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1.
In this work, the electrochemical degradation of the dye azure B in aqueous solutions was studied by electrochemical advanced oxidation processes (EAOPs), electro-Fenton, and anodic oxidation processes, using Pt/carbon-felt and boron-doped diamond (BDD)/carbon-felt cells with H2O2 electrogeneration. The higher oxidation power of the electro-Fenton (EF) process using BDD anode was demonstrated. The oxidative degradation of azure B by the electrochemically generated hydroxyl radicals (?OH) follows a pseudo-first-order kinetics. The apparent rate constants of the oxidation of azure B by ?OH were measured according to pseudo-first-order kinetic model. The absolute rate constant of azure B hydroxylation reaction was determined by competition kinetics method and found to be 1.19?×?109 M?1 s?1. It was found that the electrochemical degradation of the dye leads to the formation of aromatic by-products which are then oxidized to aliphatic carboxylic acids before their almost mineralization to CO2 and inorganic ions (sulfate, nitrate, and ammonium). The evolution of the TOC removal and time course of short-chain carboxylic acids during treatment were also investigated.  相似文献   

2.
Perfluorooctane sulfonate (PFOS), a widely used mist suppressant in hard chrome electroplating industry, has been listed in the Stockholm Convention for global ban. 6:2 Fluorotelomer sulfonate (6:2 FTS) acid and salts have been adopted as alternative products in the market, but no data about their abiotic degradation has been reported. In the present study, the degradability of 6:2 FTS potassium salt (6:2 FTS-K) was evaluated under various advanced oxidation processes, including ultraviolet (UV) irradiation, UV with hydrogen peroxide (H2O2), alkaline ozonation (O3, pH = 11), peroxone (O3/H2O2), and Fenton reagent oxidation (Fe2+/H2O2). UV/H2O2 was found to be the most effective approach, where the degradation of 6:2 FTS-K followed the pseudo-first-order kinetics. The intermediates were mainly shorter chain perfluoroalkyl carboxylic acid (C7 to C2), while sulfate (SO4 2?) and fluoride (F?) were found to be the final products. The high yields of SO4 2? and F? indicate that 6:2 FTS-K can be nearly completely desulfonated and defluorinated under UV/H2O2 condition. The degradation should firstly begin with the substitution of hydrogen atom by hydroxyl radicals, followed by desulfonation, carboxylation, and sequential “flake off” of CF2 unit. Compared with PFOS which is inert in most advanced oxidation processes, 6:2 FTS-K is more degradable as the alternative.  相似文献   

3.
4.
Chen HW  Chen CY  Wang GS 《Chemosphere》2011,85(4):591-597
The presence of various organic contaminants in water sources is of concern due to their direct threats to human health and potential to react with disinfectants to form carcinogenic byproducts including trihalomethanes, haloacetic acids and nitrosamines in finished water. This study applied both medium-pressure and low-pressure ultraviolet light coupled with hydrogen peroxide (UV/H2O2) to evaluate its efficacy for degradation of selected nitrogenous organic compounds and corresponding disinfection byproduct (DBP) formation. Six organic compounds were chosen as target precursors based on their nitrogen contents and molecular structures. The results showed that higher oxidation capacity resulted in better reduction of organic matters and DBP formation potentials (DBPFPs). However, insufficient contact time and oxidant doses could lead to a rise of DBPFPs in the early stages of UV/H2O2 reactions. A greater percentage removal was achieved for organic carbon than organic nitrogen after UV/H2O2 treatment, especially for compounds with complicated structure such as diltiazem. During the UV/H2O2 treatment, the intermediate products include tertiary amine, dimethyl amine (DMA) or DMA-like structures, which are N-nitrosodimethylamine (NDMA) precursors after chlorination or chloramination. Furthermore, it was observed that using dissolved organic nitrogen and DMA to predict NDMAFP could lead to biased conclusions because of the complex nature of nitrogenous matters in aqueous environments.  相似文献   

5.
The main disadvantage of using iron mineral in Fenton-like reactions is that the decomposition rate of organic contaminants is slower than in classic Fenton reaction using ferrous ions at acidic pH. In order to overcome these drawbacks of the Fenton process, chelating agents have been used in the investigation of Fenton heterogeneous reaction with some Fe-bearing minerals. In this work, the effect of new iron complexing agent, ethylenediamine-N,N'-disuccinic acid (EDDS), on heterogeneous Fenton and photo-Fenton system using goethite as an iron source was tested at circumneutral pH. Batch experiments including adsorption of EDDS and bisphenol A (BPA) on goethite, H2O2 decomposition, dissolved iron measurement, and BPA degradation were conducted. The effects of pH, H2O2 concentration, EDDS concentration, and goethite dose were studied, and the production of hydroxyl radical (?OH) was detected. The addition of EDDS inhibited the heterogeneous Fenton degradation of BPA but also the formation of ?OH. The presence of EDDS decreases the reactivity of goethite toward H2O2 because EDDS adsorbs strongly onto the goethite surface and alters catalytic sites. However, the addition of EDDS can improve the heterogeneous photo-Fenton degradation of BPA through the propagation into homogeneous reaction and formation of photochemically efficient Fe-EDDS complex. The overall effect of EDDS is dependent on the H2O2 and EDDS concentrations and pH value. The high performance observed at pH 6.2 could be explained by the ability of O 2 ?? to generate Fe(II) species from Fe(III) reduction. Low concentrations of H2O2 (0.1 mM) and EDDS (0.1 mM) were required as optimal conditions for complete BPA removal. These findings regarding the capability of EDDS/goethite system to promote heterogeneous photo-Fenton oxidation have important practical implications for water treatment technologies.  相似文献   

6.
The paper presents results of the studies photodegradation, photooxidation, and oxidation of phenylarsonic acid (PAA) in aquatic solution. The water solutions, which consist of 2.7 g dm?3 phenylarsonic acid, were subjected to advance oxidation process (AOP) in UV, UV/H2O2, UV/O3, H2O2, and O3 systems under two pH conditions. Kinetic rate constants and half-life of phenylarsonic acid decomposition reaction are presented. The results from the study indicate that at pH 2 and 7, PAA degradation processes takes place in accordance with the pseudo first order kinetic reaction. The highest rate constants (10.45?×?10?3 and 20.12?×?10?3) and degradation efficiencies at pH 2 and 7 were obtained at UV/O3 processes. In solution, after processes, benzene, phenol, acetophenone, o-hydroxybiphenyl, p-hydroxybiphenyl, benzoic acid, benzaldehyde, and biphenyl were identified.  相似文献   

7.
臭氧氧化及其他强化技术协同降解聚乙烯醇   总被引:3,自引:1,他引:3  
采用O3氧化降解水中聚乙烯醇(PVA),考察了O3氧化的影响因素及与其他强化技术协同下的降解效果。结果表明,经12 min处理,O3/超声波、O3/紫外光协同作用下PVA降解率较直接O3氧化的63.2%有显著提高,表现出了良好的协同效应。通过比较酸性条件下添加不同量Fenton试剂的作用效果可知,·OH的氧化作用是PVA降解的重要原因。  相似文献   

8.

A theoretical and experimental study of bisphenol A (BPA) degradation by the UV/H2O2 process in water is presented. The effects of the H2O2 concentration and the specific rate of photon emission (EP,0) on BPA degradation were investigated. A kinetic model derived from a reaction sequence was employed to predict BPA and hydrogen peroxide concentrations over time using an annular photochemical reactor in batch recirculation mode. The local volumetric rate of photon absorption (LVRPA) inside the photoreactor was computed using a Line Source with Parallel Plane emission model (LSPP). From the proposed kinetic model and the experimental data, the second order rate constants of the reactions between hydroxyl radicals and the main reacting species (H2O2 and BPA) were estimated applying a nonlinear regression method. A good agreement between the kinetic model and experimental data, for a wide range of operating conditions, was obtained. For BPA, H2O2, and TOC concentrations, the calculated root means square errors (RMSE) were 2.3?×?10??2, 9.8?×?10??1, and 9.0?×?10??2 mmol L??1, respectively. The simplified kinetic model presented in this work can be directly applied to scaling-up and reactor design, since the estimated kinetic constants are independent of the reactor size, shape, and configuration. Further experiments were made by employing low BPA initial concentration (100 μg L??1) in water and real wastewater. A lower degradation rate of BPA was observed in the real wastewater, although the UV/H2O2 process has also been able to completely degrade the target pollutant in less than 1 h.

  相似文献   

9.
In this study, an enhanced sono-Fenton process for the degradation of alachlor is presented. At high ultrasonic power, low pH, and in the presence of adequate Fenton's reagent dosages, alachlor degradation can reach nearly 100%. The toxicity of treated alachlor wastewater, which was measured by changes in cell viability, slightly decreased after the Fenton or ultrasound/H2O2 process and significantly decreased after the enhanced sono-Fenton process. A satisfactory relationship was observed between the total organic carbon removal and cell viability increment, indicating that alachlor mineralization is a key step in reducing the toxicity of the solution. The formation of alachlor degradation byproducts was observed during the oxidation process, in which the first step was the substitution of a chloride by a hydroxyl group. In conclusion, the enhanced sono-Fenton process was effective in the degradation and detoxification of alachlor within a short reaction time. Thus, the treated wastewater can then be passed through a biological treatment unit for further treatment.  相似文献   

10.
The Fenton-like degradation of nalidixic acid was studied in this work. The effects of Fe3+ concentration and initial H2O2 concentration were investigated. Increasing the initial H2O2 concentration enhances the degradation and mineralization efficiency for nalidixic acid, while Fe3+ shows an optimal concentration of 0.25 mM. A complete removal of nalidixic acid and a TOC removal of 28 % were achieved in 60 min under a reaction condition of [Fe3+]?=?0.25 mM, [H2O2]?=?10 mM, T?=?35 °C, and pH?=?3. LC–MS analysis technique was used to analyze the possible degradation intermediates. The degradation pathways of nalidixic acid were proposed according to the identified intermediates and the electron density distribution of nalidixic acid. The Fenton-like degradation reaction of nalidixic acid mainly begins with the electrophilic attack of hydroxyl radical towards the C3 position which results in the ring-opening reaction; meanwhile, hydroxyl radical attacking to the branched alkyl groups of nalidixic acid leads to the oxidation at the branched alkyl groups.  相似文献   

11.
In the present study, selected advanced oxidation processes (AOPs)—namely, photo-Fenton (with Fe2+, Fe3+, and potassium ferrioxalate—FeOx—as iron sources), solar photo-Fenton, Fenton, and UV/H2O2—were investigated for degradation of the antineoplastic drug mitoxantrone (MTX), frequently used to treat metastatic breast cancer, skin cancer, and acute leukemia. The results showed that photo-Fenton processes employing Fe(III) and FeOx and the UV/H2O2 process were most efficient for mineralizing MTX, with 77, 82, and 90 % of total organic carbon removal, respectively. MTX probably forms a complex with Fe(III), as demonstrated by voltammetric and spectrophotometric measurements. Spectrophotometric titrations suggested that the complex has a 2:1 Fe3+:MTX stoichiometric ratio and a complexation constant (K) of 1.47 × 104 M–1, indicating high MTX affinity for Fe3+. Complexation partially inhibits the involvement of iron ions and hence the degradation of MTX during photo-Fenton. The UV/H2O2 process is usually slower than the photo-Fenton process, but, in this study, the UV/H2O2 process proved to be more efficient due to complexing of MTX with Fe(III). The drug exhibited no cytotoxicity against NIH/3T3 mouse embryonic fibroblast cells when oxidized by UV/H2O2 or by UV/H2O2/FeOx at the concentrations tested.  相似文献   

12.
In this study, a three-factor, three-level Box-Behnken design with response surface methodology were used to maximize the TOC removal and minimize the H2O2 residual in the effluent of the combined UV-C/H2O2-VUV system for the treatment of an actual slaughterhouse wastewater (SWW) collected from one of the meat processing plants in Ontario, Canada. The irradiation time and the initial concentrations of total organic carbon (TOCo) and hydrogen peroxide (H2O2o) were the three predictors, as independent variables, studied in the design of experiments. The multiple response approach was used to obtain desirability response surfaces at the optimum factor settings. Subsequently, the optimum conditions to achieve the maximum percentage TOC removal of 46.19% and minimum H2O2 residual of 1.05% were TOCo of 213 mg L?1, H2O2o of 450 mg L?1, and irradiation time of 9 min. The attained optimal operating conditions were validated with a complementary test. Consequently, the TOC removal of 45.68% and H2O2 residual of 1.03% were achieved experimentally, confirming the statistical model reliability. Three individual processes, VUV alone, VUV/H2O2, and UV-C/H2O2, were also evaluated to compare their performance for the treatment of the actual SWW using the optimum parameters obtained in combined UV-C/H2O2-VUV processes. Results confirmed that an adequate combination of the UV-C/H2O2-VUV processes is essential for an optimized TOC removal and H2O2 residual. Finally, respirometry analyses were also performed to evaluate the biodegradability of the SWW and the BOD removal efficiency of the combined UV-C/H2O2-VUV processes.  相似文献   

13.
In this study, photocatalytic (photo-Fenton and H2O2/UV) and dark Fenton processes were used to remove ethylenethiourea (ETU) from water. The experiments were conducted in a photo-reactor with an 80 W mercury vapor lamp. The mineralization of ETU was determined by total organic carbon analysis, and ETU degradation was qualitatively monitored by the reduction of UV absorbance at 232 nm. A higher mineralization efficiency was obtained by using the photo-peroxidation process (UV/H2O2). Approximately 77% of ETU was mineralized within 120 min of the reaction using [H2O2]0 = 400 mg L?1. The photo-Fenton process mineralized 70% of the ETU with [H2O2]0 = 800 mg L?1 and [Fe2+] = 400 mg L?1, and there is evidence that hydrogen peroxide was the limiting reagent in the reaction because it was rapidly consumed. Moreover, increasing the concentration of H2O2 from 800 mg L?1 to 1200 mg L?1 did not enhance the degradation of ETU. Kinetics studies revealed that the pseudo-second-order model best fit the experimental conditions. The k values for the UV/H2O2 and photo-Fenton processes were determined to be 6.2 × 10?4 mg L?1 min?1 and 7.7 × 10?4 mg L?1 min?1, respectively. The mineralization of ETU in the absence of hydrogen peroxide has led to the conclusion that ETU transformation products are susceptible to photolysis by UV light. These are promising results for further research. The processes that were investigated can be used to remove pesticide metabolites from drinking water sources and wastewater in developing countries.  相似文献   

14.
The present research deals with the development of a new heterogeneous photocatalysis and Fenton hybrid system for the removal of color from textile dyeing wastewater as Rhodamine B (RhB) solutions by using Fe2+/H2O2/Nb2O5 as a photocatalytic system. The application of this photocatalytic system for the decolorization of dye contaminants is not reported in the literature yet. Different parameters like dye concentration, Nb2O5/Fe2+ catalyst amount, pH, and H2O2 concentration have been studied. The optimum conditions for the decolorization of the dye were initial concentration of 10 mg L?1 of dye, pH 4, and Nb2O5/Fe2+ catalyst concentration of 0.5 g L?1/50 mg L?1. The optimum value of H2O2 concentration for the conditions used in this study was 700 mg L?1. Moreover, the efficiency of the Nb2O5/photo-Fenton hybrid process in comparison to photo-Fenton alone and a dark Fenton process as a control experiment to decolorize the RhB solution has been investigated. The combination of photo-Fenton and Nb2O5 catalysts has been proved to be the most effective for the treatment of such type of wastewaters. The results revealed that the RhB dye was decolorized in a higher percent (78 %) by the Nb2O5/photo-Fenton hybrid process (Fe2+/H2O2/Nb2O5/UV) than by the photo-Fenton process alone (37 %) and dark Fenton process (14 %) after 120 min of treatment. Moreover, the Nb2O5 catalyst as a heterogeneous part of the photocatalytic system was demonstrated to have good stability and reusability.  相似文献   

15.
Phthalic acid esters (PAEs) are one kind of persistent organic pollutants. This study was conducted to investigate the effects of diethylphthalate (DEP) and di(2-ethyl)hexylphthalate (DEHP) with different concentrations (0, 30, 50, 100, and 200 mg L?1) on early seedling growth of Cucumis sativus L. Physiological, biochemical, and ultrastructure of seedling leaves were examined for 7-day exposure. The three antioxidant enzymes’ activities was stimulated at low-DEP treatments and decreased under higher levels (>200 mg L?1) compared to the controls. Furthermore, MDA and H2O2 gradually enhanced with the elevation of DEP and DEHP concentration. Significant impact on the chloroplast and mitochondrion was visible, possibly as a consequence of free radical generation. DEP induced bigger and more starch grains in chloroplasts than DEHP. This study concluded that the effects of DEP and DEHP on cucumber seedlings represented the adverse impacts of DEP and DEHP on the ecosystem and agricultural production. The environmental harm caused by DEP was severer than DEHP.  相似文献   

16.
A new method for the degradation of bisphenol A (BPA) in aqueous solution was developed. The oxidative degradation characteristics of BPA in a heterogeneous Fenton reaction catalyzed by Fe3O4/graphite oxide (GO) were studied. Transmission electron microscopic images showed that the Fe3O4 nanoparticles were evenly distributed and were ~6 nm in diameter. Experimental results suggested that BPA conversion was affected by several factors, such as the loading amount of Fe3O4/GO, pH, and initial H2O2 concentration. In the system with 1.0 g L?1 of Fe3O4/GO and 20 mmol L?1 of H2O2, almost 90 % of BPA (20 mg L?1) was degraded within 6 h at pH 6.0. Based on the degradation products identified by GC–MS, the degradation pathways of BPA were proposed. In addition, the reused catalyst Fe3O4/GO still retained its catalytic activity after three cycles, indicating that Fe3O4/GO had good stability and reusability. These results demonstrated that the heterogeneous Fenton reaction catalyzed by Fe3O4/GO is a promising advanced oxidation technology for the treatment of wastewater containing BPA.  相似文献   

17.
The oxidative degradation of imidacloprid (ICP) has been carried out by electrochemical advanced oxidation processes (EAOPs), anodic oxidation, and electro-Fenton, in which hydroxyl radicals are generated electrocatalytically. Carbon-felt cathode and platinum or boron-doped diamond (BDD) anodes were used in electrolysis cell. To determine optimum operating conditions, the effects of applied current and catalyst concentration were investigated. The decay of ICP during the oxidative degradation was well fitted to pseudo-first-order reaction kinetics and absolute rate constant of the oxidation of ICP by hydroxyl radicals was found to be k abs(ICP)?=?1.23?×?109 L mol?1 s?1. The results showed that both anodic oxidation and electro-Fenton process with BDD anode exhibited high mineralization efficiency reaching 91 and 94 % total organic carbon (TOC) removal at 2 h, respectively. For Pt-EF process, mineralization efficiency was also obtained as 71 %. The degradation products of ICP were identified and a plausible general oxidation mechanism was proposed. Some of the main reaction intermediates such as 6-chloronicotinic acid, 6-chloronicotinaldehyde, and 6-hydroxynicotinic acid were determined by GC-MS analysis. Before complete mineralization, formic, acetic, oxalic, and glyoxylic acids were identified as end-products. The initial chlorine and organic nitrogen present in ICP were found to be converted to inorganic anions Cl?, NO3 ?, and NH4 +.  相似文献   

18.
The treatment of 1,4-dioxane solution by electrochemical oxidation on boron-doped diamond was studied using a central composite design and the response surface methodology to investigate the use of SO4 2? and HCO3 ? as supporting electrolytes considering the applied electric current, initial chemical oxygen demand (COD) value, and treatment time. Two industrial effluents containing bicarbonate alkalinity, one just carrying 1,4-dioxane (S1), and another one including 1,4-dioxane and 2-methyl-1,3-dioxolane (S2), were treated under optimized conditions and subsequently subjected to biodegradability assays with a Pseudomonas putida culture. Electrooxidation was compared with ozone oxidation (O3) and its combination with hydrogen peroxide (O3/H2O2). Regarding the experimental design, the optimal compromise for maximum COD removal at minimum energy consumption was shown at the maximum tested concentrations of SO4 2? and HCO3 ? (41.6 and 32.8 mEq L?1, respectively) and the maximum selected initial COD (750 mg L?1), applying a current density of 11.9 mA cm?2 for 3.8 h. Up to 98 % of the COD was removed in the electrooxidation treatment of S1 effluent using 114 kWh per kg of removed COD and about 91 % of the COD from S2 wastewater applying 49 kWh per kg of removed COD. The optimal biodegradability enhancement was achieved after 1 h of electrooxidation treatment. In comparison with O3 and O3/H2O2 alternatives, electrochemical oxidation achieved the fastest degradation rate per oxidant consumption unit, and it also resulted to be the most economical treatment in terms of energy consumption and price per unit of removed COD.  相似文献   

19.
A Fenton oxidation system employing zero-valent iron (whose source was swarf, a residue of metallurgical industries, in powder form) and hydrogen peroxide for the treatment of an aqueous solution with six pesticides was developed, and the effect of the iron metal content, pH, and hydrogen peroxide concentration was evaluated. The characterization of the aqueous solution resulted in: pH 5.6, 105 mg L?1 of dissolved organic carbon, and 44.6 NTU turbidity. In addition, the characterization of the swarf by FAAS and ICP-MS showed 98.43?±?7.40 % of zero-valent iron. The removal was strongly affected by the content of iron metal, pH, and hydrogen peroxide concentration. The best degradation conditions were 2.0 g swarf, pH 2.0, and 5 mmol L?1 H2O2. At the end of the treatment, the pesticide degradation ranged from 60 to 100 %, leading to 55 % mineralization. Besides, all hydrogen peroxide was consumed and the determination of total dissolved iron resulted in 2 mg L?1. Thus, the advantages of this system are rapid degradation (up to 20 min), high-degradation rates, simple handling, and low cost.
Figure
A Fenton oxidation system employing Fe0 (in which the source of Fe0 was swarf, a residue in powder form of metallurgical industries) and H2O2 for the degradation of synthetic wastewater comprising six pesticides was developed, and the effect of the amount of Fe0, pH, and H2O2 concentration was evaluated.  相似文献   

20.
The degradation of 230 mL of a 0.6-mM sulfanilamide solution in 0.05 M Na2SO4 of pH 3.0 has been studied by electro-Fenton process. The electrolytic cell contained either a Pt or boron-doped diamond (BDD) anode and a carbon-felt cathode. Under these conditions, organics are oxidized by hydroxyl radicals formed at the anode surface from water oxidation and in the bulk from Fenton’s reaction between initially added (and then electrochemically regenerated) Fe2+ and cathodically generated H2O2. From the decay of sulfanilamide concentration determined by reversed-phase liquid chromatography, an optimum Fe2+ concentration of 0.20 mM in both cells was found. The drug disappeared more rapidly using BDD than Pt, and, in both cases, it was more quickly removed with raising applied current. Almost total mineralization was achieved using the BDD/carbon-felt cell, whereas the alternative use of Pt anode led to a slightly lower mineralization degree. In both cells, the degradation rate was accelerated at higher current but with the concomitant fall of mineralization current efficiency due to the greater increase in rate of the parasitic reactions of hydroxyl radicals. Reversed-phase liquid chromatography allowed the identification of catechol, resorcinol, hydroquinone, p-benzoquinone, and 1,2,4-trihydroxybenzene as aromatic intermediates, whereas ion exclusion chromatography revealed the formation of malic, maleic, fumaric, acetic, oxalic, formic, and oxamic acids. NH4 +, NO3 ?, and SO4 2? ions were released during the electro-Fenton process. A plausible reaction sequence for sulfanilamide mineralization involving all detected intermediates has been proposed. The toxicity of the solution was assessed from the Vibrio fischeri bacteria luminescence inhibition. Although it acquired its maximum value at short electrolysis time, the solution was completely detoxified at the end of the electro-Fenton treatment, regardless of the anode used.  相似文献   

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