Van Havenbergh K (2015) Influence of silicon nanoparticle coating on the electrolyte decomposition in Li-ion batteries. Antwerpen
Keywords: Doctoral thesis; Electron microscopy for materials research (EMAT)
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“Insertion compounds and composites made by ball milling for advanced sodium-ion batteries”. Zhang B, Dugas R, Rousse G, Rozier P, Abakumov AM, Tarascon J-M, Nature communications 7, 10308 (2016). http://doi.org/10.1038/ncomms10308
Abstract: Sodium-ion batteries have been considered as potential candidates for stationary energy storage because of the low cost and wide availability of Na sources. However, their future commercialization depends critically on control over the solid electrolyte interface formation, as well as the degree of sodiation at the positive electrode. Here we report an easily scalable ball milling approach, which relies on the use of metallic sodium, to prepare a variety of sodium-based alloys, insertion layered oxides and polyanionic compounds having sodium in excess such as the Na4V2(PO4)(2)F-3 phase. The practical benefits of preparing sodium-enriched positive electrodes as reservoirs to compensate for sodium loss during solid electrolyte interphase formation are demonstrated by assembling full C/P'2-Na-1[Fe0.5Mn0.5]O-2 and C/'Na3+xV2(PO4)(2)F-3' sodium-ion cells that show substantial increases (>10%) in energy storage density. Our findings may offer electrode design principles for accelerating the development of the sodium-ion technology.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 12.124
Times cited: 104
DOI: 10.1038/ncomms10308
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“Interface control by chemical and dimensional matching in an oxide heterostructure”. O'Sullivan M, Hadermann J, Dyer MS, Turner S, Alaria J, Manning TD, Abakumov AM, Claridge JB, Rosseinsky MJ, Nature chemistry 8, 347 (2016). http://doi.org/10.1038/NCHEM.2441
Abstract: Interfaces between different materials underpin both new scientific phenomena, such as the emergent behaviour at oxide interfaces, and key technologies, such as that of the transistor. Control of the interfaces between materials with the same crystal structures but different chemical compositions is possible in many materials classes, but less progress has been made for oxide materials with different crystal structures. We show that dynamical self-organization during growth can create a coherent interface between the perovskite and fluorite oxide structures, which are based on different structural motifs, if an appropriate choice of cations is made to enable this restructuring. The integration of calculation with experimental observation reveals that the interface differs from both the bulk components and identifies the chemical bonding requirements to connect distinct oxide structures.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 25.87
Times cited: 28
DOI: 10.1038/NCHEM.2441
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“Low-temperature plasticity of olivine revisited with in situ TEM nanomechanical testing”. Idrissi H, Bollinger C, Boioli F, Schryvers D, Cordier P, Science Advances 2, e1501671 (2016). http://doi.org/10.1126/sciadv.1501671
Abstract: The rheology of the lithospheric mantle is fundamental to understanding how mantle convection couples with plate tectonics. However, olivine rheology at lithospheric conditions is still poorly understood because experiments are difficult in this temperature range where rocks and mineral become very brittle. We combine techniques of quantitative in situ tensile testing in a transmission electron microscope and numerical modeling of dislocation dynamics to constrain the low-temperature rheology of olivine. We find that the intrinsic ductility of olivine at low temperature is significantly lower than previously reported values, which were obtained under strain-hardened conditions. Using this method, we can anchor rheological laws determined at higher temperature and can provide a better constraint on intermediate temperatures relevant for the lithosphere. More generally, we demonstrate the possibility of characterizing the mechanical properties of specimens, which can be available in the form of submillimeter-sized particles only.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Times cited: 32
DOI: 10.1126/sciadv.1501671
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“MULTEM : a new multislice program to perform accurate and fast electron diffraction and imaging simulations using graphics processing units with CUDA”. Lobato I, Van Dyck D, Ultramicroscopy 156, 9 (2015). http://doi.org/10.1016/j.ultramic.2015.04.016
Abstract: The main features and the GPU implementation of the MULTEM program are presented and described. This new program performs accurate and fast multislice simulations by including higher order expansion of the multislice solution of the high energy Schrodinger equation, the correct subslicing of the three-dimensional potential and top-bottom surfaces. The program implements different kinds of simulation for CTEM, STEM, ED, PED, CBED, ADF-TEM and ABF-HC with proper treatment of the spatial and temporal incoherences. The multislice approach described here treats the specimen as amorphous material which allows a straightforward implementation of the frozen phonon approximation. The generalized transmission function for each slice is calculated when is needed and then discarded. This allows us to perform large simulations that can include millions of atoms and keep the computer memory requirements to a reasonable level. (C) 2015 Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Vision lab
Impact Factor: 2.843
Times cited: 32
DOI: 10.1016/j.ultramic.2015.04.016
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“Structure-property relations of methylamine vapor treated hybrid perovskite CH3NH3PbI3 films and solar cells”. Conings B, Bretschneider SA, Babayigit A, Gauquelin N, Cardinaletti I, Manca JV, Verbeeck J, Snaith HJ, Boyen H-G, ACS applied materials and interfaces 9, 8092 (2017). http://doi.org/10.1021/acsami.6b15175
Abstract: The power conversion efficiency of halide perovskite solar cells is heavily dependent on the perovskite layer being sufficiently smooth and pinhole-free. It has been shown that these features can be obtained even when starting out from rough and discontinuous perovskite film, by briefly exposing it to methylamine (MA) vapor. The exact underlying physical mechanisms of this phenomenon are, however, still unclear. By investigating smooth, MA treated films, based on very rough and discontinuous reference films of methylammonium triiode (MAPbI3), considering their morphology, crystalline features, local conductive properties, and charge carrier lifetime, we unravel the relation between their characteristic physical qualities and their performance in corresponding solar cells. We discover that the extensive improvement in photovoltaic performance upon MA treatment is a consequence of the induced morphological enhancement of the perovskite layer, together with improved electron injection into TiO2, which in fact compensates for an otherwise compromised bulk electronic quality, simultaneously caused by the MA treatment.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 7.504
Times cited: 43
DOI: 10.1021/acsami.6b15175
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“A novel red Ca8.5Pb0.5Eu(PO4)7 phosphor for light emitting diodes application”. Deyneko DV, Morozov VA, Hadermann J, Savon AE, Spassky DA, Stefanovich SY, Belik AA, Lazoryak BI, Journal of alloys and compounds 647, 965 (2015). http://doi.org/10.1016/j.jallcom.2015.06.123
Abstract: Ca9-xPbxEu(PO4)(7) (0 <= x <= 1) solid solutions with a whitlockite-type (or beta-Ca-3(PO4)(2)-type) structure (sp.gr. R3c) were prepared by a standard solid-state method in air. Their luminescent properties under near-ultraviolet (n-UV) light were investigated. Excitation spectra of Ca9-xPbxEu(PO4)(7) showed the strongest absorption at about 395 nm, which matches well with commercially available n-UV-emitting GaN-based LED chips. Emission spectra indicated an intense red emission due to the D-5(0) -> F-7(2) transition of Eu3+, with a maximum in the intensity for Ca8.5Pb0.5Eu(PO4)(7). The emission intensity of Ca8.5Pb0.5Eu(PO4)(7) was about 1.8 times higher than that of a Ca9Eu(PO4)(7) phosphor. We suggest that the introduction of Pb2+ is an efficient approach to enhance luminescence properties of such phosphors. We clarified the influence of the Ca2+/Pb2+ substitution on intensities of three bands for the D-5(0) -> F-7(0) transition in excitation spectra of Ca9-xPbxEu(PO4)(7). In addition, we found a reversible first-order phase transition from R3c to R (3) over barc symmetry by second-harmonic generation in the range from 753 K (x = 1) to 846 K (x = 0). (C) 2015 Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 3.133
Times cited: 18
DOI: 10.1016/j.jallcom.2015.06.123
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“One-pot synthesis of carbon-coated nanostructured iron oxide on few-layer graphene for lithium-ion batteries”. Sun Z, Madej E, Wiktor, Sinev I, Fischer RA, Van Tendeloo G, Muhler M, Schuhmann W, Ventosa E, Chemistry: a European journal 21, 16154 (2015). http://doi.org/10.1002/chem.201501935
Abstract: Nanostructure engineering has been demonstrated to improve the electrochemical performance of iron oxide based electrodes in Li-ion batteries (LIBs). However, the synthesis of advanced functional materials often requires multiple steps. Herein, we present a facile one-pot synthesis of carbon-coated nanostructured iron oxide on few-layer graphene through high-pressure pyrolysis of ferrocene in the presence of pristine graphene. The ferrocene precursor supplies both iron and carbon to form the carbon-coated iron oxide, while the graphene acts as a high-surface-area anchor to achieve small metal oxide nanoparticles. When evaluated as a negative-electrode material for LIBs, our composite showed improved electrochemical performance compared to commercial iron oxide nanopowders, especially at fast charge/discharge rates.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 5.317
Times cited: 8
DOI: 10.1002/chem.201501935
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“Optical and photoelectrical properties of nanocrystalline indium oxide with small grains”. Forsh EA, Abakumov AM, Zaytsev VB, Konstantinova EA, Forsh PA, Rumyantseva MN, Gaskov AM, Kashkarov PK, Thin solid films : an international journal on the science and technology of thin and thick films 595, 25 (2015). http://doi.org/10.1016/j.tsf.2015.10.053
Abstract: Optical properties, spectral dependence of photoconductivity and photoconductivity decay in nanocrystalline indium oxide In2O3 are studied. A number of nanostructured In2O3 samples with various nanocrystals size are prepared by sol-gel method and characterized using various techniques. The mean nanocrystals size varies from 7 to 8 nm to 39-41 nm depending on the preparation conditions. Structural characterization of the In2O3 samples is performed by means of transmission electron microscopy and X-ray powder diffraction. The combined analysis of ultraviolet-visible absorption spectroscopy and diffuse reflectance spectroscopy shows that nanostructuring leads to the change in optical band gap: optical band gap of the In2O3 samples (with an average nanocrystal size from 7 to 41 nm) is equal to 2.8 eV. We find out the correlation between spectral dependence of photoconductivity and optical properties of nanocrystalline In2O3: sharp increase in photoconductivity was observed to begin at 2.8 eV that is equal to the optical bandgap in the In2O3 samples, and reached its maximum at 3.2-3.3 eV. The combined analysis of the slow photoconductivity decay in air, vacuum and argon, that was accurately fitted by a stretched-exponential function, and electron paramagnetic resonance (EPR) measurements shows that the kinetics of photoconductivity decay is strongly depended on the presence of oxygen molecules in the ambient of In2O3 nanocrystals. There is the quantitative correlation between EPR and photoconductivity data. Based on the obtained data we propose the model clearing up the phenomenon of permanent photoconductivity decay in nanocrystalline In2O3. (C) 2015 Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 1.879
Times cited: 18
DOI: 10.1016/j.tsf.2015.10.053
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“Post-synthesis bromination of benzene bridged PMO as a way to create a high potential hybrid material”. Huybrechts W, Mali G, Kuśtrowski P, Willhammar T, Mertens M, Bals S, Van Der Voort P, Cool P, Microporous and mesoporous materials: zeolites, clays, carbons and related materials 236, 244 (2016). http://doi.org/10.1016/j.micromeso.2016.09.003
Abstract: Periodic mesoporous organosilicas provide the best of two worlds: the strength and porosity of an inorganic framework combined with the infinite possibilities created by the organic bridging unit. In this work we focus on post-synthetical modification of benzene bridged PMO, in order to create bromobenzene PMO. In the past, this proved to be very challenging due to unwanted structural deterioration. However, now we have found a way to brominate this material whilst keeping the structure intact. In-depth structural analysis by solid state NMR and XPS shows both vast progress over previous attempts as well as potential for improvement.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA)
Impact Factor: 3.615
Times cited: 7
DOI: 10.1016/j.micromeso.2016.09.003
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“Process variability in Cu2ZnSnSe4 solar cell devices: Electrical and structural investigations”. Brammertz G, Buffiere M, Verbist C, Bekaert J, Batuk M, Hadermann J, et al, The conference record of the IEEE Photovoltaic Specialists Conference
T2 –, IEEE 42nd Photovoltaic Specialist Conference (PVSC), JUN 14-19, 2015, New Orleans, LA (2015)
Abstract: We have fabricated 9.7% efficient Cu2ZnSnSe4/CdS/ZnO solar cells by H2Se selenization of sequentially sputtered metal layers. Despite the good efficiency obtained, process control appears to be difficult. In the present contribution we compare the electrical and physical properties of two devices with nominal same fabrication procedure, but 1% and 9.7% power conversion efficiency respectively. We identify the problem of the lower performing device to be the segregation of ZnSe phases at the backside of the sample. This ZnSe seems to be the reason for the strong bias dependent photocurrent observed in the lower performing devices, as it adds a potential barrier for carrier collection. The reason for the different behavior of the two nominally same devices is not fully understood, but speculated to be related to sputtering variability.
Keywords: P1 Proceeding; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT)
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“Quantifying inflow and RANS turbulence model form uncertainties for wind engineering flows”. Gorle C, Garcia Sánchez C, Iaccarino G, Journal of wind engineering and industrial aerodynamics
T2 –, 6th International Symposium on Computational Wind Engineering (CWE), JUN 08-12, 2014, Hamburg, GERMANY 144, 202 (2015). http://doi.org/10.1016/j.jweia.2015.03.025
Abstract: Reynolds-averaged Navier-Stokes (RANS) simulations are often used in the wind engineering practice for the analysis of turbulent bluff body flows. An approach that allows identifying the uncertainty related to the use of reduced-order turbulence models in RANS simulations would significantly increase the confidence in the use of simulation results as a basis for design decisions. In the present study we apply a strategy that enables quantifying these uncertainties by introducing perturbations in the Reynolds stress tensor to simulations of the flow in downtown Oklahoma City. The method is combined with a framework to quantify uncertainties in the inflow wind direction and intensity, and the final result of the UQ approach is compared to field measurement data for the velocity at 13 locations in the downtown area. (C) 2015 Elsevier Ltd. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.049
Times cited: 22
DOI: 10.1016/j.jweia.2015.03.025
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“Doping anatase TiO2with group V-b and VI-b transition metal atoms: a hybrid functional first-principles study”. Matsubara M, Saniz R, Partoens B, Lamoen D, Physical chemistry, chemical physics 19, 1945 (2017). http://doi.org/10.1039/C6CP06882K
Abstract: We investigate the role of transition metal atoms of group V-b (V, Nb, Ta) and VI-b (Cr, Mo, W) as n- or p-type dopants in anatase TiO$_2$ using thermodynamic
principles and density functional theory with the Heyd-Scuseria-Ernzerhof HSE06 hybrid functional. The HSE06 functional provides a realistic value for the band gap, which ensures a correct classification of dopants as shallow or deep donors or acceptors. Defect formation energies and thermodynamic transition levels are calculated taking into account the constraints imposed by the stability of TiO$_2$ and the solubility limit of the impurities.
Nb, Ta, W and Mo are identified as shallow donors. Although W provides two electrons, Nb and Ta show a considerable lower formation energy, in particular under O-poor conditions. Mo donates in principle one electron, but under specific conditions can turn into a double donor. V impurities are deep donors and Cr
shows up as an amphoteric defect, thereby acting as an electron trapping center in n-type TiO$_2$ especially under O-rich conditions. A comparison with the available experimental data yields excellent agreement.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT)
Impact Factor: 4.123
Times cited: 19
DOI: 10.1039/C6CP06882K
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“RAMS and WRF sensitivity to grid spacing in large-eddy simulations of the dry convective boundary layer”. Ercolani G, Gorle C, Garcia Sánchez C, Corbari C, Mancini M, Computers and fluids 123, 54 (2015). http://doi.org/10.1016/j.compfluid.2015.09.009
Abstract: Large-eddy simulations (LESS) are frequently used to model the planetary boundary layer, and the choice of the grid cell size, numerical schemes and sub grid model can significantly influence the simulation results. In the present paper the impact of grid spacing on LES of an idealized atmospheric convective boundary layer (CBL), for which the statistics and flow structures are well understood, is assessed for two mesoscale models: the Regional Atmospheric Modeling System (RAMS) and the Weather Research and Forecasting model (WRF). Nine simulations are performed on a fixed computational domain (6 x 6 x 2 km), combining three different horizontal (120, 60, 30 m) and vertical (20, 10, 5 m) spacings. The impact of the cell size on the CBL is investigated by comparing turbulence statistics and velocity spectra. The results demonstrate that both WRF and RAMS can perform LES of the CBL under consideration without requiring extremely high computational loads, but they also indicate the importance of adopting a computational grid that is adequate for the numerical schemes and subgrid models used. In both RAMS and WRF a horizontal cell size of 30 m is required to obtain a suitable turbulence reproduction throughout the CBL height. Considering the vertical grid spacing, WRF produced similar results for all the three tested values, while in RAMS it should be ensured that the aspect ratio of the cells does not exceed a value of 3. The two models were found to behave differently in function of the grid resolution, and they have different shortcomings in their prediction of CBL turbulence. WRF exhibits enhanced damping at the smallest scales, while RAMS is prone to the appearance of spurious fluctuations in the flow when the grid aspect ratio is too high. (C) 2015 Elsevier Ltd. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.313
Times cited: 3
DOI: 10.1016/j.compfluid.2015.09.009
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“Rationalizing the influence of the Mn(IV)/Mn(III) red-Ox transition on the electrocatalytic activity of manganese oxides in the oxygen reduction reaction”. Ryabova AS, Napolskiy FS, Poux T, Istomin SY, Bonnefont A, Antipin DM, Baranchikov AY, Levin EE, Abakumov AM, Kéranguéven G, Antipov EV, Tsirlina GA, Savinova ER;, Electrochimica acta 187, 161 (2016). http://doi.org/10.1016/j.electacta.2015.11.012
Abstract: Knowledge on the mechanisms of oxygen reduction reaction (ORR) and descriptors linking the catalytic activity to the structural and electronic properties of transition metal oxides enable rational design of more efficient catalysts. In this work ORR electrocatalysis was studied on a set of single and complex Mn (III) oxides with a rotating disc electrode method and cyclic voltammetry. We discovered an exponential increase of the specific electrocatalytic activity with the potential of the surface Mn(IV)/Mn(III) red-ox couple, suggesting the latter as a new descriptor for the ORR electrocatalysis. The observed dependence is rationalized using a simple mean-field kinetic model considering availability of the Mn( III) centers and adsorbate-adsorbate interactions. We demonstrate an unprecedented activity of Mn2O3, ca. 40 times exceeding that of MnOOH and correlate the catalytic activity of Mn oxides to their crystal structure. (C) 2015 Elsevier Ltd. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.798
Times cited: 51
DOI: 10.1016/j.electacta.2015.11.012
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“Self-assembly of gas-phase synthesized magnesium nanoparticles on room temperature substrates”. Venturi F, Calizzi M, Bals S, Perkisas T, Pasquini L, Materials research express 2, 015007 (2015). http://doi.org/10.1088/2053-1591/2/1/015007
Abstract: Magnesium nanoparticles (NPs) with initial size in the 10-50 nmrange were synthesized by inert gas condensation under helium flow and deposited on room temperature substrates. The morphology and crystal structure of the NPs ensemble were investigated as a function of the deposition time by complementary electron microscopy techniques, including high resolution imaging and chemical mapping. With increasing amount of material, strong coarsening phenomena were observed at room temperature: small NPs disappeared while large faceted NPs developed, leading to a 5-fold increase of the average NPs size within a few minutes. The extent of coarsening and the final morphology depended also on the nature of the substrate. Furthermore, large single-crystal NPs were seen to arise from the self-organization of primary NPs units, providing a mechanism for crystal growth. The dynamics of the self-assembly process involves the basic steps of NPs sticking, diffusion on substrate, coordinated rotation and attachment/coalescence. Key features are the surface energy anisotropy, reflected by the faceted shape of the NPs, and the low melting point of the material. The observed phenomena have strong implications in relation to the synthesis and stability of nanostructures based on Mg or other elements with similar features.
Keywords: A1 Journal article; Engineering Management (ENM); Electron microscopy for materials research (EMAT)
Impact Factor: 1.068
Times cited: 14
DOI: 10.1088/2053-1591/2/1/015007
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“Solution-derived YBa2Cu3O7-\delta (YBCO) superconducting films with BaZrO3 (BZO) nanodots based on reverse micelle stabilized nanoparticles”. Bretos I, Schneller T, Falter M, Baecker M, Hollmann E, Woerdenweber R, Molina-Luna L, Van Tendeloo G, Eibl O, Journal of materials chemistry C : materials for optical and electronic devices 3, 3971 (2015). http://doi.org/10.1039/c4tc02543a
Abstract: Superconducting YBa2Cu3O7-delta (YBCO) films with artificial BaZrO3 (BZO) nanodots were prepared using a chemical solution deposition method involving hybrid solutions composed of trifluoroacetate-based YBCO precursors and reverse micelle stabilized BZO nanoparticle dispersions. Microemulsion-mediated synthesis was used to obtain nano-sized (similar to 12 nm) and mono-dispersed BZO nanoparticles that preserve their features once introduced into the YBCO solution, as revealed by dynamic light scattering. Phase pure, epitaxial YBCO films with randomly oriented BZO nanodots distributed over their whole microstructure were grown from the hybrid solutions on (100) LaAlO3 substrates. The morphology of the YBCO-BZO nanocomposite films was strongly influenced by the amount of nanoparticles incorporated into the system, with contents ranging from 5 to 40 mol%. Scanning electron microscopy showed a high density of isolated second-phase defects consisting of BZO nanodots in the nanocomposite film with 10 mol% of BZO. Furthermore, a direct observation and quantitative analysis of lattice defects in the form of interfacial edge dislocations directly induced by the BZO nanodots was evidenced by transmission electron microscopy. The superconducting properties (77 K) of the YBCO films improved considerably by the presence of such nanodots, which seem to enhance the morphology of the sample and therefore the intergranular critical properties. The incorporation of preformed second-phase defects (here, BZO) during the growth of the superconducting phase is the main innovation of this novel approach for the all-solution based low-cost fabrication of long-length coated conductors.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 5.256
Times cited: 19
DOI: 10.1039/c4tc02543a
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“Square-centimeter-sized high-efficiency polymer solar cells : how the processing atmosphere and film quality influence performance at large scale”. Ben Dkhil S, Pfannmöller M, Bals S, Koganezawa T, Yoshimoto N, Hannani D, Gaceur M, Videlot-Ackermann C, Margeat O, Ackermann J, Laser physics review 6, 1600290 (2016). http://doi.org/10.1002/aenm.201600290
Abstract: Organic solar cells based on two benzodithiophene-based polymers (PTB7 and PTB7-Th) processed at square centimeter-size under inert atmosphere and ambient air, respectively, are investigated. It is demonstrated that the performance of solar cells processed under inert atmosphere is not limited by the upscaling of photoactive layer and the interfacial layers. Thorough morphological and electrical characterizations of optimized layers and corresponding devices reveal that performance losses due to area enlargement are only caused by the sheet resistance of the transparent electrode reducing the effi ciency from 9.3% of 7.8% for PTB7-Th in the condition that both photoactive layer and the interfacial layers are of high layer quality. Air processing of photoactive layer and the interfacial layers into centimeter-sized solar cells lead to additional, but only slight, losses (< 10%) in all photovoltaic parameters, which can be addressed to changes in the electronic properties of both active layer and ZnO layers rather than changes in layer morphology. The demonstrated compatibility of polymer solar cells using solution-processed photoactive layer and interfacial layers with large area indicates that the introduction of a standard active area of 1 cm(2) for measuring effi ciency of organic record solar cells is feasible. However electric standards for indium tin oxides (ITO) or alternative transparent electrodes need to be developed so that performance of new photovoltaic materials can be compared at square centimeter-size.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 16.721
Times cited: 6
DOI: 10.1002/aenm.201600290
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“Strong attachment of circadian pacemaker neurons on modified ultrananocrystalline diamond surfaces”. Voss A, Wei HY, Zhang Y, Turner S, Ceccone G, Reithmaier JP, Stengl M, Popov C, Materials science and engineering: part C: biomimetic materials 64, 278 (2016). http://doi.org/10.1016/j.msec.2016.03.092
Abstract: Diamond is a promising material for a number of bio-applications, including the fabrication of platforms for attachment and investigation of neurons and of neuroprostheses, such as retinal implants. In the current work ultrananocrystalline diamond (UNCD) films were deposited by microwave plasma chemical vapor deposition, modified by UV/O-3 treatment or NH3 plasma, and comprehensively characterized with respect to their bulk and surface properties, such as crystallinity, topography, composition and chemical bonding nature. The interactions of insect circadian pacemaker neurons with UNCD surfaces with H-, O- and NH2-terminations were investigated with respect to cell density and viability. The fast and strong attachment achieved without application of adhesion proteins allowed for advantageous modification of dispersion protocols for the preparation of primary cell cultures. Centrifugation steps, which are employed for pelletizing dispersed cells to separate them from dispersing enzymes, easily damage neurons. Now centrifugation can be avoided since dispersed neurons quickly and strongly attach to the UNCD surfaces. Enzyme solutions can be easily washed off without losing many of the dispersed cells. No adverse effects on the cell viability and physiological responses were observed as revealed by calcium imaging. Furthermore, the enhanced attachment of the neurons, especially on the modified UNCD surfaces, was especially advantageous for the immunocytochemical procedures with the cell cultures. The cell losses during washing steps were significantly reduced by one order of magnitude in comparison to controls. In addition, the integration of a titanium grid structure under the UNCD films allowed for individual assignment of physiologically characterized neurons to immunocytochemically stained cells. Thus, employing UNCD surfaces free of foreign proteins improves cell culture protocols and immunocytochemistry with cultured cells. The fast and strong attachment of neurons was attributed to a favorable combination of topography, surface chemistry and wettability. (C) 2016 Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.164
Times cited: 7
DOI: 10.1016/j.msec.2016.03.092
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“Structural, electrochemical and magnetic properties of a novel KFeSO4F polymorph”. Lander L, Rousse G, Abakumov AM, Sougrati M, Van Tendeloo G, Tarascon J-M, Journal of materials chemistry A : materials for energy and sustainability 3, 19754 (2015). http://doi.org/10.1039/c5ta05548b
Abstract: In the quest for sustainable and low-cost positive electrode materials for Li-ion batteries, we discovered, as reported herein, a new low temperature polymorph of KFeSO4F. Contrary to the high temperature phase crystallizing in a KTiOPO4-like structure, this new phase adopts a complex layer-like structure built on FeO4F2 octahedra and SO4 tetrahedra, with potassium cations located in between the layers, as solved using neutron and synchrotron diffraction experiments coupled with electron diffraction. The detailed analysis of the structure reveals an alternation of edge-and corner-shared FeO4F2 octahedra leading to a large monoclinic cell of 1771.774(7) angstrom(3). The potassium atoms are mobile within the structure as deduced by ionic conductivity measurements and confirmed by the bond valence energy landscape approach thus enabling a partial electrochemical removal of K+ and uptake of Li+ at an average potential of 3.7 V vs. Li+/Li-0. Finally, neutron diffraction experiments coupled with SQUID measurements reveal a long range antiferromagnetic ordering of the Fe2+ magnetic moments below 22 K with a possible magnetoelectric behavior.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 8.867
Times cited: 11
DOI: 10.1039/c5ta05548b
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“Synthesis and cation distribution in the new bismuth oxyhalides with the Sillen-Aurivillius intergrowth structures”. Charkin DO, Akinfiev VS, Alekseeva AM, Batuk M, Abakumov AM, Kazakov SM, Journal of the Chemical Society : Dalton transactions 44, 20568 (2015). http://doi.org/10.1039/c5dt02620b
Abstract: About 20 new compounds with the Sillen-Aurivillius intergrowth structure, (MeMeBi3Nb2O11X)-Me-1-Bi-2 (Me-1 = Pb, Sr, Ba; Me-2 = Ca, Sr, Ba; X = Cl, Br, I), have been prepared. They are composed of stacking of [ANb(2)O(7)] perovskite blocks, fluorite-type [M2O2] blocks and halogen sheets. The cation distribution between the fluorite and perovskite layers has been studied for Ba2Bi3Nb2O11I, Ca1.25Sr0.75Bi3Nb2O11Cl, BaCaBi3Nb2O11Br and Sr2Bi3Nb2O11Cl. The smaller Me cations tend to reside in the perovskite block while the larger ones are situated in the fluorite-type block. The distribution of the elements was confirmed for BaCaBi3Nb2O11Br using energy dispersive X-ray analysis combined with scanning transmission electron microscopy (STEM-EDX). An electron diffraction study of this compound reveals a local symmetry lowering caused by weakly correlated rotation of NbO6 octahedra. Based on our findings, we suggest a new stability criterion for mixed-layer structures, which is that net charges of any two consecutive layers do not compensate for each other and only the whole layer sequence is electroneutral.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.029
Times cited: 5
DOI: 10.1039/c5dt02620b
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“Synthesis, structure and magnetic ordering of the mullite-type Bi2Fe4-xCrxO9 solid solutions with a frustrated pentagonal Cairo lattice”. Rozova MG, Grigoriev VV, Bobrikov IA, Filimonov DS, Zakharov KV, Volkova OS, Vasiliev AN, Antipov EV, Tsirlin AA, Abakumov AM, Journal of the Chemical Society : Dalton transactions 45, 1192 (2016). http://doi.org/10.1039/c5dt04296h
Abstract: Highly homogeneous mullite-type solid solutions Bi2Fe4-xCrxO9 (x = 0.5, 1, 1.2) were synthesized using a soft chemistry technique followed by a solid-state reaction in Ar. The crystal structure of Bi2Fe3CrO9 was investigated using X-ray and neutron powder diffraction, transmission electron microscopy and Fe-57 Mossbauer spectroscopy (S.G. Pbam, a = 7.95579(9) angstrom , b = 8.39145(9) angstrom, c = 5.98242(7) angstrom, R-F(X-ray) = 0.022, R-F(neutron) = 0.057). The ab planes in the structure are tessellated with distorted pentagonal loops built up by three tetrahedrally coordinated Fe sites and two octahedrally coordinated Fe/Cr sites, linked together in the ab plane by corner-sharing forming a pentagonal Cairo lattice. Magnetic susceptibility measurements and powder neutron diffraction show that the compounds order antiferromagnetically (AFM) with the Neel temperatures decreasing upon increasing the Cr content from T-N similar to 250 K for x = 0 to T-N similar to 155 K for x = 1.2. The magnetic structure of Bi2Fe3CrO9 at T = 30 K is characterized by a propagation vector k = (1/2,1/2,1/2). The tetrahedrally coordinated Fe cations form singlet pairs within dimers of corner-sharing tetrahedra, but spins on the neighboring dimers are nearly orthogonal. The octahedrally coordinated (Fe, Cr) cations form antiferromagnetic up-up-down-down chains along c, while the spin arrangement in the ab plane is nearly orthogonal between nearest neighbors and collinear between second neighbors. The resulting magnetic structure is remarkably different from the one in pure Bi2Fe4O9 and features several types of spin correlations even on crystallographically equivalent exchange that may be caused by the simultaneous presence of Fe and Cr on the octahedral site.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.029
DOI: 10.1039/c5dt04296h
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“Pb2MnTeO6 double perovskite : an antipolar anti-ferromagnet”. Retuerto M, Skiadopoulou S, Li MR, Abakumov AM, Croft M, Ignatov A, Sarkar T, Abbett BM, Pokorný, J, Savinov M, Nuzhnyy D, Prokleška J, Abeykoon M, Stephens PW, Hodges JP, Vaněk P, Fennie CJ, Rabe KM, Kamba S, Greenblatt M;, Inorganic chemistry 55, 4320 (2016). http://doi.org/10.1021/acs.inorgchem.6b00054
Abstract: Pb2MnTeO6, a new double perovskite, was synthesized. Its crystal structure was determined by synchrotron X-ray and powder neutron diffraction. Pb2MnTeO6 is monoclinic (I2/m) at room temperature with a regular arrangement of all the cations in their polyhedra. However, when the temperature is lowered to similar to 120 K it undergoes a phase transition from I2/m to C2/c structure. This transition is accompanied by a displacement of the Pb atoms from the center of their polyhedra due to the 6s2 lone-pair electrons, together with a surprising off-centering of Mn2+ (d5) magnetic cations. This strong first-order phase transition is also evidenced by specific heat, dielectric, Raman, and infrared spectroscopy measurements. The magnetic characterizations indicate an anti-ferromagnetic (AFM) order below TN approximate to 20 K; analysis of powder neutron diffraction data confirms the magnetic structure with propagation vector k = (0 1 0) and collinear AFM spins. The observed jump in dielectric permittivity near similar to 150 K implies possible anti-ferroelectric behavior; however, the absence of switching suggests that Pb2MnTeO6 can only be antipolar. First-principle calculations confirmed that the crystal and magnetic structures determined are locally stable and that anti-ferroelectric switching is unlikely to be observed in Pb2MnTeO6.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.857
Times cited: 9
DOI: 10.1021/acs.inorgchem.6b00054
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“Texturing of hydrothermally synthesized BaTiO3 in a strong magnetic field by slip casting”. Özen M, Mertens M, Snijkers F, Van Tendeloo G, Cool P, Ceramics international 42, 5382 (2016). http://doi.org/10.1016/j.ceramint.2015.12.073
Abstract: Barium titanate powder was processed by slip casting in a rotating strong magnetic field of 9.4 T. The orientation factor of the sintered compact was analyzed by the X-ray diffraction technique and the microstructure (grain-size) was analyzed by scanning electron microscope. The hydrothermally prepared barium titanate was used as matrix material and the molten-salt synthesized barium titanate, with a larger particle-size, was used as template for the templated grain-growth process. Addition of large template particles was observed to increase the orientation factor of the sintered cast (5 vol% loading). Template particles acted as starting grains for the abnormal grain-growth process and the average grain-size was increased after sintering. Increasing the solid loading (15 vol%) resulted in a similar orientation factor with a decrease of the average grain size by more than half. However, addition of templates to the 15 vol% cast had a negative effect on the orientation factor. The impingement of growing particles was stated as the primary cause of particle misorientation resulting in a low orientation factor after sintering. Different heating conditions were tested and it was determined that a slow heating rate gave the highest orientation factor, the smallest average grain-size and the highest relative density. (C) 2015 Elsevier Ltd and Techna Group S.r.l. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA)
Impact Factor: 2.986
Times cited: 11
DOI: 10.1016/j.ceramint.2015.12.073
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Altantzis T (2015) Three-dimensional characterization of atomic clusters, nanoparticles and their assemblies by advanced transmission electron microscopy. Antwerpen
Keywords: Doctoral thesis; Electron microscopy for materials research (EMAT)
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“Topochemical nitridation with anion vacancy -assisted N3-/O2- exchange”. Mikita R, Aharen T, Yamamoto T, Takeiri F, Ya T, Yoshimune W, Fujita K, Yoshida S, Tanaka K, Batuk D, Abakumov AM, Brown CM, Kobayashi Y, Kageyama H;, Journal of the American Chemical Society 138, 3211 (2016). http://doi.org/10.1021/jacs.6b00088
Abstract: We present how the introduction of anion vacancies in oxyhydrides enables a route to access new oxynitrides, by conducting ammonolysis of perovskite oxyhydride EuTiO3-xHx (x similar to 0.18). At 400 degrees C, similar to our studies on BaTiO3-xHx, hydride lability enables a low temperature direct ammonolysis of EUTi3.82+O-2.82/H-0.18, leading to the N3-/H--exchanged product EuTi4+O2.82No0.12 square 0.06 center dot When the ammonolysis temperature was increased up to 800 degrees C, we observed a further nitridation involving N3-/O2- exchange, yielding a fully oxidized Eu3+Ti4+O2N with the GdFeO3-type distortion (Pnma) as a metastable phase, instead of pyrochlore structure. Interestingly, the same reactions using the oxide EuTiO3 proceeded through a 1:1 exchange of N3- with O-2 only above 600 degrees C and resulted in incomplete nitridation to EuTi02.25N0.75, indicating that anion vacancies created during the initial nitridation process of EuTiO2.82H0.18 play a crucial role in promoting anion (N3-/O2-) exchange at high temperatures. Hence, by using (hydride-induced) anion-deficient precursors, we should be able to expand the accessible anion composition of perovskite oxynitrides.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 13.858
Times cited: 28
DOI: 10.1021/jacs.6b00088
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“UV effect on NO2 sensing properties of nanocrystalline In2O3”. Ilin A, Martyshov M, Forsh E, Forsh P, Rumyantseva M, Abakumov A, Gaskov A, Kashkarov P, Sensors and actuators : B : chemical 231, 491 (2016). http://doi.org/10.1016/j.snb.2016.03.051
Abstract: Nanocrystalline indium oxide films with extremely small grains in range of 7-40 nm are prepared by sol-gel method. The influence of grain size on the sensitivity of indium oxide to nitrogen dioxide in low concentration at room temperature is investigated under the UV illumination and without illumination. The sensitivity increases with the decrease of grain sizes when In2O3 is illuminated while in the dark In2O3 with intermediate grain size exhibits the highest response. An explanation of the different behavior of the In2O3 with different grain size sensitivity to NO2 under illumination and in the dark is proposed. We demonstrate that pulsed illumination may be used for NO2 detection at room temperature that significantly reduces the power consumption of sensor. (C) 2016 Elsevier B.V. All rights reserved.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 5.401
Times cited: 27
DOI: 10.1016/j.snb.2016.03.051
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“Water electrolysis on La1-xSrxCoO3-\delta perovskite electrocatalysts”. Mefford JT, Rong X, Abakumov AM, Hardin WG, Dai S, Kolpak AM, Johnston KP, Stevenson KJ, Nature communications 7, 11053 (2016). http://doi.org/10.1038/ncomms11053
Abstract: Perovskite oxides are attractive candidates as catalysts for the electrolysis of water in alkaline energy storage and conversion systems. However, the rational design of active catalysts has been hampered by the lack of understanding of the mechanism of water electrolysis on perovskite surfaces. Key parameters that have been overlooked include the role of oxygen vacancies, B-O bond covalency, and redox activity of lattice oxygen species. Here we present a series of cobaltite perovskites where the covalency of the Co-O bond and the concentration of oxygen vacancies are controlled through Sr2+ substitution into La1 – xSrxCoO3 – delta. We attempt to rationalize the high activities of La1 – xSrxCoO3 – delta through the electronic structure and participation of lattice oxygen in the mechanism of water electrolysis as revealed through ab initio modelling. Using this approach, we report a material, SrCoO2.7, with a high, room temperature-specific activity and mass activity towards alkaline water electrolysis.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 12.124
Times cited: 278
DOI: 10.1038/ncomms11053
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“Hematite-based nanocomposites for light-activated applications: Synergistic role of TiO2 and Au introduction”. Carraro G, Maccato C, Gasparotto A, Warwick MEA, Sada C, Turner S, Bazzo A, Andreu T, Pliekhova O, Korte D, Lavrenčič, Štangar U, Van Tendeloo G, Morante JR, Barreca D, Solar energy materials and solar cells 159, 456 (2017). http://doi.org/10.1016/j.solmat.2016.09.037
Abstract: Photo-activated processes have been widely recognized as cost-effective and environmentally friendly routes for both renewable energy generation and purification/cleaning technologies. We report herein on a plasma- assisted approach for the synthesis of Fe 2 O 3 -TiO 2 nanosystems functionalized with Au nanoparticles. Fe 2 O 3 nanostructures were grown by plasma enhanced-chemical vapor deposition, followed by the sequential sputtering of titanium and gold under controlled conditions, and final annealing in air. The target nanosystems were subjected to a thorough multi-technique characterization, in order to elucidate the interrelations between their chemico-physical properties and the processing conditions. Finally, the functional performances were preliminarily investigated in both sunlight-assisted H 2 O splitting and photocatalytic activity tests in view of self- cleaning applications. The obtained results highlight the possibility of tailoring the system behaviour and candidate the present Fe 2 O 3 -TiO 2 -Au nanosystems as possible multi-functional low-cost platforms for light-activated processes.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 4.784
Times cited: 15
DOI: 10.1016/j.solmat.2016.09.037
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“Shape Control of Colloidal Cu2-x S Polyhedral Nanocrystals by Tuning the Nucleation Rates”. van der Stam W, Gradmann S, Altantzis T, Ke X, Baldus M, Bals S, de Mello Donega C, Chemistry of materials 28, 6705 (2016). http://doi.org/10.1021/acs.chemmater.6b03098
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.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 9.466
Times cited: 27
DOI: 10.1021/acs.chemmater.6b03098
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