1. Synthesis of helional by hydrodechlorination reaction in the presence of mono- and bimetallic catalysts supported on aluminaOreste Piccolo, Iztok Arčon, Das Gangadhar, Giuliana Aquilanti, Andrea Prai, Stefano Paganelli, Manuela Facchin, Valentina Beghetto, 2024, izvirni znanstveni članek Opis: Hydrodechlorination reaction of 3-(benzo-1,3-dioxol-5-yl)-3-chloro-2-methylacrylaldehyde in the presence of different low metal content heterogeneous mono- or bimetallic catalysts was tested for the synthesis of the fragrance Helional® (3-[3,4-methylendioxyphenyl]-2-methyl-propionaldehyde). In particular, mono Pd/Al2O3, Rh/Al2O3 or bimetallic Pd-Cu/Al2O3, Rh-Cu/Al2O3 catalysts were tested in different reaction conditions from which it emerged that mono-Rh/Al2O3 was the best performing catalyst, allowing achievement of 100% substrate conversion and 99% selectivity towards Helional® in 24 h at 80 °C, p(H2) 1.0 MPa in the presence of a base. To establish correlations between atomic structure and catalytic activity, catalysts were characterized by Cu, Rh and Pd K-edge XANES, EXAFS analysis. These characterizations allowed verification that the formation of Pd-Cu alloys and the presence of Cu oxide/hydroxide species on the surface of the Al2O3 support are responsible for the very low catalytic efficiency of bimetallic species tested.
Ključne besede: selective hydrodechlorination, heterogeneous catalysis, XANES analysis, EXAFS analysis
Objavljeno v RUNG: 25.04.2024; Ogledov: 15; Prenosov: 0
 Celotno besedilo (446,63 KB)
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2. A Biogenerated Polymetallic Catalyst from Society's WastesOreste Piccolo, Stefano Paganelli, Petro Zanatta, Sebastiano Tieuli, Laura Sperni, Franco Baldi, Iztok Arčon, Michele Gallo, Katarina Vogel-Mikuš, 2019, izvirni znanstveni članek Opis: 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
Ključne besede: Metals
-
polymeric composite, biogenerated polymetallic exopolysaccharide, new catalyst
from metallic wastes, hydrodechlorination
of PCBs in water
Objavljeno v RUNG: 06.05.2019; Ogledov: 3327; Prenosov: 0
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3. Alternative Recovery and Valorization of Metals from Exhausted Catalytic Converters in a New Smart Polymetallic CatalystSebastiano 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: 3210; Prenosov: 0
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4. XAS and micro-XRF analysis of mono and bi-metallic exopolysaccharide (FePd-EPS) bio-generated by K. oxytocaIztok Arčon, Stefano Paganelli, Oreste Piccolo, Michele Gallo, Katarina Vogel-Mikuš, Franco Baldi, 2016, objavljeni povzetek znanstvenega prispevka na konferenci Opis: Bacteria Klebsiella oxytoca (DSM 29614) secret a specific exopolysaccharide (EPS) in the presence of Fe(III)-citrate, as sole carbon and energy source, and produces after 7 days an iron gel precipitate (Fe-EPS) [1]. In the presence of palladium or other metal species, the culture of K. oxytoca can produce other mono or bimetal species (Pd-EPS, FePd-EPS) [2]. These bio-materials may be used as green biogenerated catalysts or for other biotechnological purposes. In this work we present the analysis of the morphology and the chemical state of the metals in mono and bi-metallic (Fe-EPS, Pd-EPS, FePd-EPS) complexes, by a combination of micro X-ray fluorescence, X-ray absorption spectroscopy methods (XANES and EXAFS), and transmission electron microscopy. The results show that iron in monometallic Fe-EPS and bimetalic FePd-EPS is in the mineralized form of iron oxides/hydroxides, predominantly in the form of Fe3+, with a small amount of Fe2+ in the structure, as a mixture of different nano-crystalline iron oxides and hydroxides. Palladium on the other hand is found as Pd(0) in the form of metallic nanoparticles with fcc structure in both, bi-metallic (FePd-EPS) and mono-metallic (Pd-EPS) species. In bi-metallic species Pd and Fe nanoparticles agglomerate in larger clusters, but they remain spatially separated. Access to the SR facilities at ESRF (beamline ID21, project LS-2225), DESY (beamline C) Hamburg (project I-20110511 EC) and ELETTRA (beamline XAFS, project 20115112) is acknowledged.
Ključne besede: Klebsiella oxytoca, Fe, Pd, XANES, EXAFS, exopolysaccharide, FePd-EPS
Objavljeno v RUNG: 28.06.2016; Ogledov: 5546; Prenosov: 0
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