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Oxidative dissolution of polymer-coated CdSe/ZnS quantum dots under UV irradiation: Mechanisms and kinetics
2012
Li, Yang | Zhang, Wen | Li, Kungang | Yao, Ying | Niu, Junfeng | Chen, Yongsheng
To advance the knowledge of environmental fate of nanomaterials, we systematically investigated the dissolution of polymer-coated CdSe/ZnS quantum dots (QDs) under UV (254 nm) irradiation. The environmental effects (i.e., irradiation intensity, dissolved oxygen, temperature, and humic acid), as well as the coating effects on dissolution kinetics of QDs were investigated. Our results showed that higher irradiation intensity and temperature increased ion release rates (Cd²⁺, SeO₄ ²⁻, and Zn²⁺), whereas the different polymer coatings varied the dissolution rates. The absence of dissolved oxygen inhibited the dissolution of QDs, and we further demonstrated that the dissolution was a photo-oxidative process involved superoxide radical formation. Humic acid had a twofold effect on dissolution due to its photosensitization and photoabsorption for UV irradiation. Finally, an empirical kinetic law was proposed to interpret the above environmental effects. This study lays groundwork to better understand the environmental fate of QDs.
Show more [+] Less [-]Improvement of Photocatalytic Degradation of Naphthol Green B Under Solar Light Using Aluminum Doping of Zinc Oxide Nanoparticles
2012
Saber, Osama | El-Brolossy, Tarek A. | Al Jaafari, Abdullah A.
The photocatalytic degradation of dyes under sunlight irradiation has received much attention not only because the attempt is aimed at decomposition of pollutants but also at finding methods of making use of solar energy. Following this line, zinc oxide nano-particles were prepared using solvent thermal method in order to decompose Naphthol Green B in presence of sunlight. Complete mineralization and decolorization of Naphthol Green B were achieved in 14 h. In order to reduce the band gap of zinc oxide and increase its photocatalytic activity in sunlight, it was doped with different concentrations of aluminum (1 %, 3 %, 5 %, and 10 %). The obtained band gap energy of the Al-doped ZnO nanoparticles was investigated as a function of Al content. Reduction of band gap energy for the heavily doped ZnO nanoparticles (10 % Al) was observed from 3.29 to 3.23 eV leading to fast transfer for electron from the excited state of dye to conduction band of ZnO. Therefore, by using the 10 % Al-doped ZnO nanoparticles, the complete mineralization and decolorization of Naphthol Green B were achieved in 6 h under sunlight. These results suggested that the heavily doped ZnO nanoparticles with aluminum has a positive effect towards photocatalytic reactions with dye under solar energy.
Show more [+] Less [-]Effect of Co-Dopants in TiO2–SiO 2 Thin films on the Formaldehyde Degradation
2012
Kaewtip, Charuwan | Chadpunyanun, Pornpimon | Boonamnuayvitaya, Virote
Titanium dioxide (TiO2)–silicon dioxide (SiO2) thin films were synthesized using the peroxo titanic acid approach (PTA) combined with the sol–gel method at low temperature around 100°C. The effects of type and amount of dopants of ferric (Fe3+) or thiourea (N-S) and co-dopants of Fe3+ and N-S on the films physicochemical properties and on the photocatalytic degradation of the methylene blue and formaldehyde under UV and visible light irradiation were investigated. Physicochemical properties of photocatalysts were characterized by X-ray diffraction, transmission electron microscopy, wavelength-dispersive X-ray fluorescence spectrometry, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and UV–Vis spectroscopy. The results showed that the TiO2 crystal phases obtained from this method were exclusively anatase and the needle-like crystals have an average diameter of 10–25 nm. Compared with the single dopant of 1.0 wt.% Fe3+ or 0.125 wt.% N-S that was the optimal concentration for photocatalytic degradation of methylene blue and formaldehyde, the co-dopants of 0.125 wt.% N-S + 1.0 wt.% Fe3+ furthermore increased the degradation efficiency. Co-dopants of 0.125 wt.% N-S + 1.0 wt.% Fe3+ in TiO2–SiO2 films were considered to play synergistic roles in narrowing TiO2 band gap resulting in the higher methylene blue and formaldehyde degradation efficiency. Since the crystal grain size of TiO2–SiO2 films synthesized by the PTA method is small, in the visible light region, the high transmittance was attainable to 80% with no-doped and dropped to 50–60% with doped thin films.
Show more [+] Less [-]Effect of Nb doping on structural, optical and photocatalytic properties of flame-made TiO2 nanopowder
2012
TiO2:Nb nanopowders within a dopant concentration in the range of 0.1–15 at.% were prepared by one-step flame spray synthesis. Effect of niobium doping on structural, optical and photocatalytic properties of titanium dioxide nanopowders was studied. Morphology and structure were investigated by means of Brunauer–Emmett–Teller isotherm, X-ray diffraction and transmission electron microscopy. Diffuse reflectance and the resulting band gap energy were determined by diffuse reflectance spectroscopy. Photocatalytic activity of the investigated nanopowders was revised for the photodecomposition of methylene blue (MB), methyl orange (MO) and 4-chlorophenol under UVA and VIS light irradiation. Commercial TiO2-P25 nanopowder was used as a reference. The specific surface area of the powders was ranging from 42.9 m2/g for TiO2:0.1 at.% Nb to 90.0 m2/g for TiO2:15 at.% Nb. TiO2:Nb particles were nanosized, spherically shaped and polycrystalline. Anatase was the predominant phase in all samples. The anatase-related transition was at 3.31 eV and rutile-related one at 3.14 eV. TiO2:Nb nanopowders exhibited additional absorption in the visible range. In comparison to TiO2-P25, improved photocatalytic activity of TiO2:Nb was observed for the degradation of MB and MO under both UVA and VIS irradiation, where low doping level (Nb < 1 at.%) was the most effective. Niobium doping affected structural, optical and photocatalytic properties of TiO2. Low dopant level enhanced photocatalytic performance under UVA and VIS irradiation. Therefore, TiO2:Nb (Nb < 1 at.%) can be proposed as an efficient selective solar light photocatalyst.
Show more [+] Less [-]Improvement of biodegradability of PVA-containing wastewater by ionizing radiation pretreatment
2012
BACKGROUND: Polyvinyl alcohol (PVA) has been widely used as sizing agents in textile and manufacturing industry, and it is a refractory compound with low biodegradability. OBJECTIVE: The objective of this paper was to treat the PVA-containing wastewater using gamma irradiation as a pretreatment strategy to improve its biodegradability and to determine the roles of different kinds of radical species played during pretreatment. METHODS: Gamma radiation was carried out in a 60Cobalt source station, PVA concentration was analyzed by using a visible spectrophotometer and specific oxygen uptake rate (SOUR, milligram of O2 per gram of mixed liquor volatile suspended solids (MLVSS) per hour) was measured by a microrespirometer. RESULTS: The results showed that the biodegradability of PVA-containing wastewater with low initial concentration (e.g., 327.8 mg/l) could be improved greatly with increasing irradiation dose. However, PVA gel formation was observed at higher initial PVA concentration (e.g., 3,341.6 mg/l) and higher irradiation dose, which inhibited PVA degradation by aerobic microorganisms. However, the formed gel could be separated by microfiltration, which led to more than 90% total organic carbon (TOC) removal. CONCLUSION: Ionizing radiation could be used as a pretreatment technology for PVA-containing wastewater, and its combination with biological process is feasible.
Show more [+] Less [-]In situ photoelectrochemical/photocatalytic study of a dye discoloration in a microreactor system using TiO2 thin films
2012
Montero-Ocampo, C. | Gago, A. | Abadias, G. | Gombert, B. | Alonso-Vante, N.
INTRODUCTION: In this work, we report in situ studies of UV photoelectrocatalytic discoloration of a dye (indigo carmine) by a TiO2 thin film in a microreactor to demonstrate the driving force of the applied electrode potential and the dye flow rate toward dye discoloration kinetics. METHODS: TiO2 65-nm-thick thin films were deposited by PVD magnetron sputtering technique on a conducting glass substrate of fluorinated tin oxide. A microreactor to measure the discoloration rate, the electrode potential, and the photocurrent in situ, was developed. The dye solutions, before and after measurements in the microreactor, were analyzed by Raman spectroscopy. RESULTS: The annealed TiO2 thin films had anatase structure with preferential orientation (101). The discoloration rate of the dye increased with the applied potential to TiO2 electrode. Further, acceleration of the photocatalytic reaction was achieved by utilizing dye flow recirculation to the microreactor. In both cases the photoelectrochemical/photocatalytic discoloration kinetics of the dye follows the Langmuir–Hinshelwood model, with first-order kinetics. CONCLUSIONS: The feasibility of dye discoloration on TiO2 thin film electrodes, prepared by magnetron sputtering using a flow microreactor system, has been clearly demonstrated. The discoloration rate is enhanced by applying a positive potential (E AP) and/or increasing the flow rate. The fastest discoloration and shortest irradiation time (50 min) produced 80% discoloration with an external anodic potential of 0.931 V and a flow rate of 12.2 mL min−1.
Show more [+] Less [-]Degradation of ampicillin antibiotic in aqueous solution by ZnO/polyaniline nanocomposite as photocatalyst under sunlight irradiation
2012
Nosrati, Rahimeh | Olad, Ali | Maramifar, Roya
PURPOSE AND METHOD: ZnO/polyaniline nanocomposite in core–shell structure was prepared by the synthesis and adsorption of polyaniline chains on the structure of ZnO nanoparticles. Fourier transform infrared and ultraviolet–visible (UV–Vis) spectroscopy, X-ray diffraction patterns, field emission scanning electron microscopy, and transmission electron microscopy were used to characterize the composition and structure of the nanocomposite. The nanocomposite was used as an active photocatalyst for photodegradation and removal of ampicillin in aqueous solution. RESULTS: UV–Vis spectroscopy studies showed that ZnO/polyaniline nanocomposite absorbs visible light irradiation as well as ultraviolet spectrum, and therefore, it can be photoactivated under visible and ultraviolet lights. The photocatalytic activity of ZnO/polyaniline nanocomposite in degradation of ampicillin molecules in aqueous solution under natural sunlight irradiation was evaluated and compared with that of ZnO nanoparticles and pristine polyaniline. The ZnO/polyaniline core–shell nanocomposite exhibited higher photocatalytic activity compared to ZnO nanoparticles and pristine polyaniline. The effect of operating conditions (pH, ZnO/polyaniline nanocomposite dosage, and ampicillin concentration) in the photocatalytic degradation of ampicillin using ZnO/polyaniline nanocomposite was investigated. The optimum conditions for maximum efficiency of ampicillin degradation under 120 min sunlight irradiation were found as 10 mg L−1 dosage of ZnO/polyaniline nanocomposite, ampicillin concentration of 4.5 mg L−1, and solution pH = 5. Under optimum operating conditions, degradation efficiency was reached to 41% after 120 min of exposure to the sunlight irradiation.
Show more [+] Less [-]Adsorption and photodegradation of microcystin-LR onto sediments collected from reservoirs and rivers in Taiwan: a laboratory study to investigate the fate, transfer, and degradation of microcystin-LR
2012
Munusamy, Thirumavalavan | Hu, Ya-Lan | Lee, Jiunn-Fwu
BACKGROUND, AIM, AND SCOPE: This study demonstrated the adsorption capacity of microcystin-LR (MC-LR) onto sediment samples collected from different reservoirs (Emerald and Jade reservoirs) and rivers (Dongshan, Erhjen, and Wukai rivers) in Taiwan to investigate the fate, transport behavior, and photodegradation of MC-LR. MAIN FEATURES: Langmuir adsorption and photodegradation studies were carried out in the laboratory and tested the capability of sediments for MC-LR adsorption. These data suggested that sediments play a crucial role in microcystins degradation in aquatic systems. RESULTS AND DISCUSSION: The results of batch experiments revealed that the adsorption of MC-LR varied significantly with texture, pH, and organic matter content of sediments. Silty and clay textures of the samples were associated with larger content of organic matter, and they displayed the enhanced MC-LR adsorption. Low pH sediment showed increased adsorption of MC-LR. The effective photodegradation of MC-LR (1.6 μg/mL) was achieved within 60 min under 254 nm light irradiation. CONCLUSION: A comparative study of adsorption capacity of all sediment samples was carried out and discussed with respect to different aspects. Among all, sediments collected from Jade reservoir showed enhanced MC-LR adsorption (11.86 μg/g) due to favored textural properties (BET surface area = 20.24 m2/g and pore volume = 80.70 nm). PERSPECTIVES: These data provide important information that may be applied to management strategies for improvement of water quality in reservoirs and rivers and other water bodies in Taiwan.
Show more [+] Less [-]Transition metal-modified zinc oxides for UV and visible light photocatalysis
2012
Bloh, J. Z. | Dillert, R. | Bahnemann, D. W.
In order to use photocatalysis with solar light, finding more active and especially visible light active photocatalysts is a very important challenge. Also, studies of these photocatalysts should employ a standardized test procedure so that their results can be accurately compared and evaluated with one another. A systematic study of transition metal-modified zinc oxide was conducted to determine whether they are suitable as visible light photocatalysts. The photocatalytic activity of ZnO modified with eight different transition metals (Cu, Co, Fe, Mn, Ni, Ru, Ti, Zr) in three different concentrations (0.01, 0.1, and 1 at.%) was investigated under irradiation with UV as well as with visible light. The employed activity test is the gas-phase degradation of acetaldehyde as described by the ISO standard 22197-2. The results suggest that the UV activity can be improved with almost any modification element and that there exists an optimal modification ratio at about 0.1 at.%. Additionally, Mn- and Ru-modified ZnO display visible light activity. Especially the Ru-modified ZnO is highly active and surpasses the visible light activity of all studied titania standards. These findings suggest that modified zinc oxides may be a viable alternative to titanium dioxide-based catalysts for visible light photocatalysis. Eventually, possible underlying mechanisms are proposed and discussed.
Show more [+] Less [-]Estrogenic effects of dissolved organic matter and its impact on the activity of 17β-estradiol
2012
Chen, Lei | Shen, Chaofeng | Tang, Xianjin | Chen, Chen | Chen, Yingxu
BACKGROUND AND PURPOSE: The ubiquitous dissolved organic matter (DOM) is actually not inert as we always think, and the hormone-like effects of DOM have been reported. The objective of this study was to investigate the estrogenic effects of DOM and its impact on the activity of the natural estrogen 17β-estradiol (E2). MATERIALS AND METHODS: DOM of three different sources, HA sodium salt, Suwannee River natural organic matter (NOM), and Nordic Reservoir NOM, were used. The estrogenic activity was detected by using the yeast estrogen screen (YES) assay. Estrogenic effects of DOM without and after solar irradiation were tested. Influences on the action of E2 by DOM were also investigated. RESULTS: No direct estrogenic effects of the DOM used were observed in the YES assay. However, the estrogenic activities after 24 h of irradiation increased to 0.0288, 0.0178, and 0.0195 μM of E2 equivalents for HA sodium salt, Suwannee River NOM, and Nordic Reservoir NOM, respectively. After incubation of DOM, the estrogenic activity of E2 was increased by low concentrations (8.33 and 83.3 μM) of DOM while decreased by higher concentrations (8.33 × 102 and 8.33 × 103 μM) of DOM. CONCLUSIONS: Though direct estrogenic effects of DOM were not observed, increase in the estrogenic activity of DOM after irradiation was significant. DOM shows amphoteric influence on the natural estrogen E2, which depends on the concentration of DOM used. Because of its ubiquity, DOM may be of great ecological significance, playing an important role in regulating the reproduction of aquatic organisms.
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