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91.
Arabidopsis halleri shows hyperbioindicator behaviour for Pb and leaf Pb accumulation spatially separated from Zn
Stephan Höreth, Paula Pongrac, Marta Debeljak, Katarina Vogel-Mikuš, Matic Pečovnik, Primož Vavpetič, Iztok Arčon, original scientific article

Abstract: Lead (Pb) ranks among the most problematic environmental pollutants. Background contamination of soils is nearly ubiquitous, yet plant Pb accumulation is barely understood. In a survey covering 165 European populations of the metallophyte Arabidopsis halleri, several field samples had indicated Pb hyperaccumulation, offering a chance to dissect plant Pb accumulation. Accumulation of Pb was analysed in A. halleri individuals from contrasting habitats under controlled conditions to rule out aerial deposition as a source of apparent Pb accumulation. Several elemental imaging techniques were employed to study the spatial distribution and ligand environment of Pb. Regardless of genetic background, A. halleri individuals showed higher shoot Pb accumulation than A. thaliana. However, dose–response curves revealed indicator rather than hyperaccumulator behaviour. Xylem sap data and elemental imaging unequivocally demonstrated the in planta mobility of Pb. Highest Pb concentrations were found in epidermal and vascular tissues. Distribution of Pb was distinct from that of the hyperaccumulated metal zinc. Most Pb was bound by oxygen ligands in bidentate coordination. A. halleri accumulates Pb whenever soil conditions render Pb phytoavailable. Considerable Pb accumulation under such circumstances, even in leaves of A. thaliana, strongly suggests that Pb can enter food webs and may pose a food safety risk.
Found in: osebi
Keywords: Pb accumulation, XANES, EXAFS, Arabidopsis halleri
Published: 16.01.2020; Views: 459; Downloads: 0
.pdf Fulltext (4,46 MB)

92.
Role of Cu current collector on electrochemical mechanism of Mg–S battery
Ana Robba, Maja Mežnar, Alen Vižintin, Jan Bitenc, Jernej Bobnar, Iztok Arčon, Anna Randon-Vitanova, Robert Dominko, 2020, original scientific article

Abstract: Development of magnesium sulfur battery is accompanied with all known difficulties present in Li–S batteries, however with even more limited choice of electrolytes. In the present work, the influence of current collector on electrochemical mechanism was investigated in light of different reports where improved behavior was ascribed to electrolyte. Notable differences in cycling behavior are reported when Al current collector is replaced by Cu current collector independent of electrolyte. The initial reduction of sulfur follows similar reaction path no mater of current collector, but formation of MgS can be in competition with formation of CuS in the presence of Cu cations. With the subsequent cycling cells prepared from cathodes deposited on Cu current collector show decrease in the voltage and formation of single plateau during cycling. The change corresponds to the involvement of Cu into the reaction and formation of redox couple Mg/CuS as determined by Cu K-edge XANES measurements. Corrosion of Cu foil is identified by SEM and serves as a source of Cu cations for the chemical reaction between Cu and polysulfides. Mg/CuS redox couple shows improved cycling stability, but theoretical energy density is severely reduced due to substitution of S with CuS as cathode active material.
Found in: osebi
Keywords: Magnesium Sulfur Rechargeable batteries Current collector Copper Corrosion
Published: 16.01.2020; Views: 458; Downloads: 0
.pdf Fulltext (1,86 MB)

93.
X-ray absorption spectroscopy set-up for unstable gases: A study of 5p Hydrides
Robert Hauko, Jana Padežnik Gomilšek, Alojz Kodre, Iztok Arčon, 2020, original scientific article

Abstract: An absorption cell is constructed for x-ray absorption spectroscopy of reactive, unstable or hazardous gases at room temperature. In conjunction with in-situ micro-synthesis technique relying on handling the gas in syringes it enabled a first measurement of x-ray absorption spectra in the region of K and L edges for the series of hydrides of 5p elements (SnH4, SbH3, TeH2, HI). The signal-to-noise ratio above 103 was achieved, whereby fine detail is discerned in the spectra, in particular the small sharp features above each absorption edge, testifying of coexcitations of outer electrons in the core photoeffect.
Found in: osebi
Keywords: X-ray absorption spectroscopy Micro-synthesis absorption cell Gaseous hydrides Multielectron photoexcitations
Published: 10.02.2020; Views: 529; Downloads: 0
.pdf Fulltext (756,39 KB)

94.
Improved photocatalytic activity of anatase-rutile nanocomposites induced by low-temperature sol-gel Sn-modification of TiO2
Ksenija Maver, Iztok Arčon, Urška Lavrenčič Štangar, Mattia Fanetti, Saim Emin, Matjaž Valant, 2020, original scientific article

Abstract: The Sn-modified TiO2 photocatalysts are prepared by low-temperature sol-gel processing based on organic titanium and tin precursors with varied Sn concentrations (from 0.1–20 mol .%). The role of Sn dopant as the promotor of the formation of TiO2 rutile crystalline phase is explained and the optimal Sn concentration for preparation of efficient Sn-modified titania photocatalyst is determined. Up to 40 % increase in photocatalytic activity is achieved in Sn-modified TiO2 photocatalytic thin films dried at 150 °C with low Sn concentrations in the range from 0.1 to 1 mol .%. At low Sn concentrations optimal ratio between anatase and rutile (nano)crystals is obtained, which facilitates charge separation at the TiO2 photocatalyst’s surface. When the concentration of Sn increases above 5 mol.% or when the films are calcined at 500 °C, the relative amount of rutile phase with inferior photocatalytic activity, increases and the nanocrystals of titania grow, leading to fewer active sites per unit mass and the reduction of activity in comparison to unmodified TiO2.
Found in: osebi
Keywords: Anatase-rutile Sn-modified TiO2 XAS analysis Photocatalytic activity
Published: 10.02.2020; Views: 483; Downloads: 0
.pdf Fulltext (537,61 KB)

95.
Effects of a Mixed O/F Ligand in the Tavorite-Type LiVPO4O Structure
Sorour Semsari Parapari, Jean-Marcel Ateba Mba, Elena Tchernychova, Gregor Mali, Iztok Arčon, Gregor Kapun, Mehmet Ali Gülgün, Robert Dominko, 2020, original scientific article

Abstract: We report the synthesis and detailed structural and chemical characterization including electrochemical properties of a lithium vanadium oxy/fluoro-phosphate material. To the best of our knowledge, we have for the first time synthesized a LiVPO4O-type phase with a mixed O/F ligand. In the synthesis procedure, the LiVPO4O precursor compound was fluorinated via LiF incorporation, with preservation of the LiVPO4O framework structure. The operating potential of the synthesized material is increased compared to that of the LiVPO4O precursor (4.12 V vs 3.95 V versus metallic lithium, respectively). The related increase in operating potential was assigned to the effect of the intermixing O/F ligand, which is attained via the successful fluorine incorporation into the LiVPO4O structure. A characterization of the investigated materials was performed using microscale-covering XRD, XANES, and NMR techniques as well as nanoscale spatially resolved imaging and analytical STEM techniques. The obtained oxy/fluoro-phosphate phase is isostructural to LiVPO4O; however, the presence of the mixed O/F ligand promoted a higher symmetry of vanadium octahedra. These variations of the vanadium local environment along with the observed inhomogeneous distribution of the incorporated fluorine gave rise to the minor local deviations in vanadium valence. Our results clearly emphasize the connection among the fluorine ligand incorporation, its local distribution, and the electrochemical properties of the material.
Found in: osebi
Keywords: LiVPO4O, XRD, SEM, V XANES, Tavorite-Type, electrochemical properties
Published: 17.02.2020; Views: 438; Downloads: 0
.pdf Fulltext (3,11 MB)

96.
SnO2-Containing Clinoptilolite as a Composite Photocatalyst for Dyes Removal fromWastewater under Solar Light
Andraž Šuligoj, Jelena Pavlovič, Iztok Arčon, Nevenka Rajić, Nataša Novak Tušar, 2020, original scientific article

Abstract: Due to their adsorbent, ion exchange and catalytic properties zeolites are suitable for a variety of applications. We report on the photocatalytic activity of a readily available and inexpensive natural zeolite clinoptilolite (Z) containing SnO2 (Sn-Z). The Sn-Z samples with 3–15 wt. % of Sn were prepared by using a precipitation–deposition method. Powder X-ray diffraction analysis showed that the zeolite structure was unaffected by the introduction of the Sn-phase. Diffuse reflectance UV/VIS spectra of the Sn-Z samples confirmed the presence of SnO2 and X-Ray absorption spectroscopy analyses suggested that the SnO2 particles mainly resided on the surface of the clinoptilolite, while ATR-FTIR analysis gave some clues that part of the SnO2 phase was incorporated in the pores of the zeolite. The presence of SnO2 in Sn-Z increased both adsorption capacity and photocatalytic performance which could be partially explained by higher surface area and partially with an increased negative potential of the surface. Adsorption and total degradation of methylene blue (MB) for the Sn-Z with the highest amount of Sn (15 wt.%) was about 30% and 45%, respectively, suggesting a synergetic effect between SnO2 and the clinoptilolite lattice. Reusability tests showed that these catalysts present a promising material for water purification.
Found in: osebi
Keywords: SnO2, zeolite, SnO2-clinoptilolite composite, photocatalysis, solar light, methylene blue removal, wastewater treatment
Published: 25.02.2020; Views: 398; Downloads: 33
.pdf Fulltext (3,50 MB)

97.
Study of water adsorption on EDTA dealuminated zeolite Y
O. L. Pliekhov, Olena Pliekhova, Iztok Arčon, Federica Bondino, Elena Magnano, Gregor Mali, Nataša Zabukovec Logar, 2020, original scientific article

Abstract: Zeolite Y was synthesized and modified with EDTA dealumination procedure. The modified zeolites were analyzed by X-ray diffraction, X-ray absorption spectroscopy, chemical analysis and water adsorption measurements. We demonstrated that dealumination with bulk organic acid such as EDTA is able to reduce the original intense water affinity. Furthermore, it was found that dealumination with EDTA, in contrast with steaming and HCl dealumination, provides fully controllable, predictable and secure process of Al removal from the zeolites’ frameworks. The shift of the adsorption isotherm in the low partial pressure range represents an interesting result for adsorption-based applications.
Found in: osebi
Keywords: Zeolite Y Water sorption Dealumination Al XANES EDTA treatment
Published: 05.06.2020; Views: 368; Downloads: 0
.pdf Fulltext (667,27 KB)

98.
Ceramic synthesis of disordered lithium rich oxyfluoride materials
Jean-Marcel Ateba Mba, Iztok Arčon, Gregor Mali, Elena Tchernychova, Ralf Witte, Robert Kruk, Miran Gaberšček, Robert Dominko, 2020, original scientific article

Abstract: Disordered lithium-rich transition metal oxyfluorides with a general formula Li1þxMO2Fx (M being a transition metal) are gaining more attention due to their high specific capacity which can be delivered from the facecentered cubic (fcc) structure. The most common synthesis procedure involves use of mechanosynthesis. In this work, ceramic synthesis of lithium rich iron oxyfluoride and lithium rich titanium oxyfluoride are reported. Two ceramic synthesis routes are developed each leading to the different level of doping with Li and F and different levels of cationic disorder in the structure. Three different Li1þxMO2Fx samples (x ¼ 0.25, 0.3 and 1) are compared with a sample prepared by mechanochemical synthesis and non-doped LiFeO2 with fcc structure. The obtained lithium rich iron oxyfluoride are characterized by use of M€ossbauer spectroscopy, X-ray absorption spectroscopy, NMR and TEM. Successful incorporation of Li and F have been confirmed and specific capacity that can be obtained from the samples is in the correlation with the level of disorder introduced with doping, nevertheless oxidation state of iron in all samples is very similar. Conclusions obtained from lithium rich iron oxyfluoride are validated by lithium rich titanium oxyfluoride.
Found in: osebi
Keywords: Lithium batteries Face centered-cubic Oxyfluoride Li-rich Disorder
Published: 05.06.2020; Views: 340; Downloads: 0
.pdf Fulltext (2,37 MB)

99.
Effect of Na, Cs and Ca on propylene epoxidation selectivity over CuOx/SiO2 catalysts studied by catalytic tests, in-situ XAS and DFT
Janvit Teržan, Matej Huš, Iztok Arčon, Blaž Likozar, Petar Djinović, 2020, original scientific article

Abstract: This research focuses on epoxidation of propylene over pristine, Na, Ca and Cs modified CuOx/SiO2 catalysts using O2. The selectivity of the reaction is analyzed using a combination of catalytic tests, in-situ XAS and DFT calculations. The initially present subnanometer CuO clusters are present in all catalysts which re-disperse/flatten during reaction. During catalytic reaction, the Cu1+ becomes the predominant oxidation state. There is no correlation between propylene oxide (PO) selectivity and copper oxidation state. DFT analysis of the propylene reaction pathway revealed that Na, Cs, and Ca addition decreases the bonding strength of propylene to CuO and decreases the O2 activation barrier, while simultaneously increase the exothermicity of O2 dissociation. The Na induced Cu-O bond modification decreases the activation barrier from 0.87 to 0.71 eV for the oxametallacycle (OMC) ring closure (first step in the reaction pathway favoring selectivity towards PO) compared to pristine 5Cu catalyst. At the same time, we observed an increase (from 0.45 to 0.72 eV) of the barrier for the abstraction of allylic hydrogen. The opposite effect is achieved by Ca addition: the activation barrier for OMC ring closure increases to 1.08 eV and that for allylic hydrogen stripping decreases to 0.16 eV.
Found in: osebi
Keywords: Alkali modification, propylene epoxidation, reaction mechanism, copper oxide, activation barrier.
Published: 05.06.2020; Views: 354; Downloads: 0
.pdf Fulltext (22,78 MB)

100.
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