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1.
The present work compares the efficiency of homogenous Fenton and photo-Fenton processes in the presence of Fe(III)–EDDS complex under different experimental conditions. 4-tert-Butylphenol (4-t-BP), which is one of the endocrine disrupting chemicals, was used as a model pollutant to investigate the Fenton and photo-Fenton application. The efficiency of homogenous photo-Fenton process was significantly much higher than homogenous Fenton process, which is due to the rapid formation of Fe2+ under UV irradiation of the iron complex and the photochemical formation of HO? from the photolysis of the complex Fe(III)–EDDS. Through the degradation of 4-t-BP, the effect of Fe(III)–EDDS concentration, H2O2 concentration, pH, and oxygen was investigated in both processes. Such trend was also correlated with pH calculating the polychromatic Fe2+ quantum yield formation at pH 4.0, 6.0, and 8.6. The results showed that at high Fe(III)–EDDS and H2O2 concentrations, a negative effect was found. By the way, the Fenton process was found to be enhanced at basic pH. These results can be very useful for the use and optimization of such iron complex in water treatment process as function of different physico-chemical conditions.  相似文献   

2.
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   

3.
This work is first intended to optimize the experimental conditions for the maximum degradation of guaiacol (2-methoxyphenol) by Fenton’s reagent, and second, to improve the process efficiency through the use of solar radiation. Guaiacol is considered as a model compound of pulp and paper mill effluent. The experiments were carried out in a laboratory-scale reactor subjected or not to solar radiation. Hydrogen peroxide solution was continuously introduced into the reactor at a constant flow rate. The kinetics of organic matter decay was evaluated by means of the chemical oxygen demand (COD) and the absorbance measurements. The experimental results showed that the Fenton and solar photo-Fenton systems lead successfully to 90% elimination of COD and absorbance at 604 nm from a guaiacol solution under particular experimental conditions. The COD removal always obeyed a pseudo-first-order kinetics. The effect of pH, temperature, H2O2 dosing rate, initial concentration of Fe2+, and initial COD was investigated using the Fenton process. The solar photo-Fenton system needed less time and consequently less quantity of H2O2. Under the optimum experimental conditions, the solar photo-Fenton process needs a dose of H2O2 40% lower than that used in the Fenton process to remove 90% of COD.  相似文献   

4.
研究了1%和10%(V/V)模拟正丙醇废水在UV/TiO2体系、UV/H2O2体系、Fe2+/H2O2体系和UV/TiO2/Fe2+/H2O2体系等4种工艺条件下的降解动力学过程,对比了降解动力学特点及工艺参数对动力学常数的影响,优化工艺参数。结果表明,UV/TiO2体系和Fe2+/H2O2体系的降解过程可分为零级反应阶段和一级反应阶段,转折点分别在反应开始后2 h和氧化剂浓度为6.7 g/L,UV/H2O2体系和UV/TiO2/Fe2+/H2O2体系分别符合零级反应和一级反应规律;相同工艺参数条件下,6 h反应后,组合工艺UV/TiO2/Fe2+/H2O2体系在处理效率达85%,比前3个体系分别高52.0%、8.3%和32.0%,与UV/TiO2体系和Fe2+/H2O2体系的处理效率之和持平,其协同效应提高了速率常数,在目标物浓度降低时依然可维持较高降解速率。而目标物浓度提高10倍后,UV能量利用率提高35.5倍,氧化剂用量是Fe2+/H2O2体系的1/7.1。  相似文献   

5.
Novel photo-Fenton catalysts were prepared by immobilizing iron species on commercial bentonite plates via two methods: (1) ion exchange reaction (Fe3+ vs. Na+) by aqueous suspension powder-clay/FeCl3 followed by plate preparation, and (2) forced hydrolysis of Fe(NO3)3 onto a prefabricated clay plate. The last method led to a more photo-active Fe-oxide/bentonite plate. This material allowed, at a non-adjusted initial pH of 5.5 and in the presence of H2O2, the total degradation of resorcinol and 55% mineralization in 80 and 100 min of irradiation, respectively. The reached degradation percentages were correlated to the presence of dissolved iron, demonstrating that in these processes, the homogeneous photo-Fenton reactions were mainly responsible for the resorcinol elimination.Likewise, in slurry system, where clay has normally an increased surface area, there was no increase in activity because of a reduced leached iron probably due to the diminished light penetration in the suspension. Despite the lower surface area, in comparison to that of the slurry, the clay plates have the advantage, as heterogeneous photo-catalysts, that separation of the reaction media after treatment is not needed, and thus, a potential use for batch and continuous reaction systems is proposed.  相似文献   

6.
The application of advanced oxidation process (AOP) in the treatment of wastewater contaminated with oil was investigated in this study. The AOP investigated is the homogeneous photo-Fenton (UV/H2O2/Fe+2) process. The reaction is influenced by the input concentration of hydrogen peroxide H2O2, amount of the iron catalyst Fe+2, pH, temperature, irradiation time, and concentration of oil in the wastewater. The removal efficiency for the used system at the optimal operational parameters (H2O2?=?400 mg/L, Fe+2?=?40 mg/L, pH?=?3, irradiation time?=?150 min, and temperature?=?30 °C) for 1,000 mg/L oil load was found to be 72 %. The study examined the implementation of artificial neural network (ANN) for the prediction and simulation of oil degradation in aqueous solution by photo-Fenton process. The multilayered feed-forward networks were trained by using a backpropagation algorithm; a three-layer network with 22 neurons in the hidden layer gave optimal results. The results show that the ANN model can predict the experimental results with high correlation coefficient (R 2?=?0.9949). The sensitivity analysis showed that all studied variables (H2O2, Fe+2, pH, irradiation time, temperature, and oil concentration) have strong effect on the oil degradation. The pH was found to be the most influential parameter with relative importance of 20.6 %.  相似文献   

7.
Maezono T  Tokumura M  Sekine M  Kawase Y 《Chemosphere》2011,82(10):1422-1430
Dynamic behaviors of hydroxyl (OH) radical generation and consumption in photo-Fenton oxidation process were investigated by measuring OH radical concentration during the discoloration of azo-dye Orange II. The effects of operating parameters for photo-Fenton discoloration, i.e. dosages of H2O2 and Fe, initial dye concentration, solution pH and UV irradiation, on the generation and consumption of OH radicals playing the main role in advanced oxidation processes were extensively studied. The scavenger probe or trapping technique in which coumarin is scavenger of OH radical was applied to estimate OH radical concentration in the photoreactor during the photo-Fenton discoloration process. The OH radical generation was enhanced with increasing the dosages of Fenton regents, H2O2 and Fe. At the initial stage of photo-Fenton discoloration of Orange II, the OH radical concentration rapidly increased (Phase-I) and the OH radical concentration decreased after reaching of OH radical concentration at maximum value (Phase-II). The decrease in OH radical concentration started when the complete discoloration of Orange II was nearly achieved and the H2O2 concentration became rather low. The dynamic behavior of OH radical concentration during the discoloration of Orange II was found to be strongly linked with the change in H2O2 concentration. The generation of OH radical was maximum at solution pH of 3.0 and decreased with an increase of solution pH. The OH radical generation rate in the Fenton Process was rather slower than that in the photo-Fenton process.  相似文献   

8.
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   

9.
Y. Xu   《Chemosphere》2001,43(8):1281
The degradation of a common textile dye, Reactive-brilliant red X-3B, by several advanced oxidation technologies was studied in an air-saturated aqueous solution. The dye was resistant to the UV illumination (wavelength λ  320 nm), but was decolorized when one of Fe3+, H2O2 and TiO2 components was present. The decolorization rate was observed to be quite different for each system, and the relative order evaluated under comparable conditions followed the order of Fe2+–H2O2–UV  Fe2+–H2O2 > Fe3+–H2O2–UV > Fe3+–H2O2 > Fe3+–TiO2–UV > TiO2–UV > Fe3+–UV > TiO2–visible light (λ  450 nm) > H2O2–UV > Fe2+–UV. The mechanism for each process is discussed, and linked together for understanding the observed differences in reactivity.  相似文献   

10.
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   

11.
The removal of radiocontrast agent diatrizoic acid (DIA) from water was performed using photo-Fenton (PF) process. First, the effect of H2O2 dosage on mineralization efficiency was determined using ultraviolet (UV) irradiation. The system reached a maximum mineralization degree of 60 % total organic carbon (TOC) removal at 4 h with 20 mM initial H2O2 concentration while further concentration values led to a decrease in TOC abatement efficiency. Then, the effect of different concentrations of Fenton’s reagents was studied for homogeneous Fenton process. Obtained results revealed that 0.25 mM Fe3+ and 20 mM H2O2 were the best conditions, achieving 80 % TOC removal efficiency at 4 h treatment. Furthermore, heterogeneous PF treatment was developed using iron-activated carbon as catalyst. It was demonstrated that this catalyst is a promising option, reaching 67 % of TOC removal within 4 h treatment without formation of iron leachate in the medium. In addition, two strategies of enhancement for process efficiency are proposed: coupling of PF with electro-Fenton (EF) process in two ways: photoelectro-Fenton (PEF) or PF followed by EF (PF-EF) treatments, achieving in both cases the complete mineralization of DIA solution within only 2 h. Finally, the Microtox tests revealed the formation of more toxic compounds than the initial DIA during PF process, while, it was possible to reach total mineralization by both proposed alternatives (PEF or PF-EF) and thus to remove the toxicity of DIA solution.  相似文献   

12.
Aqueous solutions of Fenton's reagent (Fe2+ + H2O2) have been used to effect the total decomposition of the chlorophenols: 2-chlorophenol, 3-chlorophenol, 4-chlorophenol, 3,4-dichlorophenol and 2,4,5-trichlorophenol. The mineralization of these chlorinated aromatic substrates to CO2 and free Cl has been studied as a function of [Fe2+] and [HClO4]. Increasing the concentration of Fe2+ enhances the decomposition process, while an increase in the concentration of HClO4, inhibits the reaction. The presence of Fe3+ alone (without any Fe2+) with H2O2 has no effect on the degradation of the chlorophenols. In all cases, the stoichiometric quantity of free Cl was obtained at the completion of the decomposition reaction; but the rates of disappaearance of the chlorophenol and of the formation of the Cl are not similar. This suggests that some chlorinated aliphatic species may be formed as possible intemediates.  相似文献   

13.

Zero-valent iron (Fe0) has been widely used for Cr(VI) removal; however, the removal mechanisms of Cr(VI) from aqueous solution under complex hydrogeochemical conditions were poorly understood. In this research, the mixed materials containing cast iron and activated carbon were packed in columns for the treatment of aqueous Cr(VI)-Cr(III) in groundwater with high concentration of Ca2+, Mg2+, HCO3 , NO3 , and SO4 2−. We investigate the influences of those ions on Cr(VI) removal, especially emphasizing on the reaction mechanisms and associated precipitations which may lead to porosity loss by using X-ray photoelectron spectroscopy (XPS) and scanning electron microscopy (SEM) techniques. The results show that the precipitations accumulated on the material surface were (Fe/Cr) (oxy)hydroxide, mixed Fe(III)-Cr(III) (oxy)hydroxides, Fe2O3, CaCO3, and MgCO3. During these reactions, the Cr(VI) was reduced to Cr(III) coupled with the oxidated Fe0 to Fe(II) through the galvanic corrosion formed by the Fe0-C and/or the direct electron transfer between Fe0 and Cr(VI). In addition, Cr(VI) could be reduced by aqueous Fe(II), which dominated the whole removal efficiency. The primary aqueous Cr(III) was completely removed together with Cr(III) reduced from Cr(VI) even when Cr(VI) was detected in the effluent, which meant that the aqueous Cr(III) could occupy the adsorption sites. In general, the combined system was useful for the Cr(VI)-Cr(III) treatment based on galvanic corrosion, and the hardness ions had a negative effect on Cr(VI) removal by forming the carbonates which might promote the passivation of materials and decrease the removal capacity of the system.

  相似文献   

14.
The effect of irradiation with visible light-emitting diode (LED) light on the efficiency of Fenton oxidation is investigated using phenol as the target compound (100 mg/L). The H2O2 dose and temperature are tested as operating variables with the aim of minimizing consumption of the reagents. At 50 °C, 10 mg/L Fe2+, and 60 % of the stoichiometric H2O2 amount, phenol was completely oxidized into CO2, H2O, and short chain organic acids, with oxalic acid completely degraded. Up to 95 % mineralization was achieved. This high efficiency can be attributed to the effect of LED radiation on the quinones/Fe2+/Fe3+/H2O2 cycle, which significantly increases the reaction rate, as well as on the photodecomposition of the iron complexes formed along the oxidation process, which also enhanced mineralization.  相似文献   

15.
光催化氧化-Fenton组合方法降解高浓度正丙醇废水   总被引:1,自引:1,他引:0  
研究了1%和10%2种浓度正丙醇废水在光催化氧化-Fenton组合工艺条件下的降解情况,分别考察了H2O2加药方式及剂量、Fe2+浓度、TiO2浓度,以及废水的初始浓度对反应的影响,得到了优化工艺参数。结果显示,在23 W的低压汞灯照射下,当Fe2+离子浓度为0.44 g/L,TiO2为0.4 g/L,H2O2分6次等幅递增投加,增幅为均值的10%,投加总量至28.6 g/L时,反应6 h后,组合工艺可将1%浓度正丙醇废水的COD从17 200 mg/L降低至2 000 mg/L。H2O2总用量为136.5 g/L,其他条件及加药方式不变条件下,废水浓度提高至10%,紫外光能量利用率明显提高,反应15 h后,可将COD从172 000 mg/L降至1 000 mg/L以下,降解速率随浓度降低而下降。  相似文献   

16.
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   

17.
Fe2O3 and CeO2 modified activated coke (AC) synthesized by the equivalent-volume impregnation were employed to remove elemental mercury (Hg0) from simulated flue gas at a low temperature. Effects of the mass ratio of Fe2O3 and CeO2, reaction temperature, and individual flue gas components including O2, NO, SO2, and H2O (g) on Hg0 removal efficiency of impregnated AC were investigated. The samples were characterized by Brunauer–Emmett–Teller (BET), X-ray diffraction (XRD), scanning electron microscopy (SEM), and X-ray photoelectron spectroscopy (XPS). Results showed that with optimal mass percentage of 3 % Fe2O3 and 3 % CeO2 on Fe3Ce3/AC, the Hg0 removal efficiency could reach an average of 88.29 % at 110 °C. Besides, it was observed that O2 and NO exhibited a promotional effect on Hg0 removal, H2O (g) exerted a suppressive effect, and SO2 showed an insignificant inhibition without O2 to some extent. The analysis of XPS indicated that the main species of mercury on used Fe3Ce3/AC was HgO, which implied that adsorption and catalytic oxidation were both included in Hg0 removal. Furthermore, the lattice oxygen, chemisorbed oxygen, and/or weakly bonded oxygen species made a contribution to Hg0 oxidation.  相似文献   

18.
研究了辉光放电等离子体降解水中典型的环境内分泌干扰物邻苯二甲酸二丁酯(DBP)及降解过程中过氧化氢(H2O2)的生成规律。考察了电解质种类、共存污染物(甲醇、叔丁醇)及催化剂等条件对DBP降解及H2O2生成的影响。结果表明,在硫酸钠溶液中DBP降解效率和H2O2生成速率最高;甲醇、叔丁醇等共存污染物对DBP降解和H2O2生成有抑制作用;Fe2+,Fe3+和Cu2+对DBP的降解有催化作用,其催化效果为Fe2+>Fe3+>Cu2+。用高效液相色谱、离子色谱及气质联用仪等仪器分析了降解中间产物,提出了可能的降解机理。  相似文献   

19.
超声-Fenton联用技术深度处理皮革综合废水生化出水   总被引:2,自引:1,他引:1  
针对皮革综合废水生化处理出水中存在COD和色度偏高等问题,提出采用超声-Fenton联用技术对生化后的皮革综合废水进行深度处理。通过单因素实验考察了超声功率、H2O2投加量、Fe2+投加量(即H2O2/Fe2+比)、溶液pH和反应时间对水样中COD和色度去除率的影响;正交实验结果表明,当溶液初始pH值为4.0时,各因素影响显著性的先后顺序为H2O2>超声功率>反应时间>Fe2+;其优化的实验条件为:H2O2为24.0 mL/L、超声功率为85 W、反应时间为45min、Fe2+为2.2 g/L,经超声-Fenton联用技术深度处理后COD的去除率可达85.4%。在最佳实验条件下,对超声-Fenton联用技术深度处理皮革综合废水生化出水的动力学研究发现,水样中的COD降解反应符合表观一级反应动力学,速率常数增强因子可达8.64,表明存在显著的协同效应。  相似文献   

20.
ABSTRACT

Water is effective in leaching out Cr6+ from a mixture of paint powders and abrasive blast media. However, acids such as HNO3, HCl, and H2SO4 significantly enhance the leaching procedure. Cr ions in the leaching solutions are successfully removed by electrochemical precipitation. The consumable Fe electrodes generate ferrous ions to cause the reduction of Cr6+ to Cr3+. Cr3+ ions along with Fe2+ and Fe3+ are then removed mainly by precipitation as Cr(OH)3, Fe(OH)2, and Fe(OH)3 near the cathode where OH- ions are generated by water electrolysis. The electrochemical process is capable of discharging low levels of Cr6+, less than 1 mg/L, without pH adjustment.  相似文献   

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