption and Raman spectroscopy. Cs1.17In0.81Cl3 is the first example of an inorganic halide double perovskite derivative with charged-ordered In+ and In3+. Band structure and optical conductivity calculations were carried out with both generalized gradient approximation (GGA) and modified Becke-Johnson (mBJ) approach; the GGA calculations estimated the band gap and optical band gap to be 2.27 eV and 2.4 eV, respectively. The large and indirect band gap suggests that Cs1.17In0.81Cl3 is not a good candidate for photovoltaic application. |
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Place of Publication |
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Language |
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Wos |
000462950400017 |
Publication Date |
2019-02-19 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
6 |
Open Access |
OpenAccess |
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Notes |
; M.G. and X.T. were supported by the Center for Computational Design of Functional Strongly Correlated Materials and Theoretical Spectroscopy under DOE Grant No. DE-FOA-0001276. M.G. also acknowledges support of NSF-DMR-1507252 grant. G.K. and C.-J.K. were supported by the Air Force Office of Scientific Research. MRCAT operations are supported by the Department of Energy and the MRCAT member institutions. The use of the Advanced Photon Source at the Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. The works at IOPCAS were supported by NSF & MOST of China through research projects. ; |
Approved |
Most recent IF: 9.466 |
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Call Number |
UA @ admin @ c:irua:159413 |
Serial |
5262 |
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Permanent link to this record |
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Author |
Sun, M.; Rousse, G.; Abakumov, A.M.; Saubanere, M.; Doublet, M.-L.; Rodriguez-Carvajal, J.; Van Tendeloo, G.; Tarascon, J.-M. |
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Title |
Li2Cu2O(SO4)2: a possible electrode for sustainable Li-based batteries showing a 4.7 V redox activity vs Li+/Li0 |
Type |
A1 Journal article |
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Year |
2015 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
27 |
Issue |
27 |
Pages |
3077-3087 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Li-ion batteries rely on the use of insertion positive electrodes with performances scaling with the redox potential of the 31) metals accompanying Liuptake/removal. Although not commonly studied, the Cu2+/Cu3+ redox potential has been predicted from theoretical calculations to possibly offer a high operating voltage redox couple. We herein report the synthesis and crystal structure of a hitherto-unknown oxysulfate phase, Li2Cu2O(SO4)(2), which contains infinite edgesharing CuO4 chains and presents attractive electrochemical redox activity with respect to Li+/Li, namely amphoteric characteristics. Li2Cu2O(SO4)(2) shows redox activity at 4.7 V vs Li+/Li corresponding to the oxidation of Cu2+ to Cu3+ enlisting ligand holes and associated with the reversible uptake-removal of 0.3 Li. Upon reduction, this compound reversibly uptakes similar to 2 Li at an average potential of about 2.5 V vs Li+/Li, associated with the Cu2+/Cu+ redox couple. The mechanism of the reactivity upon reduction is discussed in detail, with particular attention to the occasional appearance of an oscillation wave in the discharge profile. Our work demonstrates that Cu-based compounds can indeed be fertile scientific ground in the search for new high-energy-density electrodes. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000353865800043 |
Publication Date |
2015-03-25 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756;1520-5002; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
20 |
Open Access |
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Notes |
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Approved |
Most recent IF: 9.466; 2015 IF: 8.354 |
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Call Number |
c:irua:126061 |
Serial |
3541 |
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Permanent link to this record |
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Author |
Shevchenko, V.A.; Glazkova, I.S.; Novichkov, D.A.; Skvortsova, I.; V. Sobolev, A.; Abakumov, A.M.; Presniakov, I.A.; Drozhzhin, O.A.; V. Antipov, E. |
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Title |
Competition between the Ni and Fe redox in the O3-NaNi1/3Fe1/3Mn1/3O2 cathode material for Na-ion batteries |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Chemistry of materials |
Abbreviated Journal |
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Volume |
35 |
Issue |
10 |
Pages |
4015-4025 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Sodium-ion batteries are attracting great attention due to their low cost and abundance of sodium. The O3-type NaNi1/3Fe1/3Mn1/3O2 layered oxide material is a promising candidate for positive electrodes (cathodes) in Na-ion batteries. However, its stable electrochemical performance is restricted by the upper voltage limit of 4.0 V (vs Na/Na+), which allows for reversibly removing 0.5-0.55 Na+ per formula unit, corresponding to the capacity of 120-130 mAh.g(-1). Further reduction of sodium content inevitably accelerates capacity degradation, and this issue calls for a detailed study of the redox reactions that accompany the electrochemical (de)intercalation of a large amount of sodium. Here, we present operando and ex situ studies using powder X-ray diffraction and X-ray absorption spectroscopy combined with Fe-57 Mossbauer spectroscopy. Our approach reveals the sequence of the redox transitions that occur during the charge and discharge of O3-NaNi1/3Fe1/3Mn1/3O2. Our data show that in addition to nickel and iron cations oxidizing to M+4, a part of iron transforms into the “3 + delta” state owing to the fast electron exchange Fe3+ + Fe4+ <-> Fe4+ + Fe3+. This process freezes upon cooling the material to 35 K, producing Fe4+ cations, some of which occupy tetrahedral positions. |
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Corporate Author |
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Place of Publication |
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Wos |
000985970200001 |
Publication Date |
2023-05-04 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756; 1520-5002 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
8.6 |
Times cited |
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Open Access |
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Notes |
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Approved |
Most recent IF: 8.6; 2023 IF: 9.466 |
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Call Number |
UA @ admin @ c:irua:197352 |
Serial |
9013 |
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Permanent link to this record |
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Author |
Shetty, S.; Sinha, S.K.; Ahmad, R.; Singh, A.K.; Van Tendeloo, G.; Ravishankar, N. |
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Title |
Existence of Ti2+States on the Surface of Heavily Reduced SrTiO3Nanocubes |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
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Issue |
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Pages |
acs.chemmater.7b04113 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Using advanced electron microscopy, we demonstrate the presence of Ti2+ on the 001 surfaces of heavily reduced strontium titanate nanocubes. While high-angle annular dark field images show a clear difference between the surfaces of the unreduced and reduced samples, electron energy loss spectroscopy detects the presence of Ti2+ on the surface of the reduced cubes. Conventional reduction only leads to the formation of Ti3+ and involves the use of high temperatures. In our case, reduction is achieved at relatively lower temperatures in the solid state using sodium borohydride as the reducing agent. Our findings provide insights into the optical properties of the samples and provide a convenient method to produce highly reduced surfaces that could demonstrate a range of exotic physical phenomena |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000418206600005 |
Publication Date |
2017-11-17 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
8 |
Open Access |
OpenAccess |
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Notes |
We thank Advanced Facility for Microscopy and Microanalysis (AFMM), IISc, Bangalore for providing the TEM facility. We also thank MNCF, CeNSE, IISc for providing the XPS and FT-IR facilities. We acknowledge the help from Prof. Anshu Pandey for providing the PL facility and Mr. Ashutosh Gupta for the help with measurements. SS and NR thank DST for providing the financial support. RA and AKS acknowledge Super Computing Education and Research Center (SERC) and Materials Research Center (MRC), at IISc for providing required computational facilities. RA acknowledges the financial support from INSPIRE fellowship, AORC.Science and Engineering Research Board; Federaal Wetenschapsbeleid; Department of Science and Technology, Ministry of Science and Technology; |
Approved |
Most recent IF: 9.466 |
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Call Number |
UA @ lucian @c:irua:147191 |
Serial |
4767 |
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Permanent link to this record |
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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. |
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Title |
New solid electrolyte Na9Al(MoO4)6 : structure and Na+ ion conductivity |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
29 |
Issue |
20 |
Pages |
8901-8913 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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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.')); |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
American Chemical Society |
Place of Publication |
Washington, D.C |
Editor |
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Language |
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Wos |
000413884900037 |
Publication Date |
2017-09-26 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
13 |
Open Access |
OpenAccess |
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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 |
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Call Number |
UA @ lucian @ c:irua:147432 |
Serial |
4886 |
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Permanent link to this record |
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Author |
Sathiya, M.; Thomas, J.; Batuk, D.; Pimenta, V.; Gopalan, R.; Tarascon, J.-M. |
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Title |
Dual stabilization and sacrificial effect of Na2CO3 for increasing capacities of Na-Ion cells based on P2-NaxMO2 electrodes |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
29 |
Issue |
14 |
Pages |
5948-5956 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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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. |
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Corporate Author |
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Thesis |
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Publisher |
American Chemical Society |
Place of Publication |
Washington, D.C |
Editor |
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Language |
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Wos |
000406573200026 |
Publication Date |
2017-07-03 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
26 |
Open Access |
Not_Open_Access |
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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 |
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Call Number |
UA @ lucian @ c:irua:145759 |
Serial |
4740 |
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Permanent link to this record |
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Author |
Salzmann, B.B.V.; Vliem, J.F.; Maaskant, D.N.; Post, L.C.; Li, C.; Bals, S.; Vanmaekelbergh, D. |
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Title |
From CdSe nanoplatelets to quantum rings by thermochemical edge reconfiguration |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Chemistry Of Materials |
Abbreviated Journal |
Chem Mater |
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Volume |
33 |
Issue |
17 |
Pages |
6853-6859 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
The variation in the shape of colloidal semiconductor nanocrystals (NCs) remains intriguing. This interest goes beyond crystallography as the shape of the NC determines its energy levels and optoelectronic properties. While thermodynamic arguments point to a few or just a single shape(s), terminated by the most stable crystal facets, a remarkable variation in NC shape has been reported for many different compounds. For instance, for the well-studied case of CdSe, close-to-spherical quantum dots, rods, two-dimensional nanoplatelets, and quantum rings have been reported. Here, we report how two-dimensional CdSe nanoplatelets reshape into quantum rings. We monitor the reshaping in real time by combining atomically resolved structural characterization with optical absorption and photoluminescence spectroscopy. We observe that CdSe units leave the vertical sides of the edges and recrystallize on the top and bottom edges of the nanoplatelets, resulting in a thickening of the rims. The formation of a central hole, rendering the shape into a ring, only occurs at a more elevated temperature. |
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Corporate Author |
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Publisher |
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Place of Publication |
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Language |
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Wos |
000696553600024 |
Publication Date |
2021-08-24 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756; 1520-5002 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
7 |
Open Access |
OpenAccess |
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Notes |
Hans Meeldijk is kindly acknowledged for helping with electron microscopy at Utrecht University. 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”. D.V. and L.C.P. acknowledge the Dutch NWO for financial support via the TOP-ECHO grant nr. 718.015.002. S.B acknowledges financial support from the European ERC Council, ERC Consolidator grant 815128. This project has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement no. 731019 (EUSMI). Realnano; sygmaSB |
Approved |
Most recent IF: 9.466 |
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Call Number |
UA @ admin @ c:irua:181550 |
Serial |
6839 |
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Permanent link to this record |
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Author |
Sa, J.; Hu, N.; Heyvaert, W.; Van Gordon, K.; Li, H.; Wang, L.; Bals, S.; Liz-Marzán, L.M.; Ni, W. |
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Title |
Spontaneous Chirality Evolved at the Au–Ag Interface in Plasmonic Nanorods |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem. Mater. |
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Volume |
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Issue |
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Pages |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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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. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
001052093300001 |
Publication Date |
2023-08-21 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
8.6 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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 |
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Call Number |
EMAT @ emat @c:irua:198151 |
Serial |
8810 |
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Permanent link to this record |
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Author |
Rusakov, D.; Abakumov, A.M.; Yamaura, K.; Belik, A.A.; Van Tendeloo, G.; Takayama-Muromachi, E. |
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Title |
Structural evolution of the BiFeO3-LaFeO3 system |
Type |
A1 Journal article |
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Year |
2011 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
23 |
Issue |
2 |
Pages |
285-292 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
The (1 − x)BiFeO3−xLaFeO3 system has been investigated and characterized by room-temperature and high-temperature laboratory and synchrotron powder X-ray diffraction, electron diffraction, high-resolution transmission electron microscopy, differential scanning calorimetry, and magnetization measurements. At room temperature, the ferroelectric R3c phase is observed for 0.0 ≤ x ≤ 0.10. The PbZrO3-related √2ap × 2√2ap × 4ap superstructure (where ap is the parameter of the cubic perovskite subcell) is observed for Bi0.82La0.18FeO3, while an incommensurately modulated phase is formed for 0.19 ≤ x ≤ 0.30 with the √2ap × 2ap × √2ap basic unit cell. The GdFeO3-type phase with space group Pnma (√2ap × 2ap × √2ap) is stable at 0.50 ≤ x ≤ 1. Bi0.82La0.18FeO3 has no detectable homogeneity range (space group Pnam, a = 5.6004(1) Å, b = 11.2493(3) Å, c = 15.6179(3) Å). The incommensurately modulated Bi0.75La0.25FeO3 structure was solved from synchrotron X-ray powder diffraction data (Imma(00γ)s00 superspace group, a = 5.5956(1) Å, b = 7.8171(1) Å, c = 5.62055(8) Å, q = 0.4855(4)c*, RP = 0.023, RwP = 0.033). In this structure, cooperative displacements of the Bi and O atoms occur, which order within the (AO) (where A = Bi, La) layers, resulting in an antipolar structure. Local fluctuations of the intralayer antipolar ordering are compensated by an interaction with the neighboring (AO) layers. A coupling of the antipolar displacements with the cooperative tilting distortion of the perovskite octahedral framework is proposed as the origin of the incommensurability. All the phases transform to the GdFeO3-type structure at high temperatures. Bi0.82La0.18FeO3 shows an intermediate PbZrO3-type phase with √2ap × 2√2ap × 2ap (space group Pbam; a = 5.6154(2) Å, b = 11.2710(4) Å, and c = 7.8248(2) Å at 570 K). The compounds in the compositional range of 0.18 ≤ x ≤ 0.95 are canted antiferromagnets. |
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Place of Publication |
Washington, D.C. |
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Wos |
000286160800021 |
Publication Date |
2010-12-23 |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756;1520-5002; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
133 |
Open Access |
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Notes |
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Approved |
Most recent IF: 9.466; 2011 IF: 7.286 |
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Call Number |
UA @ lucian @ c:irua:88650 |
Serial |
3236 |
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Permanent link to this record |
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Author |
Rodal-Cedeira, S.; Montes-García, V.; Polavarapu, L.; Solís, D.M.; Heidari, H.; La Porta, A.; Angiola, M.; Martucci, A.; Taboada, J.M.; Obelleiro, F.; Bals, S.; Pérez-Juste, J.; Pastoriza-Santos, I. |
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Title |
Plasmonic Au@Pd Nanorods with Boosted Refractive Index Susceptibility and SERS Efficiency: A Multifunctional Platform for Hydrogen Sensing and Monitoring of Catalytic Reactions |
Type |
A1 Journal article |
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Year |
2016 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
28 |
Issue |
28 |
Pages |
9169-9180 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Palladium nanoparticles (NPs) have received tremendous attention over the years due to their high catalytic activity for various chemical reactions. However, unlike other noble metal nanoparticles such as Au and Ag NPs, they exhibit poor plasmonic properties with broad extinction spectra and less scattering efficiency, and thus limiting their applications in the field of plasmonics. Therefore, it has been challenging to integrate tunable and strong plasmonic properties into catalytic Pd nanoparticles. Here we show that plasmonic Au@Pd nanorods (NRs) with relatively narrow and remarkably tunable optical responses in the NIR region can be obtained by directional growth of Pd on penta-twinned Au NR seeds. We found the presence of bromide ions facilitates the stabilization of facets for the directional growth of Pd shell to obtain Au@Pd nanorods (NR) with controlled length scales. Interestingly, it turns out the Au NR supported Pd NRs exhibit much narrow extinction compared to pure Pd NRs, which makes them suitable for plasmonic sensing applications. Moreover, these nanostructures display, to the best of our knowledge, one of the highest ensemble refractive index sensitivity values reported to date (1067 nm per refractive index unit, RIU). Additionally, we showed the application of such plasmonic Au@Pd NRs for localized surface plasmon resonance (LSPR)-based sensing of hydrogen both in solution as well as on substrate. Finally, we demonstrate the integration of excellent plasmonic properties in catalytic palladium enables the in situ monitoring of a reaction progress by surface-enhanced Raman scattering. We postulate the proposed approach to boost the plasmonic properties of Pd nanoparticles will ignite the design of complex shaped plasmonic Pd NPs to be used in various plasmonic applications such as sensing and in situ monitoring of various chemical reactions. |
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Wos |
000391080900036 |
Publication Date |
2016-12-27 |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
80 |
Open Access |
OpenAccess |
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Notes |
Funding from Spanish Ministerio de Economía y Competitividad (Grants MAT2013-45168-R and MAT2016-77809-R) is gratefully acknowledge. A.L.P. and S.B. acknowledge support by the European Research Council through an ERC Starting Grant (#335078-COLOURATOMS). L. P. acknowledges the financial support from by the Alexander von Humboldt-Stiftung. V. M.-G. acknowledges the financial support from FPU scholarship from the Spanish MINECO. (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); ECAS_Sara |
Approved |
Most recent IF: 9.466 |
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Call Number |
EMAT @ emat @ c:irua:139513 |
Serial |
4344 |
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Permanent link to this record |
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Author |
Recham, N.; Casas-Cabanas, M.; Cabana, J.; Grey, C.P.; Jumas, J.-C.; Dupont, L.; Armand, M.; Tarascon, J.-M. |
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Title |
Formation of a complete solid solution between the triphylite and fayalite olivine structures |
Type |
A1 Journal article |
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Year |
2008 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
20 |
Issue |
21 |
Pages |
6798-6809 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
The recent infatuation for LiFePO4 as positive electrode material in Li-ion batteries has prompted a renewed interest in olivine-type structures, with a view to enhance their conduction proper-ties. We show that the dual substitution of Li for Fe and of P for Si in the olivine LiFePO4 phase leads to a complete solid solution Li1-xFe1+xP1-xSixO4 as deduced from combined X-ray diffraction, Mossbauer, and NMR experiments. Our findings challenge the common belief that the anionic network cannot be substituted. Moreover. it is found that such a substitution promotes Li intersite mixing between the olivine M1 and M2 sites. Such mixing, together with the worsening of the conducting properties of the dually substituted samples, is believed to be responsible for the poor electrochemical performances of the member's series. Beyond x = 0.20, the samples were electrochemically inactive. While the current materials are disappointing application-wise, such a study provides clues to the rich chemistry remaining to be unveiled with olivine-type structures in particular and polyanionic compounds in general. |
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Place of Publication |
Washington, D.C. |
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Wos |
000260658100036 |
Publication Date |
2008-10-22 |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756;1520-5002; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
35 |
Open Access |
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Notes |
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Approved |
Most recent IF: 9.466; 2008 IF: 5.046 |
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Call Number |
UA @ lucian @ c:irua:103082 |
Serial |
1255 |
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Permanent link to this record |
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Author |
Ramachandran, R.K.; Filez, M.; Solano, E.; Poelman, H.; Minjauw, M.M.; Van Daele, M.; Feng, J.-Y.; La Porta, A.; Altantzis, T.; Fonda, E.; Coati, A.; Garreau, Y.; Bals, S.; Marin, G.B.; Detavernier, C.; Dendooven, J. |
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Title |
Chemical and Structural Configuration of Pt Doped Metal Oxide Thin Films Prepared by Atomic Layer Deposition |
Type |
A1 Journal article |
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Year |
2019 |
Publication |
Chemistry of materials |
Abbreviated Journal |
Chem Mater |
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Volume |
31 |
Issue |
31 |
Pages |
9673-9683 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
Pt doped semiconducting metal oxides and Pt metal clusters embedded in an oxide matrix are of interest for applications such as catalysis and gas sensing, energy storage and memory devices. Accurate tuning of the dopant level is crucial for adjusting the properties of these materials. Here, a novel atomic layer deposition (ALD) based method for doping Pt into In2O3 in specific, and metals in metal oxides in general, is demonstrated. This approach combines alternating exposures of Pt and In2O3 ALD processes in a single ‘supercycle’, followed by supercycle repetition leading to multilayered nanocomposites. The atomic level control of ALD and its conformal nature make the method suitable for accurate dopant control even on high surface area supports. Oxidation state, local structural environment and crystalline phase of the embedded Pt dopants were obtained by means of X-ray characterization methods and high angle annular dark-field scanning transmission electron microscopy (HAADF-STEM). In addition, this approach allows characterization of the nucleation stages of metal ALD processes, by stacking those states multiple times in an oxide matrix. Regardless of experimental conditions, a few Pt ALD cycles leads to the formation of oxidized Pt species due to their highly dispersed nature, as proven by X-ray absorption spectroscopy (XAS). Grazing-incidence small-angle X-ray scattering (GISAXS) and highresolution scanning transmission electron microscopy, combined with energy dispersive X-ray spectroscopy (HR-STEM/EDXS) show that Pt is evenly distributed in the In2O3 metal oxide matrix without the formation of clusters. For a larger number of Pt ALD
cycles, typ. > 10, the oxidation state gradually evolves towards fully metallic, and metallic Pt clusters are obtained within the In2O3 metal oxide matrix. This work reveals how tuning of the ALD supercycle approach for Pt doping allows controlled engineering of the Pt compositional and structural configuration within a metal oxide matrix. |
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Wos |
000502418000010 |
Publication Date |
2019-11-11 |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0897-4756 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
9.466 |
Times cited |
6 |
Open Access |
OpenAccess |
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Notes |
This research was supported by the Flemish Research Foundation (FWO-Vlaanderen), the Flemish Government (Long term structural funding – Methusalem funding and Medium scale research infrastructure funding-Hercules funding), the Special Research Fund BOF of Ghent University (GOA 01G01513) and the CALIPSO Trans National Access Program funded by the European Commission in supplying financing of travel costs. We are grateful to the SIXS and SAMBA-SOLEIL staff for smoothly running the beamline facilities. J.D. and R.K.R. are postdoctoral fellows of the FWO. |
Approved |
Most recent IF: 9.466 |
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Call Number |
EMAT @ emat @c:irua:164056 |
Serial |
5380 |
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Permanent link to this record |
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Author |
Quintelier, M.; Hajizadeh, A.; Zintler, A.; Gonçalves, B.F.; Fernández de Luis, R.; Esrafili Dizaji, L.; Vande Velde, C.M.L.; Wuttke, S.; Hadermann, J. |
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Title |
In SituStudy of the Activation Process of MOF-74 Using Three-Dimensional Electron Diffraction |
Type |
A1 Journal Article |
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Year |
2024 |
Publication |
Chemistry of Materials |
Abbreviated Journal |
Chem. Mater. |
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Pages |
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Keywords |
A1 Journal Article; 3DED; MOFs; in situ; Electron Microscopy for Materials Science (EMAT) ; |
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Abstract |
Metal–organic framework (MOF)-74 is known for its effectiveness in selectively capturing carbon dioxide (CO2). Especially the Zn and Cu versions of MOF-74 show high efficiency of this material for CO2. However, the activation of this MOF, which is a crucial step for its utilization, is so far not well understood. Here, we are closing the knowledge gap by examining the activation using, for the first time in the MOF, three-dimensional electron diffraction (3DED) during in situ heating. The use of state-of-the-art direct electron detectors enables rapid acquisition and minimal exposure times, therefore minimizing beam damage to the very electron beam-sensitive MOF material. The activation process of Zn-MOF-74 and Cu-MOF-74 is systematically studied in situ, proving the creation of open metal sites. Differences in thermal stability between Zn-MOF-74 and Cu-MOF-74 are attributed to the strength of the metal–oxygen bonds and Jahn–Teller distortions. In the case of Zn-MOF-74, we observe previously unknown remaining electrostatic potentials inside the MOF pores, which indicate the presence of remaining atoms that might impede gas flow throughout the structure when using the MOF for absorption purposes. We believe our study exemplifies the significance of employing advanced characterization techniques to enhance our material understanding, which is a crucial step for unlocking the full potential of MOFs in various applications. |
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Wos |
https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=brocade2&SrcAuth=WosAPI&KeyUT=WOS:001275 |
Publication Date |
2024-07-22 |
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Edition |
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ISSN |
0897-4756 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
8.6 |
Times cited |
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Open Access |
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Notes |
European Regional Development Fund, PID2021-122940OB-C31 ; H2020 Energy, 101022633 ; Universiteit Antwerpen, BOF TOP 38689 ; H2020 Marie Sklodowska-Curie Actions, 956099 ; Fonds Wetenschappelijk Onderzoek, I003218N ; Japan Science and Technology Agency, JPMJSC2102 ; Funda??o de Amparo ? Pesquisa do Estado de S?o Paulo; Agencia Estatal de Investigaci?n,Ministerio de Ciencia, Innovaci?n y Universidades, PID2021-122940OB-C31 TED2021-130621B-C42 ; |
Approved |
Most recent IF: 8.6; 2024 IF: 9.466 |
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Call Number |
EMAT @ emat @c:irua:207555 |
Serial |
9255 |
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Permanent link to this record |