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Photocatalytic sol-gel/P25 TiO [sub] 2 coatings for water treatment : degradation of 7 selected pharmaceuticals (CO3:IL02)
Lev Matoh, Boštjan Žener, Marin Kovačić, Hrvoje Kušić, Iztok Arčon, Meta Levstek, Urška Lavrenčič Štangar, 2022, izvirni znanstveni članek

Opis: The effect of different water matrices on the photocatalytic degradation of dissolved pharmaceuticals was explored. The focus was on the degradation efficiencies in wastewater effluent from a bioreactor and water effluent from a central wastewater treatment plant and comparing the results with degradation in deionized H2O. The compounds tested included: oxytetracycline, marbofloxacin, ibuprofen, diclofenac, phenytoin, ciprofloxacin, sulfamethoxazole. For the experiments performed in this study, a compact packed-bed photocatalytic reactor was used in which the hybrid TiO2 photocatalyst (sol-gel/P25) was deposited on ~3 mm glass beads. As expected, the reactions proceed more slowly in wastewater than in deionized water, yet it is shown that removal of the compounds from the water is still possible even when other organic molecules are present. Total organic carbon measurements have shown that complete mineralization takes place albeit at slower rates than the initial degradation of parent compounds. The results show that an acidic pH can increase the reaction rates and the adsorption on the photocatalyst surface. Analyses of the degradation intermediates were performed using tandem liquid chromatography triple-quadrupole mass spectrometry system. Additionally, X-ray absorption spectroscopy was applied to get insight into the local structure of the photocatalyst before and after use. Understanding the effects that different wastewater compositions have on photocatalytic reactions will help to refine the potential applications of the technology.
Ključne besede: titanium dioxide, sol-gel processes, functionla applications, water treatment
Objavljeno v RUNG: 30.09.2022; Ogledov: 1143; Prenosov: 0
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3.
Zr/Cu-TiO2 CATALYSTS FOR PHOTOCATALYTIC WATER TREATMENT
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: 5795; Prenosov: 135
.pdf Celotno besedilo (3,18 MB)

4.
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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5.
Correlations between photocatalytic activity and chemical structure of Cu-modified TiO2-SiO2 nanoparticle composites
T. Čižmar, doktorska disertacija

Opis: The objective of this dissertation was to examine how copper modification can improve the photocatalytic activity of TiO2-SiO2 and to explain the correlation between Cu concentration and chemical state of Cu cations in the TiO2-SiO2 matrix, as well as the photocatalytic activity under the UV/solar irradiation. The Cu-modified TiO2-SiO2 photocatalysts were prepared by a low temperature sol-gel method based on organic copper, silicon and titanium precursors with varied Cu concentrations (from 0.05 to 3 mol%). The sol-gels were dried at 150 °C to obtain the photocatalysts in the powder form. To test thermal stability, additional set of photocatalysts was obtained by calcinating dried samples in air at 500 °C for 1 h. The photocatalytic activity was determined by a fluorescence-based method of terephthalic acid decomposition. Up to three times increase in photocatalytic activity of air-dried samples is obtained when TiO2-SiO2 matrix is modified with Cu in a narrow concentration range from 0.05 to 0.1 mol%. At higher Cu loadings the photocatalytic activity of Cu-modified photocatalyst is smaller than in the unmodified reference TiO2-SiO2 photocatalyst. Calcined samples showed significantly reduced photocatalytic activity compared to air-dried samples. XRD analysis showed that all Cu-modified TiO2-SiO2 nanocomposites with different Cu concentrations have the same crystalline structure as unmodified TiO2-SiO2 nanocomposites (air-dried or calcined). The addition of Cu does not change the relative ratio between the anatase and brookite phase or unit cell parameters of the two TiO2 crystalline structures. TEM analysis showed that the addition of Cu does not change the morphology of TiO2-SiO2 catalyst dried at 150 °C. The Cu K-edge XANES and EXAFS analysis were used to determine valence state and local structure of Cu cations in Cu-modified TiO2-SiO2 photocatalyst. The results elucidate the mechanism responsible for the improved or hindered photocatalytic activity. In the air-dried samples with low Cu content, which exhibit largest activity, Cu-O-Ti connections are formed, suggesting that the activity enhancement is due to Cu(II) cations attachment on the surface of the photocatalytically active TiO2 nanoparticles, so Cu(II) cations may act as free electron traps, reducing the intensity of recombination between electrons and holes at the TiO2 photocatalyst’s surface. At higher Cu loadings no additional Cu-O-Ti connections are formed, instead only Cu-O-Cu connections are established, indicating the formation of amorphous or nanocrystalline Cu(II) oxide, which hinders the photocatalytic activity of TiO2. Calcination of Cu-modified TiO2-SiO2 photocatalysts at 500 °C induces significant structural changes: Cu-O-Ti connections are lost, Cu partially incorporates into the SiO2 matrix and amorphous copper oxides, which again reduce the photocatalytic activity of the material, are formed.
Ključne besede: titanium dioxide, Cu-modified TiO2-SiO2 photocatalyst, photocatalytic activity, Cu K-edge XANES, EXAFS.
Objavljeno v RUNG: 17.12.2018; Ogledov: 4555; Prenosov: 146
.pdf Celotno besedilo (3,05 MB)

6.
Crystal phase controlled synthesis of TiO2 nanoparticles by solution combustion method
Olena Pliekhova, Urška Lavrenčič Štangar, 2018, objavljeni znanstveni prispevek na konferenci

Ključne besede: Solution combustion, titanium dioxide, carbohydrazide, chloride ion, fluoride ion
Objavljeno v RUNG: 10.09.2018; Ogledov: 3298; Prenosov: 0
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7.
Role of Surface Cu-O-Zr Sites in the Photocatalytic Activity of TiO2 Nanoscale Particles
Olena Pliekhova, Iztok Arčon, Nataša Novak Tušar, Urška Lavrenčič Štangar, 2016, objavljeni povzetek znanstvenega prispevka na konferenci

Ključne besede: Photocatalysis, Titanium dioxide, Copper, Zirconia, co-doping, EXAFS, XANES
Objavljeno v RUNG: 23.08.2017; Ogledov: 4553; Prenosov: 0
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9.
Correlations between photocatalytic activity and Cu structure in Cu-modified TiO2-SiO2
T. Čižmar, objavljeni povzetek znanstvenega prispevka na konferenci

Ključne besede: Titanium dioxide, Cu-modified, TiO2-SiO2, photocatalysts, photocatalytic activity, Cu K-edge XANES, EXAFS
Objavljeno v RUNG: 26.06.2017; Ogledov: 4475; Prenosov: 0
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10.
HETEROGENEOUS PHOTOCATALYTIC OXIDATION FOR THE REMOVAL OF BISPHENOL A FROM AQUEOUS SOLUTION OVER TiO2/GRAPHENE OXIDE (GO) BASED NANOCOMPOSITES
Ana Veternik, 2017, magistrsko delo

Opis: Since water is an essential substance for all life on earth, it is therefore vital to prevent its pollution and to improve wastewater purification processes. There is a vast number of pollutants which can contaminate water, of which bisphenol A (known as an endocrine disruptor) is the pollutant studied herein. In this study, several TiO2/GO based nanocomposites with various GO loadings (2, 4, 10, 20 and 40%) and differently shaped nanocrystalline TiO2 phases (titanate nanotubes (TNTs) and calcined titanate nanotubes (TNTs_500)) were synthesised. All of the nanocomposites were characterised through SEM, UV-vis-DR, TGA, BET, FT-IR and CHNS analyses and were used in the heterogeneous photocatalytic degradation of bisphenol A and compared to the activity of pure TNTs and TNT_500 photocatalysts. All TiO2/GO nanocomposites exhibit much better activity than pure TNTs and TNTs_500 catalysts. The conversion of the BPA was analysed using HPLC and the mineralisation was analysed using a TOC analysis. The best experiment was performed with TNTs_500 + 10% GO composite, which can be attributed to the TiO2 crystalline structure obtained. According to the results obtained, TiO2 + 10% GO was found to exhibit the best degradation ratio, which can be ascribed to the fact that excessive GO can act as a charge carrier recombination centre and promotes the recombination of electron-hole pairs in reduced GO.
Ključne besede: heterogeneous photocatalysis, titanium dioxide, graphene oxide, bisphenol A
Objavljeno v RUNG: 23.02.2017; Ogledov: 5696; Prenosov: 289
.pdf Celotno besedilo (2,96 MB)

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