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Author Vernimmen, J.; Guidotti, M.; Silvestre-Albero, J.; Jardim, E.O.; Mertens, M.; Lebedev, O.I.; Van Tendeloo, G.; Psaro, R.; Rodríguez-Reinoso, F.; Meynen, V.; Cool, P.
Title Immersion calorimetry as a tool to evaluate the catalytic performance of titanosilicate materials in the epoxidation of cyclohexene Type A1 Journal article
Year 2011 Publication Langmuir: the ACS journal of surfaces and colloids Abbreviated Journal Langmuir
Volume 27 Issue 7 Pages 3618-3625
Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA)
Abstract Different types of titanosilicates are synthesized, structurally characterized, and subsequently catalytically tested in the liquid-phase epoxidation of cyclohexene. The performance of three types of combined zeolitic/mesoporous materials is compared with that of widely studied Ti-grafted-MCM-41 molecular sieve and the TS-1 microporous titanosilicate. The catalytic test results are correlated with the structural characteristics of the different catalysts. Moreover, for the first time, immersion calorimetry with the same substrate molecule as in the catalytic test reaction is applied as an extra means to interpret the catalytic results. A good correlation between catalytic performance and immersion calorimetry results is found. This work points out that the combination of catalytic testing and immersion calorimetry can lead to important insights into the influence of the materials structural characteristics on catalysis. Moreover, the potential of using immersion calorimetry as a screening tool for catalysts in epoxidation reactions is shown.
Address
Corporate Author Thesis
Publisher Place of Publication Washington, D.C. Editor
Language Wos 000288970900054 Publication Date 2011-02-23
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0743-7463;1520-5827; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 3.833 Times cited 19 Open Access
Notes Approved Most recent IF: 3.833; 2011 IF: 4.186
Call Number UA @ lucian @ c:irua:88366 Serial 1557
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Author Barreca, D.; Carraro, G.; Gasparotto, A.; Maccato, C.; Lebedev, O.I.; Parfenova, A.; Turner, S.; Tondello, E.; Van Tendeloo, G.
Title Tailored vapor-phase growth of CuxO-TiO2(x=1,2) nanomaterials decorated with Au particles Type A1 Journal article
Year 2011 Publication Langmuir: the ACS journal of surfaces and colloids Abbreviated Journal Langmuir
Volume 27 Issue 10 Pages 6409-6417
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract We report on the fabrication of CuxOTiO2 (x = 1, 2) nanomaterials by an unprecedented vapor-phase approach. The adopted strategy involves the growth of porous CuxO matrices by means of chemical vapor deposition (CVD), followed by the controlled dispersion of TiO2 nanoparticles. The syntheses are performed on Si(100) substrates at temperatures of 400550 °C under wet oxygen atmospheres, adopting Cu(hfa)2·TMEDA (hfa =1,1,1,5,5,5-hexafluoro-2,4-pentanedionate; TMEDA = N,N,N′,N′-tetramethylethylenediamine) and Ti(O-iPr)2(dpm)2 (O-iPr = isopropoxy; dpm = 2,2,6,6-tetramethyl-3,5-heptanedionate) as copper and titanium precursors, respectively. Subsequently, finely dispersed gold nanoparticles are introduced in the as-prepared systems via radio frequency (RF)-sputtering under mild conditions. The synthesis process results in the formation of systems with chemical composition and nano-organization strongly dependent on the nature of the initial CuxO matrix and on the deposited TiO2 amount. The decoration with low-size gold clusters paves the way to the engineering of hierarchically organized nanomaterials.
Address
Corporate Author Thesis
Publisher Place of Publication Washington, D.C. Editor
Language Wos 000290292900082 Publication Date 2011-04-25
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0743-7463;1520-5827; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 3.833 Times cited 36 Open Access
Notes Fwo Approved Most recent IF: 3.833; 2011 IF: 4.186
Call Number UA @ lucian @ c:irua:88940 Serial 3467
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Author Stefanovich, S.Y.; Belik, A.A.; Azuma, M.; Takano, M.; Baryshnikova, O.V.; Morozov, V.A.; Lazoryak, B.I.; Lebedev, O.I.; Van Tendeloo, G.
Title Antiferroelectric phase transition in Sr9In(PO4)7 Type A1 Journal article
Year 2004 Publication Physical review : B : condensed matter and materials physics Abbreviated Journal Phys Rev B
Volume 70 Issue Pages 172103,1-4
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract
Address
Corporate Author Thesis
Publisher Place of Publication Lancaster, Pa Editor
Language Wos 000225477000003 Publication Date 2004-11-12
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1098-0121;1550-235X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 3.836 Times cited 17 Open Access
Notes Iuap P5/01 Approved Most recent IF: 3.836; 2004 IF: 3.075
Call Number UA @ lucian @ c:irua:54744 Serial 135
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Author Prodi, A.; Daoud-Aladine, A.; Gozzo, F.; Schmitt, B.; Lebedev, O.; Van Tendeloo, G.; Gilioli, E.; Bolzoni, F.; Aruga-Katori, H.; Takagi, H.; Marezio, M.; Gauzzi, A.;
Title Commensurate structural modulation in the charge- and orbitally ordered phase of the quadruple perovskite (NaMn3)Mn4O12 Type A1 Journal article
Year 2014 Publication Physical review : B : condensed matter and materials physics Abbreviated Journal Phys Rev B
Volume 90 Issue 18 Pages 180101
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract By means of synchrotron x-ray and electron diffraction, we studied the structural changes at the charge order transition T-CO = 176 K in the mixed-valence quadruple perovskite (NaMn3)Mn4O12. Below T-CO we find satellite peaks indicating a commensurate structural modulation with the same propagation vector q = ( 1/2,0,-1/2) of the CE magnetic structure that orders at low temperatures, similarly to the case of simple perovskites such as La0.5Ca0.5MnO3. In the present case, the modulated structure, together with the observation of a large entropy change at T-CO, gives evidence of a rare case of full Mn3+/Mn4+ charge and orbital order, consistent with the Goodenough-Kanamori model.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000344915100001 Publication Date 2014-11-10
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1098-0121;1550-235X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 3.836 Times cited 11 Open Access
Notes Approved Most recent IF: 3.836; 2014 IF: 3.736
Call Number UA @ lucian @ c:irua:122097 Serial 406
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Author Wang, Z.-H.; Lebedev, O.I.; Van Tendeloo, G.; Cristiani, G.; Habermeier, H.-U.
Title Crosshatching on La0.5Ca0.5MnO3 ultrathin films epitaxially grown on SrTiO3(100) Type A1 Journal article
Year 2008 Publication Physical review : B : condensed matter and materials physics Abbreviated Journal Phys Rev B
Volume 77 Issue 11 Pages 1-5
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The morphological evolution in La(0.5)Ca(0.5)MnO(3)/SrTiO(3)(100) ultrathin films has been revealed by atomic force microscopy. It was found that ordered linear defects, which are in 1-2 unit cells high and oriented along the cubic [110] and [100] directions, first appear on the smooth surface of films with a thickness of 10 nm. As the epitaxial growth proceeds, these lines on surface develop into a crosshatch pattern for films with a thickness of 25 nm. Using the results of transmission electron microscopy and electrical measurements, we discuss the interplay between the surface pattern formation, the internal dislocation structure, and the variations in the electrical properties.
Address
Corporate Author Thesis
Publisher Place of Publication Lancaster, Pa Editor
Language Wos 000254542800126 Publication Date 2008-03-18
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1098-0121;1550-235X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 3.836 Times cited 8 Open Access
Notes ESTEEM nr 026019 Approved Most recent IF: 3.836; 2008 IF: 3.322
Call Number UA @ lucian @ c:irua:70022 Serial 548
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Author Lebedev, O.I.; Van Tendeloo, G.; Attfield, J.P.; McLaughlin, A.C.
Title Defect structure of ferromagnetic superconducting RuSr2GdCu2O8 Type A1 Journal article
Year 2006 Publication Physical review : B : condensed matter and materials physics Abbreviated Journal Phys Rev B
Volume 73 Issue 22 Pages
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The structure and defect structure of superconducting ferromagnetic bulk RuSr2GdCu2O8 has been investigated using high-resolution transmission electron microscopy and high-resolution scanning transmission microscopy. Two distinct, but closely related structures, due to ordering of rotated RuO6 octahedra and due to Cu substitution in the Ru-O layer, have been revealed. The structure of Ru1-xSr2GdCu2+xO8-delta can be described as a periodic alteration along the c axis of CuO4 planes and RuO6 octahedra. The unit-cell parameters of this phase are root 2a(p) x root 2a(p) x 2c. The possible influence of this phase and defect structure on the sensitivity of the superconductivity and magnetic properties is discussed. Local defects such as 90 S domain boundaries, (130) antiphase boundaries, and the associated dislocations are analyzed.
Address
Corporate Author Thesis
Publisher Place of Publication Lancaster, Pa Editor
Language Wos 000238696300115 Publication Date 2006-06-26
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1098-0121;1550-235X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 3.836 Times cited 11 Open Access
Notes Iap V-I Approved Most recent IF: 3.836; 2006 IF: 3.107
Call Number UA @ lucian @ c:irua:59707 Serial 619
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Author Blumenau, A.T.; Jones, R.; Frauenheim, T.; Willems, B.; Lebedev, O.I.; Van Tendeloo, G.; Fisher, D.; Martineau, P.M.
Title Dislocations in diamond : dissociation into partials and their glide motion Type A1 Journal article
Year 2003 Publication Physical review : B : condensed matter and materials physics Abbreviated Journal Phys Rev B
Volume 68 Issue 1 Pages 014115-14119
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The dissociation of 60degrees and screw dislocations in diamond is modeled in an approach combining isotropic elasticity theory with ab initio-based tight-binding total-energy calculations. Both dislocations are found to dissociate with a substantial lowering of their line energies. For the 60degrees dislocation, however, an energy barrier to dissociation is found. We investigate the core structure of a screw dislocation distinguishing “shuffle,” “mixed,” and “glide” cores. The latter is found to be the most stable undissociated screw dislocation. Further, the glide motion of 90degrees and 30degrees partials is discussed in terms of a process involving the thermal formation and subsequent migration of kinks along the dislocation line. The calculated activation barriers to dislocation motion show that the 30degrees partial is less mobile than the 90degrees partial. Finally, high-resolution electron microscopy is performed on high-temperature, high-pressure annealed natural brown diamond, allowing the core regions of 60degrees dislocations to be imaged. The majority of dislocations are found to be dissociated. However, in some cases, undissociated 60degrees dislocations were also observed.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000184582900050 Publication Date 2003-08-01
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0163-1829;1095-3795; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 3.836 Times cited 39 Open Access
Notes Approved Most recent IF: 3.836; 2003 IF: NA
Call Number UA @ lucian @ c:irua:103800 Serial 734
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Author Xu, T.; Nys, J.-P.; Addad, A.; Lebedev, O.I.; Urbieta, A.; Salhi, B.; Berthe, M.; Grandidier, B.; Stievenard, D.
Title Faceted sidewalls of silicon nanowires: Au-induced structural reconstructions and electronic properties Type A1 Journal article
Year 2010 Publication Physical review : B : condensed matter and materials physics Abbreviated Journal Phys Rev B
Volume 81 Issue 11 Pages 115403,1-115403,10
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Si nanowires with a ⟨111⟩ orientation, synthesized by vapor-liquid-solid process with low silane partial pressure reactant and gold as the catalyst, are known to exhibit sawtooth facets containing gold adsorbates. We report herein the study of the nanowire morphology by means of transmission electron microscopy and scanning tunneling microscopy. The nanowires consist of faceted sidewalls. The number of the sidewalls changes from 12 to 6 along the growth axis, giving rise to nanowires with an irregular hexagonal cross section at their base. The sidewalls are covered with Au-rich clusters. Their facets also exhibit atomic structures that reveal the presence of gold, resulting from the diffusion of gold during the growth. Based on these observations, the tapering of the nanowire is found to be related to two contributions: the reduction in the catalyst particle size during the growth and lateral overgrowth from the direct incorporation of Si species onto the nanowire sidewalls. Because the rearrangement of atoms at surfaces and interfaces might affect the growth kinetics, the trigonal symmetry as well as the higher lateral growth rate on the widest sidewalls are explained from the existence of an interfacial atomic structure with two inequivalent parts in the unit cell. Finally, spectroscopic measurements were performed on the major facets and revealed a metallic behavior at 77 K.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000276248800116 Publication Date 2010-03-03
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1098-0121;1550-235X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 3.836 Times cited 42 Open Access
Notes Approved Most recent IF: 3.836; 2010 IF: 3.774
Call Number UA @ lucian @ c:irua:82273 Serial 1168
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Author Fedina, L.; Lebedev, O.I.; Van Tendeloo, G.; van Landuyt, J.; Mironov, O.A.; Parker, E.H.C.
Title In situ HREM irradiation study of point-defect clustering in MBE-grown strained Si1-xGex/(001)Si structures Type A1 Journal article
Year 2000 Publication Physical review : B : condensed matter and materials physics Abbreviated Journal Phys Rev B
Volume 61 Issue 15 Pages 10336-10345
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract We present a detailed analysis of the point-defect clustering in strained Si/Si(1-x)Ge(x)/(001)Si structures, including the interaction of the point defects with the strained interfaces and the sample surface during 400 kV electron irradiation at room temperature. Point-defect cluster formation is very sensitive to the type and magnitude of the strain in the Si and Si(1-x)Ge(x) layers. A small compressive strain (-0.3%) in the SiGe alloy causes an aggregation of vacancies in the form of metastable [110]-oriented chains. They are located on {113} planes and further recombine with interstitials. Tensile strain in the Si layer causes an aggregation of interstitial atoms in the forms of additional [110] rows which are inserted on {113} planes with [001]-split configurations. The chainlike configurations are characterized by a large outward lattice relaxation for interstitial rows (0.13 +/-0.01 nm) and a very small inward relaxation for vacancy chains (0.02+/-0.01 nm). A compressive strain higher than -0.5% strongly decreases point-defect generation inside the strained SiGe alloy due to the large positive value of the formation volume of a Frenkel pair. This leads to the suppression of point-defect clustering in a strained SiGe alloy so that SiGe relaxes via a diffusion of vacancies from the Si layer, giving rise to an intermixing at the Si/SiGe interface. In material with a 0.9% misfit a strongly increased flow of vacancies from the Si layer to the SiGe layer and an increased biaxial strain in SiGe bath promote the preferential aggregation of vacancies in the (001) plane, which relaxes to form intrinsic 60 degrees dislocation loops.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000086606200082 Publication Date 2002-07-27
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0163-1829;1095-3795; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 3.836 Times cited 27 Open Access
Notes Conference Name: Microsc. Semicond. Mater. Conf. Approved Most recent IF: 3.836; 2000 IF: NA
Call Number UA @ lucian @ c:irua:103456 Serial 1577
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Author Gehrke, K.; Moshnyaga, V.; Samwer, K.; Lebedev, O.I.; Verbeeck, J.; Kirilenko, D.; Van Tendeloo, G.
Title Interface controlled electronic variations in correlated heterostructures Type A1 Journal article
Year 2010 Publication Physical review : B : condensed matter and materials physics Abbreviated Journal Phys Rev B
Volume 82 Issue 11 Pages 113101,1-113101,4
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract An interface modification of (LaCa)MnO3-BaTiO3 superlattices was found to massively influence magnetic and magnetotransport properties. Moreover it determines the crystal structure of the manganite layers, changing it from orthorhombic (Pnma) for the conventional superlattice (cSL), to rhombohedral (R3̅ c) for the modified one (mSL). While the cSL shows extremely nonlinear ac transport, the mSL is an electrically homogeneous material. The observations go beyond an oversimplified picture of dead interface layers and evidence the importance of electronic correlations at perovskite interfaces.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000281643200001 Publication Date 2010-09-07
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1098-0121;1550-235X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 3.836 Times cited 9 Open Access
Notes This work was supported by DFG via SFB 602, TPA2. Approved Most recent IF: 3.836; 2010 IF: 3.774
Call Number UA @ lucian @ c:irua:84249UA @ admin @ c:irua:84249 Serial 1691
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Author Ding, J.F.; Lebedev, O.I.; Turner, S.; Tian, Y.F.; Hu, W.J.; Seo, J.W.; Panagopoulos, C.; Prellier, W.; Van Tendeloo, G.; Wu, T.
Title Interfacial spin glass state and exchange bias in manganite bilayers with competing magnetic orders Type A1 Journal article
Year 2013 Publication Physical review : B : condensed matter and materials physics Abbreviated Journal Phys Rev B
Volume 87 Issue 5 Pages 054428-7
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The magnetic properties of manganite bilayers composed of G-type antiferromagnetic (AFM) SrMnO3 and double-exchange ferromagnetic (FM) La0.7Sr0.3MnO3 are studied. A spin-glass state is observed as a result of competing magnetic orders and spin frustration at the La0.7Sr0.3MnO3/SrMnO3 interface. The dependence of the irreversible temperature on the cooling magnetic field follows the Almeida-Thouless line. Although an ideal G-type AFM SrMnO3 is featured with a compensated spin configuration, the bilayers exhibit exchange bias below the spin glass freezing temperature, which is much lower than the Néel temperature of SMO, indicating that the exchange bias is strongly correlated with the spin glass state. The results indicate that the spin frustration that originates from the competition between the AFM super-exchange and the FM double-exchange interactions can induce a strong magnetic anisotropy at the La0.7Sr0.3MnO3/SrMnO3 interface.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000315271200002 Publication Date 2013-02-22
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1098-0121;1550-235X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 3.836 Times cited 98 Open Access
Notes FWO; COUNTATOMS; Hercules Approved Most recent IF: 3.836; 2013 IF: 3.664
Call Number UA @ lucian @ c:irua:107349 Serial 1696
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Author Maignan, A.; Lebedev, O.I.; Van Tendeloo, G.; Martin, C.; Hebert, S.
Title Metal to insulator transition in the n-type hollandite vanadate Pb1.6V8O16 Type A1 Journal article
Year 2010 Publication Physical review : B : condensed matter and materials physics Abbreviated Journal Phys Rev B
Volume 82 Issue 3 Pages 035122, 1-035122,5
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The transport and magnetic measurements of polycrystalline Pb1.6V8O16 hollandite reveal a concomitant metal to insulator and antiferromagnetic transition at TMI≈140 K. A clear localization is found below TMI, evidenced by a rapid increase in the absolute value of the negative Seebeck coefficient. The structural study by x-ray and transmission electron microscopy confirms the hollandite structure and shows that no structural transition occurs at TMI, ruling out a possible charge orbital ordering. The negative Seebeck coefficient observed from 50 K up to 900 K, with values reaching S=−38 μV K−1 at 900 K, is explained by the electron doping of ∼1.4e− in the V empty t2g orbitals responsible for the bad metal resistivity (ρ900 K∼2 mΩ cm). As this S value is close to that obtained by considering only the spin and orbital degeneracies, it is expected that |S| for such vanadates will not be sensitive at high temperature to the t2g band filling
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000280366300002 Publication Date 2010-07-27
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1098-0121;1550-235X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 3.836 Times cited 10 Open Access
Notes Approved Most recent IF: 3.836; 2010 IF: 3.774
Call Number UA @ lucian @ c:irua:84065 Serial 2009
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Author Wang, Z.-H.; Kronmüller, H.; Lebedev, O.I.; Gross, G.M.; Razavi, F.S.; Habermeier, H.U.; Shen, B.G.
Title Phase transition and magnetic anisotropy of (La,Sr)MnO3 thin films Type A1 Journal article
Year 2002 Publication Physical review : B : condensed matter and materials physics Abbreviated Journal Phys Rev B
Volume 65 Issue 5 Pages 054411-54416
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The magnetic proper-ties and their correlation with the microstructure and electrical transport are investigated in La0.88Sr0.1MnO3 films grown on (100)SrTiO3 Single crystal substrates with thickness ranging from 100 to 2500 Angstrom. The ultrathin film (t = 100 Angstrom) has a single ferromagnetic transition (FMT) at T-c of 250 K, whereas the thicker films exhibit two FMTs, with the main one at a lowered T-c of 200 K while the minor one around 300 K. Furthermore, a thickness dependent magnetic anisotropy has been found, strongly indicating the existence of strain effect, which is also revealed by the transmission electron microscopy study. The suppressed Jahn-Teller distortion (JTD) by the epitaxial strain, and the recovered JTD due to the strain relexation are suggested to explain the metallic behavior in thin films and the insulating behavior in the thick film (t = 2500 Angstrom), repectively.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000173647000058 Publication Date 2002-07-27
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0163-1829;1095-3795; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 3.836 Times cited 23 Open Access
Notes Approved Most recent IF: 3.836; 2002 IF: NA
Call Number UA @ lucian @ c:irua:103883 Serial 2592
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Author Holden, T.; Habermeier, H.-U.; Cristiani, G.; Golnik, A.; Boris, A.; Pimenov, A.; Humlicek, J.; Lebedev, O.I.; Van Tendeloo, G.; Keimer, B.; Bernhard, C.
Title Proximity induced metal-insulator transition in YBa2Cu3O7/La2/3Ca1/3MnO3 superlattices Type A1 Journal article
Year 2004 Publication Physical review : B : condensed matter and materials physics Abbreviated Journal Phys Rev B
Volume 69 Issue 6 Pages 064505,1-064505,7
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The far-infrared dielectric response of superlattices (SL) composed of superconducting YBa2Cu3O7 (YBCO) and ferromagnetic La0.67Ca0.33MnO3 (LCMO) has been investigated by ellipsometry. A drastic decrease of the free-carrier response is observed which involves an unusually large length scale of d(crit)approximate to20 nm in YBCO and d(crit)approximate to10 nm in LCMO. A corresponding suppression of metallicity is not observed in SL's where LCMO is replaced by the paramagnetic metal LaNiO3. Our data suggest that either a long-range charge transfer from the YBCO to the LCMO layers or alternatively a strong coupling of the charge carriers to the different and competitive kind of magnetic correlations in the LCMO and YBCO layers is at the heart of the observed metal-insulator transition. The low free-carrier response observed in the far-infrared dielectric response of the magnetic superconductor RuSr2GdCu2O8 is possibly related to this effect.
Address
Corporate Author Thesis
Publisher Place of Publication Lancaster, Pa Editor
Language Wos 000220092100066 Publication Date 2004-02-21
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1098-0121;1550-235X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 3.836 Times cited 101 Open Access
Notes Approved Most recent IF: 3.836; 2004 IF: 3.075
Call Number UA @ lucian @ c:irua:54743 Serial 2734
Permanent link to this record
 

 
Author Lobanov, M.V.; Balagurov, A.M.; Pomjakushin, V.J.; Fischer, P.; Gutmann, M.; Abakumov, A.M.; D'yachenko, O.G.; Antipov, E.V.; Lebedev, O.I.; Van Tendeloo, G.
Title Structural and magnetic properties of the colossal magnetoresistance perovskite La0.85Ca0.15MnO3 Type A1 Journal article
Year 2000 Publication Physical review : B : condensed matter and materials physics Abbreviated Journal Phys Rev B
Volume 61 Issue 13 Pages 8941-8949
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract
Address
Corporate Author Thesis
Publisher Place of Publication Lancaster, Pa Editor
Language Wos 000086597400059 Publication Date 2002-07-27
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0163-1829;1095-3795; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 3.836 Times cited 47 Open Access
Notes Approved Most recent IF: 3.836; 2000 IF: NA
Call Number UA @ lucian @ c:irua:54735 Serial 3197
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Author Turner, S.; Lebedev, O.I.; Verbeeck, J.; Gehrke, K.; Moshnyaga, V.; Van Tendeloo, G.
Title Structural phase transition and spontaneous interface reconstruction in La2/3Ca1/3MnO3/BaTiO3 superlattices Type A1 Journal article
Year 2013 Publication Physical review : B : condensed matter and materials physics Abbreviated Journal Phys Rev B
Volume 87 Issue 3 Pages 035418-8
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract (La2/3Ca1/3MnO3)n/(BaTiO3)m (LCMOn/BTOm) superlattices on MgO and SrTiO3 substrates with different layer thicknesses (n = 10, 38, 40 and m = 5, 18, 20) have been grown by metal organic aerosol deposition (MAD) and have been fully characterized down to the atomic scale to study the interface characteristics. Scanning transmission electron microscopy combined with spatially resolved electron energy-loss spectroscopy provides clear evidence for the existence of atomically sharp interfaces in MAD grown films, which exhibit epitaxial growth conditions, a uniform normal strain, and a fully oxidized state. Below a critical layer thickness the LCMO structure is found to change from the bulk Pnma symmetry to a pseudocubic R3̅ c symmetry. An atomically flat interface reconstruction consisting of a single Ca-rich atomic layer is observed on the compressively strained BTO on LCMO interface, which is thought to partially neutralize the total charge from the alternating polar atomic layers in LCMO as well as relieving strain at the interface. No interface reconstruction is observed at the tensile strained LCMO on BTO interface.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000313940400008 Publication Date 2013-01-23
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1098-0121;1550-235X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 3.836 Times cited 12 Open Access
Notes FWO; Hercules; Countatoms Approved Most recent IF: 3.836; 2013 IF: 3.664
Call Number UA @ lucian @ c:irua:106180 Serial 3245
Permanent link to this record
 

 
Author Lebedev, O.I.; Verbeeck, J.; Van Tendeloo, G.; Shapoval, O.; Belenchuk, A.; Moshnyaga, V.; Damaschke, B.; Samwer, K.
Title Structural phase transitions and stress accommodation in (La0.67Ca0.33MnO3)1.x:(MgO)x composite films Type A1 Journal article
Year 2002 Publication Physical review : B : condensed matter and materials physics Abbreviated Journal Phys Rev B
Volume 66 Issue 10 Pages 104421,1-10
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Composite (La0.67Ca0.33MnO3)(1-x):(MgO)(x) films were prepared by metalorganic aerosol deposition on a (100)MgO substrate for different concentrations of the (MgO) phase (0less than or equal toxless than or equal to0.8). At xapproximate to0.3 a percolation threshold in conductivity is reached, at which an infinite insulating MgO cluster forms around the La0.67Ca0.33MnO3 grains. This yields a drastic increase of the electrical resistance for films with x>0.3. The film structure is characterized by x-ray diffraction and transmission electron microscopy. The local structure of the La0.67Ca0.33MnO3 within the film depends on the MgO concentration which grows epitaxially along the domain boundaries. A different structural phase transition from the orthorhombic Pnma structure to an unusual rhombohedral R (3) over barc structure at the percolation threshold xapproximate to0.3 is found for La0.67Ca0.33MnO3. A three-dimensional stress accommodation in thick films through a phase transition is suggested.
Address
Corporate Author Thesis
Publisher Place of Publication Lancaster, Pa Editor
Language Wos 000178460900060 Publication Date 2002-09-25
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0163-1829;1095-3795; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 3.836 Times cited 48 Open Access
Notes Approved Most recent IF: 3.836; 2002 IF: NA
Call Number UA @ lucian @ c:irua:54740 Serial 3250
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Author Lebedev, O.I.; Van Tendeloo, G.; Amelinckx, S.; Leibold, B.; Habermeier, H.-U.
Title Structure and microstructure of La1-xCaxMnO3- thin films prepared by pulsed layer deposition Type A1 Journal article
Year 1998 Publication Physical review : B : condensed matter and materials physics Abbreviated Journal Phys Rev B
Volume 58 Issue 12 Pages 8065-8074
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract
Address
Corporate Author Thesis
Publisher Place of Publication Lancaster, Pa Editor
Language Wos 000076130500085 Publication Date 2002-07-27
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0163-1829;1095-3795; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 3.836 Times cited 131 Open Access
Notes Approved Most recent IF: 3.836; 1998 IF: NA
Call Number UA @ lucian @ c:irua:25679 Serial 3288
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Author Lebedev, O.I.; Van Tendeloo, G.; Cristiani, G.; Habermeier, H.-U.; Matveev, A.T.
Title Structure-properties relationship in ferromagnetic superconducting RuSr2GdCu2O8 Type A1 Journal article
Year 2005 Publication Physical review : B : condensed matter and materials physics Abbreviated Journal Phys Rev B
Volume 71 Issue Pages 134523,1-8
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract
Address
Corporate Author Thesis
Publisher Place of Publication Lancaster, Pa Editor
Language Wos 000228761800097 Publication Date 2005-04-28
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1098-0121;1550-235X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 3.836 Times cited 16 Open Access
Notes Iap V-1 Approved Most recent IF: 3.836; 2005 IF: 3.185
Call Number UA @ lucian @ c:irua:54747 Serial 3316
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Author Lebedev, O.I.; Van Tendeloo, G.; Licci, F.; Gilioli, E.; Gauzzi, A.; Prodi, A.; Marezio, M.
Title Superconductivity and microstructure of YSr2Cu3O6.875 Type A1 Journal article
Year 2002 Publication Physical review : B : condensed matter and materials physics Abbreviated Journal Phys Rev B
Volume 66 Issue Pages 132510,1-4
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract
Address
Corporate Author Thesis
Publisher Place of Publication Lancaster, Pa Editor
Language Wos 000179067900042 Publication Date 2002-10-29
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0163-1829;1095-3795; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 3.836 Times cited 9 Open Access
Notes Approved Most recent IF: 3.836; 2002 IF: NA
Call Number UA @ lucian @ c:irua:54742 Serial 3371
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Author Verbeeck, J.; Lebedev, O.I.; Van Tendeloo, G.; Mercey, B.
Title SrTiO3(100)/(LaMnO3)m(SrMnO3)n layered heterostructures: a combined EELS and TEM study Type A1 Journal article
Year 2002 Publication Physical review : B : condensed matter and materials physics Abbreviated Journal Phys Rev B
Volume 66 Issue 18 Pages 184426
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Epitaxially grown heterostructures consisting of alternating layers of LaMnO(3) (LMO, 9 or 15 unit cells) and SrMnO(3) (SMO, 4 or 6 unit cells) on a SrTiO(3)(100) (STO(100)) substrate have been studied by a combination of high resolution transmission electron microscopy (HRTEM), electron diffraction, quantitative electron energy loss spectroscopy (EELS) with model fitting, energy filtered TEM (EFTEM) and imaging spectroscopy on an atomic scale. The combination of these techniques is necessary for the structural, chemical, and electronic characterization of these heterostructures. A model is proposed containing chemically and structurally sharp interfaces. The SrMnO(3) layers are stabilized in a Pm3m structure between two LMO layers. Tensile stress causes oxygen deficiency in the SMO layers increasing the number of 3d electrons on the Mn sites to resemble the Mn(3+) sites in LMO. The energy loss near edge structure (ELNES) of O and Mn is compared for both LMO and SMO layers and shows that the Mn-O bonds have a partially covalent character. The absence of a strong valency effect in the Mn ELNES is due to the oxygen vacancies in SMO.
Address
Corporate Author Thesis
Publisher Place of Publication Lancaster, Pa Editor
Language Wos 000179633100062 Publication Date 2002-11-27
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0163-1829;1095-3795; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 3.836 Times cited 32 Open Access
Notes Approved Most recent IF: 3.836; 2002 IF: NA
Call Number UA @ lucian @ c:irua:54741 Serial 3563
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Author Barreca, D.; Gasparotto, A.; Maccato, C.; Tondello, E.; Lebedev, O.I.; Van Tendeloo, G.
Title CVD of copper oxides from a \beta-diketonate diamine precursor: tailoring the nano-organization Type A1 Journal article
Year 2009 Publication Crystal growth & design Abbreviated Journal Cryst Growth Des
Volume 9 Issue 5 Pages 2470-2480
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract A copper(II) hexafluoroacetylacetonate (1,1,1,5,5,5-hexafluoro-2,4-pentanedionate, hfa) adduct with N,N,N¡ä,N¡ä-tetramethylethylenediamine (TMEDA) [Cu(hfa)2¡¤TMEDA] is used for the first time as precursor for the chemical vapor deposition (CVD) of copper oxide nanosystems. The syntheses are carried out under both O2 and O2+H2O reaction atmospheres on Si(100) substrates, at temperatures ranging between 250 and 550 ¡ãC. Subsequently, the interrelations between the preparative conditions and the system composition, nanostructure, and morphology are elucidated by means of complementary analytical techniques [Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron and X-ray excited auger electron spectroscopies (XPS and XE-AES), glancing incidence X-ray diffraction (GIXRD), field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM)]. The obtained data revealed a gradual transformation from Cu2O, to Cu2O + CuO, to CuO nanosystems upon increasing the deposition temperature from 250 to 550 ¡ãC under both growth atmospheres. Such a phenomenon was accompanied by a progressive morphological evolution from continuous films to 1D hyperbranched nanostructures. Water vapor introduction in the deposition environment enabled to lower the deposition temperature and resulted in a higher aggregate interconnection, attributed to a higher density of nucleation centers.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000265892200066 Publication Date 2009-05-06
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1528-7483;1528-7505; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 4.055 Times cited 60 Open Access
Notes Esteem 026019 Approved Most recent IF: 4.055; 2009 IF: 4.162
Call Number UA @ lucian @ c:irua:77053 Serial 597
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Author Neira, I.S.; Kolen'ko, Y.V.; Lebedev, O.I.; Van Tendeloo, G.; Gupta, H.S.; Guitián, F.; Yoshimura, M.
Title An effective morphology control of hydroxyapatite crystals via hydrothermal synthesis Type A1 Journal article
Year 2009 Publication Crystal growth & design Abbreviated Journal Cryst Growth Des
Volume 9 Issue 1 Pages 466-474
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract A facile urea-assisted hydrothermal synthesis and systematic characterization of hydroxyapatite (HA) with calcium nitrate tetrahydrate and diammonium hydrogen phosphate as precursors are reported. The advantage of the proposed technique over previously reported synthetic approaches is the simple but precise control of the HA crystals morphology, which is achieved by employing an intensive, stepwise, and slow thermal decomposition of urea as well as varying initial concentrations of starting reagents. Whereas the plate-, hexagonal prism- and needle-like HA particles preferentially growth along the c-axis, the smaller and fine-plate-like HA crystals demonstrate crystal growth along the (102) and (211) directions, uncommon for HA. Furthermore, it was established that the hydrothermally derived powdered products are phase-pure HA containing CO32− anions in the crystal lattice, that is, AB-type carbonated hydroxyapatite. Transmission electron microscopy (TEM) and electron diffraction (ED) of selected samples reveal that the as-prepared HA crystals are single-crystalline and exhibit a nearly defect-free microstructure. The hardness and elastic modulus of the hexagonal prism-like HA crystals have been investigated on a nanoscale using the nanoindentation technique; the observed trends are discussed.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000262332700073 Publication Date 2008-11-21
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1528-7483;1528-7505; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 4.055 Times cited 183 Open Access
Notes Esteem 026019 Approved Most recent IF: 4.055; 2009 IF: 4.162
Call Number UA @ lucian @ c:irua:75740 Serial 853
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Author Bekermann, D.; Gasparotto, A.; Barreca, D.; Bovo, L.; Devi, A.; Fischer, R.A.; Lebedev, O.I.; Maccato, C.; Tondello, E.; Van Tendeloo, G.
Title Highly oriented ZnO nanorod arrays by a novel plasma chemical vapor deposition process Type A1 Journal article
Year 2010 Publication Crystal growth & design Abbreviated Journal Cryst Growth Des
Volume 10 Issue 4 Pages 2011-2018
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Strongly c-axis oriented ZnO nanorod arrays were grown on Si(100) by plasma enhanced-chemical vapor deposition (PE-CVD) starting from two volatile bis(ketoiminato) zinc(II) compounds Zn[(R′)NC(CH3)═C(H)C(CH3)═O]2, with R′ = -(CH2)xOCH3 (x = 2, 3). A systematic investigation of process parameters enabled us to obtain the selective formation of ZnO nanorods with tailored features, and provided an important insight into their growth mechanism. The morphology, structure, and composition of the synthesized ZnO nanosystems were thoroughly analyzed by field emission-scanning electron microscopy (FE-SEM), energy dispersive X-ray spectroscopy (EDXS), glancing incidence X-ray diffraction (GIXRD), X-ray photoelectron spectroscopy (XPS), and transmission electron microscopy (TEM). Photoluminescence (PL) measurements were carried out to gain information on the optical properties. Specifically, one-dimensional (1D) ZnO architectures could be grown on Si(100) substrates at temperatures as low as 200−300 °C and radio frequency (RF)-power values of 20 W, provided that a sufficiently high mass supply to the growth surface was maintained. To the best of our knowledge, the present work reports the mildest preparation conditions ever appeared in the literature for the PE-CVD of ZnO nanorods, a key result in view of potential large-scale technological applications.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000276234500080 Publication Date 2010-03-18
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1528-7483;1528-7505; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 4.055 Times cited 75 Open Access
Notes Esteem 026019 Approved Most recent IF: 4.055; 2010 IF: 4.390
Call Number UA @ lucian @ c:irua:82311 Serial 1472
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Author Li, Y.; Tan, H.; Lebedev, O.; Verbeeck, J.; Biermans, E.; Van Tendeloo, G.; Su, B.-L.
Title Insight into the growth of multiple branched MnOOH nanorods Type A1 Journal article
Year 2010 Publication Crystal growth & design Abbreviated Journal Cryst Growth Des
Volume 10 Issue 7 Pages 2969-2976
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Multiple branched manganese oxide hydroxide (MnOOH) nanorods prepared by a hydrothermal process were extensively studied by transmission electron microscopy (TEM). A model of the branch formation is proposed together with a study of the interface structure. The sword-like tip plays a crucial role for the nanorods to form different shapes. Importantly, the branching occurs at an angle of around either 57 degrees or 123 degrees. Specifically, a (111) twin plane can only be formed at the interface with a 123 degrees angle. The interfaces formed with a 57 degrees angle usually contain edge dislocations. Electron energy loss spectroscopy (EELS) demonstrates that the whole crystal has a uniform chemical composition. Interestingly, an epitaxial growth of Mn3O4 at the radial surface was also observed under electron beam irradiation; this is because of the rough purification of the products. The proposed mechanism is expected to shed light on the branched/dendrite nanostructure growth and to provide opportunities for further novel nanomaterial structure growth and design.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000279422700027 Publication Date 2010-06-08
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1528-7483;1528-7505; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 4.055 Times cited 41 Open Access
Notes Fwo; Esteem 026019 Approved Most recent IF: 4.055; 2010 IF: 4.390
Call Number UA @ lucian @ c:irua:83886UA @ admin @ c:irua:83886 Serial 1672
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Author Ahenach, J.; Cool, P.; Vansant, E.F.; Lebedev, O.; van Landuyt, J.
Title Influence of water on the pillaring of montmorillonite with aminopropyltriethoxysilane Type A1 Journal article
Year 1999 Publication Physical chemistry, chemical physics Abbreviated Journal Phys Chem Chem Phys
Volume 1 Issue Pages 3703-3708
Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA)
Abstract
Address
Corporate Author Thesis
Publisher Place of Publication Cambridge Editor
Language Wos 000081765300046 Publication Date 2002-07-26
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1463-9076;1463-9084; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 4.123 Times cited 10 Open Access
Notes Approved Most recent IF: 4.123; 1999 IF: NA
Call Number UA @ lucian @ c:irua:28250 Serial 1660
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Author Neira, I.S.; Kolen'ko, Y.V.; Lebedev, O.I.; Van Tendeloo, G.; Gupta, H.S.; Matsushita, N.; Yoshimura, M.; Guitian, F.
Title Rational synthesis of a nanocrystalline calcium phosphate cement exhibiting rapid conversion to hydroxyapatite Type A1 Journal article
Year 2009 Publication Materials science and engineering: part C: biomimetic materials Abbreviated Journal Mat Sci Eng C-Mater
Volume 29 Issue 7 Pages 2124-2132
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The rational synthesis, comprehensive characterization, and mechanical and micromechanical properties of a calcium phosphate cement are presented. Hydroxyapatite cement biomaterial was synthesized from reactive sub-micrometer-sized dicalcium phosphate dihydrate and tetracalcium phosphate via a dissolution-precipitation reaction using water as the liquid phase. As a result nanostructured, Ca-deficient and carbonated B-type hydroxyapatite is formed. The cement shows good processibility, sets in 22 ± 2 min and entirely transforms to the end product after 6 h of setting reaction, one of the highest conversion rates among previously reported for calcium phosphate cements based on dicalcium and tetracalcium phosphates. The combination of all elucidated physical-chemical traits leads to an essential bioactivity and biocompatibility of the cement, as revealed by in vitro acellular simulated body fluid and cell culture studies. The compressive strength of the produced cement biomaterial was established to be 25 ± 3 MPa. Furthermore, nanoindentation tests were performed directly on the cement to probe its local elasticity and plasticity at sub-micrometer/micrometer level. The measured elastic modulus and hardness were established to be Es = 23 ± 3.5 and H = 0.7 ± 0.2 GPa, respectively. These values are in close agreement with those reported in literature for trabecular and cortical bones, reflecting good elastic and plastic coherence between synthesized cement biomaterial and human bones.
Address
Corporate Author Thesis
Publisher Place of Publication Lausanne Editor
Language Wos 000270159200008 Publication Date 2009-04-20
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0928-4931; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 4.164 Times cited 18 Open Access
Notes Esteem 026019 Approved Most recent IF: 4.164; 2009 IF: NA
Call Number UA @ lucian @ c:irua:79312 Serial 2812
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Author Zhao, Q.; Lorenz, H.; Turner, S.; Lebedev, O.I.; Van Tendeloo, G.; Rameshan, C.; Klötzer, B.; Konzett, J.; Penner, S.
Title Catalytic characterization of pure SnO2 and GeO2 in methanol steam reforming Type A1 Journal article
Year 2010 Publication Applied catalysis : A : general Abbreviated Journal Appl Catal A-Gen
Volume 375 Issue 2 Pages 188-195
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Structural changes of a variety of different SnO, SnO2 and GeO2 catalysts upon reduction in hydrogen were correlated with associated catalytic changes in methanol steam reforming. Studied systems include SnO, SnO2 and GeO2 thin film model catalysts prepared by vapour phase deposition and growth on polycrystalline NaCl surfaces and, for comparison, the corresponding pure oxide powder catalysts. Reduction of both the SnO2 thin film and powder at around 673 K in 1 bar hydrogen leads to a substantial reduction of the bulk structure and yields a mixture of SnO2 and metallic β-Sn. On the powder catalyst this transformation is fully reversible upon oxidation in 1 bar O2 at 673 K. Strongly reduced thin films, however, can only be re-transformed to SnO2 if the reduction temperature did not exceed 573 K. For GeO2, the situation is more complex due to its polymorphism. Whereas the tetragonal phase is structurally stable during reduction, oxidation or catalytic reaction, a small part of the hexagonal phase is always transformed into the tetragonal at 673 K independent of the gas phase used. SnO2 is highly active and CO2 selective in methanol steam reforming, but the initial high activity drops considerably upon reduction between 373 and 573 K and almost complete catalyst deactivation is observed after reduction at 673 K, which is associated with the parallel formation of β-Sn. In close correlation to the structural results, the catalytic activity and selectivity can be restored upon an oxidative catalyst regeneration at 673 K. Tetragonal GeO2 exhibits only a small activity and no pronounced selectivity to either CO or CO2, at least after reduction. In its fully oxidized state release of surface/lattice oxygen results in a non-catalytic formation of CO2 by oxidation of CO originating from catalytic dehydrogenation.
Address
Corporate Author Thesis
Publisher Place of Publication Amsterdam Editor
Language Wos 000275580600002 Publication Date 2010-01-15
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0926-860X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 4.339 Times cited 20 Open Access
Notes Esteem 026019 Approved Most recent IF: 4.339; 2010 IF: 3.384
Call Number UA @ lucian @ c:irua:81741 Serial 292
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Author Lorenz, H.; Zhao, Q.; Turner, S.; Lebedev, O.I.; Van Tendeloo, G.; Kloetzer, B.; Rameshan, C.; Pfaller, K.
Title Origin of different deactivation of Pd/SnO2 and Pd/GeO2 catalysts in methanol dehydrogenation and reforming: a comparative study Type A1 Journal article
Year 2010 Publication Applied catalysis : A : general Abbreviated Journal Appl Catal A-Gen
Volume 381 Issue 1/2 Pages 242-252
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Pd particles supported on SnO2 and GeO2 have been structurally investigated by X-ray diffraction, (High-Resolution) transmission and scanning electron microscopy after different reductive treatments to monitor the eventual formation of bimetallic phases and catalytically tested in methanol dehydrogenation/ reforming. For both oxides this included a thin film sample with well-defined Pd particles and a powder catalyst prepared by incipient wetness impregnation. The hexagonal and the tetragonal polymorph were studied for powder GeO2. Pd2Ge formation was observed on all GeO2-supported catalysts, strongly depending on the specific sample used. Reduction of the thin film at 573K resulted in full transformation into the bimetallic state. The partial solubility of hexagonal GeO2 in water and its thermal structural instability yielded Pd2Ge formation at 473 K, at the cost of a structurally inhomogeneous support and Ge metal formation at higher reduction temperatures. Pd on tetragonal GeO2 entered a state of strong metalsupport interaction after reduction at 573673 K, resulting in coalescing Pd2Ge particles on a sintered and re-crystallized support, apparently partially covering the bimetallic particles and decreasing the catalytic activity. Pd2Ge on amorphous thin film and hexagonal GeO2 converted methanol primarily via dehydrogenation to CO and H2. At 573 K, formation of Pd2Sn and also PdSn occurred on the Pd/SnO2 thin film. Pd3Sn2 (and to some extent Pd2Sn) were predominantly obtained on the respective powder catalyst. Strong deactivation with increasing reduction temperature was observed, likely not based on the classical strong metalsupport interaction effect, but rather on a combination of missing active structural ensembles on Sn-enriched bimetallic phases and the formation of metallic -Sn. Correlations to Pd and its bimetallics supported on ZnO, Ga2O3 and In2O3 were also discussed.
Address
Corporate Author Thesis
Publisher Place of Publication Amsterdam Editor
Language Wos 000279100700029 Publication Date 2010-04-26
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0926-860X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 4.339 Times cited 14 Open Access
Notes Esteem 026019 Approved Most recent IF: 4.339; 2010 IF: 3.384
Call Number UA @ lucian @ c:irua:83927 Serial 2522
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Author Lorenz, H.; Turner, S.; Lebedev, O.I.; Van Tendeloo, G.; Klötzer, B.; Rameshan, C.; Pfaller, K.; Penner, S.
Title Pd-In2O3 interaction due to reduction in hydrogen: consequences for methanol steam reforming Type A1 Journal article
Year 2010 Publication Applied catalysis : A : general Abbreviated Journal Appl Catal A-Gen
Volume 374 Issue 1/2 Pages 180-188
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Two different Pd/In2O3 samples including a thin film model catalyst with well-defined Pd particles grown on NaCl(0 0 1) supports and a powder catalyst prepared by an impregnation technique are examined by electron microscopy, X-ray diffraction and catalytic measurements in methanol steam reforming in order to correlate the formation of different oxide-supported bimetallic PdIn phases with catalytic activity and selectivity. A PdIn shell around the Pd particles is observed on the thin film catalyst after embedding the Pd particles in In2O3 at 300 K, likely because alloying to PdIn and oxidation to In2O3 are competing processes. Increased PdIn bimetallic formation is observed up to 573 K reduction temperature until at 623 K the film stability limit in hydrogen is reached. Oxidative treatments at 573 K lead to decomposition of PdIn and to the formation of an In2O3 shell covering the Pd particles, which irreversibly changes the activity and selectivity pattern to clean In2O3. PdIn and Pd2In3 phases are obtained on the powder catalyst after reduction at 573 K and 673 K, respectively. Only CO2-selective methanol steam reforming is observed in the reduction temperature range between 473 K and 573 K. After reduction at 673 K encapsulation of the bimetallic particles by crystalline In2O3 suppresses CO2 formation and only activity and selectivity of clean In2O3 are measured.
Address
Corporate Author Thesis
Publisher Place of Publication Amsterdam Editor
Language Wos 000274869900023 Publication Date 2009-12-18
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0926-860X; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 4.339 Times cited 55 Open Access
Notes Esteem 026019 Approved Most recent IF: 4.339; 2010 IF: 3.384
Call Number UA @ lucian @ c:irua:81801 Serial 3553
Permanent link to this record