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1.
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   

2.
The effectiveness of ozone combined with ultrasound techniques in degrading reactive red X-3B is evaluated. A comparison among ozone (O3), ultrasonic (US), ozone/ultrasonic (O3/US) for degradation of reactive red X-3B has been performed. Results show that O3/US system was the most effective and the optimally synergetic factor reaches to 1.42 in O3/US system. The cavitation of ultrasound plays an important role during the degradation process. It is found that 99.2% of dye is degraded within 6 min of reaction at the initial concentration of 100 mg·L−1, pH of 6.52, ozone flux of 40 L·h−1 and ultrasonic intensity of 200 W·L−1. Ozonation reactions in conjunction with sonolysis indicate that the decomposition followed pseudo-first-order reaction kinetics but the degradation efficiencies are affected by operating conditions, particularly initial pH and ultrasonic intensity. A kinetic model is established based on the reaction corresponding to operational parameters. In addition, the main reaction intermediates, such as p-benzoquinone, catechol, hydroquinone, phthalic anhydride and phthalic acid, are separated and identified using GC/MS and a possible degradation pathway is proposed during the O3/US process.  相似文献   

3.
《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   

4.
《Ultrasonics sonochemistry》2014,21(3):1206-1212
The decoloration of reactive dye C.I. Reactive Blue 19 (RB 19) using combined ultrasound with the Fenton process has been investigated. The effect of varying the concentrations of hydrogen peroxide and iron sulfate, initial pH, ultrasonic power, initial dye concentration and dissolved gas on the decoloration and degradation efficiencies was measured. Calibration of the ultrasound systems was performed using calorimetric measurements and oxidative species monitoring using the Fricke dosimeter and degradations were carried out with a 20 kHz probe type transducer at 2, 4, 6 and 8 W cm−2 of acoustic intensity at 15, 25, 50 and 75 mg L−1 initial dye concentrations. First order rate kinetics was observed. It was found that while the degradation rate due to ultrasound alone was slow, sonication significantly accelerated the Fenton reaction. While the results were similar to those reported for other dyes, the effects occurred at lower concentrations. The rate and extent of decoloration of RB 19 increased with rising hydrogen peroxide concentration, ultrasonic powers and iron sulfate concentration but decreased with increasing dye concentration. An optimum pH value of pH = 3.5 was found. The rate of decoloration was higher when dissolved oxygen was present as compared with nitrogen and argon confirming the solution phase mechanism of the degradation.  相似文献   

5.
In this paper, the effect of periodate (IO4) on the ultrasonic degradation at 300 kHz of Brilliant Blue R (BBR), an organic dye pollutant, was investigated. The experiments were realized in the absence and presence of periodate for various operating conditions including initial solution pH (2–8) and delivered ultrasonic power (20–80 W). It was found that periodate greatly enhanced the sonochemical degradation of BBR. The degradation rate increased significantly with increasing IO4 concentration up to 10 mM and decreased afterward. With 10 mM of periodate, the degradation rate was 2.4-fold higher than that with ultrasound alone. The chemical probes experiments showed that periodate activation into free radicals (IO3, IO4 and OH) takes place by sonolysis and iodine radicals contribute significantly in the oxidation process. It was found that the periodate-enhanced effect was strongly experimental parameters dependent. The advantageous effect of periodate increased significantly with decreasing power and the best enhancing effect was obtained for the lowest power. Correspondingly, the periodate-enhanced effect increased with pH increase in the range 2–8 and it was more remarkable at near alkaline condition (pH 8). A reaction scheme for periodate sonolysis was proposed, for the first time, discussed and then used for interpreting the obtained results.  相似文献   

6.
《Ultrasonics sonochemistry》2014,21(5):1881-1885
In this work, the decolorization of C.I. Reactive Blue 181 (RB181), an anthraquinone dye, by Ultrasound and Fe2+ H2O2 processes was investigated. The effects of operating parameters, such as Fe2+ dosage, H2O2 dosage, pH value, reaction time and temperature were examined. Process optimisation [pH, ferrous ion (Fe2+), hydrogen peroxide (H2O2), and reaction time], kinetic studies and their comparison were carried out for both of the processes. The Sono-Fenton process was performed by indirect sonication in an ultrasonic water bath, which was operated at a fixed 35-kHz frequency. The optimum conditions were determined as [Fe2+] = 30 mg/L, [H2O2] = 50 mg/L and pH = 3 for the Fenton process and [Fe2+] = 10 mg/L, [H2O2] = 40 mg/L and pH = 3 for the Sono-Fenton process. The colour removals were 88% and 93.5% by the Fenton and Sono-Fenton processes, respectively. The highest decolorization was achieved by the Sono-Fenton process because of the production of some oxidising agents as a result of sonication. The paper also discussed kinetic parameters. The decolorization kinetic of RB181 followed pseudo-second-order reaction (Fenton study) and Behnajady kinetics (Sono-Fenton study).  相似文献   

7.
Effluents from the paper printing and textile industries are often heavily contaminated with azo dyes. Azo dyes are difficult to oxidize biologically. This work investigated the decolorization of an azo dye, C.I. Direct Red 23 (DR23), by persulfate (PS) activated with Fe0 aggregates (PS/Fe0). Ultrasound (US) and heat were used as enhancement tools in the PS oxidation system. Neither US-activated PS nor thermally activated PS was effective in oxidizing DR23. However, the decolorization was significantly enhanced by PS/Fe0 combined with US (PS/Fe0/US) or heat (PS/Fe0/55 °C). Approximately 95% decolorization of 1 × 10−4 M DR23 was achieved within 15 min in the PS/Fe0/US system at an initial pH of 6.0, PS of 5 × 10−3 M, Fe0 of 0.5 g/L and US irradiation of 106 W/cm2 (60 kHz). Complete decolorization was achieved within 10 min in the Fe0/PS/55 °C system. The rate of decolorization doubled when US was introduced in the PS/Fe0 system during the treatment of different initial dye concentrations. The dependence of dye and true color (ADMI) depletion on PS concentration has been discussed. DR23 was completely degraded based on the disappearance of aromatic groups of UV–vis spectra and the variation of TOC mineralization. The observed pseudo-first-order decolorization rate was substantially enhanced by increasing temperature. The Arrhenius activation energy for the PS activated with Fe0 was estimated as 8.98 kcal/mol, implying that higher temperature is beneficial for the DR23 decolorization. The addition of US into the PS/Fe0 system did not incur a substantial increase in electricity, whereas the mineralization of DR23 occurred quickly. Thus, both PS/Fe0/US and heated PS/Fe0 systems are practically feasible for the effective degradation of the direct azo dye in textile wastewater.  相似文献   

8.
In the present work, the degradation of methomyl has been carried out by using the ultrasound cavitation (US) and its combination with H2O2, Fenton and photo-Fenton process. The study of effect of operating pH and ultrasound power density has indicated that maximum extent of degradation of 28.57% could be obtained at the optimal pH of 2.5 and power density of 0.155 W/mL. Application of US in combination with H2O2, Fenton and photo-Fenton process has further accelerated the rate of degradation of methomyl with complete degradation of methomyl in 27 min, 18 min and 9 min respectively. Mineralization study has proved that a combination of US and photo-Fenton process is the most effective process with maximum extent of mineralization of 78.8%. Comparison of energy efficiency and cost effectiveness of various processes has indicated that the electrical cost of 79892.34 Rs./m3 for ultrasonic degradation of methomyl has drastically reduced to 2277.00 Rs./m3, 1518.00 Rs./m3 and 807.58 Rs./m3 by using US in combination with H2O2, Fenton and photo-Fenton process respectively. The cost analysis has also indicated that the combination of US and photo-Fenton process is the most energy efficient and cost effective process.  相似文献   

9.
《Journal of Molecular Liquids》2006,123(2-3):105-109
It is shown that the conductivities of LiBF4, LiPF6, LiN(SO2CF3)2 (LiTFSI), NaPF6, KPF are abnormally high in two diamine solvents: ethylenediamine (EDA) and 1,3-diaminopropane (1,3 DAP). This is particularly evident for KPF6, κMAX(EDA) = 35 mS cm 1 and κMAX(1,3 DAP) = 17.4 mS cm 1. Compared to three other organic solvents having the same viscosity, η  1.6 cP, but higher relative permittivity, NMF ε = 186.9, NMP ε = 32, γ-Bu ε = 39.1, the maxima of conductibility of EDA and 1,2 DAP, which have a low relative permittivity, ε  13–11, are largely superior or equal to those of NMF, NMP, γ-Bu. For KPF6, κMAX(NMF) = 15.4mS cm 1, κMAX(NMP) = 7.8 mS cm 1 and κMAX(γ-BL) = 10.8 mS cm 1. We assume that this is due to a non-Stokesian conductivity mechanism.  相似文献   

10.
《Solid State Ionics》2006,177(1-2):73-76
Ionic conduction in fluorite-type structure oxide ceramics Ce0.8M0.2O2−δ (M = La, Y, Gd, Sm) at temperature 400–800 °C was systematically studied under wet hydrogen/dry nitrogen atmosphere. On the sintered complex oxides as solid electrolyte, ammonia was synthesized from nitrogen and hydrogen at atmospheric pressure in the solid states proton conducting cell reactor by electrochemical methods, which directly evidenced the protonic conduction in those oxides at intermediate temperature. The rate of evolution of ammonia in Ce0.8M0.2O2−δ (M = La, Y, Gd, Sm) is up to 7.2 × 10 9, 7.5 × 10 9, 7.7 × 10 9, 8.2 × 10 9 mol s 1 cm 2, respectively.  相似文献   

11.
《Ultrasonics sonochemistry》2014,21(4):1366-1373
Porous (Ce0.5Zr0.5)O2 solid solutions were prepared by thermolysis (T = 285 °C) or sonolysis (20 kHz, I = 32 W cm−2, Pac = 0.46 W mL−1, T = 200 °C) of Ce(III) and Zr(IV) acetylacetonates in oleylamine or hexadecylamine under argon followed by heat treatment of the precipitates obtained in air at 450 °C. Transmission Electron Microscopy images of the samples show nanoparticles of ca. 4–6 nm for the two synthetic approaches. The powder X-ray diffraction, scanning electron microscopy, energy dispersive X-ray and μ-Raman spectroscopy of solids obtained after heat treatment indicate the formation of (Ce0.5Zr0.5)O2 solid solutions with a metastable tetragonal crystal structure for the two synthetic routes. The specific surface area of the samples varies between 78 and 149 m2 g−1 depending on synthesis conditions. The use of Barrett–Joyner–Halenda and t-plot methods reveal the formation of mixed oxides with a hybrid morphology that combines mesoporosity and microporosity regardless of the method of preparation. Platinum nanoparticles were deposited on the surface of the mixed oxides by sonochemical reduction of Pt(IV). It was found that the materials prepared by sonochemistry exhibit better resistance to dissolution during the deposition process of platinum. X-ray photoelectron spectroscopy analysis shows the presence of Pt(0) and Pt(II) on the surface of mixed oxides. Porous (Ce0.5Zr0.5)O2 mixed oxides loaded with 1.5 %wt. platinum exhibit high activity in catalytic wet air oxidation of formic acid at 40 °C.  相似文献   

12.
Sonoelectrochemical decomposition of organic compounds is a developing technique among advanced oxidation processes (AOPs). It has the advantage over sonication alone that it increases the efficiency of the process in terms of a more rapid decrease in chemical oxygen demand (COD) and in total organic carbon (TOC) and accelerates electrochemical oxidation which normally requires a lengthy period of time to achieve significant mineralisation. Moreover the use of an electrocatalytic electrode in the process further accelerates the oxidation reaction rates. The aim of this study was to improve the decomposition efficiency of methylene blue (MB) dye by sonoelectrochemical decomposition using environmentally friendly and cost-effective Ti/Ta2O5–SnO2 electrodes. Decolourisation was used to assess the initial stages of decomposition and COD together with TOC was used as a measure of total degradation. The effect of a range of sonication frequencies 20, 40, 380, 850, 1000 and 1176 kHz at different powers on the decolourisation efficiency of MB is reported. Frequencies of 850 and 380 kHz and the use of higher powers were found more effective towards dye decolourisation. The time for complete MB degradation was reduced from 180 min using electrolysis and from 90 min while carrying out sonolysis to 45 min when conducting a combined sonoelectrocatalytic experiments. The COD reduction of 85.4% was achieved after 2 h of combined sonication and electrolysis which is a slightly higher than after a single electrolysis (78.9%) and twice that of sonolysis (40.4%). A dramatic improvement of mineralisation values were observed within 2 h of sonoelectrocatalytic MB degradation. The TOC removal efficiency increased by a factor of 10.7 comparing to sonication alone and by a factor of 1.5 comparing to the electrolytic process. The energy consumption (kWh/m3) required for the complete degradation of MB was evaluated.  相似文献   

13.
《Solid State Ionics》2006,177(26-32):2705-2709
Lithium ions of perovskite-type lithium ion conductor La0.55Li0.35TiO3 were replaced by divalent Mg2+, Zn2+, and Mn2+ ions in an ion-exchange reaction using molten chlorides. The polycrystalline Mg-exchanged and Zn-exchanged samples are solid electrolytes for divalent Mg2+ and Zn2+ ions, whose dc ionic conductivities (σ = 2.0 × 10 6 S cm 1 at 558 K for the Mg-exchanged sample, La0.56(2)Li0.02(1)Mg0.16(1)TiO3.01(2) and σ = 1.7 × 10 6 S cm 1 at 708 K for the Zn-exchanged samples, La0.55(1)Li0.0037(2)Zn0.15(1)TiO2.98(2)) were compared to those of the known highest Mg2+ and Zn2+ inorganic solid electrolytes. The Mn-exchanged sample, then, showed paramagnetic behavior in the temperature range of 2 to 300 K. The Mn ions in the exchanged sample are divalent and the spin configuration is in high spin state (S = 5/2).  相似文献   

14.
《Ultrasonics sonochemistry》2014,21(3):1026-1029
Sonoluminescence spectra collected from 0.1 to 3.0 M aqueous solutions of formic acid sparged with argon show the OH(A2Σ+−X2Πi) and C2(d3Πg  a3Πu) emission bands and a broad continuum typical for multibubble sonoluminescence. The overall intensity of sonoluminescence and the sonochemical yield of HCOOH degradation vary in opposite directions: the sonoluminescence is quenched while the sonochemical yield increases with HCOOH concentration. By contrast, the concentration of formic acid has a relatively small effect on the intensity of C2 Swan band. It is concluded that C2 emission originates from CO produced by HCOOH degradation rather than from direct sonochemical degradation of HCOOH. The intensity of C2 band is much stronger at high ultrasonic frequency compared to 20 kHz ultrasound which is in line with higher yields of CO at high frequency. Another product of HCOOH sonolysis, carbon dioxide, strongly quenches sonoluminescence, most probably via collisional non-radiative mechanism.  相似文献   

15.
The dielectric and pyroelectric responses of MgO-modified Pb0.99(Zr0.95Ti0.05)0.98Nb0.02O3 ceramics were investigated near FR(LT)–FR(HT) phase transition. It was found that MgO additive reduced the FR(LT)–FR(HT) phase transition temperature from 41 °C to room temperature (24 °C). Superior room-temperature pyroelectric properties were obtained in the composition of 0.10 wt% MgO addition without DC bias. The largest pyroelectric coefficient, 65 × 10−8 C cm−2 K−1, was detected. Accordingly, the detectivity figures of merit Fd had maximum values of 20 × 10−5 Pa−1/2, and especially the voltage responsivity Fv = 0.91 m2C−1 is the highest value reported so far among all pyroelectric materials. It shows promising potential for application in uncooled pyroelectric infrared detector.  相似文献   

16.
《Solid State Ionics》2006,177(19-25):1725-1728
Apatite-type La10  xSi6  yAlyO27  3x/2  y/2 (x = 0–0.33; y = 0.5–1.5) exhibit predominant oxygen ionic conductivity in a wide range of oxygen partial pressures. The conductivity of silicates containing 26.50–26.75 oxygen atoms per formula unit is comparable to that of gadolinia-doped ceria at 770–870 K. The average thermal expansion coefficients are (8.7–10.8) × 10 6 K 1 at 373–1273 K. At temperatures above 1100 K, silicon oxide volatilization from the surface layers of apatite ceramics and a moderate degradation of the ionic transport with time are observed under reducing conditions, thus limiting the operation temperature of Si-containing solid electrolytes.  相似文献   

17.
《Solid State Ionics》2006,177(1-2):137-140
The thermal decomposition of lithium hexafluorophosphate was studied by using C80 calorimeter, and the samples were heated at a 0.2 K·min 1 heating rate from ambient temperature to 573 K in pressure-sensitive transducer fitted and sealed vessel with argon atmosphere. It is found that LiPF6 decomposes near 433 K, and the gas product PF5 causes the pressure increasing. The LiPF6 decomposition reaction order is calculated based on the pressure data by two methods, its average value is n = 1.5, then, the reaction is assumed to be dependent on the Arrhenius law and mass action law, and thus the activation energy and pre-exponential factor were calculated to be E = 104.2 kJ·mol 1, A = 1.12 × 107 s 1, respectively.  相似文献   

18.
A simple method for synthesis of gold nanoparticles (AuNPs) using Aspergillum sp. WL-Au was presented in this study. According to UV–vis spectra and transmission electron microscopy images, the shape and size of AuNPs were affected by different parameters, including buffer solution, pH, biomass and HAuCl4 concentrations. Phosphate sodium buffer was more suitable for extracellular synthesis of AuNPs, and the optimal conditions for AuNPs synthesis were pH 7.0, biomass 100 mg/mL and HAuCl4 3 mM, leading to the production of spherical and pseudo-spherical nanoparticles. The biosynthesized AuNPs possessed excellent catalytic activities for the reduction of 2-nitrophenol, 3-nitrophenol, 4-nitrophenol, o-nitroaniline and m-nitroaniline in the presence of NaBH4, and the catalytic rate constants were calculated to be 6.3×10−3 s−1, 5.5×10−3 s−1, 10.6×10−3 s−1, 8.4×10−3 s−1 and 13.8×10−3 s−1, respectively. The AuNPs were also able to catalyze the decolorization of various azo dyes (e.g. Cationic Red X-GRL, Acid Orange II and Acid scarlet GR) using NaBH4 as the reductant, and the decolorization rates reached 91.0–96.4% within 7 min. The present study should provide a potential candidate for green synthesis of AuNPs, which could serve as efficient catalysts for aromatic pollutants degradation.  相似文献   

19.
《Solid State Ionics》2006,177(1-2):121-127
Lithium cobalt vanadate LixCoVO4 (x = 0.8; 1.0; 1.2) has been prepared by a solid state reaction method. The XRD analysis confirms the formation of the sample. A new peak has been observed for Li1.0CoVO4 and for Li1.2CoVO4 indicating the formation of a new phase. The XPS analysis indicates the reduction in the oxidation of vanadium and oxygen with the addition of Li in LixCoVO4 (x = 0.8, 1.0, 1.2). The impedance analysis gives the conductivity value as 2.46 × 10 5, 6.16 × 10 5, 9 × 10 5 Ω 1 cm 1 for LixCoVO4 (x = 0.8; 1.0; 1.2), all at 623 K. The similarity in the bulk activation energy (Ea) and the activation enthalpy for migration of ions (Eω) indicate that the conduction in Li1.2CoVO4 has been due to hopping mechanism.  相似文献   

20.
γ-Fe2O3 nanoparticles were synthesized and loaded on activated carbon. The prepared nanomaterial was characterized by field emission scanning electron microscopy (FE-SEM), energy-dispersive X-ray spectroscopy (EDX), Fourier transforms infrared spectroscopy (FT-IR) and X-ray diffraction (XRD). The γ-Fe2O3 nanoparticle-loaded activated carbon (γ-Fe2O3-NPs-AC) was used as novel adsorbent for the ultrasonic-assisted removal of methylene blue (MB) and malachite green (MG). Response surface methodology and artificial neural network were applied to model and optimize the adsorption of the MB and MG in their individual and binary solutions followed by the investigation on adsorption isotherm and kinetics. The individual effects of parameters such as pH, mass of adsorbent, ultrasonication time as well as MB and MG concentrations in addition to the effects of their possible interactions on the adsorption process were investigated. The numerical optimization revealed that the optimum adsorption (>99.5% for each dye) is obtained at 0.02 g, 15 mg L−1, 4 min and 7.0 corresponding to the adsorbent mass, each dye concentration, sonication time and pH, respectively. The Freundlich, Langmuir, Temkin and Dubinin–Radushkevich isotherms were studied. The Langmuir was found to be most applicable isotherm which predicted maximum monolayer adsorption capacities of 195.55 and 207.04 mg g−1 for the adsorption of MB and MG, respectively. The pseudo-second order model was found to be applicable for the adsorption kinetics. Blank experiments (without any adsorbent) were run to investigate the possible degradation of the dyes studied in presence of ultrasonication. No dyes degradation was observed.  相似文献   

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