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1.
Surface modified titanium dioxide using transition metals
Andraž Šuligoj, Iztok Arčon, Matjaž Mazaj, Goran Dražić, Denis Arčon, Pegie Cool, Urška Lavrenčič Štangar, Nataša Novak Tušar, 2018, izvirni znanstveni članek

Opis: Titanium dioxide has been widely used as an antimicrobial agent, UV-filter and catalyst for pollution abatement. Herein, surface modifications with selected transition metals (Me) over colloidal TiO2 nanoparticles and immobilization with a colloidal SiO2 binder as composite films (MeTiO2/SiO2) on a glass carrier were used to enhance solar-light photoactivity. Colloidal TiO2 nanoparticles were modified by loading selected transition metals (Me ¼ Mn, Fe, Co, Ni, Cu, and Zn) in the form of chlorides on their surface. They were present primarily as oxo-nanoclusters and a portion as metal oxides. The structural characteristics of bare TiO2 were preserved up to an optimal metal loading of 0.5 wt%. We have shown in situ that metal-oxo-nanoclusters with a redox potential close to that of O2/O2  were able to function as co-catalysts on the TiO2 surface which was excited by solar-light irradiation. The materials were tested for photocatalytic activity by two opposite methods; one detecting O2  (reduction, Rz ink test) while the other detecting OH (oxidation, terephthalic acid test). It was shown that the enhancement of the solar-light activity of TiO2 by the deposition of transition metal oxo-nanoclusters on the surface depends strongly on the combination of the reduction potential of such species and appropriate band positions of their oxides. The latter prevented excessive self-recombination of the photogenerated charge carriers by the nanoclusters in Ni and Zn modification, which was probably the case in other metal modifications. Overall, only Ni modification had a positive effect on solar photoactivity in both oxidation and reduction reactions.
Najdeno v: osebi
Ključne besede: surface modified TiO2, XANES, EXAFS, Nickel, solar light photocatalyst
Objavljeno: 01.06.2018; Ogledov: 370; Prenosov: 0
.pdf Polno besedilo (1,24 MB)

2.
Unraveling the arrangement of Al and Fe within the framework explains the magnetism of mixed-metal MIL-100(Al,Fe)
Gregor Mali, Matjaž Mazaj, Iztok Arčon, Darko Hanžel, Denis Arčon, Zvonko Jagličić, 2019, izvirni znanstveni članek

Opis: Properties of mixed-metal MOFs depend on the distribution of different metals within their frameworks. Determination of this distribution is often very challenging. Using an example of aluminum- and iron-containing MIL-100, we demonstrate that 27Al NMR spectroscopy, when combined with first-principles calculations and magnetic, X-band electron paramagnetic resonance, Fe K-edge extended X-ray absorption fine structure, and Mössbauer measurements, enables one to accurately determine the arrangement of Al and Fe within the metal trimers, which are the basic building units of MIL-100. In this particular material, the incorporation of Fe and Al on the framework metal sites is random. Crucial for deciphering the arrangement is detecting NMR signals, shifted because of the strong hyperfine interaction between the 27Al nuclei and the unpaired electronic spins of Fe3+ ions, assigning the shifted signals aided by first-principles calculations of hyperfine couplings, and quantitatively evaluating the NMR intensities and the measured effective magnetic moment.
Najdeno v: osebi
Ključne besede: Fe EXAFS, XANES, MIL100, MOF, magnetizem
Objavljeno: 26.03.2019; Ogledov: 156; Prenosov: 0
.pdf Polno besedilo (2,57 MB)

3.
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).
Najdeno v: osebi
Ključne besede: MnS-1 Nanocrystals, Mn XANES, EXAFS, zeolites, microwave-assisted hydrothermal synthesis
Objavljeno: 06.05.2019; Ogledov: 107; Prenosov: 0
.pdf Polno besedilo (9,33 MB)

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