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13. Insight into the interdependence of Ni and Al in bifunctional Ni/ZSM-5 catalysts by Ni K-edge XAS analysisIztok Arčon, Hue-Tong Vu, Goran Dražić, Janez Volavšek, Gregor Mali, Nataša Zabukovec Logar, Nataša Novak Tušar, 2023, objavljeni povzetek znanstvenega prispevka na konferenci Opis: Catalyst design is crucial for improving catalytic activity and product selectivity. In a bifunctional Ni/ZSM-5
zeolite type catalyst, catalytic properties are usually tuned via varying Al and Ni contents [1]. While changes in
acid properties associated with Al sites are usually closely investigated, Ni phases, however, receive inadequate
attention. Herein, we present a systematic structural study of Ni in the Ni/ZSM-5 materials by Ni K-edge
XANES (X-ray absorption near edge structure) and EXAFS (extended X-ray absorption fine structure) analyses,
to monitor the local structure and chemical state of Ni species in the catalysts. In combination with XRD and
TEM we resolved the changes in the local environment of Ni species induced by the different Al contents of
the parent ZSM-5 prepared by a “green”, template free technique [2].
Ni species in Ni/ZSM-5 exist as NiO crystals (3–50 nm) and as charge compensating Ni2+ cations. The Ni Kedge
XANES and EXAFS results enabled the quantification of Ni-containing species. At a low Al to Si ratio
(nAl/nSi < 0.04), the NiO nanoparticles predominate in the samples and account for over 65% of Ni phases.
However, NiO is outnumbered by Ni2+ cations attached to the zeolite framework in ZSM-5 with a high Al to Si
ratio (nAl/nSi = 0.05) due to a higher number of framework negative charges imparted by Al. The obtained
results show that the number of highly reducible and active NiO crystals is strongly correlated with the
framework Al sites present in ZSM-5 zeolites, which depend greatly on the synthesis conditions. Therefore,
this kind of study is beneficial for any further investigation of the catalytic activities of Ni/ZSM-5 and other
metal-modified bifunctional catalysts.
Ključne besede: Ni/ZSM-5 catalysts, Ni EXAFS, XANES
Objavljeno v RUNG: 19.09.2023; Ogledov: 1470; Prenosov: 5
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14. Periodic anti-phase boundaries and crystal superstructures in ▫$PtCu_3$▫ nanoparticles as fuel cell electrocatalystsAna Rebeka Kamšek, Anton Meden, Iztok Arčon, Primož Jovanovič, Martin Šala, Francisco Ruiz-Zepeda, Goran Dražić, Miran Gaberšček, Marjan Bele, Nejc Hodnik, 2023, izvirni znanstveni članek Objavljeno v RUNG: 19.09.2023; Ogledov: 1528; Prenosov: 9
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15. Saturation magnetisation as an indicator of the disintegration of barium hexaferrite nanoplatelets during the surface functionalisationDarja Lisjak, Iztok Arčon, Matic Poberžnik, Gabriela Herrero‑Saboya, Ali Tufani, Andraž Mavrič, Matjaž Valant, Patricija Hribar Boštjančič, Alenka Mertelj, Darko Makovec, Layla Martin‑Samos, 2023, izvirni znanstveni članek Opis: Barium hexaferrite nanoplatelets (BHF NPLs) are permanent nanomagnets with the magnetic easy axis aligned perpendicular to their basal plane. By combining this specific property with optimised surface chemistry, novel functional materials were developed, e.g., ferromagnetic ferrofluids and porous nanomagnets. We compared the interaction of chemically different phosphonic acids, hydrophobic and hydrophilic with 1–4 phosphonic groups, with BHF NPLs. A decrease in the saturation magnetisation after functionalising the BHF NPLs was correlated with the mass fraction of the nonmagnetic coating, whereas the saturation magnetisation of the NPLs coated with a tetraphosphonic acid at 80 °C was significantly lower than expected. We showed that such a substantial decrease in the saturation magnetisation originates from the disintegration of BHF NPLs, which was observed with atomic-resolution scanning transmission electron microscopy and confirmed by a computational study based on state-of-the-art first-principles calculations. Fe K-edge XANES (X-ray absorption near-edge structure) and EXAFS (Extended X-ray absorption fine structure) combined with Fourier-transformed infrared (FTIR) spectroscopy confirmed the formation of an Fe–phosphonate complex on the partly decomposed NPLs. Comparing our results with other functionalised magnetic nanoparticles confirmed that saturation magnetisation can be exploited to identify the disintegration of magnetic nanoparticles when insoluble disintegration products are formed.
Ključne besede: barium hexaferrite, Fe XANES, EXAFS, magnetic nanoparticles
Objavljeno v RUNG: 06.07.2023; Ogledov: 2051; Prenosov: 7
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16. Multicomponent Cu-Mn-Fe silica supported catalysts to stimulate photo-Fenton-like water treatment under sunlightAndraž Šuligoj, Ivalina Trendafilova, Ksenija Maver, Albin Pintar, Alenka Ristić, Goran Dražić, Wael H. M. Abdelraheem, Zvonko Jagličić, Iztok Arčon, Nataša Zabukovec Logar, Dionysios D. Dionysiou, Nataša Novak Tušar, izvirni znanstveni članek Ključne besede: Magnetic catalyst, Photocatalyst, Water treatment, Sunlight, Contaminants of emerging concern, Photo-Fenton-like systems, Cu, Mn, Fe, XANES, EXAFS
Objavljeno v RUNG: 06.07.2023; Ogledov: 2117; Prenosov: 9
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17. Winning combination of Cu and Fe oxide clusters with an alumina support for low-temperature catalytic oxidation of volatile organic compoundsTadej Žumbar, Iztok Arčon, Petar Djinović, Giuliana Aquilanti, Gregor Žerjav, Albin Pintar, Alenka Ristić, Goran Dražić, Janez Volavšek, Gregor Mali, Margarita Popova, Nataša Zabukovec Logar, Nataša Novak Tušar, 2023, izvirni znanstveni članek Opis: A γ-alumina support functionalized with transition metals is one of the most widely used industrial catalysts for the total oxidation of volatile organic compounds (VOCs) as air pollutants at higher temperatures (280−450 °C). By rational design of a
bimetal CuFe-γ-alumina catalyst, synthesized from a dawsonite alumina precursor, the activity in total oxidation of toluene as a model VOC at a lower temperature (200−380
°C) is achieved. A fundamental understanding of the catalyst and the reaction mechanism is elucidated by advanced microscopic and spectroscopic characterizations as well as by temperature-programmed surface techniques. The nature of the metal−support bonding and the optimal abundance between Cu−O−Al and Fe−O−Al species in the catalysts leads to synergistic catalytic activity promoted by small amounts of iron (Fe/Al = 0.005).
The change in the metal oxide−cluster alumina interface is related to the nature of the
surfaces to which the Cu atoms attach. In the most active catalyst, the CuO6 octahedra are
attached to 4 Al atoms, while in the less active catalyst, they are attached to only 3 Al atoms. The oxidation of toluene occurs via the Langmuir−Hinshelwood mechanism. The presented material introduces a prospective family of low-cost and scalable oxidation catalysts with superior efficiency at lower temperatures.
Ključne besede: Iron oxide clusters, copper oxide clusters, alumina support, synergistic effect, low-temperature total catalytic oxidation, toluene, Cu, Fe XANES, EXAFS
Objavljeno v RUNG: 06.07.2023; Ogledov: 2165; Prenosov: 26
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18. Selenium affects mercury ligand environment in terrestrial food chain – a XAS studyKatarina Vogel Mikuš, Alojz Kodre, Iztok Arčon, Anja Kavčič, 2022, objavljeni povzetek znanstvenega prispevka na konferenci Opis: Selenium (Se) supplied in inorganic form (as selenate or selenite) was shown to decrease mercury (Hg) toxicity by forming HgSe in soils as well as in animal and human tissues, while for plants there is no evidence of Hg-Se complexation. Although Se in not an essential element for plants it was shown to counteract various abiotic stresses when applied at trace amounts. The aim of this work was therefore to study physiological responses and Hg speciation in plant/ fungi-animal food chain. Lettuce (Lactuca sativa) and porcini mushrooms (Boletus edulis) were taken as model plant/ fungal species and Spanish slug (Arion vulgaris) as a model animal species. The plants, fed to the slugs, were grown in HgCl2 contaminated soil or soil from the vicinity of Hg mine in Idrija with traces of HgS and methyl Hg). Physiological parameters of plants and slugs were monitored during the experiment. At the end the biological material was frozen in LN2 and freeze dried. Hg L3-edge (12284 eV) XANES and EXAFS spectra of the biological samples and standards were measured at liquid helium temperature in fluorescence detection mode at the BM30B beamline of the ESRF synchrotron in Grenoble, using the 30-segment germanium solid state detector [1]. The results showed that addition of Se alleviated Hg toxic effects in the food chain started at HgCl2-contaminated soil, while for the soil from Idrija, containing low amounts of highly toxic methyl-Hg, the beneficial effect was less prominent [2]. No Hg-Se complexes were detected in plants, while in mushrooms and slugs the complexation was confirmed. Addition of Se to the plants, however, changed Hg ligand environment in plant tissues from sulphur to nitrogen ligands. Hg and Se both target the -SH functional groups in the plant tissues, so toxic effects of Hg are rather enhanced than alleviated by addition of Se. Nevertheless, the addition of Se to the plants is beneficial for higher trophic levels and lowers Hg toxicity for the primary consumers, the slugs.
Ključne besede: mercury, toxicity, ligand environment, XANES, EXAFS, food chain, plant, slug, fungi
Objavljeno v RUNG: 05.12.2022; Ogledov: 1951; Prenosov: 0
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19. IZVOZ VIN KLETI BRDA, Z. O. O., V ZADNJIH DVAJSETIH LETIHTereza Valentinčič, 2022, diplomsko delo Opis: Izvoz je postal zelo pomemben vir prihodkov in nič drugače ni tudi za vino. Slovenska vina so vedno bolj prepoznavna na vinskem zemljevidu in vedno več držav si želi uvažati slovenska vina, zato ni čudno, da so slovenski vinarji na tujih trgih vedno bolj uspešni. Največja izvoznica slovenskih vin je Klet Brda, z. o. o, ki izvaža v že kar 26 držav po svetu. V diplomskem delu se posvetimo izvozu Kleti Brda in izpostavimo tri največje države, v katere izvaža in so si med seboj različne. To so Združene države Amerike, Kitajska in Velika Britanija. Kaj je pomembno, da je izvoz uspešen in kakšna komunikacija je potrebna, da je prodaja uspešna? Skozi intervjuje, ki smo jih opravili z zaposlenimi v Kleti Brda, smo spoznali potek in delo, ki smo ga v diplomskem delu tudi opisali. Izpostavili smo razlike med državami in kakšne metode se uporabljajo, da je prodaja na določenem trgu uspešna. Skozi delo spoznamo, kako poteka izvoz v kleti in kako se je v zadnjih dvajsetih letih spreminjal.
Ključne besede: izvoz, Klet Brda, z. o. o, Združene države Amerike, Kitajska, Velika Britanija
Objavljeno v RUNG: 04.11.2022; Ogledov: 1967; Prenosov: 39
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20. Monitoring chemical processes in (photo)catalysts and energy storage materials by operando X-ray absorption spectroscopyIztok Arčon, 2022, objavljeni povzetek znanstvenega prispevka na konferenci (vabljeno predavanje) Opis: X-ray absorption spectroscopy (XAS) is a powerful tool for characterisation of local structure and chemical state of selected elements in different new functional materials and biological or environmental samples. The XAS spectroscopy is based on extremely bright synchrotron radiation X-rays sources, which allow precise characterisation of bulk, nanostructured or highly diluted samples. The rapid development of extremely bright synchrotron sources of X-ray and ultraviolet light in recent years has opened new possibilities for research of matter at the atomic or molecular level, indispensable in the development of new functional nanostructured materials with desired properties. The talk will present the possibilities offered by X-ray absorption spectroscopy with synchrotron light for ex-situ or operando characterization of various functional porous and other nanomaterials, before, after and during their operation [1,2,3,4]. New generation of synchrotron light sources also opened the possibility of combining X-ray absorption with high-resolution emission [5] and inelastic scattering spectroscopy [6], and microscopy with sub-micron resolution [7]. Examples of operando XANES and EXAFS analysis to track changes in the valence states and local structures of selected elements in different energy storage materials and in various (photo)catalysts, during chemical reactions under controlled reaction conditions, will be presented, which provided insight into the dynamic functional properties and reaction mechanisms of these materials. Access to SR facilities of Petra III (beamlines P65, P64 and P01), ESRF (beamlines BM23, ID21, ID26) and Elettra (beamlines XAFS, XRF), for the presented research is kindly acknowledged.
Ključne besede: X-ray absorption spectroscopy, operando XANES, EXAFS, catalysts, batteries
Objavljeno v RUNG: 07.10.2022; Ogledov: 1629; Prenosov: 0
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