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Author Ati, M.; Sathiya, M.; Boulineau, S.; Reynaud, M.; Abakumov, A.; Rousse, G.; Melot, B.; Van Tendeloo, G.; Tarascon, J.-M.
Title Understanding and promoting the rapid preparation of the triplite-phase of LiFeSO4F for use as a large-potential Fe cathode Type A1 Journal article
Year 2012 Publication Journal of the American Chemical Society Abbreviated Journal J Am Chem Soc
Volume 134 Issue 44 Pages 18380-18387
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The development of new electrode materials, which are composed of Earth-abundant elements and that can be made via eco-efficient processes, is becoming absolutely necessary for reasons of sustainable production. The 3.9 V triplite-phase of LiFeSO4F, compared to the 3.6 V tavorite-phase, could satisfy this requirement provided the currently complex synthetic pathway can be simplified. Here, we present our work aiming at better understanding the reaction mechanism that govern its formation as a way to optimize its preparation. We first demonstrate, using complementary X-ray diffraction and transmission electron microscopy studies, that triplite-LiFeSO4F can nucleate from tavorite-LiFeSO4F via a reconstructive process whose kinetics are significantly influenced by moisture and particle morphology. Perhaps the most spectacular finding is that it is possible to prepare electrochemically active triplite-LiFeSO4F from anhydrous precursors using either reactive spark plasma sintering (SPS) synthesis in a mere 20 min at 320 degrees C or room temperature ball milling for 3 h. These new pathways appear to be strongly driven by the easy formation of a disordered phase with higher entropy, as both techniques trigger disorder via rapid annealing steps or defect creation. Although a huge number of phases adopts the tavorite structure-type, this new finding offers both a potential way to prepare new compositions in the triplite structure and a wealth of opportunities for the synthesis of new materials which could benefit many domains beyond energy storage.
Address
Corporate Author Thesis
Publisher Place of Publication Washington, D.C. Editor
Language Wos 000310720900041 Publication Date 2012-10-12
Series Editor (down) Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0002-7863;1520-5126; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.858 Times cited 36 Open Access
Notes Approved Most recent IF: 13.858; 2012 IF: 10.677
Call Number UA @ lucian @ c:irua:105147 Serial 3802
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Author McCalla, E.; Sougrati, M.T.; Rousse, G.; Berg, E.J.; Abakumov, A.; Recham, N.; Ramesha, K.; Sathiya, M.; Dominko, R.; Van Tendeloo, G.; Novák, P.; Tarascon, J.M.;
Title Understanding the roles of anionic redox and oxygen release during electrochemical cycling of lithium-rich layered Li4FeSbO6 Type A1 Journal article
Year 2015 Publication Journal of the American Chemical Society Abbreviated Journal J Am Chem Soc
Volume 137 Issue 137 Pages 4804-4814
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Li-rich oxides continue to be of immense interest as potential next generation Li-ion battery positive electrodes, and yet the role of oxygen during cycling is still poorly understood. Here, the complex electrochemical behavior of Li4FeSbO6 materials is studied thoroughly with a variety of methods. Herein, we show that oxygen release occurs at a distinct voltage plateau from the peroxo/superoxo formation making this material ideal for revealing new aspects of oxygen redox processes in Li-rich oxides. Moreover, we directly demonstrate the limited reversibility of the oxygenated species (O-2(n-); n = 1, 2, 3) for the first time. We also find that during charge to 4.2 V iron is oxidized from +3 to an unusual +4 state with the concomitant formation of oxygenated species. Upon further charge to 5.0 V, an oxygen release process associated with the reduction of iron +4 to +3 is present, indicative of the reductive coupling mechanism between oxygen and metals previously reported. Thus, in full state of charge, lithium removal is fully compensated by oxygen only, as the iron and antimony are both very close to their pristine states. Besides, this charging step results in complex phase transformations that are ultimately destructive to the crystallinity of the material. Such findings again demonstrate the vital importance of fully understanding the behavior of oxygen in such systems. The consequences of these new aspects of the electrochemical behavior of lithium-rich oxides are discussed in detail.
Address
Corporate Author Thesis
Publisher Place of Publication Washington, D.C. Editor
Language Wos 000353177100036 Publication Date 2015-03-26
Series Editor (down) Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0002-7863;1520-5126; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 13.858 Times cited 86 Open Access
Notes Approved Most recent IF: 13.858; 2015 IF: 12.113
Call Number c:irua:126019 Serial 3805
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Author Kazakov, S.M.; Abakumov, A.M.; Perz-Mato, J.M.; Ovchinnikov, A.V.; Roslova, M.V.; Boltalin, A.I.; Morozov, I.V.; Antipov, E.V.; Van Tendeloo, G.
Title Uniform patterns of Fe-vacancy ordering in the Kx(Fe,Co)2-ySe2 superconductors Type A1 Journal article
Year 2011 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 23 Issue 19 Pages 4311-4316
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The Fe-vacancy ordering patterns in the superconducting KxFe2ySe2 and nonsuperconducting Kx(Fe,Co)2ySe2 samples have been investigated by electron diffraction and high angle annular dark field scanning transmission electron microscopy. The Fe-vacancy ordering occurs in the ab plane of the parent ThCr2Si2-type structure, demonstrating two types of patterns. Superstructure I retains the tetragonal symmetry and can be described with the aI = bI = as√5 (as is the unit cell parameter of the parent ThCr2Si2-type structure) supercell and I4/m space group. Superstructure II reduces the symmetry to orthorhombic with the aII = as√2, bII = 2as√2 supercell and the Ibam space group. This type of superstructure is observed for the first time in KxFe2ySe2. The Fe-vacancy ordering is inhomogeneous: the disordered areas interleave with the superstructures I and II in the same crystallite. The observed superstructures represent the compositionally dependent uniform ordering patterns of two species (the Fe atoms and vacancies) on a square lattice. More complex uniform ordered configurations, including compositional stripes, can be predicted for different chemical compositions of the KxFe2ySe2 (0 < y < 0.5) solid solutions.
Address
Corporate Author Thesis
Publisher Place of Publication Washington, D.C. Editor
Language Wos 000295487800005 Publication Date 2011-09-13
Series Editor (down) Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0897-4756;1520-5002; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.466 Times cited 20 Open Access
Notes Approved Most recent IF: 9.466; 2011 IF: 7.286
Call Number UA @ lucian @ c:irua:92805 Serial 3810
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Author Abakumov, M.A.; Nukolova, N.V.; Sokolsky-Papkov, M.; Shein, S.A.; Sandalova, T.O.; Vishwasrao, H.M.; Grinenko, N.F.; Gubsky, I.L.; Abakumov, A.M.; Kabanov, A.V.; Chekhonin, V.P.;
Title VEGF-targeted magnetic nanoparticles for MRI visualization of brain tumor Type A1 Journal article
Year 2015 Publication Nanomedicine: nanotechnology, biology and medicine Abbreviated Journal Nanomed-Nanotechnol
Volume 11 Issue 11 Pages 825-833
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract This work is focused on synthesis and characterization of targeted magnetic nanoparticles as magnetic resonance imaging (MRI) agents for in vivo visualization of gliomas. Ferric oxide (Fe3O4) cores were synthesized by thermal decomposition and coated with bovine serum albumin (BSA) to form nanoparticles with D-eff of 53 +/- 9 nm. The BSA was further cross-linked to improve colloidal stability. Monoclonal antibodies against vascular endothelial growth factor (mAbVEGF) were covalently conjugated to BSA through a polyethyleneglycol linker. Here we demonstrate that 1) BSA coated nanoparticles are stable and non-toxic to different cells at concentration up to 2.5 mg/mL; 2) conjugation of monoclonal antibodies to nanoparticles promotes their binding to VEGF-positive glioma C6 cells in vitro; 3) targeted nanoparticles are effective in MRI visualization of the intracranial glioma. Thus, mAbVEGF-targeted BSA-coated magnetic nanoparticles are promising MRI contrast agents for glioma visualization. (C) 2015 Elsevier Inc. All rights reserved.
Address
Corporate Author Thesis
Publisher Place of Publication S.l. Editor
Language Wos 000354559600004 Publication Date 2015-01-31
Series Editor (down) Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1549-9634; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 5.72 Times cited 62 Open Access
Notes Approved Most recent IF: 5.72; 2015 IF: 6.155
Call Number c:irua:126351 Serial 3838
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Author Chizhov, A.S.; Rumyantseva, M.N.; Vasiliev, R.B.; Filatova, D.G.; Drozdov, K.A.; Krylov, I.V.; Abakumov, A.M.; Gaskov, A.M.
Title Visible light activated room temperature gas sensors based on nanocrystalline ZnO sensitized with CdSe quantum dots Type A1 Journal article
Year 2014 Publication Sensors and actuators : B : chemical Abbreviated Journal Sensor Actuat B-Chem
Volume 205 Issue Pages 305-312
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract This work reports the study of photoconductivity and visible light activated room temperature gas sensors properties of nanocrystalline ZnO thick films sensitized with colloidal CdSe quantum dots (QDs). Nanocrystalline zinc oxide (ZnO) was synthesized by the precipitation method. Colloidal CdSe quantum dots were obtained by high temperature colloidal synthesis. Sensitization was effectuated by three different procedures including direct adsorption of CdSe QDs stabilized with oleic acid on ZnO surface, anchoring to the ZnO surface through a bifunctional molecule of mercaptopropionic acid (MPA), and coating of CdSe QDs with a monolayer of MPA with subsequent adsorption on ZnO surface. Sensor measurements demonstrated that obtained QD CdSe/ZnO nanocomposites can be used for NO2 detection under visible (green) light illumination at room temperature without any thermal heating. (C) 2014 Elsevier B.V. All rights reserved.
Address
Corporate Author Thesis
Publisher Place of Publication Lausanne Editor
Language Wos 000343117600041 Publication Date 2014-09-06
Series Editor (down) Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0925-4005; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 5.401 Times cited 36 Open Access
Notes Approved Most recent IF: 5.401; 2014 IF: 4.097
Call Number UA @ lucian @ c:irua:121107 Serial 3848
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Author Semkina, A.; Abakumov, M.; Grinenko, N.; Abakumov, A.; Skorikov, A.; Mironova, E.; Davydova, G.; Majouga, A.G.; Nukolova, N.; Kabanov, A.; Chekhonin, V.;
Title Core-shell-corona doxorubicin-loaded superparamagnetic Fe3O4 nanoparticles for cancer theranostics Type A1 Journal article
Year 2015 Publication Colloids and surfaces: B : biointerfaces Abbreviated Journal Colloid Surface B
Volume 136 Issue 136 Pages 1073-1080
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Superparamagnetic iron oxide magnetic nanoparticles (MNPs) are successfully used as contrast agents in magnetic-resonance imaging. They can be easily functionalized for drug delivery functions, demonstrating great potential for both imaging and therapeutic applications. Here we developed new pH-responsive theranostic core-shell-corona nanoparticles consisting of superparamagentic Fe3O4 core that displays high T2 relaxivity, bovine serum albumin (BSA) shell that binds anticancer drug, doxorubicin (Dox) and poly(ethylene glycol) (PEG) corona that increases stability and biocompatibility. The nanoparticles were produced by adsorption of the BSA shell onto the Fe3O4 core followed by crosslinking of the protein layer and subsequent grafting of the PEG corona using monoamino-terminated PEG via carbodiimide chemistry. The hydrodynamic diameter, zeta-potential, composition and T2 relaxivity of the resulting nanoparticles were characterized using transmission electron microscopy, dynamic light scattering, thermogravimetric analysis and T2-relaxometry. Nanoparticles were shown to absorb Dox molecules, possibly through a combination of electrostatic and hydrophobic interactions. The loading capacity (LC) of the nanoparticles was 8 wt.%. The Dox loaded nanoparticles release the drug at a higher rate at pH 5.5 compared to pH 7.4 and display similar cytotoxicity against C6 and HEK293 cells as the free Dox. (C) 2015 Elsevier B.V. All rights reserved.
Address
Corporate Author Thesis
Publisher Place of Publication Amsterdam Editor
Language Wos 000367408100131 Publication Date 2015-11-10
Series Editor (down) Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0927-7765 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.887 Times cited 37 Open Access
Notes Approved Most recent IF: 3.887; 2015 IF: 4.152
Call Number UA @ lucian @ c:irua:131075 Serial 4157
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Author Zhang, B.; Dugas, R.; Rousse, G.; Rozier, P.; Abakumov, A.M.; Tarascon, J.-M.
Title Insertion compounds and composites made by ball milling for advanced sodium-ion batteries Type A1 Journal article
Year 2016 Publication Nature communications Abbreviated Journal Nat Commun
Volume 7 Issue 7 Pages 10308
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Sodium-ion batteries have been considered as potential candidates for stationary energy storage because of the low cost and wide availability of Na sources. However, their future commercialization depends critically on control over the solid electrolyte interface formation, as well as the degree of sodiation at the positive electrode. Here we report an easily scalable ball milling approach, which relies on the use of metallic sodium, to prepare a variety of sodium-based alloys, insertion layered oxides and polyanionic compounds having sodium in excess such as the Na4V2(PO4)(2)F-3 phase. The practical benefits of preparing sodium-enriched positive electrodes as reservoirs to compensate for sodium loss during solid electrolyte interphase formation are demonstrated by assembling full C/P'2-Na-1[Fe0.5Mn0.5]O-2 and C/'Na3+xV2(PO4)(2)F-3' sodium-ion cells that show substantial increases (>10%) in energy storage density. Our findings may offer electrode design principles for accelerating the development of the sodium-ion technology.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000369021400002 Publication Date 2016-01-18
Series Editor (down) 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 104 Open Access
Notes Approved Most recent IF: 12.124
Call Number UA @ lucian @ c:irua:131599 Serial 4197
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Author O'Sullivan, M.; Hadermann, J.; Dyer, M.S.; Turner, S.; Alaria, J.; Manning, T.D.; Abakumov, A.M.; Claridge, J.B.; Rosseinsky, M.J.
Title Interface control by chemical and dimensional matching in an oxide heterostructure Type A1 Journal article
Year 2016 Publication Nature chemistry Abbreviated Journal Nat Chem
Volume 8 Issue 8 Pages 347-353
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Interfaces between different materials underpin both new scientific phenomena, such as the emergent behaviour at oxide interfaces, and key technologies, such as that of the transistor. Control of the interfaces between materials with the same crystal structures but different chemical compositions is possible in many materials classes, but less progress has been made for oxide materials with different crystal structures. We show that dynamical self-organization during growth can create a coherent interface between the perovskite and fluorite oxide structures, which are based on different structural motifs, if an appropriate choice of cations is made to enable this restructuring. The integration of calculation with experimental observation reveals that the interface differs from both the bulk components and identifies the chemical bonding requirements to connect distinct oxide structures.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000372505500013 Publication Date 2016-02-01
Series Editor (down) Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1755-4330; 1755-4349 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 25.87 Times cited 28 Open Access
Notes Approved Most recent IF: 25.87
Call Number UA @ lucian @ c:irua:133189 Serial 4199
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Author Forsh, E.A.; Abakumov, A.M.; Zaytsev, V.B.; Konstantinova, E.A.; Forsh, P.A.; Rumyantseva, M.N.; Gaskov, A.M.; Kashkarov, P.K.
Title Optical and photoelectrical properties of nanocrystalline indium oxide with small grains Type A1 Journal article
Year 2015 Publication Thin solid films : an international journal on the science and technology of thin and thick films Abbreviated Journal Thin Solid Films
Volume 595 Issue 595 Pages 25-31
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Optical properties, spectral dependence of photoconductivity and photoconductivity decay in nanocrystalline indium oxide In2O3 are studied. A number of nanostructured In2O3 samples with various nanocrystals size are prepared by sol-gel method and characterized using various techniques. The mean nanocrystals size varies from 7 to 8 nm to 39-41 nm depending on the preparation conditions. Structural characterization of the In2O3 samples is performed by means of transmission electron microscopy and X-ray powder diffraction. The combined analysis of ultraviolet-visible absorption spectroscopy and diffuse reflectance spectroscopy shows that nanostructuring leads to the change in optical band gap: optical band gap of the In2O3 samples (with an average nanocrystal size from 7 to 41 nm) is equal to 2.8 eV. We find out the correlation between spectral dependence of photoconductivity and optical properties of nanocrystalline In2O3: sharp increase in photoconductivity was observed to begin at 2.8 eV that is equal to the optical bandgap in the In2O3 samples, and reached its maximum at 3.2-3.3 eV. The combined analysis of the slow photoconductivity decay in air, vacuum and argon, that was accurately fitted by a stretched-exponential function, and electron paramagnetic resonance (EPR) measurements shows that the kinetics of photoconductivity decay is strongly depended on the presence of oxygen molecules in the ambient of In2O3 nanocrystals. There is the quantitative correlation between EPR and photoconductivity data. Based on the obtained data we propose the model clearing up the phenomenon of permanent photoconductivity decay in nanocrystalline In2O3. (C) 2015 Elsevier B.V. All rights reserved.
Address
Corporate Author Thesis
Publisher Place of Publication Lausanne Editor
Language Wos 000365812400005 Publication Date 2015-10-27
Series Editor (down) Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0040-6090 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 1.879 Times cited 18 Open Access
Notes Approved Most recent IF: 1.879; 2015 IF: 1.759
Call Number UA @ lucian @ c:irua:130254 Serial 4219
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Author Ryabova, A.S.; Napolskiy, F.S.; Poux, T.; Istomin, S.Y.; Bonnefont, A.; Antipin, D.M.; Baranchikov, A.Y.; Levin, E.E.; Abakumov, A.M.; Kéranguéven, G.; Antipov, E.V.; Tsirlina, G.A.; Savinova, E.R.;
Title Rationalizing the influence of the Mn(IV)/Mn(III) red-Ox transition on the electrocatalytic activity of manganese oxides in the oxygen reduction reaction Type A1 Journal article
Year 2016 Publication Electrochimica acta Abbreviated Journal Electrochim Acta
Volume 187 Issue 187 Pages 161-172
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Knowledge on the mechanisms of oxygen reduction reaction (ORR) and descriptors linking the catalytic activity to the structural and electronic properties of transition metal oxides enable rational design of more efficient catalysts. In this work ORR electrocatalysis was studied on a set of single and complex Mn (III) oxides with a rotating disc electrode method and cyclic voltammetry. We discovered an exponential increase of the specific electrocatalytic activity with the potential of the surface Mn(IV)/Mn(III) red-ox couple, suggesting the latter as a new descriptor for the ORR electrocatalysis. The observed dependence is rationalized using a simple mean-field kinetic model considering availability of the Mn( III) centers and adsorbate-adsorbate interactions. We demonstrate an unprecedented activity of Mn2O3, ca. 40 times exceeding that of MnOOH and correlate the catalytic activity of Mn oxides to their crystal structure. (C) 2015 Elsevier Ltd. All rights reserved.
Address
Corporate Author Thesis
Publisher Place of Publication London Editor
Language Wos 000367235600019 Publication Date 2015-11-10
Series Editor (down) Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0013-4686 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.798 Times cited 51 Open Access
Notes Approved Most recent IF: 4.798
Call Number UA @ lucian @ c:irua:131096 Serial 4237
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Author Charkin, D.O.; Akinfiev, V.S.; Alekseeva, A.M.; Batuk, M.; Abakumov, A.M.; Kazakov, S.M.
Title Synthesis and cation distribution in the new bismuth oxyhalides with the Sillen-Aurivillius intergrowth structures Type A1 Journal article
Year 2015 Publication Journal of the Chemical Society : Dalton transactions Abbreviated Journal Dalton T
Volume 44 Issue 44 Pages 20568-20576
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract About 20 new compounds with the Sillen-Aurivillius intergrowth structure, (MeMeBi3Nb2O11X)-Me-1-Bi-2 (Me-1 = Pb, Sr, Ba; Me-2 = Ca, Sr, Ba; X = Cl, Br, I), have been prepared. They are composed of stacking of [ANb(2)O(7)] perovskite blocks, fluorite-type [M2O2] blocks and halogen sheets. The cation distribution between the fluorite and perovskite layers has been studied for Ba2Bi3Nb2O11I, Ca1.25Sr0.75Bi3Nb2O11Cl, BaCaBi3Nb2O11Br and Sr2Bi3Nb2O11Cl. The smaller Me cations tend to reside in the perovskite block while the larger ones are situated in the fluorite-type block. The distribution of the elements was confirmed for BaCaBi3Nb2O11Br using energy dispersive X-ray analysis combined with scanning transmission electron microscopy (STEM-EDX). An electron diffraction study of this compound reveals a local symmetry lowering caused by weakly correlated rotation of NbO6 octahedra. Based on our findings, we suggest a new stability criterion for mixed-layer structures, which is that net charges of any two consecutive layers do not compensate for each other and only the whole layer sequence is electroneutral.
Address
Corporate Author Thesis
Publisher Place of Publication London Editor
Language Wos 000365411500036 Publication Date 2015-10-30
Series Editor (down) Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0300-9246; 1477-9226; 1472-7773 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.029 Times cited 5 Open Access
Notes Approved Most recent IF: NA
Call Number UA @ lucian @ c:irua:130330 Serial 4256
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Author Rozova, M.G.; Grigoriev, V.V.; Bobrikov, I.A.; Filimonov, D.S.; Zakharov, K.V.; Volkova, O.S.; Vasiliev, A.N.; Antipov, E.V.; Tsirlin, A.A.; Abakumov, A.M.
Title Synthesis, structure and magnetic ordering of the mullite-type Bi2Fe4-xCrxO9 solid solutions with a frustrated pentagonal Cairo lattice Type A1 Journal article
Year 2016 Publication Journal of the Chemical Society : Dalton transactions Abbreviated Journal Dalton T
Volume 45 Issue 45 Pages 1192-1200
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Highly homogeneous mullite-type solid solutions Bi2Fe4-xCrxO9 (x = 0.5, 1, 1.2) were synthesized using a soft chemistry technique followed by a solid-state reaction in Ar. The crystal structure of Bi2Fe3CrO9 was investigated using X-ray and neutron powder diffraction, transmission electron microscopy and Fe-57 Mossbauer spectroscopy (S.G. Pbam, a = 7.95579(9) angstrom , b = 8.39145(9) angstrom, c = 5.98242(7) angstrom, R-F(X-ray) = 0.022, R-F(neutron) = 0.057). The ab planes in the structure are tessellated with distorted pentagonal loops built up by three tetrahedrally coordinated Fe sites and two octahedrally coordinated Fe/Cr sites, linked together in the ab plane by corner-sharing forming a pentagonal Cairo lattice. Magnetic susceptibility measurements and powder neutron diffraction show that the compounds order antiferromagnetically (AFM) with the Neel temperatures decreasing upon increasing the Cr content from T-N similar to 250 K for x = 0 to T-N similar to 155 K for x = 1.2. The magnetic structure of Bi2Fe3CrO9 at T = 30 K is characterized by a propagation vector k = (1/2,1/2,1/2). The tetrahedrally coordinated Fe cations form singlet pairs within dimers of corner-sharing tetrahedra, but spins on the neighboring dimers are nearly orthogonal. The octahedrally coordinated (Fe, Cr) cations form antiferromagnetic up-up-down-down chains along c, while the spin arrangement in the ab plane is nearly orthogonal between nearest neighbors and collinear between second neighbors. The resulting magnetic structure is remarkably different from the one in pure Bi2Fe4O9 and features several types of spin correlations even on crystallographically equivalent exchange that may be caused by the simultaneous presence of Fe and Cr on the octahedral site.
Address
Corporate Author Thesis
Publisher Place of Publication London Editor
Language Wos 000367614700041 Publication Date 2015-11-30
Series Editor (down) Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0300-9246; 1477-9226; 1472-7773 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.029 Times cited Open Access
Notes Approved Most recent IF: NA
Call Number UA @ lucian @ c:irua:131095 Serial 4257
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Author Retuerto, M.; Skiadopoulou, S.; Li, M.R.; Abakumov, A.M.; Croft, M.; Ignatov, A.; Sarkar, T.; Abbett, B.M.; Pokorný, J.; Savinov, M.; Nuzhnyy, D.; Prokleška, J.; Abeykoon, M.; Stephens, P.W.; Hodges, J.P.; Vaněk, P.; Fennie, C.J.; Rabe, K.M.; Kamba, S.; Greenblatt, M.;
Title Pb2MnTeO6 double perovskite : an antipolar anti-ferromagnet Type A1 Journal article
Year 2016 Publication Inorganic chemistry Abbreviated Journal Inorg Chem
Volume 55 Issue 55 Pages 4320-4329
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Pb2MnTeO6, a new double perovskite, was synthesized. Its crystal structure was determined by synchrotron X-ray and powder neutron diffraction. Pb2MnTeO6 is monoclinic (I2/m) at room temperature with a regular arrangement of all the cations in their polyhedra. However, when the temperature is lowered to similar to 120 K it undergoes a phase transition from I2/m to C2/c structure. This transition is accompanied by a displacement of the Pb atoms from the center of their polyhedra due to the 6s2 lone-pair electrons, together with a surprising off-centering of Mn2+ (d5) magnetic cations. This strong first-order phase transition is also evidenced by specific heat, dielectric, Raman, and infrared spectroscopy measurements. The magnetic characterizations indicate an anti-ferromagnetic (AFM) order below TN approximate to 20 K; analysis of powder neutron diffraction data confirms the magnetic structure with propagation vector k = (0 1 0) and collinear AFM spins. The observed jump in dielectric permittivity near similar to 150 K implies possible anti-ferroelectric behavior; however, the absence of switching suggests that Pb2MnTeO6 can only be antipolar. First-principle calculations confirmed that the crystal and magnetic structures determined are locally stable and that anti-ferroelectric switching is unlikely to be observed in Pb2MnTeO6.
Address
Corporate Author Thesis
Publisher Place of Publication Easton, Pa Editor
Language Wos 000375519700027 Publication Date 2016-04-08
Series Editor (down) Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0020-1669 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.857 Times cited 9 Open Access
Notes Approved Most recent IF: 4.857
Call Number UA @ lucian @ c:irua:134219 Serial 4258
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Author Mikita, R.; Aharen, T.; Yamamoto, T.; Takeiri, F.; Ya, T.; Yoshimune, W.; Fujita, K.; Yoshida, S.; Tanaka, K.; Batuk, D.; Abakumov, A.M.; Brown, C.M.; Kobayashi, Y.; Kageyama, H.;
Title Topochemical nitridation with anion vacancy -assisted N3-/O2- exchange Type A1 Journal article
Year 2016 Publication Journal of the American Chemical Society Abbreviated Journal J Am Chem Soc
Volume 138 Issue 138 Pages 3211-3217
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract We present how the introduction of anion vacancies in oxyhydrides enables a route to access new oxynitrides, by conducting ammonolysis of perovskite oxyhydride EuTiO3-xHx (x similar to 0.18). At 400 degrees C, similar to our studies on BaTiO3-xHx, hydride lability enables a low temperature direct ammonolysis of EUTi3.82+O-2.82/H-0.18, leading to the N3-/H--exchanged product EuTi4+O2.82No0.12 square 0.06 center dot When the ammonolysis temperature was increased up to 800 degrees C, we observed a further nitridation involving N3-/O2- exchange, yielding a fully oxidized Eu3+Ti4+O2N with the GdFeO3-type distortion (Pnma) as a metastable phase, instead of pyrochlore structure. Interestingly, the same reactions using the oxide EuTiO3 proceeded through a 1:1 exchange of N3- with O-2 only above 600 degrees C and resulted in incomplete nitridation to EuTi02.25N0.75, indicating that anion vacancies created during the initial nitridation process of EuTiO2.82H0.18 play a crucial role in promoting anion (N3-/O2-) exchange at high temperatures. Hence, by using (hydride-induced) anion-deficient precursors, we should be able to expand the accessible anion composition of perovskite oxynitrides.
Address
Corporate Author Thesis
Publisher Place of Publication Washington, D.C. Editor
Language Wos 000371945800055 Publication Date 2016-02-08
Series Editor (down) 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 28 Open Access
Notes Approved Most recent IF: 13.858
Call Number UA @ lucian @ c:irua:133156 Serial 4266
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Author Ilin, A.; Martyshov, M.; Forsh, E.; Forsh, P.; Rumyantseva, M.; Abakumov, A.; Gaskov, A.; Kashkarov, P.
Title UV effect on NO2 sensing properties of nanocrystalline In2O3 Type A1 Journal article
Year 2016 Publication Sensors and actuators : B : chemical Abbreviated Journal Sensor Actuat B-Chem
Volume 231 Issue 231 Pages 491-496
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Nanocrystalline indium oxide films with extremely small grains in range of 7-40 nm are prepared by sol-gel method. The influence of grain size on the sensitivity of indium oxide to nitrogen dioxide in low concentration at room temperature is investigated under the UV illumination and without illumination. The sensitivity increases with the decrease of grain sizes when In2O3 is illuminated while in the dark In2O3 with intermediate grain size exhibits the highest response. An explanation of the different behavior of the In2O3 with different grain size sensitivity to NO2 under illumination and in the dark is proposed. We demonstrate that pulsed illumination may be used for NO2 detection at room temperature that significantly reduces the power consumption of sensor. (C) 2016 Elsevier B.V. All rights reserved.
Address
Corporate Author Thesis
Publisher Place of Publication Lausanne Editor
Language Wos 000374330900055 Publication Date 2016-03-16
Series Editor (down) Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0925-4005 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 5.401 Times cited 27 Open Access
Notes Approved Most recent IF: 5.401
Call Number UA @ lucian @ c:irua:133630 Serial 4273
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Author Ryabova, A.S.; Bonnefont, A.; Zagrebin, P.; Poux, T.; Sena, R.P.; Hadermann, J.; Abakumov, A.M.; Kerangueven, G.; Istomin, S.Y.; Antipov, E.V.; Tsirlina, G.A.; Savinova, E.R.
Title Study of hydrogen peroxide reactions on manganese oxides as a tool to decode the oxygen reduction reaction mechanism Type A1 Journal article
Year 2016 Publication ChemElectroChem Abbreviated Journal Chemelectrochem
Volume 3 Issue 3 Pages 1667-1677
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Hydrogen peroxide has been detected as a reaction intermediate in the electrochemical oxygen reduction reaction (ORR) on transition-metal oxides and other electrode materials. In this work, we studied the electrocatalytic and catalytic reactions of hydrogen peroxide on a set of Mn oxides, Mn2O3, MnOOH, LaMnO3, MnO2, and Mn3O4, that adopt different crystal structures to shed light on the mechanism of the ORR on these materials. We then combined experiment with kinetic modeling with the objective to correlate the differences in the ORR activity to the kinetics of the elementary reaction steps, and we uncovered the importance of structural and compositional factors in the catalytic activity of the Mn oxides. We concluded that the exceptional activity of Mn2O3 in the ORR is due to its high catalytic activity both in the reduction of oxygen to hydrogen peroxide and in the decomposition of the latter, and furthermore, we proposed a tentative link between crystal structure and reactivity.
Address
Corporate Author Thesis
Publisher Wiley Place of Publication Place of publication unknown Editor
Language Wos 000388377200019 Publication Date 2016-07-14
Series Editor (down) Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2196-0216 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.136 Times cited 20 Open Access
Notes Approved Most recent IF: 4.136
Call Number UA @ lucian @ c:irua:139202 Serial 4449
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Author Kuno, Y.; Tassel, C.; Fujita, K.; Batuk, D.; Abakumov, A.M.; Shitara, K.; Kuwabara, A.; Moriwake, H.; Watabe, D.; Ritter, C.; Brown, C.M.; Yamamoto, T.; Takeiri, F.; Abe, R.; Kobayashi, Y.; Tanaka, K.; Kageyama, H.
Title ZnTaO2N: Stabilized High-Temperature LiNbO3-type Structure Type A1 Journal article
Year 2016 Publication Journal of the American Chemical Society Abbreviated Journal J Am Chem Soc
Volume 138 Issue 138 Pages 15950-15955
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract By using a high-pressure reaction, we prepared a new oxynitride ZnTaO2N that crystallizes in a centrosymmetric (R (3) over barc) high-temperature LiNbO3-type structure (HTLN-type). The stabilization of the HTLN-type structure down to low temperatures (at least 20 K) makes it possible to investigate not only the stability of this phase, but also the phase transition to a noncentrosymmetric (R3c) LiNbO3-type structure (LN-type) which is yet to be clarified. Synchrotron and neutron diffraction studies in combination with transmission electron microscopy show that Zn is located at a disordered 12c site instead of 6a, implying an order disorder mechanism of the phase transition. It is found that the dosed d-shell of Zn2+, as well as the high-valent Ta5+ ion, is responsible for the stabilization of the HTLN-type structure, affording a novel quasitriangular ZnO2N coordination. Interestingly, only 3% Zn substitution for MnTaO2N induces a phase transition from LN- to HTLN-type structure, implying the proximity in energy between the two structural types, which is supported by the first-principles calculations.
Address
Corporate Author Thesis
Publisher Place of Publication Washington, D.C. Editor
Language Wos 000389962800032 Publication Date 2016-11-18
Series Editor (down) 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 13 Open Access
Notes Approved Most recent IF: 13.858
Call Number UA @ lucian @ c:irua:140298 Serial 4452
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Author Batuk, D.; Batuk, M.; Filimonov, D.S.; Zakharov, K.V.; Volkova, O.S.; Vasiliev, A.N.; Tyablikov, O.A.; Hadermann, J.; Abakumov, A.M.
Title Crystal Structure, Defects, Magnetic and Dielectric Properties of the Layered Bi3n+1Ti7Fe3n-3,O9n+11 Perovskite-Anatase lntergrowths Type A1 Journal article
Year 2017 Publication Inorganic chemistry Abbreviated Journal Inorg Chem
Volume 56 Issue 56 Pages 931-942
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The Bi3n+1Ti7Fe3n-3,O9n+11 materials are built of (001)(p) plane parallel perovskite blocks with a thickness of n (Ti,Fe)O-6 octahedra, separated by periodic translational interfaces. The interfaces are based on anatase-like chains of edge -sharing (Ti,Fe)O-6 octahedra. Together with the octahedra of the perovskite blocks, they create S-shaped tunnels stabilized by lone pair Bi3+ cations. In this work, the structure of the n = 4-6 Bi3n+1Ti7Fe3n-3,O9n+11 homologues is analyzed in detail using advanced transmission electron microscopy, powder X-ray diffraction, and Mossbauer spectroscopy. The connectivity of the anatase-like chains to the perovskite blocks results in,a 3ap periodicity along the interfaces, so that they can be located either on top of each other or with shifts of +/- a(p) along [100](p). The ordered arrangement of the interfaces gives rise to orthorhombic Immm and monoclinic A2/m polymorphs with the unit cell parameters a = 3a(p), b = b(p), c = 2(n + 1)c(p) and a = 3a(p), b = b(p), c = 2(n + 1)c(p) – a(p), respectively. While the n = 3 compound is orthorhombic, the monoclinic modification is more favorable in higher homologues. The Bi3n+1Ti7Fe3n-3,O9n+11 structures demonstrate intricate patterns of atomic displacements in the perovskite blocks, which are supported by the stereochemical activity of the Bi3+ cations. These patterns are coupled to the cationic coordination of the oxygen atoms in the (Ti,Fe)O-2 layers at the border of the perovskite blocks. The coupling is strong in the 1/ = 3, 4 homologues, but gradually reduces with the increasing thickness of the perovskite blocks, so that, in the n = 6 compound, the dominant mode of atomic displacements is aligned along the interface planes. The displacements in the adjacent perovskite blocks tend to order antiparallel, resulting in an overall antipolar structure. The Bi3n+1Ti7Fe3n-3,O9n+11 materials demonstrate an unusual diversity of structure defects. The n = 4-6 homologues are robust antiferromagnets below T-N = 135, 220, and 295 K, respectively. They show a high dielectric constant that weakly increases with temperature and is relatively insensitive to the Ti/Fe ratio.
Address
Corporate Author Thesis
Publisher Place of Publication Easton, Pa Editor
Language Wos 000392262400029 Publication Date 2016-12-25
Series Editor (down) Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0020-1669 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.857 Times cited 3 Open Access Not_Open_Access
Notes ; The work was supported by the Russian Science Foundation (grant 14-13-00680). ; Approved Most recent IF: 4.857
Call Number UA @ lucian @ c:irua:141471 Serial 4495
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Author Rozova, M.G.; Grigoriev, V.V.; Tyablikov, O.A.; Filimonov, D.S.; Zakharov, K.V.; Volkova, O.S.; Vasiliev, A.N.; Antipov, E.V.; Abakumov, A.M.
Title Doping of Bi4Fe5O13F with pentagonal Cairo lattice with Cr and Mn: Synthesis, structure and magnetic properties Type A1 Journal article
Year 2017 Publication Materials research bulletin Abbreviated Journal Mater Res Bull
Volume 87 Issue 87 Pages 54-60
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The substitution of Cr3+ and Mn3+ for Fe3+ in the Bi4Fe6O13F oxyfluoride featuring the magnetically frustrated pentagonal Cairo lattice is reported. Bi4Fe4.1Cr0.9O13F and BiFe4.2Mn0.8O13F have been prepared using a solid state reaction in inert atmosphere. Their crystal structures were studied with transmission electron microscopy, powder X-ray diffraction and Fe-57 Mossbauer spectroscopy (S.G. P4(2)/mbc, a = 8.27836(2)angstrom, c = 18.00330(9) angstrom, R-F = 0.031 (Bi4Fe4.1Cr0.9O13F)), a= 8.29535(3)angstrom, c= 18.0060(1)angstrom, R-F = 0.027 (Bi4Fe4.1Cr0.9O13F)). The structures are formed by infinite rutile-like chains of the edge sharing BO6 octahedra (B transition metal cations) linked by the Fe2O7 groups of two corner-sharing tetrahedra. The"voids in thus formed framework are occupied by the Bi4F tetrahedra. The Fe-57 Mossbauer spectroscopy reveals that Cr3+ and Mn3+ replace Fe3+. exclusively at the octahedral positions. The Mn- and Cr-doped compounds demonstrate antiferromagnetic ordering below T-N =165 K and 120 K, respectively. (C) 2016 Elsevier Ltd. All rights reserved.
Address
Corporate Author Thesis
Publisher Place of Publication New York, N.Y. Editor
Language Wos 000392681800009 Publication Date 2016-11-17
Series Editor (down) Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0025-5408 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 2.446 Times cited 1 Open Access Not_Open_Access
Notes ; The work has been supported by the Russian Science Foundation (grant 14-13-00680). ; Approved Most recent IF: 2.446
Call Number UA @ lucian @ c:irua:141535 Serial 4498
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Author Semkina, A.S.; Abakumov, M.A.; Abakumov, A.M.; Nukolova, N.V.; Chekhonin, V.P.
Title Relationship between the Size of Magnetic Nanoparticles and Efficiency of MRT Imaging of Cerebral Glioma in Rats Type A1 Journal article
Year 2016 Publication Bulletin of experimental biology and medicine Abbreviated Journal B Exp Biol Med+
Volume 161 Issue 2 Pages 292-295
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract BSA-coated Fe3O4 nanoparticles with different hydrodynamic diameters (36 +/- 4 and 85 +/- 10 nm) were synthesized, zeta potential and T2 relaxivity were determined, and their morphology was studied by transmission electron microscopy. Studies on rats with experimental glioma C6 showed that smaller nanoparticles more effectively accumulated in the tumor and circulated longer in brain vessels. Optimization of the hydrodynamic diameter improves the efficiency of MRT contrast agent.
Address
Corporate Author Thesis
Publisher Place of Publication New York Editor
Language Wos 000380118500022 Publication Date 2016-07-07
Series Editor (down) Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0007-4888 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 0.456 Times cited 5 Open Access
Notes Approved Most recent IF: 0.456
Call Number UA @ lucian @ c:irua:144707 Serial 4684
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Author Voorhaar, L.; Diaz, M.M.; Leroux, F.; Rogers, S.; Abakumov, A.M.; Van Tendeloo, G.; Van Assche, G.; Van Mele, B.; Hoogenboom, R.
Title Supramolecular thermoplastics and thermoplastic elastomer materials with self-healing ability based on oligomeric charged triblock copolymers Type A1 Journal article
Year 2017 Publication NPG Asia materials Abbreviated Journal Npg Asia Mater
Volume 9 Issue Pages e385
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Supramolecular polymeric materials constitute a unique class of materials held together by non-covalent interactions. These dynamic supramolecular interactions can provide unique properties such as a strong decrease in viscosity upon relatively mild heating, as well as self-healing ability. In this study we demonstrate the unique mechanical properties of phase-separated electrostatic supramolecular materials based on mixing of low molar mass, oligomeric, ABA-triblock copolyacrylates with oppositely charged outer blocks. In case of well-chosen mixtures and block lengths, the charged blocks are phase separated from the uncharged matrix in a hexagonally packed nanomorphology as observed by transmission electron microscopy. Thermal and mechanical analysis of the material shows that the charged sections have a T-g closely beyond room temperature, whereas the material shows an elastic response at temperatures far above this T-g ascribed to the electrostatic supramolecular interactions. A broad set of materials having systematic variations in triblock copolymer structures was used to provide insights in the mechanical properties and and self-healing ability in correlation with the nanomorphology of the materials.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000402065300005 Publication Date 2017-05-26
Series Editor (down) Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1884-4049; 1884-4057 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 9.157 Times cited 8 Open Access OpenAccess
Notes ; This research was conducted in the framework of the SIM-SHE/NAPROM project and SIM is gratefully acknowledged for the financial support. ; Approved Most recent IF: 9.157
Call Number UA @ lucian @ c:irua:144263 Serial 4691
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Author Weber, D.; Huber, M.; Gorelik, T.E.; Abakumov, A.M.; Becker, N.; Niehaus, O.; Schwickert, C.; Culver, S.P.; Boysen, H.; Senyshyn, A.; Poettgen, R.; Dronskowski, R.; Ressler, T.; Kolb, U.; Lerch, M.
Title Molybdenum oxide nitrides of the Mo2(O,N,\square)5 type : on the way to Mo2O5 Type A1 Journal article
Year 2017 Publication Inorganic chemistry Abbreviated Journal Inorg Chem
Volume 56 Issue 15 Pages 8782-8792
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Blue-colored molybdenum oxide nitrides of the Mo-2(O,N,square)(5) type were synthesized by direct nitridation of commercially available molybdenum trioxide with a mixture of gaseous ammonia and oxygen. Chemical composition, crystal structure, and stability of the obtained and hitherto unknown compounds are studied extensively. The average oxidation state of +5 for molybdenum is proven by Mo K near-edge X-ray absorption spectroscopy; the magnetic behavior is in agreement with compounds exhibiting (MoO6)-O-v units. The new materials are stable up to similar to 773 K in an inert gas atmosphere. At higher temperatures, decomposition is observed. X-ray and neutron powder diffraction, electron diffraction, and high-resolution transmission electron microscopy reveal the structure to be related to VNb9O24.9-type phases, however, with severe disorder hampering full structure determination. Still, the results demonstrate the possibility of a future synthesis of the potential binary oxide Mo2O5. On the basis of these findings, a tentative suggestion on the crystal structure of the potential compound Mo2O5, backed by electronic-structure and phonon calculations from first principles, is given.
Address
Corporate Author Thesis
Publisher Place of Publication Easton, Pa Editor
Language Wos 000407405500026 Publication Date 2017-07-17
Series Editor (down) Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0020-1669 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.857 Times cited 3 Open Access Not_Open_Access
Notes ; Financial support from the Deutsche Forschungsgemeinschaft (SPP 1415, LE 781/ 11-1, DR 342/22-2) is gratefully acknowledged. The authors are grateful to J. Barthel, Ernst Ruska-Centre for Microscopy and Spectroscopy with Electrons Julich, Germany, for STEM image simulations. This work was further supported by Diamond Light Source (beamtime awards EE13560) within beamtime proposal SP13560. The Hamburg Synchrotron Radiation Laboratory, HASYLAB, and the FRM II, Garching, are acknowledged for providing beamtime. ; Approved Most recent IF: 4.857
Call Number UA @ lucian @ c:irua:145727 Serial 4744
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Author Lutz, L.; Corte, D.A.D.; Chen, Y.; Batuk, D.; Johnson, L.R.; Abakumov, A.; Yate, L.; Azaceta, E.; Bruce, P.G.; Tarascon, J.-M.; Grimaud, A.
Title The role of the electrode surface in Na-Air batteries : insights in electrochemical product formation and chemical growth of NaO2 Type A1 Journal article
Year 2018 Publication Advanced energy materials Abbreviated Journal Adv Energy Mater
Volume 8 Issue 4 Pages 1701581
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract The Na-air battery, because of its high energy density and low charging overpotential, is a promising candidate for low-cost energy storage, hence leading to intensive research. However, to achieve such a battery, the role of the positive electrode material in the discharge process must be understood. This issue is herein addressed by exploring the electrochemical reduction of oxygen, as well as the chemical formation and precipitation of NaO2 using different electrodes. Whereas a minor influence of the electrode surface is demonstrated on the electrochemical formation of NaO2, a strong dependence of the subsequent chemical precipitation of NaO2 is identified. In the origin, this effect stems from the surface energy and O-2/O-2(-) affinity of the electrode. The strong interaction of Au with O-2/O-2(-) increases the nucleation rate and leads to an altered growth process when compared to C surfaces. Consequently, thin (3 mu m) flakes of NaO2 are found on Au, whereas on C large cubes (10 mu m) of NaO2 are formed. This has significant impact on the cell performance and leads to four times higher capacity when C electrodes with low surface energy and O-2/O-2(-) affinity are used. It is hoped that these findings will enable the design of new positive electrode materials with optimized surfaces.
Address
Corporate Author Thesis
Publisher WILEY-VCH Verlag GmbH & Co. Place of Publication Weinheim Editor
Language Wos 000424152200009 Publication Date 2017-09-25
Series Editor (down) Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1614-6832; 1614-6840 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 16.721 Times cited 13 Open Access Not_Open_Access
Notes ; L.L. thanks ALISTORE-ERI for his PhD grant. P.G.B. is indebted to the EPSRC for financial support, including the Supergen Energy Storage grant. ; Approved Most recent IF: 16.721
Call Number UA @ lucian @ c:irua:149269 Serial 4951
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Author Grimaud, A.; Iadecola, A.; Batuk, D.; Saubanere, M.; Abakumov, A.M.; Freeland, J.W.; Cabana, J.; Li, H.; Doublet, M.-L.; Rousse, G.; Tarascon, J.-M.
Title Chemical activity of the peroxide/oxide redox couple : case study of Ba5Ru2O11 in aqueous and organic solvents Type A1 Journal article
Year 2018 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 30 Issue 11 Pages 3882-3893
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The finding that triggering the redox activity of oxygen ions within the lattice of transition metal oxides can boost the performances of materials used in energy storage and conversion devices such as Li-ion batteries or oxygen evolution electrocatalysts has recently spurred intensive and innovative research in the field of energy. While experimental and theoretical efforts have been critical in understanding the role of oxygen nonbonding states in the redox activity of oxygen ions, a clear picture of the redox chemistry of the oxygen species formed upon this oxidation process is still missing. This can be, in part, explained by the complexity in stabilizing and studying these species once electrochemically formed. In this work, we alleviate this difficulty by studying the phase Ba5Ru2O11, which contains peroxide O-2(2-) groups, as oxygen evolution reaction electrocatalyst and Li-ion battery material. Combining physical characterization and electrochemical measurements, we demonstrate that peroxide groups can easily be oxidized at relatively low potential, leading to the formation of gaseous dioxygen and to the instability of the oxide. Furthermore, we demonstrate that, owing to the stabilization at high energy of peroxide, the high-lying energy of the empty sigma* antibonding O-O states limits the reversibility of the electrochemical reactions when the O-2(2-)/O2- redox couple is used as redox center for Li-ion battery materials or as OER redox active sites. Overall, this work suggests that the formation of true peroxide O-2(2-) states are detrimental for transition metal oxides used as OER catalysts and Li-ion battery materials. Rather, oxygen species with O-O bond order lower than 1 would be preferred for these applications.
Address
Corporate Author Thesis
Publisher American Chemical Society Place of Publication Washington, D.C Editor
Language Wos 000435416600038 Publication Date 2018-05-21
Series Editor (down) 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 2 Open Access Not_Open_Access
Notes ; We thank S. Belin of the ROCK beamline (financed by the French National Research Agency (ANR) as a part of the “Investissements d'Avenir” program, reference: ANR-10-EQPX-45; proposal no. 20160095) of synchrotron SOLEIL for her assistance during XAS measurements. Authors would also like to thank V. Nassif for her assistance on the D1B beamline. A.G, G.R, and J.-M.T. acknowledge funding from the European Research Council (ERC) (FP/2014)/ERC Grant Project 670116-ARPEMA. ; Approved Most recent IF: 9.466
Call Number UA @ lucian @ c:irua:151980 Serial 5016
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Author Morozov, V.; Deyneko, D.; Basoyich, O.; Khaikina, E.G.; Spassky, D.; Morozov, A.; Chernyshev, V.; Abakumov, A.; Hadermann, J.
Title Incommensurately modulated structures and luminescence properties of the AgxSm(2-x)/3WO4 (x=0.286, 0.2) scheelites as thermographic phosphors Type A1 Journal article
Year 2018 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 30 Issue 14 Pages 4788-4798
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Ag+ for Sm3+ substitution in the scheelite-type AgxSm(2-x)/3 square(1-2x)/3WO4 tungstates has been investigated for its influence on the cation-vacancy ordering and luminescence properties. A solid state method was used to synthesize the x = 0.286 and x = 0.2 compounds, which exhibited (3 + 1)D incommensurately modulated structures in the transmission electron microscopy study. Their structures were refined using high resolution synchrotron powder X-ray diffraction data. Under near-ultraviolet light, both compounds show the characteristic emission lines for (4)G(5/2) -> H-6(J) (J = 5/2, 7/2, 9/2, and 11/2) transitions of the Sm3+ ions in the range 550-720 nm, with the J = 9/2 transition at the similar to 648 nm region being dominant for all photoluminescence spectra. The intensities of the (4)G(5/2) -> H-6(9/2) and (4)G(5/2) -> H-6(7/2) bands have different temperature dependencies. The emission intensity ratios (R) for these bands vary reproducibly with temperature, allowing the use of these materials as thermographic phosphors.
Address
Corporate Author Thesis
Publisher American Chemical Society Place of Publication Washington, D.C Editor
Language Wos 000440105500037 Publication Date 2018-06-21
Series Editor (down) 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 2 Open Access Not_Open_Access
Notes ; This research was supported by FWO (Project G039211N), Flanders Research Foundation. The research was carried out within the state assignment of FASO of Russia (Themes No. 0339-2016-0007). V.M. thanks the Russian Foundation for Basic Research (Grant 18-03-00611) for financial support. E.G.K. and O.B. acknowledge financial support from the Russian Foundation for Basic Research (Grant 16-03-00510). D.D. thanks the Foundation of the Russian Federation President (Grant MK-3502.2018.5) for financial support. We are grateful to the ESRF for granting the beamtime. V.C. is grateful for the financial support of the Russian Ministry of Science and Education (Project No. RFMEFI61616X0069). We are grateful to the ESRF for the access to ID22 station (experiment MA-3313). ; Approved Most recent IF: 9.466
Call Number UA @ lucian @ c:irua:153156 Serial 5107
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Author De Sloovere, D.; Safari, M.; Elen, K.; D'Haen, J.; Drozhzhin, O.A.; Abakumov, A.M.; Simenas, M.; Banys, J.; Bekaert, J.; Partoens, B.; Van Bael, M.K.; Hardy, A.
Title Reduced Na2+xTi4O9 composite : a durable anode for sodium-ion batteries Type A1 Journal article
Year 2018 Publication Chemistry of materials Abbreviated Journal Chem Mater
Volume 30 Issue 23 Pages 8521-8527
Keywords A1 Journal article; Condensed Matter Theory (CMT)
Abstract Sodium-ion batteries (SIBs) are potential cost-effective solutions for stationary energy storage applications. Unavailability of suitable anode materials, however, is one of the important barriers to the maturity of SIBs. Here, we report a Na2+xTi4O9/C composite as a promising anode candidate for SIBs with high capacity and cycling stability. This anode is characterized by a capacity of 124 mAh g(-1) (plus 11 mAh g(-1) contributed by carbon black), an average discharge potential of 0.9 V vs Na/Na+, a good rate capability and a high stability (89% capacity retention after 250 cycles at a rate of 1 degrees C). The mechanisms of sodium insertion/deinsertion and of the formation of Na2+xTi4O9/C are investigated with the aid of various ex/in situ characterization techniques. The in situ formed carbon is necessary for the formation of the reduced sodium titanate. This synthesis method may enable the convenient synthesis of other composites of crystalline phases with amorphous carbon.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000453489300014 Publication Date 2018-11-29
Series Editor (down) 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 7 Open Access
Notes ; This work was supported by the FWO (Research Foundation Flanders, project G040116). O.A.D. and A.M.A. are grateful to the Russian Science Foundation for financial support (Grant 17-73-30006). The authors acknowledge Pieter Samyn for Raman spectroscopy, Fulya Ulu Okudur for preliminary TEM, Bart Ruttens for XRD, Hilde Pellaers for SEM, Tom Haeldermans for elemental analysis, and Karen Leyssen and Vera Meynen for physisorption measurements. ; Approved Most recent IF: 9.466
Call Number UA @ admin @ c:irua:156235 Serial 5227
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Author Mefford, J.T.; Kurilovich, A.A.; Saunders, J.; Hardin, W.G.; Abakumov, A.M.; Forslund, R.P.; Bonnefont, A.; Dai, S.; Johnston, K.P.; Stevenson, K.J.
Title Decoupling the roles of carbon and metal oxides on the electrocatalytic reduction of oxygen on La1-xSrxCoO3-\delta perovskite composite electrodes Type A1 Journal article
Year 2019 Publication Physical chemistry, chemical physics Abbreviated Journal Phys Chem Chem Phys
Volume 21 Issue 6 Pages 3327-3338
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Perovskite oxides are active room-temperature bifunctional oxygen electrocatalysts in alkaline media, capable of performing the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) with lower combined overpotentials relative to their precious metal counterparts. However, their semiconducting nature necessitates the use of activated carbons as conductive supports to generate applicably relevant current densities. In efforts to advance the performance and theory of oxide electrocatalysts, the chemical and physical properties of the oxide material often take precedence over contributions from the conductive additive. In this work, we find that carbon plays an important synergistic role in improving the performance of La1-xSrxCoO3- (0 x 1) electrocatalysts through the activation of O-2 and spillover of radical oxygen intermediates, HO2- and O-2(-), which is further reduced through chemical decomposition of HO2- on the perovskite surface. Through a combination of thin-film rotating disk electrochemical characterization of the hydrogen peroxide intermediate reactions (hydrogen peroxide reduction reaction (HPRR), hydrogen peroxide oxidation reaction (HPOR)) and oxygen reduction reaction (ORR), surface chemical analysis, HR-TEM, and microkinetic modeling on La1-xSrxCoO3- (0 x 1)/carbon (with nitrogen and non-nitrogen doped carbons) composite electrocatalysts, we deconvolute the mechanistic aspects and contributions to reactivity of the oxide and carbon support.
Address
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Publisher Place of Publication Editor
Language Wos 000459584900049 Publication Date 2019-01-18
Series Editor (down) Series Title Abbreviated Series Title
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ISSN 1463-9076; 1463-9084 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.123 Times cited 5 Open Access OpenAccess
Notes ; Financial support for this work was provided by the R. A. Welch Foundation (grants F-1529 and F-1319). S. D. was supported as part of the Fluid Interface Reactions, Structures and Transport (FIRST) Center, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences. ; Approved Most recent IF: 4.123
Call Number UA @ admin @ c:irua:158625 Serial 5244
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Author Chizhov, A.; Vasiliev, R.; Rumyantseva, M.; Krylov, I.; Drozdov, K.; Batuk, M.; Hadermann, J.; Abakumov, A.; Gaskov, A.
Title Light-activated sub-ppm NO2 detection by hybrid ZnO/QD nanomaterials vs. charge localization in core-shell QD Type A1 Journal article
Year 2019 Publication Frontiers in materials Abbreviated Journal
Volume 6 Issue 6 Pages
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract New hybrid materials-photosensitized nanocomposites containing nanocrystal heterostructures with spatial charge separation, show high response for practically important sub-ppm level NO2 detection at room temperature. Nanocomposites ZnO/CdSe, ZnO/(CdS@CdSe), and ZnO/(ZnSe@CdS) were obtained by the immobilization of nanocrystals-colloidal quantum dots (QDs), on the matrix of nanocrystalline ZnO. The formation of crystalline core-shell structure of QDs was confirmed by HAADF-STEM coupled with EELS mapping. Optical properties of photosensitizers have been investigated by optical absorption and luminescence spectroscopy combined with spectral dependences of photoconductivity, which proved different charge localization regimes. Photoelectrical and gas sensor properties of nanocomposites have been studied at room temperature under green light (max = 535 nm) illumination in the presence of 0.12-2 ppm NO2 in air. It has been demonstrated that sensitization with type II heterostructure ZnSe@CdS with staggered gap provides the rapid growth of effective photoresponse with the increase in the NO2 concentration in air and the highest sensor sensitivity toward NO2. We believe that the use of core-shell QDs with spatial charge separation opens new possibilities in the development of light-activated gas sensors working without thermal heating.
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Publisher Place of Publication Editor
Language Wos 000487641600002 Publication Date 2019-09-24
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ISSN 2296-8016 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor Times cited 1 Open Access
Notes ; This work was financially supported by RFBR grant No. 1653-76001 (RFBR – ERA.Net FONSENS 096) and in part by a grant from the St. Petersburg State University – Event 3-2018 (id: 26520408). AC acknowledges support from the RFBR grant No. 18-33-01004. ; Approved Most recent IF: NA
Call Number UA @ admin @ c:irua:163776 Serial 5390
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Author Hadermann, J.; Abakumov, A.M.
Title Structure solution and refinement of metal-ion battery cathode materials using electron diffraction tomography Type A1 Journal article
Year 2019 Publication And Materials Abbreviated Journal
Volume 75 Issue 4 Pages 485-494
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The applicability of electron diffraction tomography to the structure solution and refinement of charged, discharged or cycled metal-ion battery positive electrode (cathode) materials is discussed in detail. As these materials are often only available in very small amounts as powders, the possibility of obtaining single-crystal data using electron diffraction tomography (EDT) provides unique access to crucial information complementary to X-ray diffraction, neutron diffraction and high-resolution transmission electron microscopy techniques. Using several examples, the ability of EDT to be used to detect lithium and refine its atomic position and occupancy, to solve the structure of materials ex situ at different states of charge and to obtain in situ data on structural changes occurring upon electrochemical cycling in liquid electrolyte is discussed.
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Publisher Place of Publication Editor
Language Wos 000480512600002 Publication Date 2019-08-05
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Impact Factor Times cited 2 Open Access
Notes ; The following funding is acknowledged: Fonds Wetenschappelijk Onderzoek (grant No. G040116N); Russian Foundation of Basic Research (grant No. 17-03-00370-a). ; Approved Most recent IF: NA
Call Number UA @ admin @ c:irua:161846 Serial 5397
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Author Kirsanova, M.A.; De Sloovere, D.; Karakulina, O.M.; Hadermann, J.; Van Bael, M.K.; Hardy, A.; Abakumov, A.M.
Title Toward unlocking the Mn3+/Mn2+ redox pair in alluaudite-type Na2+2zMn2-z(SO4)3-x(SeO4)x cathodes for sodium-ion batteries Type A1 Journal article
Year 2019 Publication Journal of solid state chemistry Abbreviated Journal J Solid State Chem
Volume 277 Issue 277 Pages 804-810
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract In polyanion cathodes, the inductive effect alters the potential of a M(n+1)+/Mn+ redox couple (M – transition metal) according to the electronegativity of the X cation in the polyanion groups (XO4m+). To manipulate the operating potential, we synthesized a series of mixed sulfate-selenate alluaudites, with structure formulas Na2+2zMn2-z(SO4)(3-x)(SeO4)(x) and Na2.81Ni1.60(SO4)(1.43)(SeO4)(1.57). Their crystal structure was determined from powder X-ray diffraction data, revealing that the Mn-based alluaudites form solid solutions with the same crystal structure for x = 0.75; 1.125 and 1.5. Na2.81Ni1.60(SO4)(1.43)(SeO4)(1.57) is isostructural to the Mn-based alluaudites. Although the Na2+2zMn2-z(SO4)(3-x)(SeO4)(x) compound with the highest selenium content demonstrates a reversible discharge capacity of 60 mAh g(-1), only a small part of this electrochemical activity can be ascribed to the Mn3+/Mn2+ redox couple. The redox potential of the Mn3+/Mn2+ pair in Na2+2zMn2-z(SO4)(3-)x(SeO4)(x) decreases with increasing values of x, in agreement with the lower electronegativity of Se compared to that of S.
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Publisher Place of Publication Editor
Language Wos 000481726300103 Publication Date 2019-07-24
Series Editor (down) Series Title Abbreviated Series Title
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ISSN 0022-4596 ISBN Additional Links UA library record; WoS full record
Impact Factor 2.299 Times cited Open Access
Notes ; The authors thank the Russian Foundation for Basic Research for financial support (grant 17-03-00370), in addition to Research Foundation-Flanders (project No G040116). ; Approved Most recent IF: 2.299
Call Number UA @ admin @ c:irua:162852 Serial 5401
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