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1.
Insight into the interdependence of Ni and Al in bifunctional Ni/ZSM-5 catalysts by Ni K-edge XAS analysis
Iztok 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: 642; Prenosov: 3
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Winning combination of Cu and Fe oxide clusters with an alumina support for low-temperature catalytic oxidation of volatile organic compounds
Tadej 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: 927; Prenosov: 11
.pdf Celotno besedilo (11,05 MB)
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4.
Insight into the interdependence of Ni and Al in bifunctional Ni/ZSM-5 catalysts at the nanoscale
Hue-Tong Vu, Iztok Arčon, Danilo Oliveira de Souza, Simone Pollastri, Goran Dražić, Janez Volavšek, Gregor Mali, Nataša Zabukovec Logar, Nataša Novak Tušar, 2022, izvirni znanstveni članek

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. 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 using Ni K-edge XANES and EXAFS analyses, complemented by XRD and TEM, to resolve 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. Ni species in Ni/ZSM-5 exist as NiO crystals (3–50 nm) and as charge compensating Ni2+ cations. The Ni K-edge 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 ¼ 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, zeolite, Ni XANES, EXAFS
Objavljeno v RUNG: 11.05.2022; Ogledov: 1457; Prenosov: 42
.pdf Celotno besedilo (1,25 MB)
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5.
SnO2-Containing Clinoptilolite as a Composite Photocatalyst for Dyes Removal fromWastewater under Solar Light
Andraž Šuligoj, Jelena Pavlovič, Iztok Arčon, Nevenka Rajić, Nataša Novak Tušar, 2020, izvirni znanstveni članek

Opis: Due to their adsorbent, ion exchange and catalytic properties zeolites are suitable for a variety of applications. We report on the photocatalytic activity of a readily available and inexpensive natural zeolite clinoptilolite (Z) containing SnO2 (Sn-Z). The Sn-Z samples with 3–15 wt. % of Sn were prepared by using a precipitation–deposition method. Powder X-ray diffraction analysis showed that the zeolite structure was unaffected by the introduction of the Sn-phase. Diffuse reflectance UV/VIS spectra of the Sn-Z samples confirmed the presence of SnO2 and X-Ray absorption spectroscopy analyses suggested that the SnO2 particles mainly resided on the surface of the clinoptilolite, while ATR-FTIR analysis gave some clues that part of the SnO2 phase was incorporated in the pores of the zeolite. The presence of SnO2 in Sn-Z increased both adsorption capacity and photocatalytic performance which could be partially explained by higher surface area and partially with an increased negative potential of the surface. Adsorption and total degradation of methylene blue (MB) for the Sn-Z with the highest amount of Sn (15 wt.%) was about 30% and 45%, respectively, suggesting a synergetic effect between SnO2 and the clinoptilolite lattice. Reusability tests showed that these catalysts present a promising material for water purification.
Ključne besede: SnO2, zeolite, SnO2-clinoptilolite composite, photocatalysis, solar light, methylene blue removal, wastewater treatment
Objavljeno v RUNG: 25.02.2020; Ogledov: 2887; Prenosov: 131
.pdf Celotno besedilo (3,50 MB)

6.
In-depth structural characterization and magnetic properties ofquaternary ferrite systems Co0.5Zn0.25M0.25Fe2O4(M¼Ni, Cu, Mn, Mg)
Radu-G. Ciocarlan, Iztok Arčon, Aurel Pui, Myrjam Mertens, Nataša Novak Tušar, Elena M. Seftel, Pegie Cool, 2019, izvirni znanstveni članek

Opis: 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.
Ključne besede: FerritesMagnetic propertiesSpinel nanoparticlesX-ray absorption spectroscopyCo-precipitation
Objavljeno v RUNG: 23.10.2019; Ogledov: 3126; Prenosov: 0
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7.
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, izvirni znanstveni članek

Opis: 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).
Ključne besede: MnS-1 Nanocrystals, Mn XANES, EXAFS, zeolites, microwave-assisted hydrothermal synthesis
Objavljeno v RUNG: 06.05.2019; Ogledov: 3277; Prenosov: 0
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8.
Cu and Zr surface sites in photocatalytic activity of TiO [sub] 2 nanoparticles : the effect of Zr distribution
Olena Pliekhova, O. L. Pliekhov, Mattia Fanetti, Iztok Arčon, Nataša Novak Tušar, Urška Lavrenčič Štangar, 2019, izvirni znanstveni članek

Opis: The present work is focused on the role of ZrO2 modification in the performance of CuO modified TiO2. Zirconia loading leads to formation of more resistant photocatalytic layers compared to samples modified with only copper containing species. Surface modification of mixed phase TiO2 with CuO/ZrO2 improves the degradation of Reactive blue 19 dye under simulated solar irradiation. An in-depth investigation of the catalysts showed that in case of CuO/ZrO2 modification, the covering of the TiO2 surface with zirconium containing species prevents morphological and harmful energetic changes induced by copper species formed on the rutile TiO2 phase at a higher copper loading.
Ključne besede: titanium dioxide, surface modification, XAS analysis, surface acidity, Hammett indicators
Objavljeno v RUNG: 26.03.2019; Ogledov: 3101; Prenosov: 0
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9.
MOŽNOSTI ZMANJŠANJA ODPADKOV HRANE V SLOVENIJI: PRIMER MLEČNIH IZDELKOV
Boštjan Gerbec, 2018, magistrsko delo

Opis: V magistrskem delu smo obravnavali problematiko zavržene hrane v Slovenji ter širše. V Sloveniji vsako leto zavržemo 73 kilogramov hrane na prebivalca, podatki zadnjih let pa kažejo na naraščanje teh količin. Polovico zavržene hrane ustvarijo gospodinjstva. Ker je hrana nepogrešljiva za življenje, veliko ljudi pa živi v pomankanju, je takšno stanje zaskrbljujoče in nas kot družbo ne prikazuje v najboljši luči. Pri razumevanju problema in pri iskanju rešitev smo poleg pregleda zakonodaje in znanstvene literature izvedeli tudi raziskavo na primeru mlečnih izdelkov. Uporabili smo tri raziskovalne pristope: anketo, intervju ter eksperiment s preizkusom izdelka. Ugotovili smo, da je literatura v večini dostopna le v obliki znanstvenih člankov in študij, prav tako še do nedavnega ni bilo sistematičnega zbiranja in vodenja evidenc o količinah zavržene hrane. V nalogi smo predlagali ukrepe in načine, kako bi lahko zmanjšali količino zavržene hrane, in izpostavili velik pomen tega, da vsak posameznik začne pri sebi. Ustrezno je treba nakupovati hrano, planirati obroke ter hrano tudi pravilno shranjevati. V nalogi smo tudi predstavili različne primere dobrih praks, ki prav tako pomagajo zmanjševati količino zavržene hrane, bodisi v Sloveniji bodisi v tujini. V nalogi smo potrdili hipotezo, ki smo jo izpostavili na začetku, da se lahko količina zavržene hrane v Slovenji zmanjša. Potrošniki lahko na to neposredno vplivamo v domačih gospodinjstvih. S spremembami nakupovalnih navad pa lahko v določeni meri vplivamo tudi na trgovce in na njihovo ponudbo živil. Na problem hrane, ki se izgublja v proizvodnem in distribucijskem delu življenjskega cikla, pa v širšem smislu lahko vplivajo tako vlade vseh držav kot tudi mednarodna skupnost.
Ključne besede: zavržena hrana, zakonodaja, gospodinjstva, primer zavrženih mlečnih izdelkov, zmanjševanje odpadne hrane z ozaveščanjem, zmanjševanje odpadne hrane z državnimi politikami
Objavljeno v RUNG: 14.09.2018; Ogledov: 4352; Prenosov: 182
.pdf Celotno besedilo (1,96 MB)

10.
The effect of Zr loading on photocatalytic activity of Cu modified TiO [sub] 2
Olena Pliekhova, O. L. Pliekhov, Mattia Fanetti, Iztok Arčon, Nataša Novak Tušar, Urška Lavrenčič Štangar, 2018, objavljeni povzetek znanstvenega prispevka na konferenci

Ključne besede: Cu Zr modified TiO2, EXAFS, XANES
Objavljeno v RUNG: 12.09.2018; Ogledov: 3327; Prenosov: 0
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