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1.
A Fenton-like disinfection process was conducted with Fenton's reagent (H2O2) at pH 3 or 5 on autochthonous drinking water biofilms grown on corroded or non-corroded pipe material. The biofilm disinfection by Fenton-like oxidation was limited by the low content of iron and copper in the biomass grown on non-corroded plumbing. It was slightly improved by spiking the distribution system with some additional iron source (soluble iron II or ferrihydrite particles appeared as interesting candidates). However successful in situ disinfection of biofilms was only achieved in fully corroded cast iron pipes using H2O2 and adjusting the pH to 5. These new results provide additional support for the use of Fenton's processes for cleaning drinking water distribution systems contaminated with biological agents or organics.  相似文献   

2.
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   

3.
The energy consumptions of conventional ozonation and the AOPs O3/H2O2 and UV/H2O2 for transformation of organic micropollutants, namely atrazine (ATR), sulfamethoxazole (SMX) and N-nitrosodimethylamine (NDMA) were compared. Three lake waters and a wastewater were assessed. With p-chlorobenzoic acid (pCBA) as a hydroxyl radical (OH) probe compound, we experimentally determined the rate constants of organic matter of the selected waters for their reaction with OH (kOH,DOM), which varied from 2.0 × 104 to 3.5 × 104 L mgC−1 s−1. Based on these data we calculated OH scavenging rates of the various water matrices, which were in the range 6.1-20 × 104 s−1. The varying scavenging rates influenced the required oxidant dose for the same degree of micropollutant transformation. In ozonation, for 90% pCBA transformation in the water with the lowest scavenging rate (lake Zürich water) the required O3 dose was roughly 2.3 mg/L, and in the water with the highest scavenging rate (Dübendorf wastewater) it was 13.2 mg/L, corresponding to an energy consumption of 0.035 and 0.2 kWh/m3, respectively. The use of O3/H2O2 increased the rate of micropollutant transformation and reduced bromate formation by 70%, but the H2O2 production increased the energy requirements by 20-25%. UV/H2O2 efficiently oxidized all examined micropollutants but energy requirements were substantially higher (For 90% pCBA conversion in lake Zürich water, 0.17-0.75 kWh/m3 were required, depending on the optical path length). Energy requirements between ozonation and UV/H2O2 were similar only in the case of NDMA, a compound that reacts slowly with ozone and OH but is transformed efficiently by direct photolysis.  相似文献   

4.
Yeo MK  Kang M 《Water research》2006,40(9):1906-1914
We investigated the relationship between the TiO2 photocatalytic decomposition of bisphenol A and biological toxicity to zebrafish (Danio rerio). TiO2 particles, which prepared using a solvothermal method, were applied to produce a nanometer-sized TiO2 thin film. An alcoholic solution containing the TiO2 particles and an inorganic binder was directly coated on the UV-lamp substrate. It was equipped in a photoreactor that was manufactured in our laboratory. The attachment of the thin TiO2 film to the UV-lamp substrate resulted in a stable and transparent coating. The TiO2 particles on the thin film were approximately 20-30 nm in size, and the resulting film thickness was approximately 200 nm after a single coat. The bisphenol A, which was eluted from epoxy resin in a drinking water tank, was completely degraded by the TiO2 photocatalysis. We initially detected approximately 7.8 ng/ml of bisphenol A in the epoxy-resin tank, but its concentration was undetectable after a 48-h photocatalytic reaction over TiO2. We observed a decreased survival rate in zebrafish that were reared in water exposed to the leaching process of the epoxy resin. After the photocatalysis, however, no toxic effects on the hatching rates or morphogenesis of the zebrafish were observed. In summary, toxicity during the TiO2 photocatalysis was observed; however, toxicity was no longer observed once the bisphenol A was completely decomposed by the TiO2 photocatalysis. On the basis of these experimental observations, we suggest that TiO2 photocatalysis can be adopted as a treatment method to purify an epoxy-resin tank.  相似文献   

5.
Kinetic modeling of electro-Fenton reaction in aqueous solution   总被引:1,自引:0,他引:1  
Liu H  Li XZ  Leng YJ  Wang C 《Water research》2007,41(5):1161-1167
To well describe the electro-Fenton (E-Fenton) reaction in aqueous solution, a new kinetic model was established according to the generally accepted mechanism of E-Fenton reaction. The model has special consideration on the rates of hydrogen peroxide (H(2)O(2)) generation and consumption in the reaction solution. The model also embraces three key operating factors affecting the organic degradation in the E-Fenton reaction, including current density, dissolved oxygen concentration and initial ferrous ion concentration. This analytical model was then validated by the experiments of phenol degradation in aqueous solution. The experiments demonstrated that the H(2)O(2) gradually built up with time and eventually approached its maximum value in the reaction solution. The experiments also showed that phenol was degraded at a slow rate at the early stage of the reaction, a faster rate during the middle stage, and a slow rate again at the final stage. It was confirmed in all experiments that the curves of phenol degradation (concentration vs. time) appeared to be an inverted "S" shape. The experimental data were fitted using both the normal first-order model and our new model, respectively. The goodness of fittings demonstrated that the new model could better fit the experimental data than the first-order model appreciably, which indicates that this analytical model can better describe the kinetics of the E-Fenton reaction mathematically and also chemically.  相似文献   

6.
Water reclamation plants frequently utilise reverse osmosis (RO), generating a concentrated reject stream as a by-product. The concentrate stream contains salts, and dissolved organic compounds, which are recalcitrant to biological treatment, and may have an environmental impact due to colour and embedded nitrogen. In this study, we characterise organic compounds in RO concentrates (ROC) and treated ROC (by coagulation, adsorption, and advanced oxidation) from two full-scale plants, assessing the diversity and treatability of colour and organic compounds containing nitrogen. One of the plants was from a coastal catchment, while the other was inland. Stirred cell membrane fractionation was applied to fractionate the treated ROC, and untreated ROC along with chemical analysis (DOC, DON, COD), colour, and fluorescence excitation-emission matrix (EEM) scans to characterise changes within each fraction. In both streams, the largest fraction contained <1 kDa molecules which were small humic substances, fulvic acids and soluble microbial products (SMPs), as indicated by EEM. Under optimal treatment conditions, alum preferentially removed >10 kDa molecules, with 17-34% of organic compounds as COD. Iron coagulation affected a wider size range, with better removal of organics (41-49% as COD) at the same molar dosage. As with iron, adsorption reduced organics of a broader size range, including organic nitrogen (26-47%). Advanced oxidation (UV/H2O2) was superior for complete decolourisation and provided superior organics removal (50-55% as COD).  相似文献   

7.
The degradation of two pesticides, bromoxynil and trifluralin, was investigated in ultrapure and natural water solutions under ultraviolet (UV) light and a combination of UV and hydrogen peroxide (H2O2). The effect of pH on the photooxidation of the pesticides was also studied. The results indicated that under direct photolysis with monochromatic light at 253.7 nm and different conditions, the photochemical rates followed first-order kinetics, with fluence-based rate constants ranging from 9.15 × 10−4 to 6.37 × 10−3 cm2 mJ−1 and 7.63 × 10−3 to 1.47 × 10−2 cm2 mJ−1 for bromoxynil and trifluralin, respectively. Quantum yields, in the range of 0.08-0.25 for bromoxynil and 0.12-0.72 for trifluralin, were observed in experiments using ultrapure water. The study also found that the UV/H2O2 process enhanced the oxidation rate in comparison to direct photolysis. A 90% degradation with UV dose of 333 and 188 mJ cm−2 was achieved for bromoxynil and trifluralin, respectively, in natural water, in presence of 8.8 × 10−4 M H2O2. To assess the aquatic toxicity, the Microtox® 81.9% screening test protocol was used before and after treatment. The test results indicated a decrease in the acute toxicity of the samples after treatment for both pesticides.  相似文献   

8.
The degradation of PbEDTA in aqueous solution by a H(2)O(2)/UV process was studied. The effect of H(2)O(2) content, pH of the solution and the presence of nitrate were investigated. PbEDTA degradation by a H(2)O(2)/UV process was shown to be accompanied by simultaneous lead precipitation. PbEDTA was decomposed rapidly in acidic solutions while lead precipitation was achieved only when the pH of the solution was higher than 6. The presence of nitrate in significant amounts (0.04 M) inhibited remarkably the degradation of the complex and metal precipitation. The degradation of CdEDTA and ZnEDTA was also studied. It was found that the decomposition of metal-EDTA complex and metal removal by the H(2)O(2)/UV process depend greatly on the nature of the metal. CdEDTA and ZnEDTA were decomposed rapidly but metal precipitation was not achieved. The major by-products of the degradation of metal-EDTA complexes observed were nitrilotriacetic acid (NTA), iminodiacetic acid (IDA), oxalic acid and nitrate.  相似文献   

9.
This work investigated the degradation of a natural (17beta-estradiol) and a synthetic (17alpha-ethinylestradiol) estrogens (pure or in the mixture) and the removal of estrogenic activity by the ozonation and O3/H2O2 process in three different pHs (3, 7 and 11). The effect of oxidation via OH radical was evaluated adding a radical scavenger (t-butanol) in the medium. Estrogenic activity was performed using the YES assay. 17beta-estradiol and 17alpha-ethinylestradiol presented similar estrogenic potential and the association of these estrogens resulted in an addictive effect for estrogenic activity. Ozonation and O3/H2O2 processes were effective in removing the estrogens in aqueous solution. In the mixture at pH 11, removals were higher than 98% and 96% for 17beta-estradiol and 17alpha-ethinylestradiol, respectively. In pH 3, 17beta-estradiol and 17alpha-ethinylestradiol removals were 100% and 99.7%, respectively. When estrogens were treated separately, the removals in pH 11 were superior to 99.7 and 98.8%, while in pH 3 were 100% and 99.5% for 17beta-estradiol and 17alpha-ethinylestradiol, respectively. 17alpha-ethinylestradiol has been always removed at lower rates (pure or in the mixture) for all applied conditions. Estrogenic activity was completely removed in pH 3 for ozonation or O3/H2O2. The samples oxidized in pH 11 presented higher estrogenic activity than those in pH 7. Estrogens removal was lower at pHs 7 and 11, when the scavenger was added to the media. The higher estrogen residual concentrations found in ozonation in presence of tert-butanol are contributing for higher estrogenic activity observed in pHs 7 and 11. By-products with estrogenic activity were formed by oxidation via OH radical. Only a few compounds could be identified in pHs 7 and 11 and they have a phenolic ring, which, probably is contributing to the estrogenic activity observed.  相似文献   

10.
This work investigates the Fenton oxidation of phenol in a semicontinuous reactor where the overall amount of H2O2 is distributed as a continuous feed upon the reaction time. The experiments were carried out at 25 °C and atmospheric pressure, with 100 mg/L initial phenol concentration and iron dosages from 1 to 100 mg/L. H2O2 aqueous solution was continuously fed during 4 h reaction time up to an overall dose varying within the range of 500-5000 mg/L. The results in terms of evolution of phenol, H2O2 and intermediates, as well as TOC abatement were compared with those obtained in conventional batch operation. It was found that the oxidation rates for phenol and intermediates were lower when adding the H2O2 continuously. However, a higher abatement of TOC was reached at the end of the 4-h reaction time, in spite of a similar overall H2O2 consumption. This is the result of a more efficient OH generation throughout the semicontinuous process, favouring the reaction with the organic species and reducing the occurrence of competitive scavenging reactions involving Fe2+, H2O2 and OH. Two kinetic models were proposed, one for describing the evolution of phenol, aromatics and H2O2 and the other for TOC. The influence of the operating conditions on the kinetic constants was also studied, looking for the optimal conditions in terms of both, environmental and economic points of view.  相似文献   

11.
Lee Y  Lee C  Yoon J 《Water research》2004,38(10):2579-2588
The objective of this study was to elucidate the degradation pathways of dimethylsulfoxide (DMSO) during its mineralization caused by UV/H(2)O(2) treatment. In order to accomplish this, we measured the concentration time-profiles of DMSO and its degradation intermediates during the UV/H(2)O(2) treatment. In addition, we proposed a kinetic model that could account for the degradation pathways of DMSO during its UV/H(2)O(2) treatment. The results show that the degradation of DMSO by the UV/H(2)O(2) treatment can be classified into two major pathways, and this is supported by both the analysis of the intermediates and total organic carbon (TOC) measurements. Firstly, DMSO was degraded into sulfate (SO(4)(2-)) through the formation of methansulfinate (CH(3)SO(2)(-)) and methansulfonate (CH(3)SO(3)(-)) as sulfur-containing intermediates. One of the two carbon constituents of DMSO was highly resistant to mineralization, due to the formation of methansulfonate, which reacted very slowly with (.-)OH k = 0.8 x 10(7) M(-1)s(-1)). Secondly, the other carbon constituent of DMSO was relatively easily mineralized through the formation of formaldehyde (HCHO) and formate (HCO(2)(-)) as non-sulfur-containing intermediates. The kinetic model proposed in this study for the degradation of DMSO by (.-)OH in the UV/H(2)O(2) process was able to successfully predict the patterns of concentration time-profiles of all components during the UV/H(2)O(2) treatment of DMSO.  相似文献   

12.
Diclofenac, a widely used anti-inflammatory drug, has been found in many Sewage Treatment Plant effluents, rivers and lake waters, and has been reported to exhibit adverse effects on fish. Advanced oxidation processes, ozonation and H2O2/UV were investigated for its degradation in water. The kinetic of the degradation reaction and the nature of the intermediate products were still poorly defined. Under the conditions adopted in the present study, both ozonation and H2O2/UV systems proved to be effective in inducing diclofenac degradation, ensuring a complete conversion of the chlorine into chloride ions and degrees of mineralization of 32% for ozonation and 39% for H2O2/UV after a 90 min treatment. The reactions were found to follow similar, but not identical, reaction pathways leading to hydroxylated intermediates (e.g. 2-[(2,6-dichlorophenyl)amino]-5-hydroxyphenylacetic acid) and C-N cleavage products (notably 2,5-dihydroxyphenylacetic acid) through competitive routes. Subsequent oxidative ring cleavage leads to carboxylic acid fragments via classic degradation pathways. In the pH range 5.0-6.0 kinetic constants (1.76 x 10(4)-1.84 x 10(4) M(-1) s(-1)) were estimated for diclofenac ozonation.  相似文献   

13.
Glyphosate is the organophosphate herbicide most widely used in the world. Any form of spill or discharge, even if unintentional, can be transferred to the water due to its high solubility. The combination of hydrogen peroxide and UV radiation could be a suitable option to decrease glyphosate concentration to acceptable limits. In this work, the effects of initial pH, hydrogen peroxide initial concentration, and incident radiation in glyphosate degradation were studied. The experimental device was a cylinder irradiated with two tubular, germicidal lamps. Conversion of glyphosate increases significantly from pH = 3-7. From this value on, the increase becomes much less noticeable. The reaction rate depends on the initial herbicide concentration and has an optimum plateau of a hydrogen peroxide to glyphosate molar concentration ratio between 7 and 19. The expected non linear dependence on the irradiation rate was observed. The identification of critical reaction intermediaries, and the quantification of the main end products were possible and it led to propose a plausible degradation path. The achieved quantification of the mineralization extent is a positive indicator for the possible application of a rather simple technology for an in situ solution for some of the problems derived from the intensive use of glyphosate.  相似文献   

14.
MM Bazri  B Barbeau  M Mohseni 《Water research》2012,46(16):5297-5304
The presence of natural organic matter (NOM) poses several challenges to the commercial practice of UV/H2O2 process for micropollutant removal. During the commercial application of UV/H2O2 advanced oxidation treatment, NOM is broken down into smaller species potentially affecting biostability by increasing Assimilable Organic Carbon (AOC) and Biodegradable Organic Carbon (BDOC) of water. This work investigated the potential impact of UV/H2O2 treatment on the molecular weight distribution of NOM and biostability of different water sources. A recently developed flow cytometric method for enumeration of bacteria was utilized to assess biological stability of the treated water at various stages through measurement of AOC. BDOC was also assessed for comparison and to better study the biostability of water. Both AOC and BDOC increased by about 3-4 times over the course of treatment, indicating the reduction of biological stability. Initial TOC and the source of NOM were found to be influencing the biostability profile of the treated water. Using high performance size exclusion chromatography, a wide range of organic molecule weights were found responsible for AOC increase; however, low molecular weight organics seemed to contribute more. Positive and meaningful correlations were observed between BDOC and AOC of different waters that underwent different treatments.  相似文献   

15.
Greater Cincinnati Water Works (GCWW) evaluated the efficacy of ultraviolet light/hydrogen peroxide advanced oxidation (UV/H2O2) for reducing trace organic contaminants in natural water with varying water qualities. A year-long UV/H2O2 pilot study was conducted to examine a variety of seasonal and granular activated carbon (GAC) breakthrough conditions. The UV pilot-scale reactors were set to consistently achieve 80% atrazine degradation, allowing comparison of low pressure (LP) and medium pressure (MP) lamp technologies for by-product formation. Because hydroxyl radicals react non-selectively with organic compounds, unintended by-product formation occurred.Total assimilable organic carbon (AOC) concentration increased through the reactors from 14 to 33% on average, depending on water quality. Natural organic matter (NOM) contains the precursors for AOC production, so when post-GAC water (versus conventionally treated water) served as reactor influent, less AOC was produced. No appreciable difference in AOC concentration was observed between LP and MP UV reactors. The Spirillum strain NOX fraction of the AOC increased from 50 to 65% on average, depending on the quality of the water. The increase in this fraction of AOC occurred because oxidation of NOM yielded smaller more assimilable organic compounds such as organic acids that are necessary for NOX growth. The Pseudomonas fluorescens strain P17 AOC concentration increased only when conventionally treated plant water was used as pilot influent. This organism thrives in waters of differing organic energy sources, but does not thrive well in carboxylic acids alone. The CONV water had more overall TOC that could contribute to higher P17 AOC counts.Biofilm coupon studies indicated that biofilms with greater heterotrophic plate counts were observed in the granular activated carbon (GAC) effluent streams receiving UV/H2O2 pre-treatment. Biofilm coupon studies additionally indicated that the effluent stream of the GAC column proceeded by the MP reactor exhibited more viable biofilm than the other GAC effluent streams based on an ATP-bioluminescence method. The increased viability of the biofilm produced by the MP UV reactor is likely a result of the multiple UV wavelengths and higher energy input characteristic of this technology.  相似文献   

16.
Suh JH  Mohseni M 《Water research》2004,38(10):2596-2604
Advanced oxidation involving O3/H2O2 was used to eliminate 1,4-dioxane and to enhance the biodegradability of dioxane-contaminated water. Oxidation experiments were carried out in a bubble column reactor operating in fed-batch. The rate of dioxane removal and enhancement in biodegradability was investigated at hydrogen peroxide to ozone ratios between 0 and 0.6 mol:mol and pH between 5 and 11. A theoretical model was also applied to predict the experimental data and to investigate the effects of dioxane concentration, pH, and H2O2 concentration. The model predictions fit the experimental data well and there was a linear correlation between dioxane oxidation and BOD enhancement. At low dioxane concentrations, the oxidation rate was first order and it gradually approached zero order with increasing dioxane concentration. Also, the biodegradability of the solution increased with pH up to about 9 and it stayed constant with further pH increase. Hydrogen peroxide initially enhanced dioxane removal and biodegradability enhancement of the solution. However, at H2O2:O3 ratios greater than about 0.4-0.45 mol:mol, i.e. about 2.90 mM for H2O2 concentration, H2O2 had negative impacts and resulted in reduced dioxane removal and biodegradability increase.  相似文献   

17.
Neamţu M  Frimmel FH 《Water research》2006,40(20):3745-3750
The photodegradation of bisphenol A (BPA) in pure water, surface water and wastewater effluents was studied. The effect of different hydrogen peroxide concentrations on degradation was investigated. The rate of BPA photolysis in the presence of hydrogen peroxide was lower in wastewater effluent than in purified water.

Phenol, 1,4-dihydroxylbenzene and 1,4-benzoquinone were identified by means of HPLC as intermediate products of the photodegradation of bisphenol A.

In addition, the disappearance of the estrogenic activity of bisphenol A during irradiation was shown by the YES test. Based upon the YES test results, there was a strong decrease of estrogenic activity of parent compound after 120 min irradiation in the presence of hydrogen peroxide.  相似文献   


18.
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   

19.
In recent years, the application of heterogeneous photocatalytic water purification processes has gained wide attention due to its effectiveness in degrading and mineralizing the recalcitrant organic compounds as well as the possibility of utilizing the solar UV and visible-light spectrum. By far, titania has played a much larger role in this scenario compared to other semiconductor photocatalysts due to its costly effectiveness, inert nature and photostability. A substantial amount of research has focused on the enhancement of TiO2 photocatalysis by modification with metal, non-metal and ion doping.This paper aims to review and summarize the recent works on the titanium dioxide (TiO2) photocatalytic oxidation of phenol and discusses various mechanisms of phenol photodegradation (indicating the intermediates products) and formation of OH radicals. Phenol degradation pathway in both systems, TiO2/UV and doped-TiO2/Vis, are described.  相似文献   

20.
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   

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