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81.
Synthesis of a Cu/ZnO Nanocomposite by Electroless Plating for the Catalytic Conversion of CO2 to Methanol
Maja Pori, Iztok Arčon, Marjan Marinšek, Goran Dražić, Blaž Likozar, Zorica Crnjak Orel, Damjan Lašič Jurković, 2019, original scientific article

Abstract: The process of methanol synthesis based on the hydrogenation of CO2 was investigated over binary Cu/ZnO catalyst materials, prepared by applying a novel electroless plating fabrication method. The activity of the produced catalytic samples was determined at temperature range between 200 and 300 °C and the feedstock conversion data were supplemented with a detailed microstructure analysis using high-resolution transmission electron microscopy (HRTEM), X-ray powder diffraction (XRD) and Cu and Zn K-edge, X-ray absorption near-edge structure (XANES) measurements and extended X-ray absorption fine-structure (EXAFS) measurements. It was confirmed that the disorder in the Cu crystallites created unique geometrical situations, which acted as the additional reactive centres for the adsorption of the reactant molecule species. Copper and zinc structural synergy (spill-over) was also demonstrated as being crucial for the carbon dioxide’s activation. EXAFS and XANES results provide strong evidence for surface alloying between copper and zinc and thus the present results demonstrate new approach applicable for explaining metal–support interactions.
Found in: osebi
Keywords: EXAFS, CuZn alloy, Spillover mechanism, CO2 valorization, Electroless deposition method, Heterogeneous catalysis
Published: 12.04.2019; Views: 907; Downloads: 0
.pdf Fulltext (1,92 MB)

82.
Alternative Recovery and Valorization of Metals from Exhausted Catalytic Converters in a New Smart Polymetallic Catalyst
Oreste Piccolo, Laura Sperni, Michele Gallo, Katarina Vogel-Mikuš, Iztok Arčon, Franco Baldi, Sebastiano Tieuli, Stefano Paganelli, 2019, original scientific article

Abstract: A new metals-polymeric composite, Metx-EPS (I), was prepared to be used as catalyst in water or in two-phase aqueous conditions. The metals source was an exhausted catalytic converter that was grinded and treated with an acidic solution at room temperature. After filtration, the solution was concentrated, neutralized and added to a broth of Klebsiella oxytoca DSM 29614 to produce (I) where metals are embedded in a peculiar polysaccharide structure (EPS). The composite was easily recovered from the fermentation broth and purified. The process protocol was verified many times and was shown to be reproducible satisfactorily. The % recovery of metals, originally present in the converter, was good as determined by atomic absorption. The morphology and the chemical state of main metals in (I) were investigated by X-ray absorption spectroscopy methods (XANES and EXAFS). No metallic alloy seems to be evident. The catalytic activity and a possible synergic effect due to the presence of the different metals was valuated in the hydrogenation of some substrates, valuable precursors for theproduction of fine chemicals.
Found in: osebi
Keywords: Biogenerated polymetallic exopolysaccharide, biphasic catalysis, hydrogenation, metals-polymeric composite, new catalyst from metallic wastes, EXAFS, XANES
Published: 06.05.2019; Views: 643; Downloads: 0
.pdf Fulltext (2,87 MB)

83.
A Biogenerated Polymetallic Catalyst from Society's Wastes
Oreste Piccolo, Stefano Paganelli, Petro Zanatta, Sebastiano Tieuli, Laura Sperni, Franco Baldi, Iztok Arčon, Michele Gallo, Katarina Vogel-Mikuš, 2019, original scientific article

Abstract: Aims:Preparation of the new metals - polymeric composite, Met x-EPS (I), to be used as a green catalyst in water or in two-phase aqueous conditions. Study Design: Recovery and valorization of polymetallic wastes to obtain directly new catalysts using a microorganism to explore their application in removal of difficult and dangerous chemical pollutants present in aqueous environment
Found in: osebi
Keywords: Metals - polymeric composite, biogenerated polymetallic exopolysaccharide, new catalyst from metallic wastes, hydrodechlorination of PCBs in water
Published: 06.05.2019; Views: 791; Downloads: 0
.pdf Fulltext (373,55 KB)

84.
New Insights into Manganese Local Environment in MnS-1Nanocrystals
Alenka Ristić, Matjaž Mazaj, Iztok Arčon, Nina Daneu, Nataša Zabukovec Logar, Roger Glaser, Nataša Novak Tušar, 2019, original scientific article

Abstract: Manganese plays an important role in redox catalysis using zeolites as inorganic support materials, but the formation of the preferred redox manganese species (framework or extraframework) is still not well understood. Herein, the influence of the amount of manganese together with conventional and microwave-assisted hydrothermal synthesis paths on the formation of manganese species within the zeolite silicalite-1 (S-1) with MFI structure was investigated. It was found out that both synthesis procedures led to the formation of framework and extraframework manganese species, but in different molar ratios. However, the conventional synthesis procedure with all Mn/Si molar ratios generates more framework Mn in comparison to the microwave procedure. Additionally, the diminution of the zeolite crystals to nanoscale from 100 to 200 nm was achieved via the conventional procedure for the first time. UV–vis, Raman, and X-ray absorption spectroscopic analyses revealed different local environments of manganese: Mn3+ incorporated into the silicalite-1 framework as “framework manganese” and Mn2+/3+ present as “extraframework manganese” (Mn2O3, Mn3O4). TEM reveals the presence of Mn3O4 nanorods. Both framework manganese and extraframework manganese exhibit good catalytic activity for styrene epoxidation. Catalytic results suggest that, in oxidation reactions of hydrocarbons, framework manganese is more active at lower Mn contents (Mn/Si < 0.015), whereas extraframework manganese is more active at higher loadings (Mn/Si > 0.015).
Found in: osebi
Keywords: MnS-1 Nanocrystals, Mn XANES, EXAFS, zeolites, microwave-assisted hydrothermal synthesis
Published: 06.05.2019; Views: 851; Downloads: 0
.pdf Fulltext (9,33 MB)

85.
86.
Effects of the molecular potential on coexcitations of valence electrons in the K-shell photoeffect of 3p and 4p elements
Robert Hauko, Jana Padežnik Gomilšek, Alojz Kodre, Iztok Arčon, Giuliana Aquilanti, 2019, original scientific article

Abstract: Photoabsorption spectra of gaseous hydrides of 3p (PH3, H2S, HCl) and 4p elements (GeH4, AsH3 , H2Se, HBr) are measured in the energy region within 50 eV above the K edge, to study coexcitations of valence electrons by photoeffect in the K shell. The analysis of the valence coexcitations is extended to Ar, Kr, and SiH4. Relative probabilities and energies of states in the individual coexcitation channels are recovered by modeling the spectral features with a minimal ansatz based on the features in the contiguous noble gas. The extracted parameters are compared to the results of theoretical calculations for molecules (ORCA code) and free atoms (Hartree-Fock code). The experimental results confirm that the valence coexcitations in the 3p and 4p hydride molecules can be satisfactorily described by a two-step process, with the shake of the outer electron following the excitation of the core electron. The total probability—relative to the K-edge jump—of the shake-up processes shows a steady decrease from 19% in Si to 14% in Cl, and from 15% in Ge to 12% in Br. The experimental values for Ar (12%) and Kr (10%) are in accord with the trend. The dominant contribution is the transition to quasiatomic orbitals, in contrast with the deeper coexcitation channels in hydride molecules where transition to molecular orbitals prevails.
Found in: osebi
Keywords: X-ray absorption spectra, gaseous hydrides, 3p K-edge spectra, DFT
Published: 05.09.2019; Views: 587; Downloads: 0
.pdf Fulltext (926,96 KB)

87.
In-depth structural characterization and magnetic properties ofquaternary ferrite systems Co0.5Zn0.25M0.25Fe2O4(M¼Ni, Cu, Mn, Mg)
Nataša Novak Tušar, Myrjam Mertens, Aurel Pui, Iztok Arčon, Radu-G. Ciocarlan, Elena M. Seftel, Pegie Cool, 2019, original scientific article

Abstract: This paper investigates the structural and magnetic properties of a mixed series of ferrites having generalformula Co0.5Zn0.25M0.25Fe2O4(M¼Ni, Cu, Mn, Mg). Insights on surface chemistry, structural andmorphological parameters are presented in order to achieve highly tuned ferrite systems with specificcharacteristics. The site occupancy of the cations in the spinel structure was determined using XAS, XRDand Raman spectroscopy. A 100% occupancy of the tetrahedral sites was observed for the Zn cations forall the samples. Co cations occupied the octahedral sites in proportion of 100% for CoeZneCu, CoeZneMg and around 80% for CoeZneNi, CoeZneMn. Ni cations were found only in the octahedral sites,while Cu 80% in the octahedral sites and Mn 60% in the octahedral sites. The cation distribution resultswere correlated with the magnetic properties data. At the same time, not only the cation distribution, butalso the particles size distribution was observed to have a great influence on magnetic and opticalproperties of the ferrites. Given the importance of the surface chemistry of the nanoparticles, XPS and FT-IR analysis were used to prove the functionalization with groups belonging to the surfactant. Moreover,the peculiar behavior of manganese in spinel structures was clarified and the origin of the multiple states(Mn2þand Mn4þ) was elucidated. Finally, parallels have been drawn between the use of different cationsin mixed ferrites in order to gain specific properties.
Found in: osebi
Keywords: FerritesMagnetic propertiesSpinel nanoparticlesX-ray absorption spectroscopyCo-precipitation
Published: 23.10.2019; Views: 626; Downloads: 0
.pdf Fulltext (2,11 MB)

88.
Comparing magnetism in isostructural oxides A[sub](0.8)La[sub](1.2)MnO[sub](4.1)
John E. Greedan, Hanna Dabkowska, Graham King, Christopher Wiebe, Meghan Rutherford, Chad Boyer, Iztok Arčon, Paul A. Dube, Mirela Dragomir, 2019, original scientific article

Abstract: This study presents the strikingly distinct magnetic properties of two isostructural compounds, Ba0.8La1.2MnO4.1 and Sr0.8La1.2MnO4.1 (K2NiF4 type, I4/mmm). Spectroscopic studies have shown that Mn is in a +3.0(1) oxidation state only, in both compounds; therefore, the charge is balanced by accommodating extra oxygen at interstitial sites, as confirmed by neutron powder diffraction. We found that the Ba compound exhibits an exceedingly rare anisotropic spin glass behavior, Tg = 26.4(4) K, with the moment freezing along the c-axis only while the in-plane spin components remain dynamic well below Tg. Experimental results including neutron diffraction, heat capacity, and magnetic (dc and ac) measurements performed on an oriented single crystal support this conclusion. This is a remarkable result, the only other known example of an anisotropic spin glass being Fe2TiO5. The spin glass state in Ba0.8La1.2MnO4.1 is argued to arise due to competing antiferromagnetic and ferromagnetic 180° Mn3+−O−Mn3+ superexchange interactions. In contrast, the Sr analogue shows 2D antiferromagnetic correlations and long-range antiferromagnetic order below 95(1) K with a remarkably reduced ordered moment of 1.449(49) μB/Mn3+ instead of the ∼4 μB expected for an S = 2 ion.
Found in: osebi
Keywords: antiferomagnetiki, Mn XANES, struktura
Published: 23.10.2019; Views: 694; Downloads: 0
.pdf Fulltext (4,14 MB)

89.
Localization, ligand environment, bioavailability and toxicity of mercury in Boletus spp. and Scutiger pes-caprae mushrooms
Anja Kavčič, Klemen Mikuš, Marta Debeljak, Johannes Teun van Elteren, Iztok Arčon, Alojz Kodre, Peter Kump, Andreas-Germanos Karydas, Alessandro Migliori, Mateusz Czyzycki, Katarina Vogel-Mikuš, 2019, original scientific article

Abstract: This study provides information on mercury (Hg) localization, speciation and ligand environment in edible mushrooms: Boletus edulis, B. aereus and Scutiger pes-caprae collected at non-polluted and Hg polluted sites, by LA-ICP-MS, SR-μ-XRF and Hg L3-edge XANES and EXAFS. Mushrooms (especially young ones) collected at Hg polluted sites can contain more than 100 μg Hg g−1 of dry mass. Imaging of the element distribution shows that Hg accumulates mainly in the spore-forming part (hymenium) of the cap. Removal of hymenium before consumption can eliminate more than 50% of accumulated Hg. Mercury is mainly coordinated to di-thiols (43–82%), followed by di-selenols (13–35%) and tetra-thiols (12–20%). Mercury bioavailability, as determined by feeding the mushrooms to Spanish slugs (known metal bioindicators owing to accumulation of metals in their digestive gland), ranged from 4% (S. pes-caprae) to 30% (B. aereus), and decreased with increasing selenium (Se) levels in the mushrooms. Elevated Hg levels in mushrooms fed to the slugs induced toxic effects, but these effects were counteracted with increasing Se concentrations in the mushrooms, pointing to a protective role of Se against Hg toxicity through HgSe complexation. Nevertheless, consumption of the studied mushroom species from Hg polluted sites should be avoided.
Found in: osebi
Keywords: edible mushrooms, HgSe complex, imaging of elemental distribution, LA-ICP-MS, alpha-XRF, XAS
Published: 24.10.2019; Views: 774; Downloads: 0
.pdf Fulltext (1,79 MB)

90.
Mineral element composition in grain of awned and awnletted wheat (Triticum aestivum L.) cultivars tissue-specific iron speciation and phytate and non-phytate ligand ratio
Hiram Castillo Michel, Iztok Arčon, Paula Pongrac, Katarina Vogel-Mikuš, 2020, original scientific article

Abstract: In wheat (Triticum aestivum L.), the awns—the bristle-like structures extending from lemmas—are photosynthetically active. Compared to awned cultivars, awnletted cultivars produce more grains per unit area and per spike, resulting in significant reduction in grain size, but their mineral element composition remains unstudied. Nine awned and 11 awnletted cultivars were grown simultaneously in the field. With no difference in 1000-grain weight, a larger calcium and manganese—but smaller iron (Fe) concentrations—were found in whole grain of awned than in awnletted cultivars. Micro X-ray absorption near edge structure analysis of different tissues of frozen-hydrated grain cross-sections revealed that differences in total Fe concentration were not accompanied by differences in Fe speciation (64% of Fe existed as ferric and 36% as ferrous species) or Fe ligands (53% were phytate and 47% were non-phytate ligands). In contrast, there was a distinct tissue-specificity with pericarp containing the largest proportion (86%) of ferric species and nucellar projection (49%) the smallest. Phytate ligand was predominant in aleurone, scutellum and embryo (72%, 70%, and 56%, respectively), while nucellar projection and pericarp contained only non-phytate ligands. Assuming Fe bioavailability depends on Fe ligands, we conclude that Fe bioavailability from wheat grain is tissue specific.
Found in: osebi
Keywords: biofortification, phytate, iron, awn, X-ray fluorescence, X-ray absorption spectrometry, phosphorus, sulphur, nicotianamine
Published: 16.01.2020; Views: 455; Downloads: 0
.pdf Fulltext (2,63 MB)

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