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Author Zalfani, M.; van der Schueren, B.; Hu, Z.-Y.; Rooke, J.C.; Bourguiga, R.; Wu, M.; Li, Y.; Van Tendeloo, G.; Su, B.-L. pdf  url
doi  openurl
  Title Novel 3DOM BiVO4/TiO2nanocomposites for highly enhanced photocatalytic activity Type A1 Journal article
  Year 2015 Publication Journal of materials chemistry A : materials for energy and sustainability Abbreviated Journal J Mater Chem A  
  Volume 3 Issue 3 Pages 21244-21256  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Novel 3DOM BiVO4/TiO2 nanocomposites with intimate contact were for the first time synthesized by a hydrothermal method in order to elucidate their visible-light-driven photocatalytic performances. BiVO4 nanoparticles and 3DOM TiO2 inverse opal were fabricated respectively. These materials were characterized by XRD, XPS, SEM, TEM, N2 adsorption–desorption and UV-vis diffuse (UV-vis) and photoluminescence spectroscopies. As references for comparison, a physical mixture of BiVO4 nanoparticles and 3DOM TiO2 inverse opal powder (0.08 : 1), and a BiVO4/P25 TiO2 (0.08 : 1) nanocomposite made also by the hydrothermal method were prepared. The photocatalytic performance of all the prepared materials was evaluated by the degradation of rhodamine B (RhB) as a model pollutant molecule under visible light irradiation. The highly ordered 3D macroporous inverse opal structure can provide more active surface areas and increased mass transfer because of its highly accessible 3D porosity. The results show that 3DOM BiVO4/TiO2 nanocomposites possess a highly prolonged lifetime and increased separation of visible light generated charges and extraordinarily high photocatalytic activity. Owing to the intimate contact between BiVO4 and large surface area 3DOM TiO2, the photogenerated high energy charges can be easily transferred from BiVO4 to the 3DOM TiO2 support. BiVO4 nanoparticles in the 3DOM TiO2 inverse opal structure act thus as a sensitizer to absorb visible light and to transfer efficiently high energy electrons to TiO2 to ensure long lifetime of the photogenerated charges and keep them well separated, owing to the direct band gap of BiVO4 of 2.4 eV, favourably positioned band edges, very low recombination rate of electron–hole pairs and stability when coupled with photocatalysts, explaining the extraordinarily high photocatalytic performance of 3DOM BiVO4/TiO2 nanocomposites. It is found that larger the amount of BiVO4 in the nanocomposite, longer the duration of photogenerated charge separation and higher the photocatalytic activity. This work can shed light on the development of novel visible light responsive nanomaterials for efficient solar energy utilisation by the intimate combination of an inorganic light sensitizing nanoparticle with an inverse opal structure with high diffusion efficiency and high accessible surface area.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000363163200049 Publication Date 2015-09-08  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2050-7488;2050-7496; ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 8.867 Times cited 88 Open Access  
  Notes This work was realized with the financial support of the Belgian FNRS (Fonds National de la Recherche Scientifique). This research used resources of the Electron Microscopy Service located at the University of Namur. This Service is a member of the “Plateforme Technologique Morphologie – Imagerie”. The XPS analyses were made in the LISE, Department of Physics of the University of Namur thanks to Dr P. Louette. This work was also supported by Changjiang Scholars and the Innovative Research Team (IRT1169) of the Ministry of Education of the People's Republic of China. B. L. Su acknowledges the Chinese Central Government for an “Expert of the State” position in the Program of the “Thousand Talents” and a Clare Hall Life Membership at the Clare Hall and the financial support of the Department of Chemistry, University of Cambridge. G. Van Tendeloo and Z. Y. Hu acknowledge support from the EC Framework 7 program ESTEEM2 (Reference 312483).; esteem2_jra4 Approved Most recent IF: 8.867; 2015 IF: 7.443  
  Call Number (up) c:irua:129476 c:irua:129476 Serial 3951  
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Author Van Aert, S.; De Backer, A.; Martinez, G.T.; den Dekker, A.J.; Van Dyck, D.; Bals, S.; Van Tendeloo, G. pdf  url
doi  openurl
  Title Advanced electron crystallography through model-based imaging Type A1 Journal article
  Year 2016 Publication IUCrJ Abbreviated Journal Iucrj  
  Volume 3 Issue 3 Pages 71-83  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT); Vision lab; Engineering Management (ENM)  
  Abstract The increasing need for precise determination of the atomic arrangement of non-periodic structures in materials design and the control of nanostructures explains the growing interest in quantitative transmission electron microscopy. The aim is to extract precise and accurate numbers for unknown structure parameters including atomic positions, chemical concentrations and atomic numbers. For this purpose, statistical parameter estimation theory has been shown to provide reliable results. In this theory, observations are considered purely as data planes, from which structure parameters have to be determined using a parametric model describing the images. As such, the positions of atom columns can be measured with a precision of the order of a few picometres, even though the resolution of the electron microscope is still one or two orders of magnitude larger. Moreover, small differences in average atomic number, which cannot be distinguished visually, can be quantified using high-angle annular dark-field scanning transmission electron microscopy images. In addition, this theory allows one to measure compositional changes at interfaces, to count atoms with single-atom sensitivity, and to reconstruct atomic structures in three dimensions. This feature article brings the reader up to date, summarizing the underlying theory and highlighting some of the recent applications of quantitative model-based transmisson electron microscopy.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000368590900010 Publication Date 2015-11-13  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2052-2525; ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 5.793 Times cited 30 Open Access OpenAccess  
  Notes The authors gratefully acknowledge the Research Foundation Flanders (FWO, Belgium) for funding and for a PhD grant to ADB. The research leading to these results has received funding from the European Union 7th Framework Program (FP7/20072013) under grant agreement No. 312483 (ESTEEM2). SB and GVT acknowledge the European Research Council under the 7th Framework Program (FP7), ERC grant No. 335078 – COLOURATOMS and ERC grant No. 246791 – COUNTATOMS.; esteem2jra2; ECASSara; (ROMEO:green; preprint:; postprint:can ; pdfversion:can); Approved Most recent IF: 5.793  
  Call Number (up) c:irua:129589 c:irua:129589 Serial 3965  
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Author Poelma, R.H.; Fan, X.; Hu, Z.-Y.; Van Tendeloo, G.; van Zeijl, H.W.; Zhang, G.Q. pdf  doi
openurl 
  Title Effects of Nanostructure and Coating on the Mechanics of Carbon Nanotube Arrays Type A1 Journal article
  Year 2016 Publication Advanced functional materials Abbreviated Journal Adv Funct Mater  
  Volume 26 Issue 26 Pages 1233-1242  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Nanoscale materials are one of the few engineering materials that can be grown from the bottom up in a controlled manner. Here, the effects of nanostructure and nanoscale conformal coating on the mechanical behavior of vertically aligned carbon nanotube (CNT) arrays through experiments and simulation are systematically investigated. A modeling approach is developed and used to quantify the compressive strength and modulus of the CNT array under large deformation. The model accounts for the porous

nanostructure, which contains multiple CNTs with random waviness, van der Waals interactions, fracture strain, contacts, and frictional forces. CNT array micropillars are grown and their porous nanostructure is controlled by the infi ltration and deposition of thin conformal coatings using chemical vapor deposition. Flat-punch nanoindentation experiments reveal signifi cant changes in material properties as a function of coating thickness. The simulations explain the experimental results and show the novel failure transition regime that changes from collective CNT buckling toward structural collapse due to fracture. The compressive strength and the elastic

modulus increase exponentially as a function of the coating thickness and demonstrate a unique dependency on the CNT waviness. More interestingly, a design rule is identifi ed that predicts the optimum coating thickness for porous materials.
 
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000371078100010 Publication Date 2016-01-04  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1616-301X ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 12.124 Times cited 17 Open Access  
  Notes The research leading to the TEM/HAADF-STEM results received funding from the EC Framework 7 Program ESTEEM2 (Reference 312483). We wish to acknowledge the support of the Else Kooi Laboratory for their assistance during the clean room processing.; esteem2_ta Approved Most recent IF: 12.124  
  Call Number (up) c:irua:130060 c:irua:130060 Serial 3996  
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Author Bertoni, G.; Fabbri, F.; Villani, M.; Lazzarini, L.; Turner, S.; Van Tendeloo, G.; Calestani, D.; Gradečak, S.; Zappettini, A.; Salviati, G. pdf  url
doi  openurl
  Title Nanoscale mapping of plasmon and exciton in ZnO tetrapods coupled with Au nanoparticles Type A1 Journal article
  Year 2016 Publication Scientific reports Abbreviated Journal Sci Rep-Uk  
  Volume 6 Issue 6 Pages 19168  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Metallic nanoparticles can be used to enhance optical absorption or emission in semiconductors, thanks to a strong interaction of collective excitations of free charges (plasmons) with electromagnetic fields. Herein we present the direct imaging at the nanoscale of plasmon-exciton coupling in Au/ZnO nanostructures by combining scanning transmission electron energy loss and cathodoluminescence spectroscopy and mapping. The Au nanoparticles (~30 nm in diameter) are grown in-situ on ZnO nanotetrapods by means of a photochemical process without the need of binding agents or capping molecules. This results in clean interfaces, enabling to prove the occurrence of the plasmon-exciton coupling and the straightforward mapping of its spatial localization. Interestingly, the Au plasmon resonance is localized at the Au/vacuum interface, rather than presenting an isotropic distribution around the nanoparticle. On the contrary, a strong localization of the ZnO excitons, has been observed inside the Au nanoparticle, revealing the existence of the plasmon-exciton coupling, as also confirmed by numerical simulations.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000368111900001 Publication Date 2016-01-12  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2045-2322 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 4.259 Times cited 15 Open Access  
  Notes The research leading to these results has received funding from the European Union FP7 Grant Agreement n. 265073 ITN-Nanowiring, and FP7 Grant Agreement n. 312483 ESTEEM2 for Integrated Infrastructure Initiative – I3. S.T. gratefully acknowledges the FWO Vlaanderen. G.V.T. acknowledges the European Research Council (ERC grant N°246791 – COUNTATOMS). The authors thank Alessandra Catellani and Arrigo Calzolari for helpful discussions.; Esteem2_jra3 Approved Most recent IF: 4.259  
  Call Number (up) c:irua:130406 c:irua:130406 Serial 3999  
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Author Paria Sena, R.; Babaryk, A.A.; Khainakov, S.; Garcia-Granda, S.; Slobodyanik, N.S.; Van Tendeloo, G.; Abakumov, A.M.; Hadermann, J. pdf  url
doi  openurl
  Title A pseudo-tetragonal tungsten bronze superstructure: a combined solution of the crystal structure of K6.4(Nb,Ta)36.3O94 with advanced transmission electron microscopy and neutron diffraction Type A1 Journal article
  Year 2016 Publication Journal of the Chemical Society : Dalton transactions Abbreviated Journal Dalton T  
  Volume 45 Issue 45 Pages 973-979  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract The crystal structure of the K6.4Nb28.2Ta8.1O94 pseudo-tetragonal tungsten bronze-type oxide was determined using a combination of X-ray powder diffraction, neutron diffraction and transmission electron microscopy techniques, including electron diffraction, high angle annular dark field scanning transmission electron microscopy (HAADF-STEM), annular bright field STEM (ABF-STEM) and energy-dispersive X-ray compositional mapping (STEM-EDX). The compound crystallizes in the space group Pbam with unit cell parameters a = 37.468(9) A, b = 12.493(3) A, c = 3.95333(15) A. The structure consists of corner sharing (Nb,Ta)O6 octahedra forming trigonal, tetragonal and pentagonal tunnels. All tetragonal tunnels are occupied by K(+) ions, while 1/3 of the pentagonal tunnels are preferentially occupied by Nb(5+)/Ta(5+) and 2/3 are occupied by K(+) in a regular pattern. A fractional substitution of K(+) in the pentagonal tunnels by Nb(5+)/Ta(5+) is suggested by the analysis of the HAADF-STEM images. In contrast to similar structures, such as K2Nb8O21, also parts of the trigonal tunnels are fractionally occupied by K(+) cations.  
  Address Electron Microscopy for Materials Research (EMAT), University of Antwerp, Groenenborgerlaan 171, B-2020, Antwerp, Belgium. joke.hadermann@uantwerpen.be babaryk@univ.kiev.ua  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language English Wos 000367614700018 Publication Date 2015-11-23  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1477-9226 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 4.029 Times cited 6 Open Access  
  Notes We thank Dr E. Suard and Dr O. Fabello for assistance in collecting the neutron diffraction data. R.P.S. acknowledges funding from the European Research Council under the 7th Framework Program (FP7), ERC Grant No. 246791-COUNTATOMS. The titan microscope was partly funded by the Hercules fund from the Flemish Government. The authors acknowledge financial support from the European Union under the Seventh Framework Program under a contract for an Integrated Infrastructure Initiative. Reference No. 312483-ESTEEM2. AAB acknowledges the JSPDS ICDD Grant-in-Aid program (12-02).; esteem2jra1; esteem2jra2 Approved Most recent IF: 4.029  
  Call Number (up) c:irua:130408 c:irua:130408 Serial 3998  
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Author Zanaga, D.; Bleichrodt, F.; Altantzis, T.; Winckelmans, N.; Palenstijn, W.J.; Sijbers, J.; de Nijs, B.; van Huis, M.A.; Sanchez-Iglesias, A.; Liz-Marzan, L.M.; van Blaaderen, A.; Joost Batenburg, K.; Bals, S.; Van Tendeloo, G. pdf  url
doi  openurl
  Title Quantitative 3D analysis of huge nanoparticle assemblies Type A1 Journal article
  Year 2016 Publication Nanoscale Abbreviated Journal Nanoscale  
  Volume 8 Issue 8 Pages 292-299  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Vision lab  
  Abstract Nanoparticle assemblies can be investigated in 3 dimensions using electron tomography. However, it is not straightforward to obtain quantitative information such as the number of particles or their relative position. This becomes particularly difficult when the number of particles increases. We propose a novel approach in which prior information on the shape of the individual particles is exploited. It improves the quality of the reconstruction of these complex assemblies significantly. Moreover, this quantitative Sparse Sphere Reconstruction approach yields directly the number of particles and their position as an output of the reconstruction technique, enabling a detailed 3D analysis of assemblies with as many as 10 000 particles. The approach can also be used to reconstruct objects based on a very limited number of projections, which opens up possibilities to investigate beam sensitive assemblies where previous reconstructions with the available electron tomography techniques failed.  
  Address EMAT, University of Antwerp, Groenenborgerlaan 171, B-2020 Antwerp, Belgium. sara.bals@uantwerpen.be  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language English Wos 000366911700028 Publication Date 2015-11-19  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2040-3364 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 7.367 Times cited 34 Open Access OpenAccess  
  Notes The authors acknowledge financial support from European Research Council (ERC Starting Grant # 335078-COLOURATOMS, ERC Advanced Grant # 291667 HierarSACol and ERC Advanced Grant 267867 – PLASMAQUO), the European Union under the FP7 (Integrated Infrastructure Initiative N. 262348 European Soft Matter Infrastructure, ESMI and N. 312483 ESTEEM2), and from the Netherlands Organisation for Scientific Research (NWO), project number 639.072.005 and NWO CW 700.57.026. Networking support was provided by COST Action MP1207.; esteem2jra4; ECASSara; (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:cannot); Approved Most recent IF: 7.367  
  Call Number (up) c:irua:131062 c:irua:131062 Serial 3979  
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Author Ren, X.-N.; Wu, L.; Jin, J.; Liu, J.; Hu, Z.-Y.; Li, Y.; Hasan, T.; Yang, X.-Y.; Van Tendeloo, G.; Su, B.-L. pdf  url
doi  openurl
  Title 3D interconnected hierarchically macro-mesoporous TiO2networks optimized by biomolecular self-assembly for high performance lithium ion batteries Type A1 Journal article
  Year 2016 Publication RSC advances Abbreviated Journal Rsc Adv  
  Volume 6 Issue 6 Pages 26856-26862  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract Biomolecular self-assembly is an effective synthesis strategy for materials fabrication with unique structural complexity and properties. For the first time, we intergrate inner-particle mesoporosity in a three-dimensional (3D) interconnected macroporous TiO2 structure via the mediation of biomolecular self-assembly of the lipids and proteins from rape pollen coats and P123 to optimize the structure for high performance lithium storage. Benefitting from the hierarchically 3D interconnected macro-mesoporous structure with high surface area, small nanocrystallites and good electrolyte permeation, such unique porous structure demonstrates superior electrochemical performance, with high initial coulombic efficiency (94.4% at 1C) and a reversible discharge capacity of 161, 145, 127 and 97 mA h g-1 at 2, 5, 10 and 20C for 1000 cycles, with 79.3%, 89.9%, 90.1% and 87.4% capacity retention, respectively. Using SEM, TEM and HRTEM observations on the TiO2 materials before and after cycling, we verify that the inner-particle mesoporosity and the Li2Ti2O4 nanocrystallites formed during the cycling process in interconnected macroporous structure largely enhance the cycle life and rate performance. Our demonstration here offers opportunities towards developing and optimizing hierarchically porous structures for energy storage applications via biomolecular self-assembly.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000372253700043 Publication Date 2016-03-07  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2046-2069 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 3.108 Times cited 16 Open Access  
  Notes G. Van Tendeloo and Z. Y. Hu acknowledge support from the EC Framework 7 program ESTEEM2 (Reference 312483).; esteem2_jra4 Approved Most recent IF: 3.108  
  Call Number (up) c:irua:131915 c:irua:131915 c:irua:131915 Serial 4022  
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Author Yang, Z.; Altantzis, T.; Zanaga, D.; Bals, S.; Van Tendeloo, G.; Pileni, M.-P. pdf  url
doi  openurl
  Title Supracrystalline Colloidal Eggs: Epitaxial Growth and Freestanding Three-Dimensional Supracrystals in Nanoscaled Colloidosomes Type A1 Journal article
  Year 2016 Publication Journal of the American Chemical Society Abbreviated Journal J Am Chem Soc  
  Volume 138 Issue 138 Pages 3493-3500  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract The concept of template-confined chemical reactions allows the synthesis of complex molecules that would hardly be producible through conventional method. This idea was developed to produce high quality nanocrystals more than 20 years ago. However, template-mediated assembly of colloidal nanocrystals is still at an elementary level, not only because of the limited templates suitable for colloidal assemblies, but also because of the poor control over the assembly of nanocrystals within a confined space. Here, we report the design of a new system called “supracrystalline colloidal eggs” formed by controlled assembly of nanocrystals into complex colloidal supracrystals through superlattice-matched epitaxial overgrowth along the existing colloidosomes. Then, with this concept, we extend the supracrystalline growth to lattice-mismatched binary nanocrystal superlattices, in order to reach anisotropic superlattice growths, yielding freestanding binary nanocrystal supracrystals that could not be produced previously.  
  Address CEA/IRAMIS , CEA Saclay F-91191 Gif-sur-Yvette, France  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language English Wos 000372477700034 Publication Date 2016-02-24  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 0002-7863 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 13.858 Times cited 57 Open Access OpenAccess  
  Notes The research leading to these results has been supported by an Advanced Grant of the European Research Council under Grant 267129. The authors appreciate financial support by the European Union under the Framework 7 program under a contract for an Integrated Infrastructure Initiative (Reference No. 312483 ESTEEM2). The authors thank Dr. P. A. Albouy for the SAXS measurement.; esteem2_ta Approved Most recent IF: 13.858  
  Call Number (up) c:irua:131923 c:irua:131923 Serial 4018  
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Author Sathiya, M.; Abakumov, A.M.; Foix, D.; Rousse, G.; Ramesha, K.; Saubanère, M.; Doublet, M. .; Vezin, H.; Laisa, C.P.; Prakash, A.S.; Gonbeau, D.; Van Tendeloo, G.; Tarascon, J.M. pdf  url
doi  openurl
  Title Origin of voltage decay in high-capacity layered oxide electrodes Type A1 Journal article
  Year 2015 Publication Nature materials Abbreviated Journal Nat Mater  
  Volume 14 Issue 14 Pages 230-238  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract Although Li-rich layered oxides (Li1+xNiyCozMn1−x−y−zO2 > 250 mAh g−1) are attractive electrode materials providing energy densities more than 15% higher than todays commercial Li-ion cells, they suffer from voltage decay on cycling. To elucidate the origin of this phenomenon, we employ chemical substitution in structurally related Li2RuO3 compounds. Li-rich layered Li2Ru1−yTiyO3 phases with capacities of ~240 mAh g−1 exhibit the characteristic voltage decay on cycling. A combination of transmission electron microscopy and X-ray photoelectron spectroscopy studies reveals that the migration of cations between metal layers and Li layers is an intrinsic feature of the chargedischarge process that increases the trapping of metal ions in interstitial tetrahedral sites. A correlation between these trapped ions and the voltage decay is established by expanding the study to both Li2Ru1−ySnyO3 and Li2RuO3; the slowest decay occurs for the cations with the largest ionic radii. This effect is robust, and the finding provides insights into new chemistry to be explored for developing high-capacity layered electrodes that evade voltage decay.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication London Editor  
  Language Wos 000348600200024 Publication Date 2014-12-01  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1476-1122;1476-4660; ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 39.737 Times cited 395 Open Access  
  Notes 246791 Countatoms; 312483 Esteem2; esteem2_ta Approved Most recent IF: 39.737; 2015 IF: 36.503  
  Call Number (up) c:irua:132555 c:irua:132555 Serial 2528  
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Author Liao, Z.; Huijben, M.; Zhong, Z.; Gauquelin, N.; Macke, S.; Green, R.J.; Van Aert, S.; Verbeeck, J.; Van Tendeloo, G.; Held, K.; Sawatzky, G.A.; Koster, G.; Rijnders, G. url  doi
openurl 
  Title Controlled lateral anisotropy in correlated manganite heterostructures by interface-engineered oxygen octahedral coupling Type A1 Journal article
  Year 2016 Publication Nature materials Abbreviated Journal Nat Mater  
  Volume 15 Issue 15 Pages 425-431  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract Controlled in-plane rotation of the magnetic easy axis in manganite heterostructures by tailoring the interface oxygen network could allow the development of correlated oxide-based magnetic tunnelling junctions with non-collinear magnetization, with possible practical applications as miniaturized high-switching-speed magnetic random access memory (MRAM) devices. Here, we demonstrate how to manipulate magnetic and electronic anisotropic properties in manganite heterostructures by engineering the oxygen network on the unit-cell level. The strong oxygen octahedral coupling is found to transfer the octahedral rotation, present in the NdGaO3 (NGO) substrate, to the La2/3Sr1/3MnO3 (LSMO) film in the interface region. This causes an unexpected realignment of the magnetic easy axis along the short axis of the LSMO unit cell as well as the presence of a giant anisotropic transport in these ultrathin LSMO films. As a result we possess control of the lateral magnetic and electronic anisotropies by atomic-scale design of the oxygen octahedral rotation.  
  Address MESA+ Institute for Nanotechnology, University of Twente, PO Box 217, 7500 AE Enschede, The Netherlands  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language English Wos 000372591700017 Publication Date 2016-03-07  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1476-1122 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 39.737 Times cited 273 Open Access  
  Notes We would like to acknowledge Dr. Evert Houwman for stimulated discussion. M.H., G.K. and G.R. acknowledge funding from DESCO program of the Dutch Foundation for Fundamental Research on Matter (FOM) with financial support from the Netherlands Organization for Scientific Research (NWO). This work was funded by the European Union Council under the 7th Framework Program (FP7) grant nr NMP3-LA-2010- 246102 IFOX. J.V. and S.V.A. acknowledges funding from FWO project G.0044.13N and G. 0368.15N. The Qu-Ant-EM microscope was partly funded by the Hercules fund from the Flemish Government. N.G. acknowledges funding from the European Research Council under the 7th Framework Program (FP7), ERC Starting Grant 278510 VORTEX. N.G., S.V.A., J.V. and G.V.T. acknowledge financial support from the European Union under the Seventh Framework Program under a contract for an Integrated Infrastructure Initiative (Reference No. 312483-ESTEEM2). The Canadian work was supported by NSERC and the Max Planck-UBC Centre for Quantum Materials. Some experiments for this work were performed at the Canadian Light Source, which is funded by the Canada Foundation for Innovation, NSERC, the National Research Council of Canada, the Canadian Institutes of Health Research, the Government of Saskatchewan, Western Economic Diversification Canada, and the University of Saskatchewan. Z.Z. acknowledges funding from the SFB ViCoM (Austrian Science Fund project ID F4103- N13), and Calculations have been done on the Vienna Scientific Cluster (VSC).; esteem2jra2; esteem2jra3 ECASJO_; Approved Most recent IF: 39.737  
  Call Number (up) c:irua:133190 c:irua:133190UA @ admin @ c:irua:133190 Serial 4041  
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Author Lottini, E.; López-Ortega, A.; Bertoni, G.; Turner, S.; Meledina, M.; Van Tendeloo, G.; de Julián Fernández, C.; Sangregorio, C. url  doi
openurl 
  Title Strongly Exchange Coupled Core|Shell Nanoparticles with High Magnetic Anisotropy: A Strategy toward Rare-Earth-Free Permanent Magnets Type A1 Journal article
  Year 2016 Publication Chemistry of materials Abbreviated Journal Chem Mater  
  Volume 28 Issue 28 Pages 4214-4222  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract Antiferromagnetic(AFM)|ferrimagnetic(FiM) core|shell (CS) nanoparticles (NPs) of formula Co0.3Fe0.7O|Co0.6Fe2.4O4 with mean diameter from 6 to 18 nm have been synthesized through a one-pot thermal decomposition process. The CS structure has been generated by topotaxial oxidation of the core region, leading to the formation of a highly monodisperse single inverted AFM|FiM CS system with variable AFM-core diameter and constant FiM-shell thickness (~2 nm). The sharp interface, the high structural matching between both phases and the good crystallinity of the AFM material have been structurally demonstrated and are corroborated by the robust exchange-coupling between AFM and FiM phases, which gives rise to one among the largest exchange bias (HE) values ever reported for CS NPs (8.6 kOe) and to a strongly enhanced coercive field (HC). In addition, the investigation of the magnetic properties as a function of the AFM-core size (dAFM), revealed a non-monotonous trend of both HC and HE, which display a maximum value for dAFM = 5 nm (19.3 and 8.6 kOe, respectively). These properties induce a huge improvement of the capability of storing energy of the material, a result which suggests that the combination of highly anisotropic AFM|FiM materials can be an efficient strategy towards the realization of novel Rare Earth-free permanent magnets.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000378973100013 Publication Date 2016-05-20  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 9.466 Times cited 48 Open Access  
  Notes This work was supported by the EU-FP7 through NANOPYME Project (No. 310516) and Integrated Infrastructure Initiative ESTEEM2 (No. 312483). S.T. gratefully acknowledges the FWO Flanders for a post-doctoral scholarship.; esteem2_ta Approved Most recent IF: 9.466  
  Call Number (up) c:irua:134084 c:irua:134084 Serial 4092  
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Author Altantzis, T.; Coutino-Gonzalez, E.; Baekelant, W.; Martinez, G.T.; Abakumov, A.M.; Van Tendeloo, G.; Roeffaers, M.B.J.; Bals, S.; Hofkens, J. pdf  url
doi  openurl
  Title Direct Observation of Luminescent Silver Clusters Confined in Faujasite Zeolites Type A1 Journal article
  Year 2016 Publication ACS nano Abbreviated Journal Acs Nano  
  Volume 10 Issue 10 Pages 7604-7611  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract One of the ultimate goals in the study of metal clusters is the correlation between the atomic-scale organization and their physicochemical properties. However, direct observation of the atomic organization of such minuscule metal clusters is heavily hindered by radiation damage imposed by the different characterization techniques. We present direct evidence of the structural arrangement, at an atomic level, of luminescent silver species stabilized in faujasite (FAU) zeolites using aberration-corrected scanning transmission electron microscopy. Two different silver clusters were identified in Ag-FAU zeolites, a trinuclear silver species associated with green emission and a tetranuclear silver species related to yellow emission. By combining direct imaging with complementary information obtained from X-ray powder diffraction and Rietveld analysis, we were able to elucidate the main differences at an atomic scale between luminescent (heat-treated) and nonluminescent (cation-exchanged) Ag-FAU zeolites. It is expected that such insights will trigger the directed synthesis of functional metal nanocluster-zeolite composites with tailored luminescent properties.  
  Address RIES, Hokkaido University , N20W10, Kita-Ward Sapporo 001-0020, Japan  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language English Wos 000381959100043 Publication Date 2016-07-08  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 13.942 Times cited 57 Open Access OpenAccess  
  Notes The authors gratefully acknowledge financial support from the Belgian Federal government (Belspo through the IAP-VI/27 and IAP-VII/05 programs), the European Union’s Seventh Framework Programme (FP7/2007-2013 under grant agreement no. 310651 SACS and no. 312483-ESTEEM2), the Flemish government in the form of long-term structural funding “Methusalem” grant METH/15/04 CASAS2, the Hercules foundation (HER/11/14), the “Strategisch Initiatief Materialen” SoPPoM program, and the Fund for Scientific Research Flanders (FWO) grants G.0349.12 and G.0B39.15. S.B. acknowledges funding from ERC Starting Grant COLOURATOMS (335078). The authors thank Prof. S. Van Aert for helpful discussions, Dr. T. De Baerdemaeker for XRD measurements, Mr. B. Dieu for the preparation of graphical material, and UOP Antwerp for the kind donation of zeolite samples.; esteem2jra4; ECASSara; (ROMEO:white; preprint:; postprint:restricted 12 months embargo; pdfversion:cannot); Approved Most recent IF: 13.942  
  Call Number (up) c:irua:134576 c:irua:134576 Serial 4102  
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Author Ying, J.; Hu, Z.-Y.; Yang, X.-Y.; Wei, H.; Xiao, Y.-X.; Janiak, C.; Mu, S.-C.; Tian, G.; Pan, M.; Van Tendeloo, G.; Su, B.-L. pdf  url
doi  openurl
  Title High viscosity to highly dispersed PtPd bimetallic nanocrystals for enhanced catalytic activity and stability Type A1 Journal article
  Year 2016 Publication Chemical communications Abbreviated Journal Chem Commun  
  Volume 52 Issue 52 Pages 8219-8222  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract A facile high-viscosity-solvent method is presented to synthesize PtPd bimetallic nanocrystals highly dispersed in different mesostructures (2D and 3D structures), porosities (large and small pore sizes), and compositions (silica and carbon). Further, highly catalytic activity, stability and durability of the nanometals have been proven in different catalytic reactions.  
  Address State Key Laboratory Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, 122, Luoshi Road, Wuhan, 430070, China. xyyang@whut.edu.cn  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language English Wos 000378715400006 Publication Date 2016-05-16  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1359-7345 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 6.319 Times cited 19 Open Access  
  Notes This work was supported by NFSC (51472190 and 51503166), ISTCP (2015DFE52870), PCSIRT (IRT15R52) of China, and the Integrated Infrastructure Initiative of EU (312483-ESTEEM2).; esteem2jra4 Approved Most recent IF: 6.319  
  Call Number (up) c:irua:134660 c:irua:134660 Serial 4110  
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Author Zalfani, M.; Hu, Z.-Y.; Yu, W.-B.; Mahdouani, M.; Bourguig, R.; Wu, M.; Li, Y.; Van Tendeloo, G.; Djoued, Y.; Su, B.-L. pdf  url
doi  openurl
  Title BiVO4/3DOM TiO2 nanocomposites: Effect of BiVO4 as highly efficient visible light sensitizer for highly improved visible light photocatalytic activity in the degradation of dye pollutants Type A1 Journal article
  Year 2016 Publication Applied Catalysis B-Environmental Abbreviated Journal Appl Catal B-Environ  
  Volume 205 Issue 205 Pages 121-132  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract A series of BiVO4/3DOM TiO2 nanocomposites have been synthesized and their photocatalytic activity was investigated under visible light irradiation using the RhB dye as model pollutant molecule in an aqueous solution. The effect of the amount of BiVO4 as visible light sensitizer on the photocatalytic activity of BiVO4/3DOM TiO2 nanocomposites was highlighted. The heterostructured composite system leads to much higher photocatalytic efficiencies than bare 3DOM TiO2 and BiVO4 nanoparticles. As the proportion of BiVO4 in BiVO4/3DOM TiO2 nanocomposites increases from 0.04 to 0.6, the photocatalytic performance of the BiVO4/3DOM TiO2 nanocomposites increases and then decreases after reaching a maximum at 0.2. This improvement in photocatalytic perfomance is related to 1) the interfacial electron transfer efficiency between the coupled materials, 2) the 3DOM TiO2 inverse opal structure with interconnected pores providing an easy mass transfer of the reactant molecules and high accessibility to the active sites and large surface area and 3) the effect of light sensitizer of BiVO4. Intensive studies on structural, textural, optical and surface properties reveal that the electronic interactions between BiVO4 and TiO2 lead to an improved charge separation of the coupled BiVO4/TiO2 system. The photogenerated charge carrier densities increase with increasing the BiVO4 content, which acts as visible light sensitizer to the TiO2 and is responsible for the enhancement in the rate of photocatalytic degradation. However, the photocatalytic activity is reduced when the BiVO4 amount is much higher than that of 3DOM TiO2. Two reasons could account for this behavior. First, with increasing BiVO4 content, the photogenerated electron/hole pairs are accumulated at the surface of the BiVO4 nanoparticles and the recombination rate increases as shown by the PL results. Second, decreasing the amount of 3DOM TiO2 in the nanocomposite decreases the surface area as shown by the BET results. Moreover, the poor adsorptive properties of the BiVO4 photocatalyst also affect the photocatalytic performance, in particular at higher BiVO4 content. The present work demonstrates that BiVO4/3DOM TiO2 is a very promising heterojunction system for visible light photocatalytic applications.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000393931000013 Publication Date 2016-12-08  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 0926-3373 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 9.446 Times cited 52 Open Access OpenAccess  
  Notes Z. Y. Hu and G. Van Tendeloo acknowledge support from the EC Framework 7 program ESTEEM2 (Reference 312483). Approved Most recent IF: 9.446  
  Call Number (up) EMAT @ emat @ Serial 4323  
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Author Barreca, D.; Carraro, G.; Gasparotto, A.; Maccato, C.; Warwick, M.E.A.; Turner, S.; Van Tendeloo, G. pdf  doi
openurl 
  Title Fabrication and Characterization of Fe2O3-Based Nanostructures Functionalized with Metal Particles and Oxide Overlayers Type A1 Journal article
  Year 2015 Publication Journal of advanced microscopy research Abbreviated Journal  
  Volume 10 Issue 10 Pages 239-243  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract We report on the design of nanosystems based on functionalized -Fe 2 O 3 nanostructures supported on fluorine-doped tin oxide (FTO) substrates. The target materials were developed by means of hybrid vapor phase approaches, combining plasma assisted-chemical vapor deposition (PA-CVD) for the production of iron(III) oxide systems and the subsequent radio frequency (RF)-sputtering or atomic layer deposition (ALD) for the functionalization with Au nanoparticles or TiO 2 overlayers, respectively. The interplay between material characteristics and the adopted processing parameters was investigated by complementary analytical techniques, encompassing X-ray photoelectron spectroscopy (XPS), field emission-scanning electron microscopy (FE-SEM), high angle annular dark field-scanning transmission electron microscopy (HAADF-STEM), and energy dispersive X-ray spectroscopy (EDXS). The obtained results highlight the possibility of fabricating Au/ -Fe 2 O 3 nanocomposites, with a controlled dispersion and distribution of metal particles, and TiO 2 / -Fe 2 O 3 heterostructures, characterized by an intimate coupling between the constituent oxides.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos Publication Date 2015-12-01  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2156-7573 ISBN Additional Links UA library record  
  Impact Factor Times cited Open Access  
  Notes The authors acknowledge the financial support under the FP7 project “SOLARO- GENIX” (NMP4-SL-2012-310333), as well as Padova University ex-60% 2012–2015 projects, grant n CPDR132937/13 (SOLLEONE), and Regione Lombardia- INSTM ATLANTE program. Stuart Turner acknowledges the FWO Flanders for a post-doctoral scholarship. Thanks are also due to Dr. L. Borgese and Prof. E. Bontempi (Chemistry for Technologies Laboratory, Brescia Univer- sity, Italy) for precious assistance in ALD experiments. Approved Most recent IF: NA  
  Call Number (up) EMAT @ emat @ c:irua:132798 Serial 4058  
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Author De Keukeleere, K.; Cayado, P.; Meledin, A.; Vallès, F.; De Roo, J.; Rijckaert, H.; Pollefeyt, G.; Bruneel, E.; Palau, A.; Coll, M.; Ricart, S.; Van Tendeloo, G.; Puig, T.; Obradors, X.; Van Driessche, I. url  doi
openurl 
  Title Superconducting YBa2Cu3O7-δNanocomposites Using Preformed ZrO2Nanocrystals: Growth Mechanisms and Vortex Pinning Properties Type A1 Journal article
  Year 2016 Publication Advanced Electronic Materials Abbreviated Journal  
  Volume 2 Issue 2 Pages 1600161  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Although high temperature superconductors are promising for power applications, the production of low-cost coated conductors with high current densities—at high magnetic fields—remains challenging. A superior superconducting YBa2Cu3O7–δ nanocomposite is fabricated via chemical solution deposition (CSD) using preformed nanocrystals (NCs). Preformed, colloidally stable ZrO2 NCs are added to the trifluoroacetic acid based precursor solution and the NCs' stability is confirmed up to 50 mol% for at least 2.5 months. These NCs tend to disrupt the epitaxial growth of YBa2Cu3O7–δ, unless a thin seed layer is applied. A 10 mol% ZrO2 NC addition proved to be optimal, yielding a critical current density JC of 5 MA cm−2 at 77 K in self-field. Importantly, this new approach results in a smaller magnetic field decay of JC(H//c) for the nanocomposite compared to a pristine film. Furthermore, microstructural analysis of the YBa2Cu3O7–δ nanocomposite films reveals that different strain generation mechanisms may occur compared to the spontaneous segregation approach. Yet, the generated nanostrain in the YBa2Cu3O7–δ nanocomposite results in an improvement of the superconducting properties similar to the spontaneous segregation approach. This new approach, using preformed NCs in CSD coatings, can be of great potential for high magnetic field applications.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000386624100003 Publication Date 2016-09-05  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2199160X ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor Times cited 26 Open Access  
  Notes This work was financially supported by a BOF research fund of Ghent University (BOF11/DOC/286), FWO Flanders (F08512), and Eurotapes, a collaborative project funded by the European Community’s Seven Framework Program (EU-FP7 NMP-LA-2012-280432). We also acknowledge MINECO and FEDER funds for MAT2014-51778-C2-1-R and the Center of Excellence award Severo Ochoa SEV-2015-0496, and SGR753 from the Generalitat of Catalunya. MC acknowledges RyC contract 2013-12448 Approved Most recent IF: NA  
  Call Number (up) EMAT @ emat @ c:irua:135171 Serial 4118  
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Author Spadaro, M.C.; Luches, P.; Bertoni, G.; Grillo, V.; Turner, S.; Van Tendeloo, G.; Valeri, S.; D'Addato, S. pdf  url
doi  openurl
  Title Influence of defect distribution on the reducibility of CeO2-x nanoparticles Type A1 Journal article
  Year 2016 Publication Nanotechnology Abbreviated Journal Nanotechnology  
  Volume 27 Issue 27 Pages 425705  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract Ceria nanoparticles (NPs) are fundamental in heterogeneous catalysis because of their ability to store or release oxygen depending on the ambient conditions. Their oxygen storage capacity is strictly related to the exposed planes, crystallinity, density and distribution of defects. In this work a study of ceria NPs produced with a ligand-free, physical synthesis method is presented. The NP films were grown by a magnetron sputtering based gas aggregation source and studied by high resolution- and scanning-transmission electron microscopy and x-ray photoelectron spectroscopy. In particular, the influence of the oxidation procedure on the NP reducibility has been investigated. The different reducibility has been correlated to the exposed planes, crystallinity and density and distribution of structural defects. The results obtained in this work represent a basis to obtain cerium oxide NP with desired oxygen transport properties.  
  Address Dipartimento FIM, Universita di Modena e Reggio Emilia, via G. Campi 213/a, I-41125 Modena, Italy. CNR-NANO, via G. Campi 213/a, I-41125 Modena, Italy  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language English Wos 000385483900004 Publication Date 2016-09-15  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 0957-4484 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 3.44 Times cited 11 Open Access  
  Notes The authors gratefully acknowledge financial support by the Italian MIUR under grant FIRB RBAP115AYN (Oxides at the nanoscale: multifunctionality and applications). The activity is performed within the COST Action CM1104 'Reducible oxide chemistry, structure and functions'. The research leading to these results has received funding also from the European Union Seventh Framework Programme under Grant Agreement 312483—ESTEEM2 (Integrated Infrastructure Initiative–I3).; esteem2_ta Approved Most recent IF: 3.44  
  Call Number (up) EMAT @ emat @ c:irua:135424 Serial 4130  
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Author Carraro, G.; Maccato, C.; Gasparotto, A.; Warwick, M.E.A.; Sada, C.; Turner, S.; Bazzo, A.; Andreu, T.; Pliekhova, O.; Korte, D.; Lavrenčič Štangar, U.; Van Tendeloo, G.; Morante, J.R.; Barreca, D. pdf  doi
openurl 
  Title Hematite-based nanocomposites for light-activated applications: Synergistic role of TiO2 and Au introduction Type A1 Journal article
  Year 2017 Publication Solar energy materials and solar cells Abbreviated Journal Sol Energ Mat Sol C  
  Volume 159 Issue 159 Pages 456-466  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Photo-activated processes have been widely recognized as cost-effective and environmentally friendly routes for both renewable energy generation and purification/cleaning technologies. We report herein on a plasma- assisted approach for the synthesis of Fe 2 O 3 -TiO 2 nanosystems functionalized with Au nanoparticles. Fe 2 O 3 nanostructures were grown by plasma enhanced-chemical vapor deposition, followed by the sequential sputtering of titanium and gold under controlled conditions, and final annealing in air. The target nanosystems were subjected to a thorough multi-technique characterization, in order to elucidate the interrelations between their chemico-physical properties and the processing conditions. Finally, the functional performances were preliminarily investigated in both sunlight-assisted H 2 O splitting and photocatalytic activity tests in view of self- cleaning applications. The obtained results highlight the possibility of tailoring the system behaviour and candidate the present Fe 2 O 3 -TiO 2 -Au nanosystems as possible multi-functional low-cost platforms for light-activated processes.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000388053600053 Publication Date 2016-10-07  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 0927-0248 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 4.784 Times cited 15 Open Access Not_Open_Access  
  Notes The research leading to these results has received funding from the FP7 project “SOLAROGENIX” (NMP4-SL-2012-310333), as well as from Padova University ex-60% 2013-2016 projects, grant no. CPDR132937/13 (SOLLEONE) and the post-doc fellowship ACTION. INFINITY project in the framework of the EU Erasmus Mundus Action 2 is also acknowledged to provide a Ph.D. financial support as well as Slovenian Research Agency (program P2-0377). The authors are grateful to Dr. E. Toniato (Department of Chemistry, Padova University, Italy) for synthetic assistance and to Prof. E. Bontempi and Dr. M. Brisotto (Chemistry for Technologies Laboratory, Brescia University, Italy) for XRD analyses. Approved Most recent IF: 4.784  
  Call Number (up) EMAT @ emat @ c:irua:135833 Serial 4284  
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Author Perez, A.J.; Batuk, D.; Saubanère, M.; Rousse, G.; Foix, D.; Mc Calla, E.; J. Berg, E.; Dugas, R.; van den Bos, K. H. W.; Doublet, M.-L.; Gonbeau, D.; Abakumov, A.M.; Van Tendeloo, G.; Tarascon, J.-M. pdf  url
doi  openurl
  Title Strong oxygen participation in the redox governing the structural and electrochemical properties of Na-rich layered oxide Na2IrO3 Type A1 Journal article
  Year 2016 Publication Chemistry of materials Abbreviated Journal Chem Mater  
  Volume 28 Issue 28 Pages 8278-8288  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract The recent revival of the Na-ion battery concept has prompted intense activities in the search for new Na-based layered oxide positive electrodes. The largest capacity to date was obtained for a Na-deficient layered oxide that relies on cationic redox processes only. To go beyond this limit, we decided to chemically manipulate these Na-based layered compounds in a way to trigger the participation of the anionic network. We herein report the electrochemical properties of a Na-rich phase Na2IrO3, which can reversibly cycle 1.5 Na+ per formula unit while not suffering from oxygen release nor cationic migrations. Such large capacities, as deduced by complementary XPS, X-ray/neutron diffraction and transmission electron microscopy measurements, arise from cumulative cationic and anionic redox processes occurring simultaneously at potentials as low as 3.0 V. The inability to remove more than 1.5 Na+ is rooted in the formation of an O1-type phase having highly stabilized Na sites as confirmed by DFT calculations, which could rationalize as well the competing metal/oxygen redox processes in Na2IrO3. This work will help to define the most fertile directions in the search for novel high energy Na-rich materials based on more sustainable elements than Ir.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000388914500021 Publication Date 2016-10-17  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 9.466 Times cited 45 Open Access  
  Notes The authors thank Montse Casas-Cabanas and Marine Reynaud for discussions about the FAULTS program, Sandra Van Aert for her great help in guiding us towards the use of the statistical parameter estimation method for establishing the O-O histogram, and Thomas Hansen and Vladimir Pomjakushin for their precious help in neutron diffraction experiments. This work is based on experiments performed at the Swiss spallation neutron source SINQ, Paul Scherrer Institute, Villigen, Switzerland, and at Institut Laue Langevin, Grenoble, France. Use of the 11-BM mail service of the APS at Argonne National Laboratory was supported by the U.S. department of Energy under contract No. DE-AC02-06CH11357 and is greatly acknowledged. Approved Most recent IF: 9.466  
  Call Number (up) EMAT @ emat @ c:irua:135994 Serial 4287  
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Author Meledin, A.; Turner, S.; Cayado, P.; Mundet, B.; Solano, E.; Ricart, S.; Ros, J.; Puig, T.; Obradors, X.; Van Tendeloo, G. url  doi
openurl 
  Title Unique nanostructural features in Fe, Mn-doped YBCO thin films Type A1 Journal article
  Year 2016 Publication Superconductor science and technology Abbreviated Journal Supercond Sci Tech  
  Volume 29 Issue 29 Pages 125009  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract An attempt to grow a thin epitaxial composite film of YBa2Cu3O7−δ (YBCO) with spinel MnFe2O4 (MFO) nanoparticles on a LAO substrate using the CSD approach resulted in a decomposition of the spinel and various doping modes of YBCO with the Fe and Mn cations. These nanostructural effects lead to a lowering of T c and a slight J c increase in field. Using a combination of advanced transmission electron microscopy (TEM) techniques such as atomic resolution high-angle annular dark field scanning TEM, energy dispersive x-ray spectroscopy and electron energy-loss spectroscopy we have been able to decipher and characterize the effects of the Fe and Mn doping on the film architecture. The YBaCuFeO5 anion-deficient double perovskite phase was detected in the form of 3D inclusions as well as epitaxially grown lamellas within the YBCO matrix. These nano-inclusions play a positive role as pinning centers responsible for the J c/J sf (H) dependency smoothening at high magnetic fields in the YBCO-MFO films with respect to the pristine YBCO films.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000387680100001 Publication Date 2016-10-31  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 0953-2048 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 2.878 Times cited 6 Open Access  
  Notes The authors gratefully acknowledge Prof. Dr. A. Abakumov and Dr. J. Gazquez for discussions and corrections. Part of this work was performed within the framework of the EUROTAPES project (FP7-NMP.2011.2.2-1 Grant no. 280432), funded by the European Union. ICMAB research was financed by the Ministry of Economy and Competitiveness, and FEDER funds under the projects MAT2011-28874-C02-01, MAT2014-51778-C2-1-R, ENE2014-56109-C3-3-R and Consolider Nanoselect CSD2007-00041, and by Generalitat de Catalunya (2009 SGR 770, 2015 SGR 753 and Xarmae). ICMAB acknowledges support from Severo Ochoa Program (MINECO, Grant SEV-2015-0496). Approved Most recent IF: 2.878  
  Call Number (up) EMAT @ emat @ c:irua:136444 Serial 4295  
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Author Yu, W.-B.; Hu, Z.-Y.; Yi, M.; Huang, S.-Z.; Chen, D.-S.; Jin, J.; Li, Y.; Van Tendeloo, G.; Su, B.-L. pdf  url
doi  openurl
  Title Probing the electrochemical behavior of {111} and {110} faceted hollow Cu2O microspheres for lithium storage Type A1 Journal article
  Year 2016 Publication RSC advances Abbreviated Journal Rsc Adv  
  Volume 6 Issue 6 Pages 97129-97136  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract Transition metal oxides with exposed highly active facets have become of increasing interest as anode materials for lithium ion batteries, because more dangling atoms exposed at the active surface facilitate the reaction between the transition metal oxides and lithium. In this work, we probed the electrochemical behavior of hollow Cu2O microspheres with {111} and {110} active facets on the polyhedron surface as anodes for lithium storage. Compared to commercial Cu2O nanoparticles, hollow Cu2O microspheres with {111} and {110} active facets show a rising specific capacity at 30 cycles which then decreases after 110 cycles during the cycling process. Via advanced electron microscopy characterization, we reveal that this phenomenon can be attributed to the highly active {111} and {110} facets with dangling “Cu” atoms facilitating the conversion reaction of Cu2O and Li, where part of the Cu2O is oxidized to CuO during the charging process. However, as the reaction proceeds, more and more formed Cu nanoparticles cannot be converted to Cu2O or CuO. This leads to a decrease of the specific capacity. We believe that our study here sheds some light on the progress of the electrochemical behavior of transition metal oxides with respect to their increased specific capacity and the subsequent decrease via a conversion reaction mechanism. These results will be helpful to optimize the design of transition metal oxide micro/nanostructures for high performance lithium storage.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000386242500084 Publication Date 2016-10-06  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2046-2069 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 3.108 Times cited 5 Open Access  
  Notes Z. Y. Hu and G. Van Tendeloo acknowledge support from the EC Framework 7 program ESTEEM2 (Reference 312483). Approved Most recent IF: 3.108  
  Call Number (up) EMAT @ emat @ c:irua:138199 Serial 4322  
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Author Jany, B.R.; Gauquelin, N.; Willhammar, T.; Nikiel, M.; van den Bos, K.H.W.; Janas, A.; Szajna, K.; Verbeeck, J.; Van Aert, S.; Van Tendeloo, G.; Krok, F. url  doi
openurl 
  Title Controlled growth of hexagonal gold nanostructures during thermally induced self-assembling on Ge(001) surface Type A1 Journal article
  Year 2017 Publication Scientific reports Abbreviated Journal Sci Rep-Uk  
  Volume 7 Issue 7 Pages 42420  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract Nano-sized gold has become an important material in various fields of science and technology, where control over the size and crystallography is desired to tailor the functionality. Gold crystallizes in the face-centered cubic (fcc) phase, and its hexagonal closed packed (hcp) structure is a very unusual and rare phase. Stable Au hcp phase has been reported to form in nanoparticles at the tips of some Ge nanowires. It has also recently been synthesized in the form of thin graphene-supported sheets which are unstable under electron beam irradiation. Here, we show that stable hcp Au 3D nanostructures with well-defined crystallographic orientation and size can be systematically created in a process of thermally induced self-assembly of thin Au layer on Ge(001) monocrystal. The Au hcp crystallite is present in each Au nanostructure and has been characterized by different electron microscopy techniques. We report that a careful heat treatment above the eutectic melting temperature and a controlled cooling is required to form the hcp phase of Au on a Ge single crystal. This new method gives scientific prospects to obtain stable Au hcp phase for future applications in a rather simple manner as well as redefine the phase diagram of Gold with Germanium.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000393940700001 Publication Date 2017-02-14  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2045-2322 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 4.259 Times cited 25 Open Access OpenAccess  
  Notes The authors gratefully acknowledge the financial support from the Polish National Science Center, grant no. DEC-2012/07/B/ST5/00906. N.G., G.V.T. and J.V. acknowledge the European Union (EU) Council under the 7th Framework Program (FP7) ERC Starting Grant 278510 VORTEX for support. The Research Foundation Flanders is acknowledged through project fundings (G.0374.13N, G.0368.15N, G.0369.15N) and for a Ph.D. research grant to K.H.W.v.d.B. The microscope was partly funded by the Hercules Fund from the Flemish Government. T.W. acknowledges the Swedish Research Council for an international postdoc grant. The research leading to these results has received funding from the European Union Seventh Framework Programme under Grant Agreement 312483–ESTEEM2 (Integrated Infrastructure Initiative–I3). Part of the research was carried out with equipment purchased with financial support from the European Regional Development Fund in the framework of the Polish Innovation Economy Operational Program (Contract No. POIG.02.01.00-12-023/08). Approved Most recent IF: 4.259  
  Call Number (up) EMAT @ emat @ c:irua:140846UA @ admin @ c:irua:140846 Serial 4423  
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Author Tarasov, A.; Hu, Z.-Y.; Meledina, M.; Trusov, G.; Goodilin, E.; Van Tendeloo, G.; Dobrovolsky, Y. pdf  url
doi  openurl
  Title One-Step Microheterogeneous Formation of Rutile@Anatase Core–Shell Nanostructured Microspheres Discovered by Precise Phase Mapping Type A1 Journal article
  Year 2017 Publication The journal of physical chemistry: C : nanomaterials and interfaces Abbreviated Journal J Phys Chem C  
  Volume 121 Issue 121 Pages 4443-4450  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Nanostructured core−shell microspheres with a rough rutile core and a thin anatase shell are synthesized via a one-step heterogeneous templated hydrolysis process of TiCl4 vapor on the aerosol water−air interface. The rutile-in-anatase core−shell structure has been evidenced by different electron microscopy techniques, including electron energy-loss spectroscopy and 3D electron tomography. A new mechanism for the formation of a crystalline rutile core inside the anatase shell is proposed based on a statistical evaluation of a large number of electron microscopy data. We found that the control over the TiCl4 vapor pressure, the ratio between TiCl4 and H2O aerosol, and the reaction conditions plays a crucial role in the formation of the core−shell morphology and increases the yield of nanostructured microspheres.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000395616200038 Publication Date 2017-03-02  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1932-7447 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 4.536 Times cited 4 Open Access OpenAccess  
  Notes Z.-Y.H., M. M., and G.V.T. acknowledge support from the the EC Framework 7 program ESTEEM2 (Reference 312483). Approved Most recent IF: 4.536  
  Call Number (up) EMAT @ emat @ c:irua:141720 Serial 4472  
Permanent link to this record
 

 
Author Willhammar, T.; Sentosun, K.; Mourdikoudis, S.; Goris, B.; Kurttepeli, M.; Bercx, M.; Lamoen, D.; Partoens, B.; Pastoriza-Santos, I.; Pérez-Juste, J.; Liz-Marzán, L.M.; Bals, S.; Van Tendeloo, G. pdf  url
doi  openurl
  Title Structure and vacancy distribution in copper telluride nanoparticles influence plasmonic activity in the near-infrared Type A1 Journal article
  Year 2017 Publication Nature communications Abbreviated Journal Nat Commun  
  Volume 8 Issue 8 Pages 14925  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT)  
  Abstract Copper chalcogenides find applications in different domains including photonics, photothermal therapy and photovoltaics. CuTe nanocrystals have been proposed as an alternative to noble metal particles for plasmonics. Although it is known that deviations from stoichiometry are a prerequisite for plasmonic activity in the near-infrared, an accurate description of the material and its (optical) properties is hindered by an insufficient understanding of the atomic structure and the influence of defects, especially for materials in their nanocrystalline form. We demonstrate that the structure of Cu1.5±xTe nanocrystals canbe determined using electron diffraction tomography. Real-space high-resolution electron tomography directly reveals the three-dimensional distribution of vacancies in the structure. Through first-principles density functional theory, we furthermore demonstrate that the influence of these vacancies on the optical properties of the nanocrystals is determined. Since our methodology is applicable to a variety of crystalline nanostructured materials, it is expected to provide unique insights concerning structure–property correlations.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000397799700001 Publication Date 2017-03-30  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2041-1723 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 12.124 Times cited 37 Open Access OpenAccess  
  Notes The work was financially supported by the European Research Council through an ERC Starting Grant (#335078-COLOURATOMS). T.W. acknowledges the Swedish Research Council for an international postdoc grant. We acknowledge financial support of FWO-Vlaanderen through project G.0216.14N, G.0369.15N and a postdoctoral research grant to B.G. The computational resources and services used in this work were provided by the VSC (Flemish Supercomputer Center) and the HPC infrastructure of the University of Antwerp (CalcUA), both funded by the FWO-Vlaanderen and the Flemish Government–Department EWI. The work was further supported by the Spanish MINECO (MAT2013-45168-R). S.M. thanks the Action ooSupporting Postdoctoral Researchers44 of the Operational Program ‘Education and Lifelong Learning’ (Action’s Beneficiary: General Secretariat for Research and Technology of Greece), which was co-financed by the European Social Fund (ESF) and the Greek State. (ROMEO:green; preprint:; postprint:can ; pdfversion:can); ECAS_Sara Approved Most recent IF: 12.124  
  Call Number (up) EMAT @ emat @ c:irua:142203UA @ admin @ c:irua:142203 Serial 4538  
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Author Pulinthanathu Sree, S.; Dendooven, J.; Geerts, L.; Ramachandran, R.K.; Javon, E.; Ceyssens, F.; Breynaert, E.; Kirschhock, C.E.A.; Puers, R.; Altantzis, T.; Van Tendeloo, G.; Bals, S.; Detavernier, C.; Martens, J.A. pdf  url
doi  openurl
  Title 3D porous nanostructured platinum prepared using atomic layer deposition Type A1 Journal article
  Year 2017 Publication Journal of materials chemistry A : materials for energy and sustainability Abbreviated Journal J Mater Chem A  
  Volume 5 Issue 5 Pages 19007-19016  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract A robust and easy to handle 3D porous platinum structure was created via replicating the 3D channel system

of an ordered mesoporous silica material using atomic layer deposition (ALD) over micrometer distances.

After ALD of Pt in the silica material, the host template was digested using hydrogen fluoride (HF). A fully

connected ordered Pt nanostructure was obtained with morphology and sizes corresponding to that of

the pores of the host matrix, as revealed with high-resolution scanning transmission electron

microscopy and electron tomography. The Pt nanostructure consisted of hexagonal Pt rods originating

from the straight mesopores (11 nm) of the host structure and linking features resulting from Pt

replication of the interconnecting mesopore segments (2–4 nm) present in the silica host structure.

Electron tomography of partial replicas, made by incomplete infilling of Zeotile-4 material with Pt,

provided insight in the connectivity and formation mechanism of the Pt nanostructure by ALD. The Pt

replica was evaluated for its potential use as electrocatalyst for the hydrogen evolution reaction, one of

the half-reactions of water electrolysis, and as microelectrode for biomedical sensing. The Pt replica

showed high activity for the hydrogen evolution reaction and electrochemical characterization revealed

a large impedance improvement in comparison with reference Pt electrodes.
 
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000411232100010 Publication Date 2017-06-28  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2050-7488 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 8.867 Times cited 9 Open Access OpenAccess  
  Notes This work was supported by the Flemish government through long-term structural funding (Methusalem) to JAM and FWO for a research project (G0A5417N). JD, TA and FC acknowledge Flemish FWO for a post-doctoral fellowship. S. B. acknowledges funding from ERC Starting Grant COLOURATOMS (335078). (ROMEO:yellow; preprint:; postprint:restricted ; pdfversion:cannot); saraecas; ECAS_Sara; Approved Most recent IF: 8.867  
  Call Number (up) EMAT @ emat @ c:irua:144624 c:irua:144624 c:irua:144624UA @ admin @ c:irua:144624 Serial 4634  
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Author Sieger, M.; Pahlke, P.; Ottolinger, R.; Stafford, B.H.; Lao, M.; Meledin, A.; Bauer, M.; Eisterer, M.; Van Tendeloo, G.; Schultz, L.; Nielsch, K.; Hühne, R. url  doi
openurl 
  Title Influence of substrate tilt angle on the incorporation of BaHfO3 in thick YBa2Cu3O7-δ films Type A1 Journal article
  Year 2016 Publication IEEE transactions on applied superconductivity Abbreviated Journal  
  Volume 27 Issue 27 Pages 1-4  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract High critical current densities can be realized in high-temperature superconductors such as YBa2Cu3O7-δ (YBCO) by controlling density, shape, size and direction of a secondary phase. Whereas the dependence on the growth rate and deposition temperature has been widely studied as key parameters for nano-engineering the pinning landscape, the vicinal tilt of the substrate surface might have an additional influence. Therefore, we deposited 6 mol% BaHfO3 (BHO) doped YBCO on SrTiO3 (STO) substrates with vicinal angles α between 0° and 40° to identify the influence of the tilt on the growth mode of BHO. An undisturbed epitaxial growth of the superconductor as well as an epitaxial integration of the BHO phase in the YBCO matrix is observed for all vicinal angles investigated. The critical temperature is constant up to α = 20°, whereas the self-field critical current density at 77 K starts to decrease above 10°. A detailed structural analysis of the film cross sections showed that the growth mode of BHO changes already for a vicinal tilt of 2° from a pure c-axis oriented growth to a layered structure with BHO aligned parallel to the YBCO ab-plane. We identified a strong influence of such a microstructure on the current flow in BHO doped YBCO films on STO substrates as well as on MgO based coated conductors prepared by inclined substrate deposition  
  Address  
  Corporate Author Thesis  
  Publisher Institute of Electrical and Electronics Engineers (IEEE) Place of Publication Editor  
  Language Wos 000418469400001 Publication Date 2016-11-22  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1051-8223 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor Times cited 3 Open Access  
  Notes This work was supported by EUROTAPES, a collaborative project funded by the European Commission’s Seventh Framework Program (FP7 / 2007 – 2013) under Grant Agreement n.280432.The authors would like to thank R. Nast, M. Reitner, M. Kühnel, U. Fiedler and J. Scheiter for technical assistance. Approved Most recent IF: NA  
  Call Number (up) EMAT @ emat @ Sieger_2016a c:irua:138603 Serial 4317  
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Author Li, J.; Pereira, P.J.; Yuan, J.; Lv, Y.-Y.; Jiang, M.-P.; Lu, D.; Lin, Z.-Q.; Liu, Y.-J.; Wang, J.-F.; Li, L.; Ke, X.; Van Tendeloo, G.; Li, M.-Y.; Feng, H.-L.; Hatano, T.; Wang, H.-B.; Wu, P.-H.; Yamaura, K.; Takayama-Muromachi, E.; Vanacken, J.; Chibotaru, L.F.; Moshchalkov, V.V. url  doi
openurl 
  Title Nematic superconducting state in iron pnictide superconductors Type A1 Journal article
  Year 2017 Publication Nature communications Abbreviated Journal Nat Commun  
  Volume 8 Issue 1 Pages 1880  
  Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)  
  Abstract Nematic order often breaks the tetragonal symmetry of iron-based superconductors. It arises from regular structural transition or electronic instability in the normal phase. Here, we report the observation of a nematic superconducting state, by measuring the angular dependence of the in-plane and out-of-plane magnetoresistivity of Ba 0.5 K 0.5 Fe 2 As 2 single crystals. We find large twofold oscillations in the vicinity of the superconducting transition, when the direction of applied magnetic field is rotated within the basal plane. To avoid the influences from sample geometry or current flow direction, the sample was designed as Corbino-shape for in-plane and mesa-shape for out-of-plane measurements. Theoretical analysis shows that the nematic superconductivity arises from the weak mixture of the quasi-degenerate s-wave and d-wave components of the superconducting condensate, most probably induced by a weak anisotropy of stresses inherent to single crystals.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000416933400002 Publication Date 2017-11-27  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 2041-1723 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 12.124 Times cited 8 Open Access OpenAccess  
  Notes The authors J.L., P.J.P., and J.Y. contributed equally to this work. J.L. and J.Y. designed the experiments. J.L., H.-L.F., K.Y., and E.T.-M. grew the single crystals. J.L., J.Y., Y.-Y.L., M.-P.J., D.L., M.-Y.L., T.H., H.-B.W., P.-H.W., K.Y., E.T.-M., J.V., and V.V.M. fabricated the devices and measured transport properties. J.L., Y.-Y.L., Z.-Q.L., Y.-J.L., J.-F.W., and L.L. studied on the pulsed high field measurements. X.K. and G.V.T. measured the low temperature TEM. All authors discussed the data. J.L., P.J.P., and L.F.C. proposed the model and simulated the results. J.L., P.J.P., K.Y., E.T.-M., and L.F.C. analyzed the data and prepared the manuscript. Approved Most recent IF: 12.124  
  Call Number (up) EMAT @ emat @c:irua:147348 Serial 4772  
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Author Pearce, P.E.; Perez, A.J.; Rousse, G.; Saubanère, M.; Batuk, D.; Foix, D.; McCalla, E.; Abakumov, A.M.; Van Tendeloo, G.; Doublet, M.-L.; Tarascon, J.-M. url  doi
openurl 
  Title Evidence for anionic redox activity in a tridimensional-ordered Li-rich positive electrode β-Li2IrO3 Type A1 Journal article
  Year 2017 Publication Nature materials Abbreviated Journal Nat Mater  
  Volume 16 Issue 5 Pages 580-586  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract Lithium-ion battery cathode materials have relied on cationic redox reactions until the recent discovery of anionic redox activity in Li-rich layered compounds which enables capacities as high as 300 mAh g(-1). In the quest for new high-capacity electrodes with anionic redox, a still unanswered question was remaining regarding the importance of the structural dimensionality. The present manuscript provides an answer. We herein report on a beta-Li2IrO3 phase which, in spite of having the Ir arranged in a tridimensional (3D) framework instead of the typical two-dimensional (2D) layers seen in other Li-rich oxides, can reversibly exchange 2.5 e(-) per Ir, the highest value ever reported for any insertion reaction involving d-metals. We show that such a large activity results from joint reversible cationic (Mn+) and anionic (O-2)(n-) redox processes, the latter being visualized via complementary transmission electron microscopy and neutron diffraction experiments, and confirmed by density functional theory calculations. Moreover, beta-Li2IrO3 presents a good cycling behaviour while showing neither cationic migration nor shearing of atomic layers as seen in 2D-layered Li-rich materials. Remarkably, the anionic redox process occurs jointly with the oxidation of Ir4+ at potentials as low as 3.4 V versus Li+/Li-0, as equivalently observed in the layered alpha-Li2IrO3 polymorph. Theoretical calculations elucidate the electrochemical similarities and differences of the 3D versus 2D polymorphs in terms of structural, electronic and mechanical descriptors. Our findings free the structural dimensionality constraint and broaden the possibilities in designing high-energy-density electrodes for the next generation of Li-ion batteries.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000400004200018 Publication Date 2017-02-27  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 1476-1122 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 39.737 Times cited Open Access Not_Open_Access  
  Notes The authors thank Q. Jacquet for fruitful discussions and V. Pomjakushin for his valuable help in neutron diffraction experiments. This work is based on experiments performed at the Swiss Spallation Neutron Source SINQ, Paul Scherrer Institute, Villigen, Switzerland. Use of the 11-BM mail service of the APS at Argonne National Laboratory was supported by the US Department of Energy under contract No. DE-AC02-06CH11357 and is greatly acknowledged. J.-M.T. acknowledges funding from the European Research Council (ERC) (FP/2014)/ERC Grant-Project 670116-ARPEMA. E.M. acknowledges financial support from the Fonds de Recherche du Quebec-Nature et Technologies. Approved Most recent IF: 39.737  
  Call Number (up) EMAT @ emat @c:irua:147502 Serial 4773  
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Author Jacquet, Q.; Perez, A.; Batuk, D.; Van Tendeloo, G.; Rousse, G.; Tarascon, J.-M. url  doi
openurl 
  Title The Li3RuyNb1-yO4 (0 ≤y≤ 1) System: Structural Diversity and Li Insertion and Extraction Capabilities Type A1 Journal article
  Year 2017 Publication Chemistry of materials Abbreviated Journal Chem Mater  
  Volume 29 Issue 12 Pages 5331-5343  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract Searching for novel high-capacity electrode materials combining cationic and anionic redox processes is an ever-growing activity within the field of Li-ion batteries. In this respect, we report on the exploration of the Li3RuyNb1-yO4 (O <= y <= 1) system with an O/M ratio of 4 to maximize the number of oxygen lone pairs, responsible for the anionic redox. We show that this system presents a very rich crystal chemistry with the existence of four structural types, which derive from the rocksalt structure but differ in their cationic arrangement, creating either zigzag, helical, jagged chains or clusters. From an electrochemical standpoint, these compounds are active on reduction via a classical cationic insertion process. The oxidation process is more complex, because of the instability of the delithiated phase. Our results promote the use of the rich Li3MO4 family as a viable platform for a better understanding of the relationships between structure and anionic redox activity.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000404493100036 Publication Date 2017-06-27  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 9.466 Times cited 17 Open Access Not_Open_Access  
  Notes The authors thank Paul Pearce, Alexis Grimaud, Matthieu Saubanere, and Marie-Liesse Doublet for fruitful discussions, Vivian Nassif for her help in neutron diffraction experiment at the D1B diffractometer at ILL, and Dominique Foix for XPS analysis. Use of the Advanced Photon Source at Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. Q.J. thanks the ANR “Deli-Redox” for Ph.D. funding. J.-M.T. and D.B. acknowledge funding from the European Research Council (ERC) (FP/2014)/ERC Grant -Project 670116-ARPEMA. Approved Most recent IF: 9.466  
  Call Number (up) EMAT @ emat @c:irua:147506 Serial 4776  
Permanent link to this record
 

 
Author Pearce, P.E.; Rousse, G.; Karakulina, O.M.; Hadermann, J.; Van Tendeloo, G.; Foix, D.; Fauth, F.; Abakumov, A.M.; Tarascon, J.-M. pdf  url
doi  openurl
  Title β-Na1.7IrO3: A Tridimensional Na-Ion Insertion Material with a Redox Active Oxygen Network Type A1 Journal article
  Year 2018 Publication Chemistry of materials Abbreviated Journal Chem Mater  
  Volume 30 Issue 10 Pages 3285-3293  
  Keywords A1 Journal article; Electron microscopy for materials research (EMAT)  
  Abstract The revival of the Na-ion battery concept has prompted an intense search for new high capacity Na-based positive electrodes. Recently, emphasis has been placed on manipulating Na-based layered compounds to trigger the participation of the anionic network. We further explored this direction and show the feasibility of achieving anionic-redox activity in three-dimensional Na-based compounds. A new 3D β-Na1.7IrO3 phase was synthesized in a two-step process, which involves first the electrochemical removal of Li from β-Li2IrO3 to produce β-IrO3, which is subsequently reduced by electrochemical Na insertion. We show that β-Na1.7IrO3 can reversibly uptake nearly 1.3 Na+ per formula unit through an uneven voltage profile characterized by the presence of four plateaus related to structural transitions. Surprisingly, the β-Na1.7IrO3 phase was found to be stable up to 600 °C, while it could not be directly synthesized via conventional synthetic methods. Although these Na-based iridate phases are of limited practical interest, they help to understand how introducing highly polarizable guest ions (Na+) into host rocksalt-derived oxide structures affects the anionic redox mechanism.  
  Address  
  Corporate Author Thesis  
  Publisher Place of Publication Editor  
  Language Wos 000433403800014 Publication Date 2018-05-22  
  Series Editor Series Title Abbreviated Series Title  
  Series Volume Series Issue Edition  
  ISSN 0897-4756 ISBN Additional Links UA library record; WoS full record; WoS citing articles  
  Impact Factor 9.466 Times cited 6 Open Access OpenAccess  
  Notes The authors thank A. Perez for fruitful discussions and his valuable help in synchrotron XRD experiment and Matthieu Courty for carrying out the DSC measurements. The authors also greatly thank Matthieu Saubanère and Marie-Liesse Doublet for valuable discussions on theoretical aspects of this work. This work is based on experiments performed on the Materials Science and Powder Diffraction Beamline at ALBA synchrotron (Proposal 2016091814), Cerdanyola del Vallès, E- 08290 Barcelona, Spain. J.-M.T. acknowledges funding from the European Research Council (ERC) (FP/2014)/ERC Grant- Project 670116-ARPEMA. G.R. acknowledges funding from ANR DeliRedox. O.M.K., J.H., and A.M.A. are grateful to FWO Vlaanderen for financial support under Grant G040116N. Approved Most recent IF: 9.466  
  Call Number (up) EMAT @ emat @c:irua:152048 Serial 4996  
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