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1.
Polyacrylonitrile (PAN) fiber was modified with hydroxylamine hydrochloride to introduce amidoxime groups onto the fiber surface. These amidoxime groups were used to react with Fe (III) ions to prepare Fe (III)-amidoximated PAN fiber complex, which was characterized using SEM, XRD, FTIR, XPS, DMA, and DRS respectively. Then the photocatalytic activity of Fe-AO-PAN was evaluated in the degradation of a typical azo dye, C. I. Reactive Red 195 in the presence of H2O2 under visible light irradiation. Moreover, the effect of the Fe content of Fe-AO-PAN on dye degradation was also investigated. The results indicated that Fe (III) ions can crosslink between the modified PAN fiber chains by the coordination of Fe (III) ions with the amino nitrogen atoms and hydroxyl oxygen atoms of the amidoximation groups to form Fe (III)-amidoximated PAN fiber complex, and the Fe content of which is mainly determined by Fe (III) ions and amidoximation groups. Fe (III)-amidoximated PAN fiber complex is found to be activated in the visible light region. Moreover, Fe (III)-amidoximated PAN fiber complex shows the catalytic activity for dye degradation by H2O2 at pH = 6.0 in the dark, and can be significantly enhanced by increasing light irradiation and Fe content, therefore, it can be used as a new heterogeneous Fenton photocatalyst for the effective decomposition of the dye in water. In addition, ESR spectra confirm that Fe (III)-amidoximated PAN fiber complex can generate more OH radicals from H2O2 under visible light irradiation, leading to dye degradation. A possible mechanism of photocatalysis is proposed.  相似文献   

2.
The kinetics of photodegradation of the pesticide metaldehyde by UV/H2O2 and UV/TiO2 in laboratory grade water and a natural surface water were studied. Experiments were carried out in a bench scale collimated beam device using UVC radiation. Metaldehyde was efficiently degraded by both processes in laboratory grade water at identical rates of degradation (0.0070 and 0.0067 cm2 mJ−1 for UV/TiO2 and UV/H2O2 respectively) when optimised doses were used. The ratio between oxidant and metaldehyde was significantly higher for H2O2 due to its low photon absorption efficiency at 254 nm. However, the presence of background organic compounds in natural water severely affected the rate of degradation, and whilst the pseudo first-order rate constant of degradation by UV/H2O2 was slowed down (0.0020 cm2 mJ−1), the degradation was completely inhibited for the UV/TiO2 process (k′ = 0.00007 cm2 mJ−1) due to the blockage of active sites on TiO2 surface by the background organic material.  相似文献   

3.
The discharge of dyes into water is an ecological problem that can be alleviated by advanced oxidation processes (AOPs), such as UV/H2O2 treatments. Searching for more efficient light sources is a way to improve AOPs’ efficiency. This work tested the efficiency of an amalgam lamp on the degradation of an azo dye, studying the effect of dye and H2O2 concentrations and pH, and the influence of some salts on the decolouration rate of methyl orange. Actinometry showed that the amalgam lamp system was able to provide a high incident photon irradiance (6.30·10?5 mol/cms). The amalgam lamp‐driven AOP was able to decolourize the dye at pseudo‐first‐order rates of 0.654–4.008 1/min, with increasing rates at low dye concentration and low pH and at high H2O2 concentrations until a maximum value is reached. The results show that the amalgam lamp can be an alternative light source for fast dye degradation by AOPs.  相似文献   

4.
The photocatalytic degradation of two phenolic compounds, p-coumaric acid and caffeic acid, was performed with a suspended mixture of TiO2 and powdered activated carbon (PAC) (at pH = 3.4 and 8). Adsorption, direct photolysis and photocatalytic degradation were studied under different pH and UV light sources (sunlight vs. 365 nm UV lamps). The potential for reusing this catalyst mixture in sequential photocatalytic runs was examined as well. Quantum yields for the direct photolysis of caffeic acid under solar and artificial 365 nm light were calculated (for the first time) as 0.005 and 0.011, respectively.A higher removal rate of contaminants by either adsorption or photocatalysis was obtained at a low pH (pH 4). Furthermore, the addition of PAC increased the removal efficiency of the phenolic compounds. Fast removal of the pollutants from the solution over three sequential runs was achieved only when both TiO2 and PAC were present. This suggests that at medium phenolic concentrations, the presence of PAC as a co-sorbent reduces surface poisoning of the TiO2 catalyst and hence improves photocatalysis degradation of phenolic pollutants.The adsorption equilibrium of caffeic acid or p-coumaric acid on TiO2, PAC and the combined mixture of TiO2 and PAC follows the Langmuir isotherm model. Experiments with PAC TiO2 mixture and olive mill wastewater (anaerobically treated and diluted by a factor of 10) showed higher removal of polyphenols than of chemical oxygen demand (COD). 87% removal of total polyphenols, compared to 58% of COD, was achieved after 24 h of exposure to 365 nm irradiation (7.6 W/m2) in the presence of a suspended mixture of TiO2 and PAC, indicating “self-selectivity” of polyphenols.  相似文献   

5.
This article examines the oxidative disposal of Prozac® (also known as Fluoxetine, FXT) through several oxidative processes with and without UV irradiation: for example, TiO2 alone, O3 alone, and the hybrid methods comprised of O3 + H2O2 (PEROXONE process), TiO2 + O3 and TiO2 + O3 + H2O2 at the laboratory scale. Results show a strong pH dependence of the adsorption of FXT on TiO2 and the crucial role of adsorption in the whole degradation process. Photolysis of FXT is remarkable only under alkaline pH. The heterogeneous photoassisted process removes 0.11 mM FXT (initial concentration) within ca. 60 min with a concomitant 50% mineralization at pH 11 (TiO2 loading, 0.050 g L−1). The presence of H2O2 enhances the mineralization further to >70%. UV/ozonation leads to the elimination of FXT to a greater extent than does UV/TiO2: i.e., 100% elimination of FXT is achieved by UV/O3 in the first 10 min of reaction and almost 97% mineralization is attained under UV irradiation in the presence of H2O2. The hybrid configuration UV + TiO2 + O3 + H2O2 enhances removal of dissolved organic carbon (DOC) in ca. 30 min leaving, however, an important inorganic carbon (IC) content. In all cases, the presence of H2O2 improves the elimination of DOC, but not without a detrimental effect on the biodegradability of FXT owing to the low organic carbon content in the final treated effluent, together with significant levels of inorganic byproducts remaining. The photoassisted TiO2/O3 hybrid method may prove to be an efficient combination to enhance wastewater treatment of recalcitrant drug pollutants in aquatic environments.  相似文献   

6.
Wang C  Zhu L  Wei M  Chen P  Shan G 《Water research》2012,46(3):845-853
Bi2WO6 displayed great photolytic degradation efficiency to bisphenol A (BPA) under simulated solar light irradiation but its reaction mechanism and the impacts of coexisting substances on the degradation remain unclear. In present study, the reaction mechanism was investigated using DMPO spin-trapping ESR spectra and experiments with scavengers of hydroxyl radicals (OH) and holes. The results supported that hole oxidation mainly governed the photodegradation process. As a common humic substance in natural water, humic acid accelerated the degradation of BPA when its concentration was 1 mg/L, while the photodegradation was impeded with the increase of humic acid concentration in the range of 5-20 mg/L. Almost all anions, including NO3, HCO3, Cl, SO42− inhibited the degradation of BPA by Bi2WO6 and their inhibition effects followed the order of SO42− > Cl > HCO3 > NO3. Cations of Na+, K+, Ca2+ and Mg2+ displayed slight suppressing effect on BPA degradation mainly due to the impact of Cl coexisting in the solution. However, Cu2+ hindered the BPA photodegradation heavily. Fe3+ and H2O2 affected the photodegradation in a complicated way: they suppressed or promoted the photodegradation depending on their concentrations. This could be the result of competition between photolyitc hole generated by Bi2WO6 and OH produced by Fe3+ or H2O2.  相似文献   

7.
Aqueous solutions of atrazine (ATZ, 2-chloro-4-ethylamino-6-isopropylamino-1, 3, 5-triazine) were photolysed (λ = 254 nm) by low pressure UV/H2O2 process (LP/UV/H2O2) under a variety of parameters including hydrogen peroxide, the initial concentration of ATZ, pH, and humic acid. The results show that the most favourable reaction condition appears to be a moderate concentration of H2O2 from 100 mg/L to 120 mg/L. The presence of humic acid in the solution has a negative impact on the LP/UV/H2O2 treatment because of scavenging effects. Ninety percent of ATZ is destroyed in one hour under the optimum conditions. In this study, LP/UV/ H2O2 treatment of ATZ yielded several organic by products which are identified, including DIA, DEA, OHDIA, OHDEA, DAA and OAAT. They are quantified over the range of treatment tested and the ATZ degradation scheme is proposed combined with by products information.  相似文献   

8.
The typical antibiotic Oxytetracycline (OTC) remained in the environment and it was widely used. And the migration and transformation of OTC in natural environment and its harmfulness had become the focus of attention. Thus, the influence of Fe(II/III)‐OTC complex on degradation of OTC by Fe(II)/H2O2 under simulated solar light was investigated. The results showed that the average ratio of OTC‐Fe(II/III) complexes formed by OTC and Fe(III) was 1:1 at pH = 2.5. In addition, it was difficult to obtain the stability constant of Fe(III)‐OTC complexes effectively considering the morphology of Fe(III) and the complexation sites of OTC. And when OTC:Fe(II):H2O2 = 1:1.5:2, the removal rate of OTC was 82% after 1 h, however, simulated solar light could not improve the degradation of OTC effectively. Furthermore, the existence of OTC‐Fe(II/III) complex led to the slow degradation stage of OTC degradation by Fe(II)/H2O2. It could be concluded that the Fe(III)‐OTC complex might prolong the retention time of OTC in the environment.  相似文献   

9.
Tokumura M  Znad HT  Kawase Y 《Water research》2008,42(18):4665-4673
The decolorization of dark brown colored coffee effluent by solar photo-Fenton process has been studied. Effects of accumulated solar light energy and dosage of Fenton reagents (iron and hydrogen peroxide) on the color removal have been examined. With increasing Fe dosage the rate of the decolorization increased but the enhancement was not pronounced beyond 10 mg L−1. Although addition of H2O2 increased the decolorization rate up to around 1000 mg L−1 of H2O2, further addition of H2O2 could not enhance the color removal. At excess dosages of Fenton reagents, the color removal was not improved due to their scavenging of hydroxyl radicals. It was found that the pseudo-first order decolorization kinetic constant based on the accumulated solar energy is a sole parameter unifying solar photo-Fenton decolorization processes under the different weather conditions. The kinetic constant can be readily used to calculate the amount of solar energy required to achieve a certain degree of color removal. The mineralization was rather slower as compared with the decolorization. The decolorization capability with solar irradiation was found to be comparable to UV light irradiation. The present results suggest that abundant solar energy driving decolorization of coffee effluent by photo-Fenton reaction is highly efficient.  相似文献   

10.
Photocatalytic oxidation by TiO2 has been shown to deactivate biological pollutants. Most previous studies evaluated TiO2's antimicrobial performance using bacteria, with Escherichia coli most commonly applied as the test microbe. There have not been concentrated studies focusing on the photocatalytic disinfection of fungi which widely exist in buildings and cause health problems. In this study, the antifungal activity of TiO2 photocatalytic reaction against Aspergillus niger was investigated for moist wood boards during periods of several weeks. TiO2 coated film in the presence of UVA (365 nm) irradiation exhibited antifungal capability. No visible growth was observed on specimens during the photo-process. Re-growth appeared in subsequent dark, indicating that the photocatalytic reaction was not sufficient for total disinfection against mold fungi but did suppress fungi growth. The study sheds light on conditions and potential applications of photocatalytic deactivation of fungi.  相似文献   

11.
Peng Wang  Irene M.C. Lo   《Water research》2009,43(15):3727-3734
In this study, mesoporous magnetic iron-oxide (γ-Fe2O3) was synthesized as an adsorbent for Cr(VI) removal. For material synthesis, mesoporous silica (KIT-6) was used as a hard template and to drive iron precursor into KIT-6, a ‘greener’, affinity based impregnation method was employed, which involved using a nonpolar solvent (xylene) and led to recycling of the solvent. The results of Cr(VI) removal experiments showed that the synthesized mesoporous γ-Fe2O3 has a Cr(VI) adsorption capacity comparable with 10 nm nonporous γ-Fe2O3 but simultaneously has a much faster separation than 10 nm nonporous γ-Fe2O3 in the presence of an external magnetic field under the same experimental conditions. Cr(VI) adsorption capacity onto the mesoporous γ-Fe2O3 increased with decreasing solution pH and could be readily regenerated. Therefore, mesoporous γ-Fe2O3 presents a reusable adsorbent for a fast, convenient, and highly efficient removal of Cr(VI) from contaminated water.  相似文献   

12.
This study focuses on the removal of 32 selected micropollutants (pharmaceuticals, corrosion inhibitors and biocides/pesticides) found in an effluent coming from a municipal wastewater treatment plant (MWTP) based on activated sludge. Dissolved organic matter was present, with an initial total organic carbon of 15.9 mg L−1, and a real global quantity of micropollutants of 29.5 μg L−1. The treatments tested on the micropollutants removal were: UV-light emitting at 254 nm (UV254) alone, dark Fenton (Fe2+,3+/H2O2) and photo-Fenton (Fe2+,3+/H2O2/light). Different irradiation sources were used for the photo-Fenton experiences: UV254 and simulated sunlight. Iron and H2O2 concentrations were also changed in photo-Fenton experiences in order to evaluate its influence on the degradation. All the experiments were developed at natural pH, near neutral. Photo-Fenton treatments employing UV254, 50 mg L−1 of H2O2, with and without adding iron (5 mg L−1 of Fe2+ added or 1.48 mg L−1 of total iron already present) gave the best results. Global percentages of micropollutants removal achieved were 98 and a 97% respectively, after 30 min of treatments. As the H2O2 concentration increased (10, 25 and 50 mg L−1), best degradations were observed. UV254, Fenton, and photo-Fenton under simulated sunlight gave less promising results with lower percentages of removal.The highlight of this paper is to point out the possibility of the micropollutants degradation in spite the presence of DOM in much higher concentrations.  相似文献   

13.
Metal loaded semiconductors in general possess greater photocatalytic activity than pure semiconductors. Hence, with an attempt to achieve higher photocatalytic activity, Au-TiO2 photocatalysts were prepared by deposition-precipitation method and used for the photocatalytic degradation of an azo dye (Acid Red 88; AR88). The materials were characterized by different analytical techniques. A possible mechanism for the photocatalytic degradation of AR88 by Au-TiO2 in the absence and presence of other oxidizing agents (peroxomonosulfate (PMS), peroxodisulfate (PDS) & hydrogen peroxide (H2O2)) has been proposed. The extent of mineralization of the target pollutant was also evaluated using Total Organic Carbon (TOC) analysis.  相似文献   

14.
This study investigated the treatment performances of H2O2 oxidation alone and its combination with granular activated carbon (GAC) adsorption for raw leachate from the NENT landfill (Hong Kong) with a very low biodegradability ratio (BOD5/COD) of 0.08. The COD removal of refractory compounds (as indicated by COD values) by the integrated H2O2 and GAC treatment was evaluated, optimized and compared to that by H2O2 treatment alone with respect to dose, contact time, pH, and biodegradability ratio. At an initial COD concentration of 8000 mg/L and NH3-N of 2595 mg/L, the integrated treatment has substantially achieved a higher removal (COD: 82%; NH3-N: 59%) than the H2O2 oxidation alone (COD: 33%; NH3-N: 4.9%) and GAC adsorption alone (COD: 58%) at optimized experimental conditions (p ≤ 0.05; t-test). The addition of an Fe(II) dose at 1.8 g/L further improved the removal of refractory compounds by the integrated treatment from 82% to 89%. Although the integrated H2O2 oxidation and GAC adsorption could treat leachate of varying strengths, treated effluents were unable to meet the local COD limit of less than 200 mg/L and the NH3-N of lower than 5 mg/L. However, the integrated treatment significantly improved the biodegradability ratio of the treated leachate by 350% from 0.08 to 0.36, enabling the application of subsequent biological treatments for complementing the degradation of target compounds in the leachate prior to their discharge.  相似文献   

15.
A comparative study on the photocatalytic activities of four different catalysts, P-25 TiO2, TiO2 nanofibers, tin-doped TiO2 nanofibers under UV light irradiation at 350 nm, and coumarin (C-343) coated TiO2 nanofibers at 436 nm light emitting diodes (LED) is reported. Catalysts performance has been compared based on their reflectance spectrum and activity. A common water contaminant 4-chlorophenol was used as a substrate to compare the activity of the different catalysts under both direct and dye sensitized conditions. Results indicated that amongst the four different catalysts the activity of P-25 was the highest. However the activity of C-343 coated TiO2 nanofibers in the LED (436 nm) based reactor was competitive. Identification of reaction intermediates implied that the reaction pathways under UV (band gap) and visible (dye sensitized) irradiation were different. Nonetheless, ring opening took place in all reactions with both maleic and dihydroxymaleic have been identified as intermediates. The study indicates that ordered arrays of TiO2 irradiated by panels of arrays of low cost high intensity LEDs might be used for the design of reactors. The near monochromaticity, long life, and operation under direct currents are advantages of using LEDs.  相似文献   

16.
Advanced oxidation with ultraviolet light and hydrogen peroxide (UV/H2O2) produces hydroxyl radicals that have the potential to degrade a wide-range of organic micro-pollutants in water. Yet, when this technology is used to reduce target contaminants, natural organic matter can be altered. This study evaluated disinfection by-product (DBP) precursor formation for UV/H2O2 while reducing trace organic contaminants in natural water (>90% for target pharmaceuticals, pesticides and taste and odor producing compounds and 80% atrazine degradation). A year-long UV/H2O2 pilot study was conducted to evaluate DBP precursor formation with varying water quality. The UV pilot reactors were operated to consistently achieve 80% atrazine degradation, allowing comparison of low pressure (LP) and medium pressure (MP) lamp technologies for DBP precursor formation. Two process waters of differing quality were used as pilot influent, i.e., before and after granular activated carbon adsorption. DBP precursors increased under most of the conditions studied. Regulated trihalomethane formation potential increased through the UV/H2O2 reactors from 20 to 118%, depending on temperature and water quality. When Post-GAC water served as reactor influent, less DBPs were produced in comparison to conventionally treated water. Haloacetic acid (HAA5) increased when conventionally treated water served as UV/H2O2 pilot influent, but only increased slightly (MP lamp) when GAC treated water served as pilot influent. No difference in 3-day simulated distribution system DBP concentration was observed between LP and MP UV reactors when 80% atrazine degradation was targeted.  相似文献   

17.
The article has studied the impact of various physicochemical factors (the concentration of H2O2: alcohol ratio, the presence of oxygen, of Fe(III) ions, etc.) on the consumption and buildup of H2O2 in oxidation of aliphatic alcohols in aqueous solutions under the effect of UV light (200–360 nm). Based on the obtained data the kinetic model of generating H2O2 has been proposed in the processes being considered.  相似文献   

18.
Cho M  Gandhi V  Hwang TM  Lee S  Kim JH 《Water research》2011,45(3):1063-1070
A sequential application of UV as a primary disinfectant with and without H2O2 addition followed by free chlorine as secondary, residual disinfectant was performed to evaluate the synergistic inactivation of selected indicator microorganisms, MS-2 bacteriophage and Bacillus subtilis spores. No synergism was observed when the UV irradiation treatment was followed by free chlorine, i.e., the overall level of inactivation was the same as the sum of the inactivation levels achieved by each disinfection step. With the addition of H2O2 in the primary UV disinfection step, however, enhanced microbial inactivation was observed. The synergism was observed in two folds manners: (1) additional inactivation achieved by hydroxyl radicals generated from the photolysis of H2O2 in the primary UV disinfection step, and (2) damage to microorganisms in the primary step which facilitated the subsequent chlorine inactivation. Addition of H2O2 in the primary disinfection step was also found to be beneficial for the degradation of selected model organic pollutants including bisphenol-A (endocrine disruptor), geosmin (taste and odor causing compound) and 2,4-D (herbicide). The results suggest that the efficiency of UV/free chlorine sequential disinfection processes, which are widely employed in drinking water treatment, could be significantly enhanced by adding H2O2 in the primary step and hence converting the UV process to an advanced oxidation process.  相似文献   

19.
Xiong Z  Ma J  Ng WJ  Waite TD  Zhao XS 《Water research》2011,45(5):2095-2103
Mesoporous anatase (TiO2) was modified with silver (Ag) nanoparticles using a photoreduction method. Performance of the resulting TiO2-Ag nanocomposites for water purification was evaluated using degradation of Rhodamine B (RhB) and disinfection of Escherichia coli (E. coli) under ultraviolet (UV) irradiation. The composites with different Ag loadings were characterized using physical adsorption of nitrogen, X-ray diffraction, X-ray photoelectron spectroscopy and UV-Visible diffuse reflectance spectroscopic techniques. The results showed that metallic Ag nanoparticles were firmly immobilized on the TiO2 surface, which improved electron-hole separation by forming the Schottky barrier at the TiO2-Ag interface. Photocatalytic degradation of RhB and inactivation of E. coli effectively occurred in an analogical trend. The deposited Ag slightly decreased adsorption of target pollutants, but greatly increased adsorption of molecular oxygen with the latter enhancing production of reactive oxygen species (ROSs) with concomitant increase in contaminant photodegradation. The optimal Ag loadings for RhB degradation and E. coli disinfection were 0.25 wt% and 2.0 wt%, respectively. The composite photocatalysts were stable and could be used repeatedly under UV irradiation.  相似文献   

20.
De Laat J  Dao YH  El Najjar NH  Daou C 《Water research》2011,45(17):5654-5664
The decomposition rate of H2O2 by iron(III)-nitrilotriacetate complexes (FeIIINTA) has been investigated over a large range of experimental conditions: 3 < pH < 11, [Fe(III)]T,0: 0.05-1 mM; [NTA]T,0/[Fe(III)]T,0 molar ratios : 1-250; [H2O2]0: 1 mM-4 M) and concentrations of HO radical scavengers: 0-53 mM. Spectrophotometric analyses revealed that reactions of H2O2 with FeIIINTA (1 mM) at neutral pH immediately lead to the formation of intermediates (presumably peroxocomplexes of FeIIINTA) which absorb light in the region 350-600 nm where FeIIINTA and H2O2 do not absorb. Kinetic experiments showed that the decomposition rates of H2O2 were first-order with respect to H2O2 and that the apparent first-order rate constants were found to be proportional to the total concentration of FeIIINTA complexes, were at a maximum at pH 7.95 ± 0.10 and depend on the [NTA]T,0/[Fe(III)]T,0 and [H2O2]0/[Fe(III)]T,0 molar ratios. The addition of increasing concentrations of tert-butanol or sodium bicarbonate significantly decreased the decomposition rate of H2O2, suggesting the involvement of HO radicals in the decomposition of H2O2. The decomposition of H2O2 by FeIIINTA at neutral pH was accompanied by a production of dioxygen and by the oxidation of NTA. The degradation of the organic ligand during the course of the reaction led to a progressive decomplexation of FeIIINTA followed by a subsequent precipitation of iron(III) oxyhydroxides and by a significant decrease in the catalytic activity of Fe(III) species for the decomposition of H2O2.  相似文献   

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