“Nitrogen control in nanodiamond produced by detonation shock-wave-assisted synthesis”. Shenderova OA, Vlasov II, Turner S, Van Tendeloo G, Orlinskii SB, Shiryaev AA, Khomich AA, Sulyanov SN, Jelezko F, Wrachtrup J, The journal of physical chemistry: C : nanomaterials and interfaces 115, 14014 (2011). http://doi.org/10.1021/jp202057q
Abstract: Development of efficient production methods of nanodiamond (ND) particles containing substitutional nitrogen and nitrogen-vacancy (NV) complexes remains an important goal in the nanodiamond community. ND synthesized from explosives is generally not among the preferred candidates for imaging applications owing to lack of optically active particles containing NV centers. In this paper, we have systematically studied representative classes of NDs produced by detonation shock wave conversion of different carbon precursor materials, namely, graphite and a graphite/hexogen mixture into ND, as well as ND produced from different combinations of explosives using different cooling methods (wet or dry cooling). We demonstrate that (i) the N content in nanodiamond particles can be controlled through a correct selection of the carbon precursor material (addition of graphite, explosives composition); (ii) particles larger than approximately 20 nm may contain in situ produced optically active NV centers, and (iii) in ND produced from explosives, NV centers are detected only in ND produced by wet synthesis. ND synthesized from a mixture of graphite/explosive contains the largest amount of NV centers formed during synthesis and thus deserves special attention.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.536
Times cited: 54
DOI: 10.1021/jp202057q
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“Identification of substitutional nitrogen and surface paramagnetic centers in nanodiamond of dynamic synthesis by electron paramagnetic resonance”. Orlinskii SB, Bogomolov RS, Kiyamova AM, Yavkin BV, Mamin GM, Turner S, Van Tendeloo G, Shiryaev AA, Vlasov II, Shenderova O, Nanoscience and nanotechnology letters 3, 63 (2011). http://doi.org/10.1166/nnl.2011.1121
Abstract: Production of nanodiamond particles containing substitutional nitrogen is important for a wide variety of advanced applications. In the current work nanodiamond particles synthesized from a mixture of graphite and hexogen were analyzed to determine the presence of substitutional nitrogen using pulsed electron paramagnetic resonance (EPR) spectroscopy. Nitrogen paramagnetic centers in the amount of 1.2 ppm have been identified. The spin relaxation characteristics for both nitrogen and surface defects are also reported. A new approach for efficient depletion of the strong non-nitrogen EPR signal in nanodiamond material by immersing nanodiamond particles into ice matrix is suggested. This approach allows an essential decrease of the spin relaxation time of the dominant non-nitrogen defects, while preserving the substitutional nitrogen spin relaxation time.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 1.889
Times cited: 14
DOI: 10.1166/nnl.2011.1121
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“Solving the structure of Li ion battery materials with precession electron diffraction : application to Li2CoPo4F”. Hadermann J, Abakumov AM, Turner S, Hafideddine Z, Khasanova NR, Antipov EV, Van Tendeloo G, Chemistry of materials 23, 3540 (2011). http://doi.org/10.1021/cm201257b
Abstract: The crystal structure of the Li2CoPO4F high-voltage cathode for Li ion rechargeable batteries has been completely solved from precession electron diffraction (PED) data, including the location of the Li atoms. The crystal structure consists of infinite chains of CoO4F2 octahedra sharing common edges and linked into a 3D framework by PO4 tetrahedra. The chains and phosphate anions together delimit tunnels filled with the Li atoms. This investigation demonstrates that PED can be successfully applied for obtaining structural information on a variety of Li-containing electrode materials even from single micrometer-sized crystallites.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 9.466
Times cited: 46
DOI: 10.1021/cm201257b
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“Graphitic nanocrystals inside the pores of mesoporous silica : synthesis, characterization and an adsorption study”. de Clippel F, Harkiolakis A, Vosch T, Ke X, Giebeler L, Oswald S, Houthoofd K, Jammaer J, Van Tendeloo G, Martens JA, Jacobs PA, Baron GV, Sels BF, Denayer JFM, Microporous and mesoporous materials: zeolites, clays, carbons and related materials 144, 120 (2011). http://doi.org/10.1016/j.micromeso.2011.04.003
Abstract: This work presents a new carbonsilica hybrid material, denoted as CSM, with remarkable sorption properties. It consists of intraporous graphitic nanocrystals grown in the pores of mesoporous silica. CSM is obtained by a subtle incipient wetness impregnation of Al-containing mesoporous silica with furfuryl alcohol (FA)/hemelitol solutions. Both the volume match of the impregnation solution with that of the silica template pore volume, and the presence of Al3+ in the silica, are crucial to polymerize FA selectively inside the mesopores. Carbonization of the intraporous polymer was then performed by pyrolysis under He up to 1273 K. The resulting CSMs were examined by SEM, HRTEM, 27Al MAS NMR, N2 adsorption, XRD, TGA, TPD, XPS, pycnometry and Raman spectroscopy. Mildly oxidized graphitic-like carbon nanoblocks, consisting of a few graphene-like sheets, were thus identified inside the template mesopores. Random stacking of these carbon crystallites generates microporosity resulting in biporous materials at low carbon content and microporous materials at high carbon loadings. Very narrow pore distributions were obtained when pyrolysis was carried out under slow heating rate, viz. 1 K min−1. Adsorption and shape selective properties of the carbon filled mesoporous silica were studied by performing pulse chromatography and breakthrough experiments, and by measuring adsorption isotherms of linear and branched alkanes. Whereas the parent mesoporous silica shows unselective adsorption, their CSM analogues preferentially adsorb linear alkanes. The sorption capacity and selectivity can be adjusted by changing the pore size of the template or by varying the synthesis conditions. A relation between the carbon crystallites size and the shape selective behaviour of the corresponding CSM for instance is demonstrated. Most interestingly, CSM shows separation factors for linear and branched alkanes up to values comparable to those of zeolitic molecular sieves.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.615
Times cited: 15
DOI: 10.1016/j.micromeso.2011.04.003
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“High resolution mapping of surface reduction in ceria nanoparticles”. Turner S, Lazar S, Freitag B, Egoavil R, Verbeeck J, Put S, Strauven Y, Van Tendeloo G, Nanoscale 3, 3385 (2011). http://doi.org/10.1039/c1nr10510h
Abstract: Surface reduction of ceria nano octahedra with predominant {111} and {100} type surfaces is studied using a combination of aberration-corrected Transmission Electron Microscopy (TEM) and spatially resolved electron energy-loss spectroscopy (EELS) at high energy resolution and atomic spatial resolution. The valency of cerium ions at the surface of the nanoparticles is mapped using the fine structure of the Ce M4,5 edge as a fingerprint. The valency of the surface cerium ions is found to change from 4+ to 3+ owing to oxygen deficiency (vacancies) close to the surface. The thickness of this Ce3+ shell is measured using atomic-resolution Scanning Transmission Electron Microscopy (STEM)-EELS mapping over a {111} surface (the predominant facet for this ceria morphology), {111} type surface island steps and {100} terminating planes. For the {111} facets and for {111} surface islands, the reduction shell is found to extend over a single fully reduced surface plane and 12 underlying mixed valency planes. For the {100} facets the reduction shell extends over a larger area of 56 oxygen vacancy-rich planes. This finding provides a plausible explanation for the higher catalytic activity of the {100} surface facets in ceria.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 7.367
Times cited: 127
DOI: 10.1039/c1nr10510h
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“Selective organic functionalization of graphene bulk or graphene edges”. Quintana M, Montellano A, Esau del Rio Castillo A, Van Tendeloo G, Bittencourt C, Prato M, Chemical communications 47, 9330 (2011). http://doi.org/10.1039/c1cc13254g
Abstract: Graphene sheets have been functionalized with a PAMAM dendron, finding that graphene can be efficiently functionalized all over the surface, or only at the edges, depending on the reactions used in the functionalization process.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 6.319
Times cited: 84
DOI: 10.1039/c1cc13254g
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“Three-dimensional atomic imaging of colloidal core-shell nanocrystals”. Bals S, Casavola M, van Huis MA, Van Aert S, Batenburg KJ, Van Tendeloo G, Vanmaekelbergh D, Nano letters 11, 3420 (2011). http://doi.org/10.1021/nl201826e
Abstract: Colloidal coreshell semiconductor nanocrystals form an important class of optoelectronic materials, in which the exciton wave functions can be tailored by the atomic configuration of the core, the interfacial layers, and the shell. Here, we provide a trustful 3D characterization at the atomic scale of a free-standing PbSe(core)CdSe(shell) nanocrystal by combining electron microscopy and discrete tomography. Our results yield unique insights for understanding the process of cation exchange, which is widely employed in the synthesis of coreshell nanocrystals. The study that we present is generally applicable to the broad range of colloidal heteronanocrystals that currently emerge as a new class of materials with technological importance.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Vision lab
Impact Factor: 12.712
Times cited: 121
DOI: 10.1021/nl201826e
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“Light-assisted nucleation of silver nanowires during polyol synthesis”. Lin H, Ohta T, Paul A, Hutchison JA, Kirilenko D, Lebedev O, Van Tendeloo G, Hofkens J, Uji-i H, Journal of photochemistry and photobiology: A: chemistry 221, 220 (2011). http://doi.org/10.1016/j.jphotochem.2011.04.015
Abstract: This report describes the effect of light irradiation on the synthesis of silver nanowires by the well-known polyol method. High quality nanowires are produced in high yields when the reaction suspension is irradiated with 400500 nm light during the nucleation stage. These studies suggest that light accelerates the formation of the nanoparticle seeds most appropriate for nanowire growth.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.625
Times cited: 24
DOI: 10.1016/j.jphotochem.2011.04.015
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“Quantum cutting in Li (770 nm) and Yb (1000 nm) co-dopant emission bands by energy transfer from the ZnO nano-crystalline host”. Shestakov MV, Tikhomirov VK, Kirilenko D, Kuznetsov AS, Chibotaru LF, Baranov AN, Van Tendeloo G, Moshchalkov VV, Optics express 19, 15955 (2011). http://doi.org/10.1364/OE.19.015955
Abstract: Li-Yb co-doped nano-crystalline ZnO has been synthesized by a method of thermal growth from the salt mixtures. X-ray diffraction, transmission electron microscopy, atomic absorption spectroscopy and optical spectroscopy confirm the doping and indicate that the dopants may form Li-Li and Yb3+-Li based nanoclusters. When pumped into the conduction and exciton absorption bands of ZnO between 250 to 425 nm, broad emission bands of about 100 nm half-height-width are excited around 770 and 1000 nm, due to Li and Yb dopants, respectively. These emission bands are activated by energy transfer from the ZnO host mostly by quantum cutting processes, which generate pairs of quanta in Li (770 nm) and Yb (1000 nm) emission bands, respectively, out of one quantum absorbed by the ZnO host. These quantum cutting phenomena have great potential for application in the down-conversion layers coupled to the Si solar cells.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.307
Times cited: 19
DOI: 10.1364/OE.19.015955
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“2D atomic mapping of oxidation states in transition metal oxides by scanning transmission electron microscopy and electron energy-loss spectroscopy”. Tan H, Turner S, Yücelen E, Verbeeck J, Van Tendeloo G, Physical review letters 107, 107602 (2011). http://doi.org/10.1103/PhysRevLett.107.107602
Abstract: Using a combination of high-angle annular dark-field scanning transmission electron microscopy and atomically resolved electron energy-loss spectroscopy in an aberration-corrected transmission electron microscope we demonstrate the possibility of 2D atom by atom valence mapping in the mixed valence compound Mn3O4. The Mn L2,3 energy-loss near-edge structures from Mn2+ and Mn3+ cation sites are similar to those of MnO and Mn2O3 references. Comparison with simulations shows that even though a local interpretation is valid here, intermixing of the inelastic signal plays a significant role. This type of experiment should be applicable to challenging topics in materials science, such as the investigation of charge ordering or single atom column oxidation states in, e.g., dislocations.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 8.462
Times cited: 115
DOI: 10.1103/PhysRevLett.107.107602
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“Uniform patterns of Fe-vacancy ordering in the Kx(Fe,Co)2-ySe2 superconductors”. Kazakov SM, Abakumov AM, Perz-Mato JM, Ovchinnikov AV, Roslova MV, Boltalin AI, Morozov IV, Antipov EV, Van Tendeloo G, Chemistry of materials 23, 4311 (2011). http://doi.org/10.1021/cm201203h
Abstract: The Fe-vacancy ordering patterns in the superconducting KxFe2ySe2 and nonsuperconducting Kx(Fe,Co)2ySe2 samples have been investigated by electron diffraction and high angle annular dark field scanning transmission electron microscopy. The Fe-vacancy ordering occurs in the ab plane of the parent ThCr2Si2-type structure, demonstrating two types of patterns. Superstructure I retains the tetragonal symmetry and can be described with the aI = bI = as√5 (as is the unit cell parameter of the parent ThCr2Si2-type structure) supercell and I4/m space group. Superstructure II reduces the symmetry to orthorhombic with the aII = as√2, bII = 2as√2 supercell and the Ibam space group. This type of superstructure is observed for the first time in KxFe2ySe2. The Fe-vacancy ordering is inhomogeneous: the disordered areas interleave with the superstructures I and II in the same crystallite. The observed superstructures represent the compositionally dependent uniform ordering patterns of two species (the Fe atoms and vacancies) on a square lattice. More complex uniform ordered configurations, including compositional stripes, can be predicted for different chemical compositions of the KxFe2ySe2 (0 < y < 0.5) solid solutions.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 9.466
Times cited: 20
DOI: 10.1021/cm201203h
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“Resistive switching at manganite/manganite interfaces”. Kalkert C, Krisponeit J-O, Esseling M, Lebedev OI, Moshnyaga V, Damaschke B, Van Tendeloo G, Samwer K, Applied physics letters 99, 132512 (2011). http://doi.org/10.1063/1.3643425
Abstract: We report bipolar resistive switching between the interfaces of manganite nanocolumns. La0.7Sr0.3MnO3 films were prepared on Al2O3 substrates, where the films grow in nanocolumns from the substrate to the surface. Conductive atomic force microscopy directly detects that the resistive switching is located at the boundaries of the grains. Furthermore, mesoscopic transport measurements reveal a tunnel magnetoresistance. In combination with the resistive switching, this leads to a total of four different resistive states.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.411
Times cited: 10
DOI: 10.1063/1.3643425
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“Article Structure and magnetic properties of BiFe0.75Mn0.25O3 perovskite prepared at ambient and high pressure”. Belik AA, Abakumov AM, Tsirlin AA, Hadermann J, Kim J, Van Tendeloo G, Takayama-Muromachi E, Chemistry of materials 23, 4505 (2011). http://doi.org/10.1021/cm201774y
Abstract: Solid solutions of BiFe1xMnxO3 (0.0 ≤ x ≤ 0.4) were prepared at ambient pressure and at 6 GPa. The ambient-pressure (AP) phases crystallize in space group R3c similarly to BiFeO3. The high-pressure (HP) phases crystallize in space group R3c for x = 0.05 and in space group Pnma for 0.15 ≤ x ≤ 0.4. The structure of HP-BiFe0.75Mn0.25O3 was investigated using synchrotron X-ray powder diffraction, electron diffraction, and transmission electron microscopy. HP-BiFe0.75Mn0.25O3 has a PbZrO3-related √2ap × 4ap × 2√2ap (ap is the parameter of the cubic perovskite subcell) superstructure with a = 5.60125(9) Å, b = 15.6610(2) Å, and c = 11.2515(2) Å similar to that of Bi0.82La0.18FeO3. A remarkable feature of this structure is the unconventional octahedral tilt system, with the primary ab0a tilt superimposed on pairwise clockwise and counterclockwise rotations around the b-axis according to the oioi sequence (o stands for out-of-phase tilt, and i stands for in-phase tilt). The (FeMn)O6 octahedra are distorted, with one longer metaloxygen bond (2.222.23 Å) that can be attributed to a compensation for covalent BiO bonding. Such bonding results in the localization of the lone electron pair on Bi3+ cations, as confirmed by electron localization function analysis. The relationship between HP-BiFe0.75Mn0.25O3 and antiferroelectric structures of PbZrO3 and NaNbO3 is discussed. On heating in air, HP-BiFe0.75Mn0.25O3 irreversibly transforms to AP-BiFe0.75Mn0.25O3 starting from about 600 K. Both AP and HP phases undergo an antiferromagnetic ordering at TN ≈ 485 and 520 K, respectively, and develop a weak net magnetic moment at low temperatures. Additionally, ceramic samples of AP-BiFe0.75Mn0.25O3 show a peculiar phenomenon of magnetization reversal.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 9.466
Times cited: 57
DOI: 10.1021/cm201774y
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“GaN@ZIF-8 : selective formation of gallium nitride quantum dots inside a zinc methylimidazolate framework”. Esken D, Turner S, Wiktor C, Kalidindi SB, Van Tendeloo G, Fischer RA, Journal of the American Chemical Society 133, 16370 (2011). http://doi.org/10.1021/ja207077u
Abstract: The microporous zeolitic imidazolate framework [Zn(MeIM)2; ZIF-8; MeIM = imidazolate-2-methyl] was quantitatively loaded with trimethylamine gallane [(CH3)3NGaH3]. The obtained inclusion compound [(CH3)3NGaH3]@ZIF-8 reveals three precursor molecules per host cavity. Treatment with ammonia selectively yields the caged cyclotrigallazane intermediate (H2GaNH2)3@ZIF-8, and further annealing gives GaN@ZIF-8. This new composite material was characterized with FT-IR spectroscopy, solid-state NMR spectroscopy, powder X-ray diffraction, elemental analysis, (scanning) transmission electron microscopy combined with electron energy-loss spectroscopy, photoluminescence (PL) spectroscopy, and N2 sorption measurements. The data give evidence for the presence of GaN nanoparticles (13 nm) embedded in the cavities of ZIF-8, including a blue-shift of the PL emission band caused by the quantum size effect.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 13.858
Times cited: 82
DOI: 10.1021/ja207077u
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“New insights in the formation of combined zeolitic/mesoporous materials by using a one-pot templating synthesis”. Vernimmen J, Meynen V, Herregods SJF, Mertens M, Lebedev OI, Van Tendeloo G, Cool P, European journal of inorganic chemistry , 4234 (2011). http://doi.org/10.1002/ejic.201100268
Abstract: Zeolitic growth is often absent or occurs in separate phases when synthetic strategies based on the combination of zeolite templates and mesopore templating agents are applied. In this work, zeolitic growth and mesopore formation have been investigated at different temperatures by applying a one-pot templating approach, based on a TS-1 zeolite synthesis whereby part of the microtemplate (tetrapropylammonium hydroxide, TPAOH) is replaced by a mesotemplate (hexadecyltrimethylammonium bromide, CTMABr). Moreover, the synthesis duration and the molar ratio of the microtemplate/mesotemplate have also been studied. The different syntheses clearly show the inherent competitive mechanism between zeolitic growth and mesopore formation. These insights have led to the conclusion that by following a one-pot templating strategy with standard, nonexotic commercial templates, i.e. CTMABr and TPAOH, it is not possible to develop a true hierarchical mesoporous zeolite, meaning a mesoporous siliceous material with highly crystalline zeolitic walls. The resultant materials are instead combined zeolitic/mesoporous composite structures with, however, highly tuneable and controllable porosity characteristics.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA)
Impact Factor: 2.444
Times cited: 7
DOI: 10.1002/ejic.201100268
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“Atomic oxygen functionalization of vertically aligned carbon nanotubes”. Bittencourt C, Navio C, Nicolay A, Ruelle B, Godfroid T, Snyders R, Colomer J-F, Lagos MJ, Ke X, Van Tendeloo G, Suarez-Martinez I, Ewels CP, The journal of physical chemistry: C : nanomaterials and interfaces 115, 20412 (2011). http://doi.org/10.1021/jp2057699
Abstract: Vertically aligned multiwalled carbon nanotubes (v-MWCNTs) are functionalized using atomic oxygen generated in a microwave plasma. X-ray photoelectron spectroscopy depth profile analysis shows that the plasma treatment effectively grafts oxygen exclusively at the v-MWCNT tips. Electron microscopy shows that neither the vertical alignment nor the structure of v-MWCNTs were affected by the plasma treatment. Density functional calculations suggest assignment of XPS C 1s peaks at 286.6 and 287.5 eV, to epoxy and carbonyl functional groups, respectively.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.536
Times cited: 31
DOI: 10.1021/jp2057699
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“A cyclic catalyst pretreatment in CO2 for high yield production of Carbon nanofibers with narrow diameter distribution”. Corthals S, van Noyen J, Liang D, Ke X, Van Tendeloo G, Jacobs P, Sels B, Catalysis letters 141, 1621 (2011). http://doi.org/10.1007/s10562-011-0690-3
Abstract: This paper presents a cyclic catalyst pretreatment process to improve the CNF yield with narrow size distribution by sequentially feeding the CVD reactor with CH4/CO2 mixtures (carbon deposition) and CO2 (carbon removal) prior to the actual growth process. A mechanism based on a break-up of large Ni particles tentatively explains the beneficial effect of the cyclic carbon deposition/removal CVD procedure.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.799
Times cited: 1
DOI: 10.1007/s10562-011-0690-3
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“Multimodal zeolite-beta-based catalysts with a hierarchical, three-level pore structure”. Chen L-H, Li X-Y, Tian G, Li Y, Tan H-Y, Van Tendeloo G, Zhu G-S, Qiu S-L, Yang X-Y, Su B-L, Chemsuschem 4, 1452 (2011). http://doi.org/10.1002/cssc.201100181
Abstract: Hole diggers: The hierarchically structured porous solid-acid catalyst described in this report possess a remarkable pore system, encompassing well-defined macrochannels, interconnected mesopores, intracrystalline mesopores, and tunable zeolite micropores. Importantly, the catalyst exhibits very strong acidity and superior catalytic activity for esterification reactions.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 7.226
Times cited: 33
DOI: 10.1002/cssc.201100181
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“Nickel/carbon composite materials based on expanded graphite”. Afanasov IM, Lebedev OI, Kolozhvary BA, Smirnov AV, Van Tendeloo G, New carbon materials 26, 335 (2011). http://doi.org/10.1016/S1872-5805(11)60085-1
Abstract: Monolithic nickel/carbon (Ni/C) composites were prepared from coal tar pitch-impregnated compressed expanded graphite pre-decorated with NiO particles (EGNiO) by pyrolysis at 550 °C and subsequent steam activation at 800 °C. The microstructural arrangement of the Ni-comprising nanoparticles in the composites was investigated using transmission electron microscopy. The specific surface area and porosity of the composites were analyzed by nitrogen adsorption. The catalytic activity of the composites was compared with the material obtained by the conventional H2 treatment of EGNiO using hydrocracking of 2,2,3-trimethylpentane as a model reaction.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Times cited: 7
DOI: 10.1016/S1872-5805(11)60085-1
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“New anion-conducting solid solutions Bi1-xTex(O,F)2+\delta (x >, 0.5) and glassceramic material on their base”. Prituzhalov VA, Ardashnikova EI, Vinogradov AA, Dolgikh VA, Videau J-J, Fargin E, Abakumov AM, Tarakina NV, Van Tendeloo G, Journal of fluorine chemistry 132, 1110 (2011). http://doi.org/10.1016/j.jfluchem.2011.06.042
Abstract: The anion-excess fluorite-like solid solutions with general composition Bi1−xTex(O,F)2+δ (x > 0.5) have been synthesized by a solid state reaction of TeO2, BiF3 and Bi2O3 at 873 K with following quenching. The homogeneity areas and polymorphism of the I ↔ IV Bi1−xTex(O,F)2+δ phases were investigated. The crystal structure of the low temperature IV-Bi1−xTex(O,F)2+δ phase has been solved using electron diffraction and X-ray powder diffraction (a = 11.53051(9) Å, S.G. Ia-3, RI = 0.046, RP = 0.041). Glass formation area in the Bi2O3BiF3TeO2 (10% TiO2) system was investigated. IVBi1−xTex(O,F)2+δ phase starts to crystallize at short-time (0.53 h) annealing of oxyfluoride glasses at temperatures above Tg (600615 K). The ionic conductivity of the crystalline Bi1−xTex(O,F)2+δ phase and corresponding glass-ceramics was investigated. Activation energy of conductivity Ea = 0.41(2) eV for the IV-Bi1−xTex(O,F)2+δ crystalline samples and Ea = 0.73 eV for the glass-ceramic samples were obtained. Investigation of the oxyfluoride samples with a constant cation ratio demonstrates essential influence of excess fluorine anions on the ionic conductivity.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.101
Times cited: 2
DOI: 10.1016/j.jfluchem.2011.06.042
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“Plasma-assisted synthesis of Ag/ZnO nanocomposites : first example of photo-induced H2 production and sensing”. Simon Q, Barreca D, Bekermann D, Gasparotto A, Maccato C, Comini E, Gombac V, Fornasiero P, Lebedev OI, Turner S, Devi A, Fischer RA, Van Tendeloo G, International journal of hydrogen energy 36, 15527 (2011). http://doi.org/10.1016/j.ijhydene.2011.09.045
Abstract: Ag/ZnO nanocomposites were developed by a plasma-assisted approach. The adopted strategy exploits the advantages of Plasma Enhanced-Chemical Vapor Deposition (PE-CVD) for the growth of columnar ZnO arrays on Si(100) and Al2O3 substrates, in synergy with the infiltration power of the Radio Frequency (RF)-sputtering technique for the subsequent dispersion of different amounts of Ag nanoparticles (NPs). The resulting composites, both as-prepared and after annealing in air, were thoroughly characterized with particular attention on their morphological organization, structure and composition. For the first time, the above systems have been used as catalysts in the production of hydrogen by photo-reforming of alcoholic solutions, yielding a stable H2 evolution even by the sole use of simulated solar radiation. In addition, Ag/ZnO nanocomposites presented an excellent response in the gas-phase detection of H2, opening attractive perspectives for advanced technological applications.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.582
Times cited: 62
DOI: 10.1016/j.ijhydene.2011.09.045
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“The beneficial effect of CO2 in the low temperature synthesis of high quality carbon nanofibers and thin multiwalled carbon nanotubes from CH_{4} over Ni catalysts”. Corthals S, van Noyen J, Geboers J, Vosch T, Liang D, Ke X, Hofkens J, Van Tendeloo G, Jacobs P, Sels B, Carbon 50, 372 (2012). http://doi.org/10.1016/j.carbon.2011.08.047
Abstract: A low temperature chemical vapor deposition method is described for converting CH4 into high-quality carbon nanofibers (CNFs) using a Ni catalyst supported on either spinel or perovskite oxides in the presence of CO2. The addition of CO2 has a significant influence on CNF purity and stability, while the CNF diameter distribution is significantly narrowed. Ultimately, the addition of CO2 changes the CNF structure from fishbone fibers to thin multiwalled carbon nanotubes. A new in situ cooling principle taking into account dry reforming chemistry and thermodynamics is introduced to account for the structural effects of CO2.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 6.337
Times cited: 26
DOI: 10.1016/j.carbon.2011.08.047
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“F-doped Co3O4 photocatalysts for sustainable H2 generation from water/ethanol”. Gasparotto A, Barreca D, Bekermann D, Devi A, Fischer RA, Fornasiero P, Gombac V, Lebedev OI, Maccato C, Montini T, Van Tendeloo G, Tondello E, Journal of the American Chemical Society 133, 19362 (2011). http://doi.org/10.1021/ja210078d
Abstract: p-Type Co3O4 nanostructured films are synthesized by a plasma-assisted process and tested in the photocatalytic production of H2 from water/ethanol solutions under both near-UV and solar irradiation. It is demonstrated that the introduction of fluorine into p-type Co3O4 results in a remarkable performance improvement with respect to the corresponding undoped oxide, highlighting F-doped Co3O4 films as highly promising systems for hydrogen generation. Notably, the obtained yields were among the best ever reported for similar semiconductor-based photocatalytic processes.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 13.858
Times cited: 114
DOI: 10.1021/ja210078d
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“Measuring the corrugation amplitude of suspended and supported graphene”. Kirilenko DA, Dideykin AT, Van Tendeloo G, Physical review : B : condensed matter and materials physics 84, 235417 (2011). http://doi.org/10.1103/PhysRevB.84.235417
Abstract: Nanoscale corrugation is a fundamental property of graphene arising from its low-dimensional nature. It places a fundamental limit to the conductivity of graphene and influences its properties. However the degree of the influence of the corrugation has not been well established because of the little knowledge about its spectrum in suspended graphene. We present a transmission electron microscopy technique that enables us to measure the average corrugation height and length. We applied the technique also to measure the temperature dependence of the corrugation. The difference in corrugation between suspended and supported graphene has been illustrated.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.836
Times cited: 31
DOI: 10.1103/PhysRevB.84.235417
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“Atomic scale electron vortices for nanoresearch”. Verbeeck J, Schattschneider P, Lazar S, Stöger-Pollach M, Löffler S, Steiger-Thirsfeld A, Van Tendeloo G, Applied physics letters 99, 203109 (2011). http://doi.org/10.1063/1.3662012
Abstract: Electron vortex beams were only recently discovered and their potential as a probe for magnetism in materials was shown. Here we demonstrate a method to produce electron vortex beams with a diameter of less than 1.2 Å. This unique way to prepare free electrons to a state resembling atomic orbitals is fascinating from a fundamental physics point of view and opens the road for magnetic mapping with atomic resolution in an electron microscope.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.411
Times cited: 90
DOI: 10.1063/1.3662012
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“Point defect clusters and dislocations in FIB irradiated nanocrystalline aluminum films : an electron tomography and aberration-corrected high-resolution ADF-STEM study”. Idrissi H, Turner S, Mitsuhara M, Wang B, Hata S, Coulombier M, Raskin J-P, Pardoen T, Van Tendeloo G, Schryvers D, Microscopy and microanalysis 17, 983 (2011). http://doi.org/10.1017/S143192761101213X
Abstract: Focused ion beam (FIB) induced damage in nanocrystalline Al thin films has been characterized using advanced transmission electron microscopy techniques. Electron tomography was used to analyze the three-dimensional distribution of point defect clusters induced by FIB milling, as well as their interaction with preexisting dislocations generated by internal stresses in the Al films. The atomic structure of interstitial Frank loops induced by irradiation, as well as the core structure of Frank dislocations, has been resolved with aberration-corrected high-resolution annular dark-field scanning TEM. The combination of both techniques constitutes a powerful tool for the study of the intrinsic structural properties of point defect clusters as well as the interaction of these defects with preexisting or deformation dislocations in irradiated bulk or nanostructured materials.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 1.891
Times cited: 25
DOI: 10.1017/S143192761101213X
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“Defect controlled room temperature ferromagnetism in Co-doped barium titanate nanocrystals”. Ray S, Kolen'ko YV, Kovnir KA, Lebedev OI, Turner S, Chakraborty T, Erni R, Watanabe T, Van Tendeloo G, Yoshimura M, Itoh M, Nanotechnology 23, 025702 (2012). http://doi.org/10.1088/0957-4484/23/2/025702
Abstract: Defect mediated high temperature ferromagnetism in oxide nanocrystallites is the central feature of this work. Here, we report the development of room temperature ferromagnetism in nanosized Co-doped barium titanate particles with a size of around 14 nm, synthesized by a solvothermal drying method. A combination of x-ray diffraction with state-of-the-art electron microscopy techniques confirms the intrinsic doping of Co into BaTiO3. The development of the room temperature ferromagnetism was tracked down to the different donor defects, namely hydroxyl groups at the oxygen site (\mathrm {OH}\mathrm {(O)}
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.44
Times cited: 19
DOI: 10.1088/0957-4484/23/2/025702
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“Nanoscale spectroscopy with polarized X-rays by NEXAFS-TXM”. Guttmann P, Bittencourt C, Rehbein S, Umek P, Ke X, Van Tendeloo G, Ewels CP, Schneider G, Nature photonics 6, 25 (2012). http://doi.org/10.1038/NPHOTON.2011.268
Abstract: Near-edge X-ray absorption spectroscopy (NEXAFS)1 is an essential analytical tool in material science. Combining NEXAFS with scanning transmission X-ray microscopy (STXM) adds spatial resolution and the possibility to study individual nanostructures2, 3. Here, we describe a full-field transmission X-ray microscope (TXM) that generates high-resolution, large-area NEXAFS data with a collection rate two orders of magnitude faster than is possible with STXM. The TXM optical design combines a spectral resolution of E/ΔE = 1 × 104 with a spatial resolution of 25 nm in a field of view of 1520 µm and a data acquisition time of ~1 s. As an example, we present image stacks and polarization-dependent NEXAFS spectra from individual anisotropic sodium and protonated titanate nanoribbons. Our NEXAFS-TXM technique has the advantage that one image stack visualizes a large number of nanostructures and therefore already contains statistical information. This new high-resolution NEXAFS-TXM technique opens the way to advanced nanoscale science studies.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 37.852
Times cited: 76
DOI: 10.1038/NPHOTON.2011.268
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“Well-organized zeolite nanocrystal aggregates with interconnected hierarchically micro-meso-macropore systems showing enhanced catalytic performance”. Yang X-Y, Tian G, Chen L-H, Li Y, Rooke JC, Wei Y-X, Liu Z-M, Deng Z, Van Tendeloo G, Su B-L, Chemistry: a European journal 17, 14987 (2011). http://doi.org/10.1002/chem.201101594
Abstract: Preparation and characterization of well-organized zeolitic nanocrystal aggregates with an interconnected hierarchically micromesomacro porous system are described. Amorphous nanoparticles in bimodal aluminosilicates were directly transformed into highly crystalline nanosized zeolites, as well as acting as scaffold template. All pores on three length scales incorporated in one solid body are interconnected with each other. These zeolitic nanocrystal aggregates with hierarchically micromesomacroporous structure were thoroughly characterized. TEM images and 29Si NMR spectra showed that the amorphous phase of the initial material had been completely replaced by nanocrystals to give a micromesomacroporous crystalline zeolitic structure. Catalytic testing demonstrated their superiority due to the highly active sites and the presence of interconnected micromesomacroporosity in the cracking of bulky 1,3,5-triisopropylbenzene (TIPB) compared to traditional zeolite catalysts. This synthesis strategy was extended to prepare various zeolitic nanocrystal aggregates (ZSM-5, Beta, TS-1, etc.) with well-organized hierarchical micromesomacroporous structures.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 5.317
Times cited: 61
DOI: 10.1002/chem.201101594
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“TXM-NEXAFS of TiO2-based nanostructures”. Guttmann P, Bittencourt C, Ke X, Van Tendeloo G, Umek P, Arcon D, Ewels CP, Rehbein S, Heim S, Schneider G, AIP conference proceedings 1365, 437 (2011). http://doi.org/10.1063/1.3625396
Abstract: In this work, electronic properties of individual TiOx-pristine nanoribbons (NR) prepared by hydrothermal treatment of anatase TiO(2) micro-particles were studied using the HZB transmission x-ray microscope (TXM) at the BESSY II undulator beamline U41-FSGM. NEXAFS is ideally suited to study TiO(2)-based materials because both the O K-edge and Ti L-edge features are very sensitive to the local bonding environment, providing diagnostic information about the crystal structures and oxidation states of various forms of titanium oxides and sub-oxides. TXM-NEXAFS combines full-field x-ray microscopy with spectroscopy, allowing the study of the electronic structure of individual nanostructures with spatial resolution better than 25 nm and a spectral resolution of up to E/Delta E = 10000. The typical image field in TXM-NEXAFS measurements is about 10 mu m. 10 mu m, which is large compared to the individual nanoparticle. Therefore, one image stack already contains statistically significant data. In addition, the directional electric field vector ((E) over bar) of the x-rays can be used as a “search tool” for the direction of chemical bonds of the atom selected by its absorption edge.
Keywords: P1 Proceeding; Electron microscopy for materials research (EMAT)
Times cited: 2
DOI: 10.1063/1.3625396
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