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1.
《Ultrasonics sonochemistry》2014,21(4):1310-1317
A novel sonoelectrochemical catalytic oxidation-driven process using a nanocoated electrode to treat methylene blue (MB) wastewater was developed. The nano-scale (nanocoated) electrode generated more hydroxyl radicals than non-nano-scale (non-nanocoated) electrodes did. However, hydroxyl radicals were easily adsorbed by the nanomaterial and thus were not able to enter the solution. Supersonic waves were found to enhance the mass-transfer effect on the nanocoated electrode surface, resulting in rapid diffusion of the generated hydroxyl radicals into the solution. In solution, the hydroxyl radicals then reacted with organic pollutants in the presence of ultrasonic waves. The effect of the nanocoated electrode on the MB wastewater treatment process was enhanced by ultrasound when compared to the non-nanocoated electrode used under the same conditions. The synergy of the nanocoated electrode and ultrasonic waves towards MB degradation was then studied. The optimum operating conditions resulted in a 92% removal efficiency for TOC and consisted of a current of 600 mA, an ultrasound frequency of 45 kHz, and a supersonic power of 250 W. The mechanism of ultrasound enhancement of the nanocoated electrode activity with respect to MB treatment is discussed. The reaction intermediates of the sonoelectrochemical catalytic oxidation process were monitored, and degradation pathways were proposed. The sonoelectrochemical catalytic oxidation-driven process using nanocoated electrodes was found to be a very efficient method for the treatment of non-biodegradable wastewater.  相似文献   

2.
《Ultrasonics sonochemistry》2014,21(6):1982-1987
Sonophotolytic degradation of THMs mixture with different electrical energy ratio was carried out for efficient design of process. The total consumed electrical energy was fixed around 50 W, and five different energy conditions were applied. The maximum degradation rate showed in conditions of US:UV = 1:3 and US:UV = 0:4. This is because the photolytic degradation of bromate compounds is dominant degradation mechanism for THMs removal. However, the fastest degradation of total organic carbon was observed in a condition of US:UV = 1:3. Because hydrogen peroxide generated by sonication was effectively dissociated to hydroxyl radicals by ultraviolet, the concentration of hydroxyl radical was maintained high. This mechanism provided additional degradation of organics. This result was supported by comparison between the concentration of hydrogen peroxide sole and combined process. Consequently, the optimal energy ratio was US:UV = 1:3 for degradation of THMs in sonophotolytic process.  相似文献   

3.
Degradation of azo dye Acid Orange 7 (AO7) by zero-valent aluminum (ZVAl) in combination with ultrasonic irradiation was investigated. The preliminary studies of optimal degradation methodology were conducted with sole ultrasonic, sole ZVAl/air system, ultrasonication + ZVAl/air system (US-ZVAl). In ZVAl/air system, the degradation of AO7 could almost not be observed within 30 min. The degradation of AO7 by ZVAl/air system was obviously enhanced under ultrasound irradiation, and the enhancement is mainly attributed to that the production of hydroxyl radicals in ultrasound-ZVAl process was much higher than that in sole ultrasonic or in sole ZVAl/air system. The variables considered for the effect of degradation were the power of ultrasound, the initial concentration of AO7, as well as the initial pH value and the dosage of zero-valent aluminum. The results showed that the decolorization rate increased with the increase of power density and the dosage of ZVAl, but decreased with the increase of initial pH value and initial concentration of AO7. More than 96% of AO7 removal was achieved within 30 min under optimum operational conditions (AO7: 20 mg/L, ZVAl: 2 g/L, pH: 2.5, ultrasound: 20 kHz, 300 W). This study demonstrates that ultrasound-ZVAl process can effectively decolorize the azo dye AO7 in wastewater.  相似文献   

4.
The plasma-treated pyrite (PTP) nanostructures were prepared from natural pyrite (NP) utilizing argon plasma due to its sputtering and cleaning effects resulting in more active surface area. The NP and PTP were characterized using X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), Brunauer–Emmett–Teller (BET) and scanning electron microscopy (SEM) methods. The performance of the PTP was greater than NP for treatment of Reactive Red 84 (RR84) by the heterogeneous sono-Fenton process. The optimum amounts of main operational parameters were obtained as PTP of 4 g/L, initial dye concentration of 10 mg/L, pH of 5, and ultrasonic power of 300 W after 120 min of reaction time. Also, the effects of enhancers, and inorganic salts and t-butanol as hydroxyl radical scavengers on the degradation efficiency were investigated. Gas chromatography–mass spectroscopy analysis (GC–MS) was applied for detection of some degradation intermediates. Environmentally friendly plasma modification of the NP, in situ production of H2O2 and OH radicals, low leached iron concentration and repeated reusability at the milder pH are the significant benefits of the PTP utilization.  相似文献   

5.
A sonophotochemical oxidation process has been used for the treatment of an aqueous solution of phenol. The aim of this work is to evaluate the effect of nitrate ions on hydroxyl radical production and on phenol oxidation. It has been demonstrated that ultrasound can produce NOx (nitrate and nitrite), with a production rate of 2.2 μM min−1. The photolysis of nitrate can significantly improve the hydroxyl radical production. The apparent rate constant for hydroxyl radical production increased from 0.0015 min−1 to 0.0073 min−1 while increasing initial nitrate concentration from 0 to 0.5 mM. The concentration of hydroxyl radical was directly proportional to the initial nitrate concentration. Using US/UV process, the apparent reaction rate constant of phenol degradation in the presence of nitrate reached 0.020 min−1, which was relatively lower than the value obtained (0.027 min−1) in the absence of nitrate. It appeared that, nitrate ions can inhibit the sonochemical degradation of organic compounds such as phenol.  相似文献   

6.
Hydrolytic enzymes released by the microorganisms in activated sludge are responsible for the organic matter degradation; however, the optimal extraction procedure of this valuable resource has not been well established until now. The present study evaluates the recovery of protease and lipase from the activated sludge by using stirring and ultrasonication, varying different parameters such as extraction time, concentration of additives (Triton X100, Cation Exchange Resin and Tris buffer), stirring velocity, ultrasonic power and sludge source. Sludge was collected from two urban wastewater treatment plants located in Prague (Czech Republic) and Reus (Spain). It was found that stirring using 2% v/v Triton X100 for 1 h was enough to extract 57.4 protease units/g VSS, and that the same method using a combination of 10 mM Tris pH 7.5 + 0.48 g/mL CER + 0.5% TX100 as an additive allowed to extract 15.5 lipase units/g VSS from sludge collected from Reus Wastewater Treatment Plant. Ultrasonication allowed reducing the extraction time to 10 min for protease (using 2% v/v Triton X100 yielding 52.9 units/g VSS) and to 20 min for lipase (without any additive yielding nearly 21.4 units/g VSS), which makes this method appropriate for the extraction of enzymes from the activated sludge, and suitable to be scaled up for its application in the industry.  相似文献   

7.
《Ultrasonics sonochemistry》2014,21(4):1358-1365
Ultrasonic-assisted heterogeneous Fenton reaction was used for degradation of nitrobenzene (NB) at neutral pH conditions. Nano-sized oxides of α-Fe2O3 and CuO were prepared, characterized and tested in degradation of NB (10 mg L−1) under sonication of 20 kHz at 25 °C. Complete degradation of NB was effected at pH 7 in presence of 10 mM H2O2 after 10 min of sonication in presence of α-Fe2O3 (1.0 g L−1), (k = 0.58 min−1) and after 25 min in case of CuO (k = 0.126 min−1). α-Fe2O3 showed also effective degradation under the conditions of 0.1 g L−1 oxide and 5.0 mM of H2O2, even though with a lower rate constant (0.346 min−1). Sonication plays a major role in enhancing the production of hydroxyl radicals in presence of solid oxides. Hydroxyl radicals-degradation pathway is suggested and adopted to explain the differences noted in rate constants recorded on using different oxides.  相似文献   

8.
A system of ultrasound radiation coupled with Zn0 was applied to degrade diclofenac. The effects of initial pH, dosage of Zn0 and ultrasound density were investigated. To further explore the mechanism of the microcosmic reaction, the fresh and used Zn0 powders were characterized by SEM, XRD and XPS. Radical scavengers were used to determine the oxidation performance of strong oxidizing free radicals on diclofenac, including hydroxyl radicals and superoxide radicals. The results showed that the optimum removal of diclofenac reached to over 85% at pH of 2.0 in 15 min, with Zn0 dosage of 0.1 g/L and ultrasound density of 0.6 W/cm3. TOC removal of 72.6% in 15 min and dechlorination efficiency of diclofenac reached 70% in 30 min. Characterization results showed that a ZnO membrane was generated on the surface of Zn particles after use. According to the mass spectrometry results, several possible pathways of diclofenac degradation were proposed, and most diclofenac was turned into micro-molecules or CO2 finally. The synergistic effect of US/Zn0 in the reactions led to a proposed degradation mechanism in which zinc could directly attack the target contaminant diclofenac because of its good reducibility with the auxiliary functions of ultrasonic irradiation, mechanical shearing and free radical oxidation.  相似文献   

9.
To augment the removal of pharmaceuticals different conventional and alternative wastewater treatment processes and their combinations were investigated. We tested the efficiency of (1) two distinct laboratory scale biological processes: suspended activated sludge and attached-growth biomass, (2) a combined hydrodynamic cavitation–hydrogen peroxide process and (3) UV treatment. Five pharmaceuticals were chosen including ibuprofen, naproxen, ketoprofen, carbamazepine and diclofenac, and an active metabolite of the lipid regulating agent clofibric acid.Biological treatment efficiency was evaluated using lab-scale suspended activated sludge and moving bed biofilm flow-through reactors, which were operated under identical conditions in respect to hydraulic retention time, working volume, concentration of added pharmaceuticals and synthetic wastewater composition. The suspended activated sludge process showed poor and inconsistent removal of clofibric acid, carbamazepine and diclofenac, while ibuprofen, naproxen and ketoprofen yielded over 74% removal. Moving bed biofilm reactors were filled with two different types of carriers i.e. Kaldnes K1 and Mutag BioChip? and resulted in higher removal efficiencies for ibuprofen and diclofenac. Augmentation and consistency in the removal of diclofenac were observed in reactors using Mutag BioChip? carriers (85% ± 10%) compared to reactors using Kaldnes carriers and suspended activated sludge (74% ± 22% and 48% ± 19%, respectively). To enhance the removal of pharmaceuticals hydrodynamic cavitation with hydrogen peroxide process was evaluated and optimal conditions for removal were established regarding the duration of cavitation, amount of added hydrogen peroxide and initial pressure, all of which influence the efficiency of the process. Optimal parameters resulted in removal efficiencies between 3–70%. Coupling the attached-growth biomass biological treatment, hydrodynamic cavitation/hydrogen peroxide process and UV treatment resulted in removal efficiencies of >90% for clofibric acid and >98% for carbamazepine and diclofenac, while the remaining compounds were reduced to levels below the LOD. For ibuprofen, naproxen, ketoprofen and diclofenac the highest contribution to overall removal was attributed to biological treatment, for clofibric acid UV treatment was the most efficient, while for carbamazepine hydrodynamic cavitation/hydrogen peroxide process and UV treatment were equally efficient.  相似文献   

10.
Nano-sized magnetic Fe0/polyaniline (Fe0/PANI) nanofibers were used as an effective material for sonocatalytic degradation of organic anionic Congo red (CR) dye. Fe0/PANI, was synthesized via reductive deposition of nano-Fe0 onto the PANI nanofibers at room temperature. Prepared catalyst was characterized using HR-TEM, FE-SEM, XRD, FTIR instruments. The efficacy of catalyst in removing CR was assessed colorimetrically using UV–visible spectroscopy under different experimental conditions such as % of Fe0 loading into the composite material, solution pH, initial concentration of dye, catalyst dosage, temperature and ultrasonic power. The optimum conditions for sonocatalytic degradation of CR were obtained at catalyst concentrations = 500 mg.L−1, concentration of CR = 200 ppm, solution pH = neutral (7.0), temperature = 30 °C, % of Fe0 loading = 30% and 500 W ultrasonic power. The experimental results showed that ultrasonic process could remove 98% of Congo red within 30 min with higher Qmax value (Qmax = 446.4 at 25 °C). The rate of degradation of CR dye was much faster in this ultrasonic technique rather than conventional adsorption process. The degradation efficiency declined with the addition of common inorganic salts (NaCl, Na2CO3, Na2SO4 and Na3PO4). The rate of degradation suppressed more with increasing salt concentration. Kinetic and isotherm studies indicated that the degradation of CR provides pseudo-second order rate kinetic and Langmuir isotherm model compared to all other models tested. The excellent high degradation capacity of Fe0/PANI under ultrasonic irradiation can be explained on the basis of the formation of active hydroxyl radicals (OH) and subsequently a series of free radical reactions.  相似文献   

11.
The effects of critical factors such as Henry’s Law constant, atmospheric OH rate constant, initial concentration, H2O2, FeSO4 and tert-butanol on the sonochemical degradation of fumaric acid have been investigated. The pseudo first-order rate constant for the sonochemical degradation of 1 mM fumaric acid is much lower than those for chloroform and phenol degradation, and is related to solute concentration at the bubble/water interface and reactivity towards hydroxyl radicals. Furthermore, fumaric acid is preferentially oxidized at the lower initial concentration. It is unreactive to H2O2 under agitation at room temperature. However, the degradation rate of fumaric acid increases with the addition of H2O2 under sonication. 0.1 mM of fumaric acid suppresses H2O2 formation thanks to water sonolysis, while degradation behavior is also dramatically affected by the addition of an oxidative catalyst (FeSO4) or radical scavenger (tert-butanol), indicating that the degradation of fumaric acid is caused by hydroxyl radicals generated during the collapse of high-energy cavities.  相似文献   

12.
Micropollutants are becoming an increasing problem for the environment and wastewater treatment. One example is Bisphenol A (BPA), an endocrinic disruptor, which is widely used in plastic production. Due to its endocrine disrupting effects on aquatic (micro-)organisms and its ubiquity, in surface- and wastewater alike, adequate treatment techniques are necessary.In this study, the degradation of BPA by a sonoelectrochemical hybrid system was investigated, using a low frequency (24 kHz) ultrasound horn and two boron doped diamond electrodes. It was found that by the combination of the individual processes, i.e. ultrasound and electrochemical oxidation, more than 90% of BPA could be removed within 30 min at an initial concentration of 1 mg L−1. Moreover, synergistic effects were discovered and a considerable improvement compared to the individual processes could be achieved by using a potential of 5 V, whereas synergistic effects were absent at a potential of 10 V. This study provides investigation of ultrasound amplitude, potential and electrode positioning on BPA degradation. The reaction was found to follow pseudo first order kinetics with a rate constant of 0.089 min−1. Samples were analysed by high pressure liquid chromatography (HPLC) using a diode array detector. Moreover, the presence and distribution of hydroxyl radicals within the reactor was visualized by using sonochemiluminescence.  相似文献   

13.
The degradation of a reactive azo dye, Direct Red 81 (DR81), by Fenton process and in conjunction with sonolysis (SonoFenton) was studied. The synergistic effect of Fenton process and sonolysis enhanced the degradation of Direct Red 81 in aqueous solutions and the reaction followed the mechanism of hydroxyl radical (HO) oxidation. The influence of the initial substrate concentration, pH and catalyst loading on the rate of decolorisation were studied. The dye decolorisation followed apparent first order kinetics. The optimum conditions for decolorisation were pH = 3.0, [Fe2+] = 0.2 g/l, [H2O2] = 5.1 × 10−3 mol/l and ultrasonic frequency = 120 kHz, 60 W. These conditions yielded 99% decolorisation of DR81 within 75 min. The sonolytic degradation products of DR81 were identified using Electrospray Ionization-Mass Spectrometry (ESI-MS). The presence of CO32−, HCO3, Cl, NO3, and SO42− ions in the dye solution did not have a considerable effect on the decolorisation efficiency. This study demonstrates that Fenton and SonoFenton methods can effectively decolorize DR81 dye in waste water. The dye concentration used in this study is higher compared to earlier studies illustrating the effective mineralization by the SonoFenton process. The mechanism of dye degradation is also proposed.  相似文献   

14.
We examined the feasibility of using two types of fly ash (an industrial waste from thermal power plants) as a low-cost catalyst to enhance the ultrasonic (US) degradation of ibuprofen (IBP) and sulfamethoxazole (SMX). Two fly ashes, Belews Creek fly ash (BFA), from a power station in North Carolina, and Wateree Station fly ash (WFA), from a power station in South Carolina, were used. The results showed that >99% removal of IBP and SMX was achieved within 30 and 60 min of sonication, respectively, at 580 kHz and pH 3.5. Furthermore, the removal of IBP and SMX achieved, in terms of frequency, was in the order 580 kHz > 1000 kHz > 28 kHz, and in terms of pH, was in the order of pH 3.5 > pH 7 > pH 9.5. WFA showed significant enhancement in the removal of IBP and SMX, which reached >99% removal within 20 and 50 min, respectively, at 580 kHz and pH 3.5. This was presumably because WFA contains more silicon dioxide than BFA, which can enhance the formation of OH radicals during sonication. Additionally, WFA has finer particles than BFA, which can increase the adsorption capacity in removing IBP and SMX. The sonocatalytic degradation of IBP and SMX fitted pseudo first-order rate kinetics and the synergistic indices of all the reactions were determined to compare the efficiency of the fly ashes. Overall, the findings have showed that WFA combined with US has potential for treating organic pollutants, such as IBP and SMX, in water and wastewater.  相似文献   

15.
The purpose of this study, is to compare the sequences: 1) proton density (PD) BLADE (BLADE is a PROPELLER-equivalent implementation of the Siemens Medical System) with fat saturation (FS) coronal (COR), 2) PD FS COR, 3) multi-planar reconstruction (MPR) with 3 mm slice thickness and 4) multi-planar reconstruction (MPR) with 1.5 mm slice thickness, both from the T2 3D-double-echo steady state (DESS) with water excitation (WE) sagittal (SAG), regarding their abilities to identify changes in the femorotibial condyle cartilage in knee MRI examinations. Thirty three consecutive patients with osteoarthritis (18 females, 15 males; mean age 56 years, range 37–71 years), who had been routinely scanned for knee examination using the previously mentioned image acquisition techniques, participated in the study. A quantitative analysis was performed based on the relative contrast (ReCON) measurements, which were taken both on normal tissues as well as on pathologies. Additionally, a qualitative analysis was performed by two radiologists. Motion and pulsatile flow artifacts were evaluated. The PD BLADE FS COR sequence produced images of higher contrast between Menisci and Cartilage, Fluid and Cartilage, Pathologies and Cartilage as well as of the Conspicuousness Superficial Cartilage and it was found to be superior to the other sequences (p < 0.001). The sequences T2 3D DESS 1.5 mm and T2 3D DESS 3 mm were significantly superior to the PD BLADE FS COR and the PD FS COR sequences in the visualization of Bone and Cartilage and the Conspicuousness Deep Surface Cartilage. This pattern of results is also confirmed by the quantitative analysis. PD FS BLADE sequences are ideal for the depiction of the cartilage pathologies compared to the conventional PD FS and T2 3D DESS sequences.  相似文献   

16.
Ultrasonic frequencies of 20 kHz, 382 kHz, 584 kHz, 862 kHz (and 998 kHz) have been compared with regard to energy output and hydroxyl radical formation utilising the salicylic acid dosimeter. The 862 kHz frequency inputs 6 times the number of Watts into water, as measured by calorimetry, with the other frequencies having roughly the same value under very similar conditions. A plausible explanation involving acoustic fountain formation is proposed although enhanced coupling between this frequency and water cannot be discounted. Using the salicylic acid dosimeter and inputting virtually the same Wattages it is established that 862 kHz is around 10% more efficient at generating hydroxyl radicals than the 382 kHz but both of these are far more effective than the other frequencies. Also, it is found that as temperature increases to 42 °C then the total dihydroxybenzoic acid (Total DHBA) produced is virtually identical for 382 kHz and 862 kHz, though 582 kHz is substantially lower, when the power levels are set at approximately 9 W for all systems. An equivalent power level of 9 W could not be obtained for the 998 kHz transducer so a direct comparison could not be made in this instance. These results have implications for the optimum frequencies chosen for both Advanced Oxidation Processes (AOPs) and organic synthesis augmented by ultrasound.  相似文献   

17.
Ultrasonic irradiation (640 kHz) leads to the effective degradation of 5-methyl-benzotriazole (5-MBT) in O2 saturated aqueous solution. Up to 97% of 5-MBT is eliminated within 2 h of treatment. Upon extended treatment of 6 h, UV absorbance of the n  π1 and π  π1 transitions associated with aromatic and conjugated systems are completely removed, indicating complete destruction of the aromatic system in 5-MBT. The decomposition of 5-MBT follows pseudo-first order kinetics and the observed decomposition rate dropped significantly in the presence of tertiary butyl alcohol. Detailed product studies were performed employing a negative mode ESI LC–MS. Twenty eight intermediate products were detected during ultrasonic mediated degradation of 5-MBT. Reaction pathways are proposed based on the structures of products assigned to observed 28 masses from LC–MS and commonly accepted degradation pathways observed by thermal and hydroxyl radical mediated pathways often associated with ultrasonic treatment.  相似文献   

18.
The aim of this research was to evaluate the efficiency of an ultrasonication process in combination with METIX-AC technology, a chemical process, for metal removal and dewatering ability, with preservation of fertilizing properties of sewage sludge. Waste activated sludge samples having a total solids concentration of 4 and 20 g L?1, were enriched with Cu and Zn in order to exceed the limiting values recommended by Québec regulation for sludge valorization. Ultrasonication was applied at low frequency (22 kHz) at specific energies ranging from 180 to 66,000 kJ kg?1 of dry sludge. Ultrasound-assisted leaching rates and yields were similar to chemical leaching alone for Zn, whereas solubilisation was reduced for Cu, regardless the specific energy. Fertilizing properties preservation and dewatering ability were similar in ultrasound-assisted leaching, compared to chemical leaching alone. These trends were mainly attributed to the changes of metal speciation, particle size and morphology during ultrasonication, in addition to untreated sludge properties.  相似文献   

19.
The present study demonstrated that the combined use of the sonocatalytic reaction (using ultrasound and titanium dioxide) and the Fenton reaction exhibited synergistically enhanced hydroxyl (OH) radical generation. Dihydroxybenzoic acid (DHBA) concentration as index of OH radical generation was 13 and 115 μM at 10 min in the sonocatalytic reaction and Fenton reaction, respectively. On the other hand, the DHBA concentration was 378 μM at 10 min in the sonocatalytic–Fenton reaction. The sonocatalytic–Fenton reaction was used for degradation of lignin. The lignin degradation ratio was 1.8%, 49.9%, and 60.0% at 180 min in the sonocatalytic reaction, Fenton reaction, and sonocatalytic–Fenton reaction, respectively. Moreover, the sonocatalytic–Fenton reaction was applied to pretreatment of lignocellulosic biomass to enhance subsequent enzymatic saccharification. The cellulose saccharification ratio was 11%, 14%, 16% and 25% at 360 min of pretreatment by control reaction, the sonocatalytic reaction, Fenton reaction, and sonocatalytic–Fenton reaction, respectively.  相似文献   

20.
The effects and mechanism of phycocyanin removal from water by high-frequency ultrasound treatment were studied. The efficiency of sonication treatment in removing proteins derived from algal cells was investigated, and the factors influencing the process, including the effects of coagulation, were also studied. In addition, sodium dodecyl sulfate polyacrylamide gel electrophoresis (SDS-PAGE), the three-dimensional fluorescence spectrum, and mass spectrum were used to illustrate the removal mechanism. The results indicated that phycocyanin can be degraded to the point where it is barely detectable in water samples after 180 min of high-frequency sonication. While the total nitrogen (TN) concentration remained consistent during the entire sonication process (240 min), about 78.9% of the dissolved organic nitrogen (DON) was oxidized into inorganic nitrogen. The sonication effect was greatly influenced by the ultrasound frequency, with 200 kHz having the highest removal performance due to the large production of hydroxyl (HO) radicals. Coagulation was adversely influenced by sonication in the first 60 min due to the cross-linking reaction between protein molecules caused by the sonication. The influence of sonication weakened with sonication time due to the further degradation of the proteins by ultrasound. The variation of the TN, DON, and inorganic nitrogen indicated that the main mechanism occurring during the high-frequency sonication of the phycocyanin was the direct oxidation of the radicals, which was totally different from of the mechanism occurring during ultrasound with low frequency.  相似文献   

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