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11.
Alternative Recovery and Valorization of Metals from Exhausted Catalytic Converters in a New Smart Polymetallic Catalyst
Sebastiano Tieuli, Franco Baldi, Iztok Arčon, Katarina Vogel-Mikuš, Michele Gallo, Laura Sperni, Oreste Piccolo, Stefano Paganelli, 2019, izvirni znanstveni članek

Opis: 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.
Ključne besede: Biogenerated polymetallic exopolysaccharide, biphasic catalysis, hydrogenation, metals-polymeric composite, new catalyst from metallic wastes, EXAFS, XANES
Objavljeno v RUNG: 06.05.2019; Ogledov: 3149; Prenosov: 0
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12.
In-situ XAS analysis of nanoshaped CuO/CeO2 catalysts used for N2O decomposition
Iztok Arčon, Maxim Zabilsky, Petar Djinović, Albin Pintar, 2018, objavljeni povzetek znanstvenega prispevka na konferenci

Opis: The goal of this research is to establish the working state and correlations between atomic structure and catalytic activity of nanoshaped CuO/CeO2 catalysts used in N2O decomposition reaction. The catalysts contained CuO nanoclusters dispersed over different CeO2 morphologies: nano-rods and nano-cubes. N2O is a side product of nitric and adipic acid production and a very potent greenhouse gas that is formed in amounts estimated at about 400 Mt/a of CO2 equivalent. Consequently, the development of robust, active and selective catalysts for N2O decomposition is of a great environmental and economical interest. CeO2-based materials promoted by CuO represent a new class of catalysts that exhibit considerable activity in N2O decomposition reaction between 300 and 500 °C [1-3], and are significantly cheaper and more efficient than Pt, Pd or Rh based catalysts. In order to maximize the efficiency of the catalyst, the active site in this reaction needs to be identified and the mechanism clarified. In-situ Cu K-edge and Ce L3-edge XANES and EXAFS analysis was done on a set of CuO/CeO2 catalysts with different ceria morphology (nano-cubes, nano-rods) and Cu loadings between 2 to 8 wt. %, during N2O decomposition reaction, under controlled reaction conditions at 400 °C. The XAS spectra were measured in-situ, in a tubular reactor, filled with protective He atmosphere at 1 bar, first at RT, then during heating, and at final temperature of 400 °C, during catalytic reaction, when the catalyst was exposed to a small amount (0.2 vol%) of N2O mixed with He. The Cu K-edge and Ce L3-edge XANES and EXAFS analysis reveals changes in valence and local structure of Cu and Ce in the CuO/CeO2 catalysts. In the initial state (in He at RT), copper is present in the form of CuO nanoparticles attached to the CeO2 surface. After heating in He to 400 °C, partial (10%) reduction of Ce [Ce(IV)→Ce(III)] is detected, significant part of Cu(II) is reduced to Cu(I) and Cu(0) species, and direct Cu-Cu bonds are formed. During catalytic N2O decomposition at 400°C, all Ce(III) is oxidized back to Ce(VI), and a major part of Cu is oxidized back to Cu(II), with about 5% of Cu(I) remaining in equilibrium state. Observed structural and valence changes of copper strongly depend on its loading and CeO2 morphology. With systematic In-situ XAS analysis of different nanoshaped CuO/CeO2 catalysts, we identified the structural characteristics and changes of Cu and Ce phases during catalytic N2O decomposition reaction, which could lead to identification of the active catalytic site during the reaction and further improve the performance of these promising catalytic materials.
Ključne besede: EXAFS, CuO/CeO2 catalyst, N2O decomposition
Objavljeno v RUNG: 12.09.2018; Ogledov: 3678; Prenosov: 0
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13.
14.
Diclofenac removal by simulated solar assisted photocatalysis using TiO2-based zeolite catalyst; mechanisms, pathways and environmental aspects
Subhan Salaeh, Daria Juretic Perisic, Martina Biosic, Hrvoje Kušić, Sandra Babich, Urška Lavrenčič Štangar, Dionysios D. Dionysiou, Ana Lončarić Božić, 2016, izvirni znanstveni članek

Opis: The study explores the potential of immobilized TiO2-based zeolite composite photocatalyst (TiO2-FeZ) made of commercial AEROXIDE TiO2 P25 and iron-exchanged zeolite of ZSM5 type (FeZ), for solar assisted treatment of diclofenac (DCF), pharmaceutical included in the ‘‘watch list” during last prioritization in water legislation by EU. In this study the efficiency of applied photocatalytic treatment, solar/TiO2-FeZ/H2O2, of DCF water solution was evaluated on basis of DCF removal and conversion kinetics, as well as the changes of common parameters for assessing water quality. Hence, the changes in the removal and mineralization of overall organic content, biodegradability, toxicity to Vibrio fischeri, dechlorination of DCF and its formed by-products, were monitored during the treatment. The obtained data were correlated with the evolution of DCF by-products, identified and monitored during the treatment by HPLC/MSMS analysis. In order to estimate the influence of water matrix, all experiments were performed in the presence of chloride or sulphate as counter ions. The obtained data revealed that degradation mechanism of DCF by applied treatment process using immobilized TiO2-FeZ includes the adsorption onto photocatalyst surface and consequent degradation. The contribution of homogeneous Fenton reaction due to leached iron ions was found to be negligible. The adsorption and degradation pathway of DCF were influenced by the type of counter ions, which was reflected in the observed changes of water quality parameters.
Ključne besede: Solar photocatalysis, TiO2-FeZ catalyst, Diclofenac, Degradation pathway, Biodegradability, Toxicity
Objavljeno v RUNG: 21.07.2016; Ogledov: 5391; Prenosov: 0
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