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1.
Pifer AD  Fairey JL 《Water research》2012,46(9):2927-2936
Several challenges with disinfection byproduct (DBP) control stem from the complexity and diversity of dissolved organic matter (DOM), which is ubiquitous in natural waters and reacts with disinfectants to form DBPs. Fluorescence parallel factor (PARAFAC) analysis and asymmetric flow-field flow fractionation (AF4) were used in combination with free chlorine DBP formation potential (DBPFP) tests to study the physicochemical DOM properties and DBP formation in raw- and alum-coagulated waters. Enhanced coagulation with alum became more effective at removing DBP-precursors as the pH decreased from 8 to 6. AF4-UV254 fractograms indicated enhanced coagulation at pH 6 preferentially removed larger DOM, whereas no preferential size removal occurred at pH 8. Fluorescence-PARAFAC analysis revealed the presence of one protein-like and three humic-like fluorophore groups; stronger linear correlations were found between chloroform and the maximum intensity (FMAX) of a humic-like fluorophore (r2 = 0.84) than with SUVA254 (r2 = 0.51). This result indicated that the fluorescence-PARAFAC approach used here was an improvement on SUVA254, i.e., fluorescence-based measurements were stronger predictors of chloroform formation.  相似文献   

2.
During membrane treatment of secondary effluent from wastewater treatment plants, a reverse osmosis concentrate (ROC) containing trace organic contaminants is generated. As the latter are of concern, effective and economic treatment methods are required. Here, we investigated electrochemical oxidation of ROC using Ti/Ru0.7Ir0.3O2 electrodes, focussing on the removal of dissolved organic carbon (DOC), specific ultra-violet absorbance at 254 nm (SUVA254), and 28 pharmaceuticals and pesticides frequently encountered in secondary treated effluents. The experiments were conducted in a continuously fed reactor at current densities (J) ranging from 1 to 250 A m−2 anode, and a batch reactor at J = 250 A m−2. Higher mineralization efficiency was observed during batch oxidation (e.g. 25.1 ± 2.7% DOC removal vs 0% removal in the continuous reactor after applying specific electrical charge, Q = 437.0 A h m−3 ROC), indicating that DOC removal is depending on indirect oxidation by electrogenerated oxidants that accumulate in the bulk liquid. An initial increase and subsequent slow decrease in SUVA254 during batch mode suggests the introduction of auxochrome substituents (e.g. -Cl, NH2Cl, -Br, and -OH) into the aromatic compounds. Contrarily, in the continuous reactor ring-cleaving oxidation products were generated, and SUVA254 removal correlated with applied charge. Furthermore, 20 of the target pharmaceuticals and pesticides completely disappeared in both the continuous and batch experiments when applying J ≥ 150 A m−2 (i.e. Q ≥ 461.5 A h m−3) and 437.0 A h m−3 (J = 250 A m−2), respectively. Compounds that were more persistent during continuous oxidation were characterized by the presence of electrophilic groups on the aromatic ring (e.g. triclopyr) or by the absence of stronger nucleophilic substituents (e.g. ibuprofen). These pollutants were oxidized when applying higher specific electrical charge in batch mode (i.e. 1.45 kA h m−3 ROC). However, baseline toxicity as determined by Vibrio fischeri bioluminescence inhibition tests (Microtox) was increasing with higher applied charge during batch and continuous oxidation, indicating the formation of toxic oxidation products, possibly chlorinated and brominated organic compounds.  相似文献   

3.
Zhou T  Lim TT  Wu X 《Water research》2011,45(9):2915-2924
The sonophotolytic advance oxidation system (US/UV/Fe3+) could achieve synergistic degradation of reactive black 5 (RB5), as compared to UV/Fe3+ and US/Fe3+ systems. A synergy factor of 2.5 based on the pseudo-first-order degradation rate constant (kobs) was found, along with enhancements in organic detoxification and mineralization. The presence of organic ligands could affect the US/UV/Fe3+ system differently. Oxalate, citrate, tartrate and succinate could enhance the RB5 degradation, while NTA and EDTA exhibited strong inhibitions. The influence of these ligands on kobs(RB5) in the US/UV/Fe(III)-ligand systems followed the sequence of oxalate > tartrate > succinate > citrate > without ligand > NTA > EDTA, while they could be degraded simultaneously with the kobs(ligand) order of oxalate > citrate > tartrate > succinate > NTA > EDTA. Monitoring of iron species and the generated H2O2 and •OH revealed that the ligands in the US/UV/Fe(III)-ligand system could play different mechanistic roles: (1) promoting H2O2 production, (2) accelerating Fenton reaction, and (3) competing with RB5 for reacting with •OH. Among the ligands, oxalate exhibited the most significant enhancement of RB5 oxidation in the sonophotolytic system, and the process was pH-dependent. An initial reaction lag in RB5 degradation was observed when Fe2+ was used in lieu of Fe3+ as the catalyst in the sonophotolytic system.  相似文献   

4.
The photoassisted reduction of metal ions and organic dye by metal-deposited Degussa P25 TiO2 nanoparticles was investigated. Copper and silver ions were selected as the target metal ions to modify the surface properties of TiO2 and to enhance the photocatalytic activity of TiO2 towards methylene blue (MB) degradation. X-ray powder diffraction (XRPD), X-ray photoelectron spectroscopy (XPS), and transmission electron microscopy (TEM) were used to characterize the crystallinity, chemical species and morphology of metal-deposited TiO2, respectively. Results showed that the particle size of metal-deposited TiO2 was larger than that of Degussa P25 TiO2. Based on XRPD patterns and XPS spectra, it was observed that the addition of formate promoted the photoreduction of metal ion by lowering its oxidation number, and subsequently enhancing the photodegradation efficiency and rate of MB. The pseudo-first-order rate constant (kobs) for MB photodegradation by Degussa P25 TiO2 was 3.94 × 10− 2 min− 1 and increased by 1.4-1.7 times in kobs with metal-deposited TiO2 for MB photodegradation compared to simple Degussa P25 TiO2. The increase in mass loading of metal ions significantly enhanced the photodegradation efficiency of MB; the kobs for MB degradation increased from 3.94 × 10− 2 min− 1 in the absence of metal ion to 4.64-7.28 × 10− 2 min− 1 for Ag/TiO2 and to 5.14-7.61 × 10− 2 min− 1 for Cu/TiO2. In addition, the electrons generated from TiO2 can effectively reduce metal ions and MB simultaneously under anoxic conditions. However, metal ions and organic dye would compete for electrons from the illuminated TiO2.  相似文献   

5.
A screening concept is suggested for evaluating the effectiveness of fluids to thermally suppress fires. It is based on measuring a fluid's ability to inhibit (or quench) the temperature rise of a material that is rapidly heated. The experimental design is similar to the transient hot wire technique, in which the evolution of the average material temperature is recorded for a given input power, and internal temperature gradients in the material are minimized. A gold wire (100 μm long and 5 μm diameter) is used as the surface which heats the fluid. The wire temperature response due to a power pulse provides a measure of the effectiveness of the fluid to suppress thermally the temperature increase. The results indicate that the “quenching effectiveness”, QE=(TmaxT)/(Tmax,refT)QE=(TmaxT)/(Tmax,refT), correlates with the ratio of the fluid thermal conductivity to that of the wire, kfluid/ksolid, using different Nusselt numbers (representing both conduction and natural convection) for the liquids or gases. The concept developed here could be included in a more comprehensive screening protocol, which would assess the thermal potential of candidate fire suppressants.  相似文献   

6.
Modeling monochloramine loss in the presence of natural organic matter   总被引:2,自引:0,他引:2  
A comprehensive model describing monochloramine loss in the presence of natural organic matter (NOM) is presented. The model incorporates simultaneous monochloramine autodecomposition and reaction pathways resulting in NOM oxidation. These competing pathways were resolved numerically using an iterative process evaluating hypothesized reactions describing NOM oxidation by monochloramine under various experimental conditions. The reaction of monochloramine with NOM was described as biphasic using four NOM specific reaction parameters. NOM pathway 1 involves a direct reaction of monochloramine with NOM (kdoc1=1.05×104-3.45×104 M−1 h−1). NOM pathway 2 is slower in terms of monochloramine loss and attributable to free chorine (HOCl) derived from monochloramine hydrolysis (kdoc2=5.72×105-6.98×105 M−1 h−1), which accounted for the majority of monochloramine loss. Also, the free chlorine reactive site fraction in the NOM structure was found to correlate to specific ultraviolet absorbance at 280 nm (SUVA280). Modeling monochloramine loss allowed for insight into disinfectant reaction pathways involving NOM oxidation. This knowledge is of value in assessing monochloramine stability in distribution systems and reaction pathways leading to disinfection by-product (DBP) formation.  相似文献   

7.
Parshetti GK  Doong RA 《Water research》2011,45(14):4198-4210
The coupled removal of priority pollutants by nanocomposite materials has recently been receiving much attention. In this study, trichloroethylene (TCE) and 2,4-dichlorophenol (DCP) in aqueous solutions were simultaneously removed by Fe/TiO2 nanocomposites under anoxic conditions in the presence of nickel ions and UV light at 365 nm. Both TCE and DCP were effectively dechlorinated by Fe/TiO2 nanocomposites, and the pseudo-first-order rate constants (kobs) for TCE and DCP dechlorination were (1.39 ± 0.05)×10−2 and (1.08 ± 0.05)×10−2 h−1, respectively, which were higher than that by nanoscale zerovalent iron alone. In addition, the kobs for DCP dechlorination was enhanced by a factor of 77 when Fe/TiO2 was illuminated with UV light for 2 h. Hydrodechlorination was found to be the major reaction pathway for TCE dechlorination, while DCP could undergo reductive dechlorination or react with hydroxyl radicals to produce 1,4-benzoquinone and phenol. TCE was a stronger electron acceptor than DCP, which could inhibit the dechlorination efficiency and rate of DCP during simultaneous removal processes. The addition of nickel ions significantly enhanced the simultaneous photodechlorination efficiency of TCE and DCP under the illumination of UV light. The kobs values for DCP and TCE photodechlorination by Fe/TiO2 in the presence of 20-100 μM Ni(II) were 30.4-136 and 13.2-192 times greater, respectively, when compared with those in the dark. Electron spin resonance analysis showed that the photo-generated electron-hole pairs could be effectively separated through Ni ions cycling, leading to the improvement of electron transfer efficiency of TCE and DCP by Fe/TiO2.  相似文献   

8.
Haomin Xu 《Water research》2011,45(2):632-638
Amoxicillin is a widely used antibiotic and has been detected in natural waters. Its environmental fate is in part determined by hydrolysis, and, direct and indirect photolysis. The hydrolysis rate in distilled water and water to which five different isolated of dissolved organic matter (DOM) was added, were evaluated. In the five different DOM solutions hydrolysis accounted for 5-18% loss of amoxicillin. Direct and indirect photolysis rates were determined using a solar simulator and it appeared that indirect photolysis was the dominant loss mechanism. Direct photolysis, in a solar simulator, accounted for 6-21% loss of amoxicillin in the simulated natural waters. The steady-state concentrations of singlet oxygen, 1ΔO2 (∼10−13 M) and hydroxyl radical, •OH (∼10−17 M) were obtained in aqueous solutions of five different dissolved organic matter samples using a solar simulator. The bimolecular reaction rate constant of 1ΔO2 with amoxicillin was measured in the different solutions, kΔO2 = 1.44 × 104 M−1 s−1. The sunlight mediated amoxicillin loss rate with 1ΔO2 (∼10−9 s−1), and with •OH (∼10−7 s−1), were also determined for the different samples of DOM. While 1ΔO2 only accounted for 0.03-0.08% of the total loss rate, the hydroxyl radical contributed 10-22%. It appears that the direct reaction of singlet and triplet excited state DOM (3DOM) with amoxicillin accounts for 48-74% of the loss of amoxicillin. Furthermore, the pseudo first-order photodegradation rate showed a positive correlation with the sorption of amoxicillin to DOM, which further supported the assumption that excited state DOM plays a key role in the photochemical transformation of amoxicillin in natural waters. This is the first study to report the relative contribution of all five processes to the fate of amoxicillin in aqueous solution.  相似文献   

9.
Dissolved organic matter (DOM) in 20 surface waters in Eastern Finland were characterized to examine relationships between structural and compositional properties of DOM and partition coefficients (Kp) describing sorption of four model contaminants to DOM and the bioavailability of contaminants by Daphnia magna. The hydrophobic acids (HbA), hydrophobic neutrals (HbN) and hydrophilic (HI) fractions of DOM were separated by XAD-8 resin. The KPs were measured by equilibrium dialysis. Model contaminants were benzo(a)pyrene (BaP), naphthalene (NAPH), 3.3′,4.4′-tetrachlorobiphenyl (TCB) and dehydroabietic acid (DHAA).DOM concentrations varied from 2.0 to 38.3 mg org. C/l in the water series. The percentage of HbA and the aromaticity of DOM, as indicated by the absorptivity at 270 nm (A270) and hydrogen/carbon ratio (H/C ratio), increased with increasing DOM concentration. Significant correlations were observed between KP of BAP, A270 and HbA content of the DOM from different sources. For the other contaminants similar kinds of relationships between Kps and quality parameters of DOM could not be found.The bioavailability of model compounds was decreased by increasing DOM concentration in the water series. For all four model contaminants, measured bioconcentration factors (BCF) correlated well with the A270 of a water and HbA content of the DOM. These results show that the total DOM concentration is an important factor controlling the bioavailability of xenobiotics in natural waters. Besides the quantity also the quality of DOM, like proportion of HbA, can contribute in bioavailability.  相似文献   

10.
The objective of this study was to evaluate the formation and speciation of iodinated trihalomethanes (I-THMs) from preformed chloramination of waters containing bromide (Br) and iodide (I) at a Br/I weight ratio of 10:1. The factors investigated were pH, iodide to dissolved organic carbon (I/DOC) ratio, and NOM characteristics, specifically SUVA254. A Br/I ratio of 1:2 was also evaluated to determine the importance of Br and I concentrations and ratio on I-THM formation and speciation. Regulated triholamethanes (THMs) were measured alongside I-THMs for a more complete understanding of trihalomethane formation. The results showed that, in general, both I-THM and THM formation increased with decreased pH. Greater formation at lower pH was likely attributed to monochloramine decomposition and the formation of additional oxidants and substituting agents, most notably chlorine. For pH ≥ 7.5, I-THM yield increased with increasing I/DOC ratio and decreasing specific ultraviolet absorbance (SUVA254) of the water. The Br/I, Br/DOC and I/DOC ratios were important factors for I-THM and THM speciation. At pH 6, dichloroiodomethane (CHCl2I) and bromochloroiodomethane (CHBrClI) were the dominant species at the common bromide and iodide levels. For pH ≥ 7.5 and for elevated bromide and iodide levels, iodoform (CHI3) was always the dominant specie regardless of the Br/I ratio. The results demonstrated that it is important to examine I-THM formation and speciation at typical Br/I ratios (∼10) of natural waters, which have often been overlooked in previous investigations, in order to obtain practical and relevant results.  相似文献   

11.
The influences of various geochemical constituents, such as humic acid, HCO3, and Ca2+, on Cr(VI) removal by zero-valent iron (Fe0) were investigated in a batch setting. The collective impacts of humic acid, HCO3, and Ca2+ on the Cr(VI) reduction process by Fe0 appeared to significantly differ from their individual impacts. Humic acid introduced a marginal influence on Fe0 reactivity toward Cr(VI) reduction, whereas HCO3 greatly enhanced Cr(VI) removal by maintaining the solution pH near neutral. The Cr(VI) reduction rate constants (kobs) were increased by 37.8% and 78.3%, respectively, with 2 mM and 6 mM HCO3 in solutions where humic acid and Ca2+ were absent. Singly present Ca2+ did not show a significant impact to Cr(VI) reduction. However, probably due to the formation of passivating CaCO3, further addition of Ca2+ to HCO3 containing solutions resulted in a decrease of kobs compared to solutions containing HCO3 alone. Ca2+ enhanced humic acid adsorption led to a minor decrease of Cr(VI) reduction rates. In Ca2+-free solutions, humic acid increased the amount of total dissolved iron to 25 mg/l due to the formation of soluble Fe-humate complexes and stably dispersed fine Fe (oxy)hydroxide colloids, which appeared to suppress iron precipitation. In contrast, the coexistence of humic acid and Ca2+ significantly promoted the aggregation of Fe (oxy)hydroxides, with which humic acid co-aggregated and co-precipitated. These aggregates would progressively be deposited on Fe0 surfaces and impose long-term impacts on the permeability of PRBs.  相似文献   

12.
A survey study conducted randomly in the cities of Erzurum, Erzincan and Kars included 360 subjects interviewed face to face. It was aimed to detect the subjective features of the participants such as gender, marital status, age, educational status and income level and the reflections of these features on the city parks. Conclusively, it was determined that those who are male, unmarried, at the age of between 19 and 24, university graduate and with a monthly income of 65–125 USD use the parks in majority. In the statistical analysis, the SPSS software was used and variables were compared. Chi-square (χ2) test was used to determine the independency correlations. According to the analysis, gender and income had no significant effect on the use of city parks, but marital status, age and education status had significant effects at 5% significance levels (*p<0.05p<0.05, χ2: 27.805; *p<0.05p<0.05, χ2: 44.073; *p<0.05p<0.05, χ2: 39.998, respectively).  相似文献   

13.
14.
A series of reduced-scale experiments were carried out in order to investigate thermal behaviors of window flame, which exposes the upper floors as well as the adjacent buildings to potential risks of fire spread. A stainless pan filled with alcohol was used as the fire source and was placed inside a cubic compartment of 900 mm side. Temperatures and velocities at various points inside and outside of the compartment were measured. The compartment was pressurized during the experiment by mechanically supplying air at several mass inflow rates through an inlet duct set at the bottom part of the compartment. This was for simulating fire conditions under the effect of external wind pressure. On the basis of the experimental observation, line (i.e., two-dimensional) heat source assumption was adopted for developing a model of window flame behavior. A dimensionless parameter Q*Q* was derived from the governing differential equations in order to generalize the measurement results. Expressions for temperature rise along the trajectory ΔTm and characteristic flame width bT were developed incorporating the parameter Q*Q*.  相似文献   

15.
This study focuses on the removal of 32 selected micropollutants (pharmaceuticals, corrosion inhibitors and biocides/pesticides) found in an effluent coming from a municipal wastewater treatment plant (MWTP) based on activated sludge. Dissolved organic matter was present, with an initial total organic carbon of 15.9 mg L−1, and a real global quantity of micropollutants of 29.5 μg L−1. The treatments tested on the micropollutants removal were: UV-light emitting at 254 nm (UV254) alone, dark Fenton (Fe2+,3+/H2O2) and photo-Fenton (Fe2+,3+/H2O2/light). Different irradiation sources were used for the photo-Fenton experiences: UV254 and simulated sunlight. Iron and H2O2 concentrations were also changed in photo-Fenton experiences in order to evaluate its influence on the degradation. All the experiments were developed at natural pH, near neutral. Photo-Fenton treatments employing UV254, 50 mg L−1 of H2O2, with and without adding iron (5 mg L−1 of Fe2+ added or 1.48 mg L−1 of total iron already present) gave the best results. Global percentages of micropollutants removal achieved were 98 and a 97% respectively, after 30 min of treatments. As the H2O2 concentration increased (10, 25 and 50 mg L−1), best degradations were observed. UV254, Fenton, and photo-Fenton under simulated sunlight gave less promising results with lower percentages of removal.The highlight of this paper is to point out the possibility of the micropollutants degradation in spite the presence of DOM in much higher concentrations.  相似文献   

16.
Yonkyu Choi 《Water research》2010,44(1):115-122
UV treatment is a cost-effective disinfection process for drinking water, but concerned to have negative effects on water quality in distribution system by changed DOM structure. In the study, the authors evaluated the effects of UV disinfection on the water quality in the distribution system by investigating structure of DOM, concentration of AOC, chlorine demand and DBP formation before and after UV disinfection process. Although UV treatment did not affect concentration of AOC and characteristics of DOM (e.g., DOC, UV254, SUVA254, the ratio of hydrophilic/hydrophobic fractions, and distribution of molecular weight) significantly, the increase of low molecular fraction was observed after UV treatment, in dry season. Chlorine demand and THMFP are also increased with chlorination of UV treated water. This implies that UV irradiation can cleave DOM, but molecular weights of broken DOM are not low enough to be used directly by microorganisms in distribution system. Nonetheless, modification of DOM structure can affect water quality of distribution system as it can increase chlorine demands and DBPs formation by post-chlorination.  相似文献   

17.
The formation of disinfection by-products (DBPs) is a public health concern. An important way to evaluate the presence of DBPs is in terms of the total organic halogen (TOX), which can be further specified into total organic chlorine (TOCl), bromine (TOBr), and iodine (TOI). The formation and distribution of halogen-specific TOX during chlorination and chloramination of natural organic matter (NOM) isolates in the presence of bromide and iodide ions were studied. As expected, chloramination produced significantly less TOX than chlorination. TOCl was the dominant species formed in both chlorination and chloramination. TOI was always produced in chloramination, but not in chlorination when high chlorine dose was used, due to the limited presence of HOI in chlorination as a result of the oxidation of iodide to iodate in the presence of excess chlorine. The formation of TOI during chloramination increased as the initial iodide ion concentration increased, with a maximum of ∼60% of the initial iodide ion becoming incorporated into NOM. Iodine incorporation in NOM was consistently higher than bromine incorporation, demonstrating that the competitive reactions between bromine and iodine species in chloramination favoured the formation of HOI and thus TOI, rather than TOBr. Correlations between the aromatic character of the NOM isolates (SUVA254 and % aromatic C) and the concentrations of overall TOX and halogen-specific TOX in chloramination were observed. This indicates that the aromatic moieties in NOM, as indicated by SUVA254 and % aromatic C, play an important role in the formation of overall TOX and halogen-specific TOX in chloramination. THMs comprised only a fraction of TOX, up to 7% in chloramination and up to 47% in chlorination. Although chloramine produces less TOX than chlorine, it formed proportionally more non-THM DBPs than chlorine. These non-THM DBPs are mostly unknown, corresponding to unknown health risks. Considering the higher potential for formation of iodinated DBPs and unknown DBPs associated with the use of chloramine, water utilities need to carefully balance the risks and benefits of using chloramine as an alternative disinfectant to chlorine in order to satisfy guideline values for THMs.  相似文献   

18.
19.
20.
Sorption processes involving secondary iron minerals may significantly contribute to immobilisation of metals in soils and surface waters. In the present work the effect of dissolved organic matter (DOM) from a concentrated bog-water on the adsorption of Cu(II) onto schwertmannite (Fe8O8(OH)6SO4) and goethite (α-FeOOH) has been studied. The acid/base behaviour of DOM up to pH 6 was explained by assuming a diprotic acid with a density of carboxylate groups of 6.90 μeq (mg C)−1. The resulting acidity constants, recalculated to zero ionic strength were and .The uptake of DOM to schwertmannite and goethite was highest at low pH although adsorption was significant also under mildly alkaline conditions. Adsorption to the two minerals was similar although at high pH more DOM was adsorbed to schwertmannite than to goethite.DOM enhanced the adsorption of Cu(II) at moderately low pH in the goethite system but there was no effect of DOM in the case of schwertmannite. The presence of Cu(II) resulted in a decreased adsorption of DOM to goethite at weakly acidic pH and increased adsorption at high pH. In the case of schwertmannite, Cu(II) did not affect DOM uptake.  相似文献   

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