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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: 75; Prenosov: 0
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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: 303; Prenosov: 1
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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: 369; Prenosov: 4
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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: 681; Prenosov: 16
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Opis: The effect of different water matrices on the photocatalytic degradation of dissolved pharmaceuticals was explored. The focus was on the degradation efficiencies in wastewater effluent from a bioreactor and water effluent from a central wastewater treatment plant and comparing the results with degradation in deionized H2O. The compounds tested included: oxytetracycline, marbofloxacin, ibuprofen, diclofenac, phenytoin, ciprofloxacin, sulfamethoxazole. For the experiments performed in this study, a compact packed-bed photocatalytic reactor was used in which the hybrid TiO2 photocatalyst (sol-gel/P25) was deposited on ~3 mm glass beads. As expected, the reactions proceed more slowly in wastewater than in deionized water, yet it is shown that removal of the compounds from the water is still possible even when other organic molecules are present. Total organic carbon measurements have shown that complete mineralization takes place albeit at slower rates than the initial degradation of parent compounds. The results show that an acidic pH can increase the reaction rates and the adsorption on the photocatalyst surface. Analyses of the degradation intermediates were performed using tandem liquid chromatography triple-quadrupole mass spectrometry system. Additionally, X-ray absorption spectroscopy was applied to get insight into the local structure of the photocatalyst before and after use. Understanding the effects that different wastewater compositions have on photocatalytic reactions will help to refine the potential applications of the technology.
Ključne besede: titanium dioxide, sol-gel processes, functionla applications, water treatment
Objavljeno v RUNG: 30.09.2022; Ogledov: 667; Prenosov: 0
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