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1.
《分离科学与技术》2012,47(7):1521-1534
Abstract

Aqueous solutions of Acid Blue 74, Acid Orange 10, and Acid Violet 19 were subjected to Fenton/Fenton‐like oxidation and its combination with lime coagulation. The analysis indicated no dependence of chemical oxidation efficacy on dye concentration in the range of 0.1–1 g L?1. Complete or nearly complete (higher than 95%) color removal of all treated samples was observed. Dye:H2O2 weight ratio of 1∶2 proved optimal for treatment of all dye solutions by means of Fenton/Fenton‐like oxidation. Moderate doses of hydrogen peroxide led to the improvement of biodegradability of dye solutions. No formation of any toxic intermediates during the oxidation of Acid Orange 10 and Acid Violet 19 was detected. Only a slight toxicity increase was observed after Acid Blue 74 degradation by Fenton chemistry. H2O2/Fe3+ system with pH adjusted to 3 proved the most effective oxidation process. The combination of Fenton chemistry and subsequent lime coagulation was the most feasible treatment method of removing COD and UV254 and UVmax absorbance of dye solutions. Combined oxidation and coagulation was more effective for Acid Blue 74 and Acid Orange 10 elimination than for Acid Violet 19.  相似文献   

2.
BACKGROUND: The Fenton process is a popular advanced oxidation process (AOP) for treating textile wastewater. However, high consumption of chemical reagents and high production of sludge are typical problems when using this process and in addition, textile wastewater has wide‐ranging characteristics. Therefore, dynamically regulating the Fenton process is critical to reducing operation costs and enhancing process performance. The artificial neural network (ANN) model has been adopted extensively to optimize wastewater treatment. This study presents a novel Fenton process control strategy using ANN models and oxygen reduction potential (ORP) monitoring to treat two synthetic textile wastewaters containing two common dyes. RESULTS: Experimental results indicated that the ANN models can predict precisely the colour and chemical oxygen demand (COD) removal efficiencies for synthetic textile wastewaters with correlation coefficients (R2) of 0.91–0.99. The proposed control strategy based on these ANN models effectively controls the Fenton process for various effluent colour targets. For treating the RB49 synthetic wastewater to meet the effluent colour targets of 550 and 1500 ADMI units, the required Fe+2 doses were 13.0–84.3 and 5.5–34.6 mg L?1 (Fe+2/H2O2 = 3.0), resulting in average effluent colour values of 520 and 1494 units. On the other hand, an effluent colour target of 550 ADMI units was achieved for RBB synthetic wastewater. The required Fe+2 doses were 14.6–128.0 mg L?1; the average effluent colour values were 520 units. CONCLUSION: The Fenton process for textile wastewater treatment was effectively controlled using a control strategy applying the ANN models and ORP monitoring, giving the benefit of chemical cost savings. Copyright © 2009 Society of Chemical Industry  相似文献   

3.
BACKGROUND: Heterogeneous Fenton catalysts have been used to treat various organic pollutants in an aqueous environment. The present study has investigated the degradation of 2,4‐dinitrophenol (2,4‐DNP), a priority pollutant generated by such industries as pharmaceuticals, pesticides, pigments and dyes. Degradation of 2,4‐DNP (100 mg L?1) was studied using Fe3+ loaded on Al2O3 as a heterogeneous catalyst in the presence of H2O2, and the efficiency compared with the homogeneous Fe3+/H2O2 based Fenton‐like process. The effect of different parameters for both processes, such as catalyst loading, H2O2 concentration, initial solution pH, initial substrate concentration and temperature were investigated and the optimum operating conditions determined. RESULTS: Under optimal operating conditions of the homogeneous system ([Fe3+] 125 mg L?1; [H2O2] 250 mg L?1; pH 3; room temperature), 92.5% degradation was achieved in 35 min for an initial 2,4‐DNP concentration of 100 mg L?1. In the case of immobilized Fe (Fe3+–Al2O3 catalyst), degradation improved to 98.7% under the condition 10 wt% [Fe3+–Al2O3] 1 g L?1 catalyst loading; [H2O2] 250 mg L?1; pH 3; at room temperature for the same duration. CONCLUSIONS: This study demonstrated the stability and reusability of the prepared heterogeneous catalyst. This process is a viable technique for treatment of aqueous solutions containing contaminants. Copyright © 2012 Society of Chemical Industry  相似文献   

4.
《分离科学与技术》2012,47(14):2294-2303
ABSTRACT

In this study, the experiments were carried out to evaluate the effect of five independent variables on the Chemical Oxygen Demand (COD) removal in a pharmaceutical wastewater contaminated with sodium diclofenac. The parameters were statistically optimized under response surface mythology. The optimum conditions for 97.21% of COD removal experimentally were at reaction time of 59.68 min, current density of 58.47 mA/cm2, pH of 2.89, volume ratio of 0.32 ml/l and H2O2/Fe2+ molar ratio of 3.60.  相似文献   

5.
《分离科学与技术》2012,47(7):1597-1611
Abstract

Some advanced oxidation processes (AOP's) such as Fenton H2O2/Fe2+, photo assisted Fenton UV/H2O2/Fe2+, UV photolysis, and photo assisted Fenton—like UV/O2/Fe2+ have been tested for the degradation of Gemfibrozil in aqueous solution in a batch system and then in a membrane reactor. A nanofiltration/reverse osmosis type cross‐linked polyamide, UTC‐60 (Toray) membrane (19 cm2) was used. In the batch degradation tests, the gemfibrozil, used at 5 mg/L, was degraded by employing the four AOP's but numerous peaks of intermediates were observed at the HPLC. Indeed DOC analyses showed poor mineralization in the case of photolysis (3.1%) and UV/O2/Fe (10%), while it was 62% using the photo assisted Fenton and 24% using the Fenton. Thus in the membrane reactor only the Fenton and the photo assisted Fenton were tested. Obtained results showed a drug degradation higher than 92%, a mineralization higher than 55%, and a membrane retention of the catalyst in solution higher than 95%.  相似文献   

6.
BACKGROUND: The degradation and mineralisation of the antibiotic amoxicillin by photo‐Fenton reactions, mediated by artificial UVA or solar irradiation, were investigated. Experiments were conducted with 30 mg L?1 amoxicillin solutions prepared with deionised or surface water at Fe2+ and H2O2 concentrations in the range 0.0179–0.0895 and 1–10 mmol L?1, respectively. Black‐light irradiation at 365 nm was provided by a 13 W m?2 lamp, while samples were exposed to sunlight at 20 W m?2 for solar experiments. RESULTS: In all cases, quantitative amoxicillin degradation occurred within 5 min and this was accompanied by lower mineralisation rates. Mineralisation followed first‐order kinetics with respect to organic carbon content and it was not affected by the water matrix with either type of illumination. Solar‐induced reactions were only marginally faster than artificial irradiation. Increasing the H2O2 to Fe2+ concentration ratio increases the extent of mineralisation up to a point beyond which degradation is impeded due to radical scavenging associated with the high concentrations of the Fenton reagents. CONCLUSION: Amoxicillin is readily degradable by homogeneous photocatalysis, being converted to more stable intermediates as indicated by lower mineralisation rates. The process can be driven by solar irradiation, thus providing a sustainable treatment technology. Copyright © 2009 Society of Chemical Industry  相似文献   

7.
This study analyzes the performances of 2 methods of oxidation based on ozone, namely ozonation and ozone combined with hydrogen peroxide (O3/H2O2), on two biotreated municipal wastewater effluents. The main parameters monitored to evaluate the effectiveness of the processes were Chemical Oxygen Demand (COD), Dissolved Organic Carbon (DOC) and Biochemical Oxygen Demand (BOD5). Ozonation and O3/H2O2 treatment removed 44% and 48%, respectively, of the COD, after 90 min, of the secondary effluent of Calafell wastewater treatment plant (Spain). On the secondary effluent from the Grasse wastewater treatment plant (France), these same treatments (O3; O3/H2O2) achieved, respectively, a degradation of 52% and 100% of the COD after 60 min. The transferred ozone dose (TOD) during Calafell and Grasse effluents' ozonation were 122 mg·L?1 and 77 mg·L?1 after 90 min, respectively. A low removal of DOC was monitored during both O3 or O3/H2O2 treatments applied to Calafell wastewater, respectively 12% and 14%. Better DOC reductions were obtained on the water of Grasse treated with O3 or O3/H2O2, respectively, 48% and 60%. In addition, ammonia nitrogen was oxidized to nitrate nitrogen thus giving rise to an over ozone consumption. And finally, both processes proceeded with an increase of pH values. These results highlight the strong dependency of O3 or O3/H2O2 treatment effectiveness in terms of dissolved organic matter (DOM) removal and ozone consumption on wastewater composition (organic and inorganic substances).  相似文献   

8.
A Fenton‐like process, involving oxidation and coagulation, was evaluated for the removal of odorous compounds and treatment of a pulp and paper wastewater. The main parameters that govern the complex reactive system [pH and Fe(III) and hydrogen peroxide concentrations] were studied. Concentrations of Fe(III) between 100 and 1000 mg L?1 and of H2O2 between 0 and 2000 mg L?1 were chosen. The main mechanism for color removal was coagulation. The maximum COD, color and aromatic compound removals were 75, 98 and 95%, respectively, under optimal operating conditions ([Fe(III)] = 400 mg L?1; [H2O2] = 500–1000 mg L?1; pH = 2.5; followed by coagulation at pH 5.0). The biodegradability of the wastewater treated increased from 0.4 to 0.7 under optimal conditions and no residual hydrogen peroxide was found after treatment. However, partially or non‐oxidized compounds present in the treated wastewater presented higher acute toxicity to Artemia salina than the untreated wastewater. Based on the optimum conditions, pilot‐scale experiments were conducted and revealed a high efficiency in relation to the mineralization of organic compounds. Terpenes [(1S)‐α‐pinene, β‐pinene, (1R)‐α‐pinene and limonene] were identified in the wastewater and were completely eliminated by the Fenton‐like treatment. Copyright © 2006 Society of Chemical Industry  相似文献   

9.
《分离科学与技术》2012,47(7):1505-1520
Abstract

Fenton‐and Fenton‐like AOPs systems have been utilized for the oxidative degradation of some chlorinated pollutants such as chloral hydrate or 1,1,1‐trichloroethane, and for the treatment of real industrial wastewaters. Both ferrous sulfate (FeSO4 · 7 H2O) and Mohr's salt (NH4)2Fe(SO4)2. 6 H2O have been used as Fe2+ ion sources. With Mohr's salt (MS) the Fenton‐and Fenton‐like reaction has been successfully carried out under acidic (pH 3) and neutral (pH 7) reaction conditions. The new Fenton‐like system utilizes zero‐valent iron (Feo) instead of ferrous sulfate has been applied for the 1,1,1‐trichloroethane and chloral hydrate degradation. Similarly, the application of catechol‐ and hydroquinone‐driven Fenton reaction for the degradation of chloral hydrate under acidic and neutral pH is a new Fenton‐like AOPs approach. The photo‐Fenton‐like reactions such as Fe3+/hν, Fe2+/H2O2/hν, and ferrioxalate system have been also studied for the degradation of chloral hydrate. As an irradiation source a daily light or sun light have been used. In comparison with photoreactor experiments the best system was observed to be Fe3+/hν. In some experiments the influence of standing time prolongation after Fenton reaction on the final degradation efficiency due to hydrolysis of intermediates such as phosgene (CCl2?O) has also been studied. The Fenton reaction was successfully utilized for the treatment of real industrial wastewaters, in two cases even in plant‐scale applications.  相似文献   

10.
BACKGROUND: A mesoporous alumina supported nanosized Fe2O3 was prepared through an original synthesis procedure and used as a heterogeneous catalyst for the Fenton process degradation of the model azo dye C.I. Acid Orange 7 enhanced by ultrasound irradiation (US/Fe2O3‐Al2O3‐meso/H2O2 system). The effect of various operating conditions was investigated, namely hydrogen peroxide concentration, initial pH, ultrasonic power and catalyst loading. RESULTS: The results indicated that the degradation of C.I. Acid Orange 7 followed a pseudo‐first‐order kinetic model. There exists an optimal hydrogen peroxide concentration, initial pH, ultrasonic power and catalyst loading for decolorization. The aggregate size of the spent catalyst was reduced after dispersion in water by ultrasonic irradiation. A very low level of iron leaching was observed ranging from < 0.1 to 0.23 mg L?1. The intermediate products of C.I. Acid Orange 7 degradation were identified using gas chromatography–mass spectrometry (GC‐MS). CONCLUSION: The optimal conditions for efficient C.I. Acid Orange 7 degradation were pH close to 3, hydrogen peroxide concentration 4 mmol L?1, catalyst loading 0.3 g L?1, and ultrasonic power 80 W. Copyright © 2011 Society of Chemical Industry  相似文献   

11.
BACKGROUND: Microwave‐enhanced advanced oxidation processes with and without the addition of ferrous sulfate (MW/H2O2/Fe2+‐AOP and MW/H2O2‐AOP respectively) were studied for reduction of solids and solubilisation of nutrients from secondary sewage sludge. RESULTS: For the MW/H2O2/Fe2+‐AOP the yields of solubilisation of orthophosphate and ammonia decreased with increasing temperature. The best results (88.1 mg L?1 for orthophosphate and 22.7 mg L?1 for ammonia) were obtained at a treatment temperature of 40 °C. In contrast, the MW/H2O2‐AOP had an advantage when it was operated at higher temperatures of 60 and 80 °C. The highest yields of solubilisation were obtained at 60 °C for orthophosphate (81.1 mg L?1) and at 80 °C for both ammonia (35.0 mg L?1) and soluble chemical oxygen demand (1954 mg L?1). Over the temperature range used in this study, the MW/H2O2‐AOP gave a better performance than the MW/H2O2/Fe2+‐AOP. CONCLUSION: For sewage sludge treatment the MW/H2O2‐AOP is more effective than the MW/H2O2/Fe2+‐AOP in terms of solid reduction and nutrient solubilisation. It will also be more cost‐effective, as it does not require iron addition in the process. Copyright © 2008 Society of Chemical Industry  相似文献   

12.
Wastewater sludge usually contains large amounts of water and organic materials; therefore, its stabilization and dewatering are of particular importance. The present study aimed to investigate the possibility of sludge stabilization and dewatering from wastewater sludge by bioleaching (Thiobacillus ferrooxidans), Fenton/bioleaching, and bioleaching/Fenton-like processes. To evaluate sludge stabilization and dewatering, specific resistance to filtration (SRF), volatile suspended solids (VSS), total suspended solids (TSS), and soluble chemical oxygen demand (SCOD) were measured. In biological treatment with T. ferrooxidans with Fe2+ (2?g?L?1), 99.75, 33, 37, and 72% reduction were observed in SRF, VSS, TSS, SCOD, respectively, after 2 days. In the combined treatment of Fenton before bioleaching (including Fe2+ 2?g?L?1 and H2O2 1?g?L?1 with Fenton oxidation for 30?min followed by biological treatment with T. ferrooxidans for 2 days), the reduction rates in TSS, VSS, SCOD, and SRF were 40.18, 40.88, 60.95, and 75.43%, respectively. In treatment with the combined method of bioleaching before Fenton-like oxidation, the removal rates of the aforementioned parameters were 52.5, 54.4, 88, and 99.82%, respectively. In comparison to Fenton oxidation and bioleaching alone, combined biological method of bioleaching/Fenton-like oxidation using a lower dose of H2O2 and Fe2+ significantly improved sludge dewatering and stabilization.  相似文献   

13.
In the present study, Fenton and sono‐Fenton processes were applied to the oxidative decolorisation of synthetic textile wastewater including CI Reactive Orange 127 and polyvinyl alcohol. Process optimisation [pH, ferrous ion (Fe2+) and hydrogen peroxide (H2O2)], kinetic studies and their comparison were carried out for both of the processes. The sono‐Fenton process was performed by indirect sonication in an ultrasonic water bath, which was operated at a fixed 35‐kHz frequency and 80 W power. The optimum conditions were determined as [Fe2+] = 20 mg l?1, [H2O2] = 15 mg l?1 and pH = 3 for the Fenton process and [Fe2+] = 25 mg l?1, [H2O2] = 5 mg l?1 and pH = 3 for the sono‐Fenton process. The colour removals were 89.9% and 91.8% by the Fenton and sono‐Fenton processes, respectively. The highest decolorisation was achieved by the sono‐Fenton process because of the production of some oxidising agents as a result of sonication. Consequently, ultrasonic irradiation in the sono‐Fenton process slightly increased the colour removal to 91.8%, while decreasing the hydrogen peroxide dosage to one‐third of that of the Fenton process.  相似文献   

14.
A coupled O3/Fenton process is applied to study the degradation ef?ciency of organic pollutants. The C.I. Acid Blue 80 (AB80), a kind of anthraquinone dye, is used as target contaminant. The results show that the combination of ozonation and Fenton process is a highly effective way of removing color from wastewater. Response surface methodology is applied to optimize the working conditions and the effects and interactions among initial pH (X1), mole ratio of H2O2/Fe2+ (X2) and ozone flux (X3) are investigated. Regression equations determines that the best condition is that initial pH = 2.85, [H2O2]/[Fe2+] = 18.10 and ozone flux = 55.70 L.h?1. It turns out the relative error of 1.32% with the predicted model when the actual value which is 88.76% in the best condition, compared to the predictive value of 88.95% under same condition. UV-Vis and FT-IR analysis are used as an assisted technique to study degradation mechanism during the oxidation process. The intermediate products are determined by gas chromatography/mass spectrometry (GC/MS) analysis and the plausible degradation pathway is proposed.  相似文献   

15.
An initial set of 12 kinetic experiments was carried out to remove naphthalene from an aqueous effluent by photo-Fenton involving Fe0 and Fe2+ at two different concentrations of H2O2 (150 and 300?mg?L?1) and three different pHs (3, 5, and 7) (22×31 experiments). The rate constants (k) for the reaction of naphthalene degradation by involving Fe2+ as reactant were in general higher than those with Fe0, but the use of Fe2+ increased the concentration of naphthalene at equilibrium (Ce) when compared with the same response obtained with Fe0 at analogous conditions. A second set of twelve kinetic experiments of photo-Fenton degradation was also performed with persulfate as additive at the conditions already reported, but at a constant concentration of H2O2 of 150?mg?L?1 (21×31 experiments with NaCl +21×31 experiments without NaCl). In almost all the runs in which only the source of iron was varied, k from the kinetic data involving Fe2+ was higher than that involving Fe0, but no difference was observed in terms of Ce that was always zero. The addition of persulfate to treat the effluent either containing or not containing salt enhanced the chemical kinetics, and shifted the equilibrium toward the full removal of naphthalene. A final set of nine experiments of UV photo degradation of naphthalene by involving persulfate without iron, with Fe0 and Fe2+ in the pH range from 3 to 7 (32 experiments) mainly showed that the use of H2O2 may be avoided to remove rapidly and completely naphthalene from wastewater.  相似文献   

16.
The performance and economic cost of the removal of phenol with TiO2 photocatalysis, photo‐Fenton reactions, biological aerated filter (BAF), and constructed wetland (CW) reactors has been studied. The BAF achieved complete removal with a maximum phenol concentration of 200 mg·L?1. The BAF‐CW combination provided a phenol‐free effluent with a maximum phenol concentration of 650 mg·L?1. In both cases, a complete detoxification of the treated water was achieved at the concentrations studied. The efficiency of TiO2 photocatalysis was limited to concentrations below 50 mg L?1 to minimize removal reduction and toxicity of the intermediates. Photo‐Fenton was more efficient, but also more expensive because of the high cost of H2O2. The photo‐Fenton‐BAF combination is proposed to be the most suitable one.  相似文献   

17.
BACKGROUND: The discharge of azo dyes into the environment poses concerns due to their limited biodegradability. The electro‐Fenton process (EF) is a good method to effectively degrade these dyes. The aim of this work was to study the mechanism and the feasibility of the EF reaction using an activated carbon fibre (ACF) cathode. In this study, two methods were used to measure the reactive species generated in anodic oxidation (AO), anodic oxidation with electrogenerated H2O2 (AO‐H2O2) and the EF process. Acid Red 14 (AR14) was chosen as a model pollutant. The effects of the operational parameters, pH and initial concentrations were investigated. A short‐term biodegradability test was also carried out to evaluate the EF process from a biological point of view. RESULTS: After 2 h EF reaction 118.7 µmol L?1?OH were produced, which was much higher than that of the AO‐H2O2 (63.2 µmol L?1) process. H2O2 is largely generated and Fe3+ efficiently reduced on the high surface area of the ACF cathode. The EF process provides more effective degradation of AR14 than the conventional Fenton process, and its current efficiency is significantly affected by the initial pH and the initial AR14 concentration. Following EF treatment, the biodegradability of AR14 is significantly increased. CONCLUSION: The higher formation of ?OH in the EF process suggests it is an effective method for pollutant removal. This process also leads to increased biodegradability, which is expected to facilitate subsequent biological treatment. Copyright © 2010 Society of Chemical Industry  相似文献   

18.
Humic acids are often found in surface and ground waters as a result of organic matter decay. In this study, water samples containing 50 mgL?1 humic acid were treated by conventional application of coagulation/flocculation technique. The results showed 70% ±10 turbidity, ≥82% ±10 UV254 absorbance and 85% ±10 total organic carbon removal under pH 5–9 and above 5 mgL?1 Fe3+ coagulant doses. Application of post-ozonation significantly increased the UV254 absorbance and turbidity removal under low dose Fe3+ application. On the other hand ozonation prior to coagulation/flocculation process altered the structure of HA and caused no significant improvement in removal efficiencies.  相似文献   

19.
Fe2-xYxW3O12 powder has been synthesized by the citrate sol-gel process. A model was proposed to calculate the concentration of species in a citric solution. The calculated results could provide valuable information for determining the optimal molar ratio of cation to citric acid and pH value of solution for Fe2-xYxW3O12 preparation. The predicted parameters derived from this model are in good agreement with the experimental results. The prepared gel and the Fe2-xYxW3O12 powder were characterized by X-ray diffraction (XRD) and differential thermal analysis-thermogravimetry (DTA-TG). The results show that it is very difficult to obtain pure Fe2W3O12 powder by the citrate sol-gel process in the temperature range 500°–1000°C, however, Y2W3O12 can easily be prepared even at 500°C. Y2W3O12 annealed at 1000°C for 10 h is favorable for absorbing moisture in air to form Y2W3O12·3.3H2O. The thermal expansion coefficients of Y2W3O12·3.3H2O are: αa = ? 8.01 × 10?6°C?1, αb = ? 2.51 × 10?7°C?1, and αc = ? 5.55 × 10?6°C?1 in 473–1173 K.  相似文献   

20.
In this study, phenol, aromatic, and non‐biodegradable organic matter were investigated and found to be removed from the model solution through chemical oxidation using Fenton reagent. The effects of the initial phenol concentration, hydrogen peroxide, and ferrous sulfate concentrations on the removal efficiency were investigated. Performance of the chemical oxidation process was monitored with phenol and COD (Chemical Oxygen Demand) analyses. In the experimental studies, phenol removal of over 98 % and COD removal of nearly 70 % were achieved. The optimum conditions for Fenton reaction both for initial phenol concentrations of 200 and 500 mg/L were found at a ratio [Fe2+]/[H2O2] (mol/mol) equal to 0.11. According to the results, chemical oxidation using Fenton reagent was found to be too effective, especially for phenol removal. However, this method has limited removal efficiency for COD.  相似文献   

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