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Olena Pliekhova, 2019, doktorska disertacija

Opis: This work entitled «Zr/Cu-TiO2 catalysts for photocatalytic water treatment» tackles a problem of tons of dyes discharged everyday mainly from textile industries. This is a huge concern because of dyes persistence, toxicity and potential to the bioaccumulation in living organisms. Here, a small contribution to overall problem is presented. The research work consists of three main parts: Theoretical background, Experimental and Results and discussion. In the Theoretical background chapter the overall problem is identified and discussed. The main water treatment techniques are presented briefly with their advantages and drawbacks. Photocatalysis assisted with TiO2 is shown as an alternative additional technique with its own pros and cons. Further, a cursory overview of TiO2 modification techniques is made and advantages in using copper and zirconium oxides for TiO2 modification are presented. The reason and possible positive effect of using of two oxides simultaneously for TiO2 modification is indicated. Additionally, a positive impact of solar light for overall rate of dyes degradation assisted with TiO2 is discussed. Within the framework of photosensitization effect, the problem of using dyes for assessment of photocatalytic properties of materials under the visible light is touched on. Photothermal methods as possible beneficial techniques for this purpose are proposed. In the Experimental chapter, all experimental techniques used in current research work with the technical details specific for the research work are presented. There are methods of materials preparation, photocatalytic tests under different conditions and varying model pollutants, and physico-chemical characterization techniques. The Results and discussion chapter is divided by three subchapters. Each chapter is dedicated to one hypothesis, which was checked and confirmed or disproved. The first hypothesis is about beneficial loading of copper and zirconium oxides to TiO2. After numerous experiments held, it was concluded that the pair of copper and zirconium oxides is beneficial for simultaneous application on TiO2 surface to promote its performance. The second subchapter is about zirconium distribution and its impact on the activity of studied materials towards the antraquinone dye Reactive Blue 19. Different techniques such as XRD, TEM, EXAFS and many others were used in order to characterize the materials and to understand the details of the processes taking place. The existence of upper limit of copper oxide loading for its beneficial effect on TiO2 performance was demonstrated. It was observed that zirconium species loading leads to improvement in performance of materials with higher copper loading, which otherwise lowers activity of TiO2 – this is in case when copper only above its optimal level is present. It was concluded that zirconium oxide containing species occupy rutile surface sites in mixed phase TiO2 and this way beneficially influence the material performance towards the dye removal. The third subchapter is about the visible light TiO2 assisted dye degradation. It is well known that photosensitization mechanism of dye degradation appears under the visible and as a consequence under the solar light irradiation. This leads to the overall enhancement of dyes degradation, which is positive and may be used as a benefit for faster pollutant destruction. However, this fact leads to mishmash in the determination of real photocatalytic activity of materials towards the dye. It was hypothesized that the impact of photosensitization mechanism on the overall material performance against Reactive blue 19 dye (RB19) descends with the dye concentration lowering. Thermal lens spectrometry (TLS) which is sensitive to chemicals at low concentrations was used for hypothesis evaluation. To summarize the research work achievements, the conclusions of the thesis are given at the end.
Ključne besede: titanium dioxide, photocatalysis, zirconium/copper, surface modification, water treatment, dyes
Objavljeno v RUNG: 03.12.2019; Ogledov: 5667; Prenosov: 134
.pdf Celotno besedilo (3,18 MB)

The effect of Zr loading on photocatalytic activity of Cu modified TiO2
Olena Pliekhova, O. L. Pliekhov, Mattia Fanetti, Iztok Arčon, Nataša Novak Tušar, Urška Lavrenčič Štangar, 2018, objavljeni znanstveni prispevek na konferenci

Ključne besede: Titanium diokside, acidic sites, surface titration, copper, zirconium
Objavljeno v RUNG: 10.09.2018; Ogledov: 3730; Prenosov: 0
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Photocatalytic Activity of Zirconium- and Manganese- Codoped Titania in Aqueous Media: The Role of the Metal Dopant and its Incorporation Site
O. L. Pliekhov, Iztok Arčon, Nataša Novak Tušar, Urška Lavrenčič Štangar, 2016, izvirni znanstveni članek

Opis: The development of efficient TiO2-based photocatalysts for water treatment is mainly performed by doping with transition metals or by establishing junctions between different phases, metal–semiconductor or semiconductor–semiconductor. We present, for the first time, the synthesis of Zr- and Mn-modified TiO2 by a redesigned sol–gel technique that allows the formation of heterometallic bridges on the TiO2 surface. Cations of the doping metals are located in the pores of mesoporous anatase and attached to the crystalline TiO2 walls. The presence of the Zr enhances the photoactivity of the TiO2 catalyst. However, the introduction of Mn decreases the photocatalytic efficiency in a nonadditive manner. The inhibition effect was assigned to the side reaction between hydroxyl radicals and Mn ions. The fact that Mn effectively scavenges the hydroxyl radicals and, consequently, inhibits the whole oxidation process is direct proof that hydroxyl radicals are the main reactive species in the photocatalytic oxidative processes on TiO2 surfaces in aqueous media and the process of COH generation is the rate-determining step, which was confirmed using a method based on the decolorization of a commercial dye Bezaktiv Blau in a reaction with Fenton’s reagent as a source of hydroxyl radicals.
Ključne besede: doping, manganese, oxidation, X-ray absorption spectroscopy, zirconium
Objavljeno v RUNG: 21.07.2016; Ogledov: 4031; Prenosov: 0
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