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1.
The characteristics and influencing factors for dinitrotoluene degradation by nano-Fe3O4-H2O2 were studied, and the nano-scale Fe3O4 catalyst was prepared by the coprecipitation method, with dinitrotoluene wastewater as the degradation object. The results showed that the catalytic reaction system within the pH value range of 1 to 9 could effectively degrade dinitrotoluene, and the optimal pH value was 3; with the increase of catalyst dosage, the degradation efficiency and the catalytic reaction rate of dinitrotoluene grew as well. The optimal catalyst dosage was 1.0 g/L when the H2O2 dosage was within the range of 0 to 0.8 mL/L; the degradation efficiency and reaction rate grew with the increase of H2O2 dosage. With further increase of H2O2 dosage, degradation efficiency and reaction rate decreased; under the best conditions with the H2O2 dosage of 0.8 mL/L, the catalyst concentration of 1 g/L and the pH value of 3 at room temperature (25 °C), the degradation rate of the 100-mg/L dinitrotoluene in 120 min reached 97.6%. Through the use of the probe compounds n-butyl alcohol and benzoquinone, it was proved that the oxidation activity species in the nano-Fe3O4-H2O2 catalytic system were mainly hydroxyl radical (?OH) and superoxide radicals (HO2 ?), based on which, the reaction mechanism was hypothesized.  相似文献   

2.
This laboratory study was designed to investigate the degradation of 4-chloronitrobenzene ([CNB] = 2.4 × 10?6 mol L?1; pH = 7.5) by H2O2/UV and by O3/UV oxidation processes which involve the generation of very reactive and oxidizing hydroxyl free radicals. The effects of the oxidant doses (H2O2 or aqueous O3), liquid flow rate (or the contact time), and bicarbonate ions acting as OH· radical scavengers on the CNB removal rates were studied. For a constant oxidant dose, the results show that the O3/UV system appears to be more efficient than the H2O2/UV system to remove CNB because of the greatest rate of OH· generation by ozone photodecomposition compared to H2O2 photolysis. However, for a given amount of oxidant decomposed, the H2O2/UV oxidant system was found to be more efficient than O3/UV. Moreover, high levels of bicarbonate ions in solution (4 × 10?3 mol L?1) significantly decrease the efficiency of CNB removal by H2O2/UV and by O3/UV oxidation processes.  相似文献   

3.
Fe2-xYxW3O12 powder has been synthesized by the citrate sol-gel process. A model was proposed to calculate the concentration of species in a citric solution. The calculated results could provide valuable information for determining the optimal molar ratio of cation to citric acid and pH value of solution for Fe2-xYxW3O12 preparation. The predicted parameters derived from this model are in good agreement with the experimental results. The prepared gel and the Fe2-xYxW3O12 powder were characterized by X-ray diffraction (XRD) and differential thermal analysis-thermogravimetry (DTA-TG). The results show that it is very difficult to obtain pure Fe2W3O12 powder by the citrate sol-gel process in the temperature range 500°–1000°C, however, Y2W3O12 can easily be prepared even at 500°C. Y2W3O12 annealed at 1000°C for 10 h is favorable for absorbing moisture in air to form Y2W3O12·3.3H2O. The thermal expansion coefficients of Y2W3O12·3.3H2O are: αa = ? 8.01 × 10?6°C?1, αb = ? 2.51 × 10?7°C?1, and αc = ? 5.55 × 10?6°C?1 in 473–1173 K.  相似文献   

4.
The stability and the activity of Fe2O3/Cr2O3 and ZnO/Cr2O3 catalysts were examined for a reverse-watergas-shift reaction (RWReaction). The initial activities of those catalysts were quite high so that the conversion reached close to equilibrium. The activity of Fe2O3/Cr2O3 catalyst decreased from 33.5 to 29.8% during the RWReaction for 75 h at 873 K with GHSV (ml/gcat · h) of 100,000. Moreover, the coke formation on the Fe2O3/Cr2O3 catalyst caused clogging in the RWReactor of the CAMERE process. On the other hand, the ZnO/Cr2O3 catalyst showed no coke formation and no deactivation for the RWReaction at 873 K with GHSV (ml/gcat · h) of 150,000. The ZnO/Cr2O3 was a good catalyst for the RWReaction of the CAMERE process.  相似文献   

5.
BACKGROUND: Heterogeneous Fenton catalysts have been used to treat various organic pollutants in an aqueous environment. The present study has investigated the degradation of 2,4‐dinitrophenol (2,4‐DNP), a priority pollutant generated by such industries as pharmaceuticals, pesticides, pigments and dyes. Degradation of 2,4‐DNP (100 mg L?1) was studied using Fe3+ loaded on Al2O3 as a heterogeneous catalyst in the presence of H2O2, and the efficiency compared with the homogeneous Fe3+/H2O2 based Fenton‐like process. The effect of different parameters for both processes, such as catalyst loading, H2O2 concentration, initial solution pH, initial substrate concentration and temperature were investigated and the optimum operating conditions determined. RESULTS: Under optimal operating conditions of the homogeneous system ([Fe3+] 125 mg L?1; [H2O2] 250 mg L?1; pH 3; room temperature), 92.5% degradation was achieved in 35 min for an initial 2,4‐DNP concentration of 100 mg L?1. In the case of immobilized Fe (Fe3+–Al2O3 catalyst), degradation improved to 98.7% under the condition 10 wt% [Fe3+–Al2O3] 1 g L?1 catalyst loading; [H2O2] 250 mg L?1; pH 3; at room temperature for the same duration. CONCLUSIONS: This study demonstrated the stability and reusability of the prepared heterogeneous catalyst. This process is a viable technique for treatment of aqueous solutions containing contaminants. Copyright © 2012 Society of Chemical Industry  相似文献   

6.
《应用陶瓷进展》2013,112(6):331-336
Abstract

Homogeneous precipitation method was applied to synthesise Ca2Co2O5 powders using calcium nitrate, cobalt nitrate and urea as raw materials. Uniform plate-like Ca2Co2O5 powders with an average grain size of 1 μm can be obtained by calcining the precursor for 8 h at 1073 K in the air. The Ca2Co2O5 ceramics were gained after sintering for 4 h at 1083 K using uniaxial pressure moulding and then sintering technique. The thermoelectric properties of ceramic samples were measured from 303 to 973 K, and the result shows that the electrical conductivity, Seebeck coefficient, thermal conductivity and figure of merit of the sample are 2236·85 S m?1, 175·95 μV K?1, 1·01 W m?1 K?1 and 0·69 at 973 K respectively.  相似文献   

7.
《应用陶瓷进展》2013,112(4):234-239
Abstract

In the present study, the effect of temperature and oxidising agents such as Fe2O3 and Co3O4 on physical and mechanical properties of glass foam is investigated. The glass foam is made of panel glass from dismantled cathode ray tubes and SiC as a foaming agent. In the process, powdered waste glass (mean particle size below 63 μm) in addition to 4 wt-% SiC powder (mean particle size below 45 μm) are combined with Fe2O3 and Co3O4 (0·4, 0·8 and 1·2 wt-%) have been sintered at 950 and 1050°C. The glass foamed containing 1·2 wt-% Co3O4 has good physical properties, with porosity more than 80% and bending strength more than 1·57±0·12 MPa. However, by adding different amounts of Fe2O3 in comparison with samples without iron oxide, little changes in porosity and strength are obtained.  相似文献   

8.
BACKGROUND: A mesoporous alumina supported nanosized Fe2O3 was prepared through an original synthesis procedure and used as a heterogeneous catalyst for the Fenton process degradation of the model azo dye C.I. Acid Orange 7 enhanced by ultrasound irradiation (US/Fe2O3‐Al2O3‐meso/H2O2 system). The effect of various operating conditions was investigated, namely hydrogen peroxide concentration, initial pH, ultrasonic power and catalyst loading. RESULTS: The results indicated that the degradation of C.I. Acid Orange 7 followed a pseudo‐first‐order kinetic model. There exists an optimal hydrogen peroxide concentration, initial pH, ultrasonic power and catalyst loading for decolorization. The aggregate size of the spent catalyst was reduced after dispersion in water by ultrasonic irradiation. A very low level of iron leaching was observed ranging from < 0.1 to 0.23 mg L?1. The intermediate products of C.I. Acid Orange 7 degradation were identified using gas chromatography–mass spectrometry (GC‐MS). CONCLUSION: The optimal conditions for efficient C.I. Acid Orange 7 degradation were pH close to 3, hydrogen peroxide concentration 4 mmol L?1, catalyst loading 0.3 g L?1, and ultrasonic power 80 W. Copyright © 2011 Society of Chemical Industry  相似文献   

9.
Photocatalytic degradation of 4-chlrophenol (4-CP) using UVA-LED assisted persulfate and hydrogen peroxide activated by the nZVI (Nano Zero Valent Iron) in a batch photocatalytic reactor was investigated. The reaction involved a lab-scale photoreactor irradiated with UVA-LED light emitted at 390 nm. The efficiency of the reaction was evaluted in terms of 4-CP degradation and mineralization degree at different pH of solution, initial concentrations of nZVI, persulfate, hydrogen peroxide and 4-CP. In UVA-LED/H2O2/nZVI process, complete degradation of 4-CP (>99%) and 75% mineralization was achieved at pH of 3, hydrogen peroxide concentration of 0.75 mM, nZVI dosage of 1mM and initial 4-CP concentration of 25mg/L at the reaction time of 30 min. The optimum conditions obtained for the best 4-CP degradation rate were at an initial concentration of 25mg/l, persulfate concentration of 1.5mM, nZVI dosage of 1mM, pH of 3 and reaction time of 120min for UVA-LED/persulfate/nZVI process. It was also observed that the 4-CP degradation rate is dependent on initial 4-CP concentrations for both processes. The pseudo-first-order kinetic constant at 25mg/L initial concentration of 4-CP was found to be 1.4×10?1 and 3.8×10?2 in UVA-LED/H2O2/nZVI and UVA-LED/persulfate/nZVI processes, respectively. Briefly, the UVA-LED/H2O2/nZVI process enhanced the degradation rate of 4-CP by 3.67-times in comparison to UVA-LED/persulfate/nZVI process at 30min contact time, which serves as a new and feasible approach for the degradation of 4-CP as well as other organic contaminants containing wastewater.  相似文献   

10.
In the catalytic ozonation process used in this study, adsorption and chemical reactions were performed at the catalyst surface. This process can increase the efficiency of plain ozonation. The main aim of this study was to investigate the efficiency of the catalytic ozonation process in removing Alizarin Red S dye from colored water by Fe2O3 coated on PAC. In this work, activated carbon powder/γ-Fe2O3 nano-composite was modified. The BET results showed that the surface area in PAC and PAC-γ-Fe2O3 nano-composite was 654 and 450?m2 g?1, respectively. In this study, the best pH for removal of ARS was found to be 9. At a higher pH, the efficiency of the process decreased gradually. According to studies, catalysts increase surface area and active sites for more ozone degradation. Also, the characterization of the catalyst will play a very important role in the COP. Also, the maximum removal efficiency was observed in catalyst dose 1.1?g l?1. The study results showed that the highest mineralization rate in ARS degradation was related to O3/PAC/γ-Fe2O3. The amount of mineralization in the SOP, O3-PAC, and O3/PAC/γ-Fe2O3 was 13, 25, and 40%, respectively. The finding of mineralization of ARS using the SOP reflected the low power of the ozonation process for the mineralization of pollutants.  相似文献   

11.
An initial set of 12 kinetic experiments was carried out to remove naphthalene from an aqueous effluent by photo-Fenton involving Fe0 and Fe2+ at two different concentrations of H2O2 (150 and 300?mg?L?1) and three different pHs (3, 5, and 7) (22×31 experiments). The rate constants (k) for the reaction of naphthalene degradation by involving Fe2+ as reactant were in general higher than those with Fe0, but the use of Fe2+ increased the concentration of naphthalene at equilibrium (Ce) when compared with the same response obtained with Fe0 at analogous conditions. A second set of twelve kinetic experiments of photo-Fenton degradation was also performed with persulfate as additive at the conditions already reported, but at a constant concentration of H2O2 of 150?mg?L?1 (21×31 experiments with NaCl +21×31 experiments without NaCl). In almost all the runs in which only the source of iron was varied, k from the kinetic data involving Fe2+ was higher than that involving Fe0, but no difference was observed in terms of Ce that was always zero. The addition of persulfate to treat the effluent either containing or not containing salt enhanced the chemical kinetics, and shifted the equilibrium toward the full removal of naphthalene. A final set of nine experiments of UV photo degradation of naphthalene by involving persulfate without iron, with Fe0 and Fe2+ in the pH range from 3 to 7 (32 experiments) mainly showed that the use of H2O2 may be avoided to remove rapidly and completely naphthalene from wastewater.  相似文献   

12.
To facilitate the recovery of Pb/SiO2 catalyst, magnetic Pb/Fe3O4/SiO2 samples were prepared separately by emulsification, sol-gel and incipient impregnation methods. The catalyst samples were characterized by means of X-ray diffraction and N2 adsorption-desorption, and their catalytic activity was investigated in the reaction for synthesizing propylene carbonate from urea and 1,2-propylene glycol. When the gelatin was applied in the preparation of Fe3O4 at 60°C and the pH value was controlled at 4 in the preparation of Fe3O4/SiO2, the Pb/Fe3O4/SiO2 sample shows good catalytic activity and magnetism. Under the reaction conditions of a reaction temperature of 180°C, reaction time of 2 h, catalyst percentage of 1.7 wt-% and a molar ratio of urea to PG of 1:4, the yield of propylene carbonate attained was 87.7%.  相似文献   

13.
The oxidative dehydrogenation of 4-vinylcyclohexene (VCH) into styrene was carried out in the presence of oxygen over a ZrO2 catalyst promoted with Fe2O3 and CaO. Intrinsically, ZrO2 showed high dehydrogenation activity, which resulted in 80% styrene selectivity with 45% conversion at 425 °C and LHSV 3 h−1. When the ZrO2 was further promoted with calcium and iron, CaO/Fe2O3/ZrO2, the highest styrene selectivity of 88.9% was obtained as well as the lowest deactivation. The deactivation of catalyst was prohibited properly through the introduction of oxygen in the reactant together with the modification of Fe2O3/ZrO2 with CaO. The CaO/Fe2O3/ZrO2 showed constant catalytic activity and selectivity for more than 50 h without deactivation. The selectivity of styrene was strongly influenced by the mole ratio of O2/VCH and 95% selectivity with 80% conversion was obtained at O2/VCH mole ratio of 6 over Fe2O3/ZrO2. It is thought that the oxidative dehydrogenation proceeds through the dehydrogenation (DH) of ring-hydrocarbon of VCH followed by selective combustion of hydrogen (SHC) and the high selectivity of styrene was achieved by the bi-functional role of ZrO2 for DH and SHC reactions. This revised version was published online in July 2006 with corrections to the Cover Date.  相似文献   

14.
《分离科学与技术》2012,47(9):2132-2145
Abstract

MgAl2O4 nanopowder has been prepared by alkoxides hydrolysis with further calcination at temperature of 700°C. The adsorption of a leather dye, Direct Black 38, onto this material was investigated. The sample was characterized by X-ray-diffraction (XRD), N2 adsorption–desorption isotherm and Fourier transform infrared spectroscopy. The results showed that sample present a pure phase, and the average nanocrystal size of 8 nm, the BET surface area is about 206.5 m2 · g?1 and total pore volume is about 1.44 cm3 · g?1. Adsorption kinetics data were modeled by film and pore diffusion model. The experimental isotherm was described by the Langmuir model. MgAl2O4 nanopowder presented a great removal efficiency of leather dye by adsorption process, with a maximum adsorption capacity of 833 mg of dye per gram of adsorbent.  相似文献   

15.
Abstract

The oxidation-precipitation method was used for the synthesis of Fe3O4/AC. The characterization of the catalyst was accomplished by XRD, FT-IR, FE-SEM, BET, and VSM techniques. The obtained results indicated that magnetite nanoparticles were successfully prepared with cubic spinel structures and uniform distribution on the surface of activated carbon by the oxidation-precipitation method. The effect of operating parameters was evaluated to determine the optimum operating condition for the electro-Fenton (EF) removal of catechol as a phenolic pollutant model. At the optimum operating conditions (pH 3, Fe3O4/AC: 0.9?g L?1, Catechol: 8.0?×?10?4?mol L?1 at I: 120?mA), the catechol and COD removal reached 98.2 and 76.1% in 120?min, respectively. Only 2.1% of ferrous and 3.44% of ferric ions were leached into the solution. Regarding the results from utilization of oxidant scavengers (isopropanol and BQ), it can be inferred that hydroxyl radical (responsible for 57% catechol removal) and superoxide anion radical (responsible for 40% catechol removal) is the main oxidants in acidic (pH 3) and basic (pH 10) conditions, respectively. The kinetics of EF removal of catechol was studied and the rate constant for the pseudo-first-order kinetic model was found to be 3.37?×?10?2min?1 (R2 = 0.9924). The GC-MS analysis was carried out to detect the intermediate products and a possible degradation mechanism was proposed. The reusability of Fe3O4/AC was examined for six cycles. It can be concluded that Fe3O4/AC is an applicable ultimate catalyst for EF removal of organic pollutants.  相似文献   

16.
An economical method was proposed to develop an efficient alumina-supported manganese (Mn) and copper (Cu) oxides (Mn-Cu-O/Al2O3) catalyst with a high surface area, 184.06 cm2 g?1. The catalyst was utilized for degradation refinery wastewater by heterogeneous catalytic ozonation. The effects of various operating variables including pH, ozone and catalyst dosages, and temperature were systematically investigated in detail to obtain the optimized conditions for accelerated degradation of refinery wastewater. The optimum values were as follows: ozone dose 50.0 mg L?1, catalyst dose 3.0 g L?1, initial pH = 6.8, T = 17 °C. Refinery wastewater samples were analyzed by chemical oxygen demand (COD) and the results indicated that kinetics of COD followed a pseudo–first-order degradation. Moreover, hydroxyl radical mechanism rather than absorption was proposed, indicating that the surface hydroxyl groups were the active sites that played a significant role in catalytic ozonation.  相似文献   

17.
The compatibilities and conductivities of K2NiF4 typed La2Ni0·9Fe0·1O4+δ (L2NF91) and LaNi0·6Fe0·4O3?δ (LNF64) perovskites, promising cathode materials for solid oxide fuel cell, with Gd0·1Ce0·9O1·95 (GDC) electrolyte were investigated. L2NF91 and LNF64 were synthesised using citrate and modified citrate methods with the calcination temperature of 1000°C for 5 h. The single phased oxides with the average particle sizes of L2NF91 and LNF64 ~0·2 μm were obtained. The thermal expansion coefficients of L2NF91 and LNF64 were 12·7×10?6 and 13·2×10?6 K?1 respectively. The mixtures of cathode materials and the electrolytes were heated between 800 and 1200°C to observe the formation of secondary phases at the operation temperatures of solid oxide fuel cell. The X-ray diffraction and scanning electron microscopy–energy dispersive X-ray results indicated that L2NF91 and LNF64 had good chemical compatibility with GDC from room temperature up to 900°C. Both L2NF91 and LNF64 showed higher conductivities when in contact with GDC electrolyte than with Zr0·92Y0·08O1·96 electrolyte.  相似文献   

18.
BACKGROUND: The removal of antibiotic ampicillin sodium using H2O2 and modified granular activated carbon (GAC) is discussed. Two types of modified activated carbons were used in experiment to catalyze ·OH production from H2O2. One was modified with base (NaOH; called B‐GAC), the other was modified with Fe(NO3)3 (Fe‐GAC) and the nominal Fe metal loading was 5 wt%. In the experiment, pH, contact time, dosage of activated carbon and H2O2 and initial concentration of ampicillin sodium were investigated to determine their influence on the removal efficiency. The stability of Fe‐GAC was also evaluated. RESULTS: With an initial ampicillin sodium concentration of 200 mg L?1, 85.2% of chemical oxygen demand (COD) and 76.4% of total organic carbon (TOC) can be removed with 8.0 g L?1 of B‐GAC and 80 mg L?1 of H2O2 (at pH 5.0). For the Fe‐GAC/H2O2 process, with 5.0 g L?1 of activated carbon and 80 mg L?1 of H2O2, COD and TOC removal can be elevated to 91.2% and 79.5% (at pH 3.0), respectively. CONCLUSION: The integration of activated carbon and H2O2 treatment was more effective for the removal of ampicillin from aqueous solution than using activated carbon alone. In the process, adsorption played a dominant role and the addition of a small amount of H2O2 accelerated the reaction rate and improved the removal efficiency. pH also greatly affected removal efficiency. Copyright © 2011 Society of Chemical Industry  相似文献   

19.
《分离科学与技术》2012,47(3):456-470
ABSTRACT

We present a way of synthesizing nanocomposite Fe3O4@SiO2@CTAB–SiO2 by employing simple sol–gel technique with selective etching for extreme selectivity adsorption of cyclophosphamide (CP). The transmission electron microscopy (TEM); scanning electron microscopy (SEM); X-ray diffraction (XRD); Fourier transform infrared (FT-IR); vibrating sample magnetometer (VSM); pHPZC; and Brunauer, Emmett and Teller (BET) techniques were used for nanocomposite characterization. These nanoparticles have an SBET of 157.8 m2 g?1 and a high saturation magnetization of 67.5 emu g?1. First, the adsorption system was examined as a function of contact time under various initial CP contents, ionic strength, initial solution pH, adsorbent dose and temperature in batch test. The optimum dose, pH and contact time were obtained to be 0.01 g, 7.0 and 30 min, respectively. Ultimately, experimental isotherm and kinetics data of adsorption of CP onto nanocomposite Fe3O4@SiO2@CTAB–SiO2 were fitted to classical models. Additionally, it was found that the maximum adsorption process capacity of CP on adsorbent was 342.8 mg g?1.  相似文献   

20.
A novel waterborne polyurethane-silanized CoFe2O-acrylate magnetic pressure-sensitive adhesive was prepared. With the increase of PU content, gel content, swelling capability, and SAFT increased, and fracture energy increased first, then decreased. The T-peeling strength increased from 8.93 to 19.07 N · m?1, tack force increased from No.3 to No.10, while shear resistance increased from 35 to 72 h, and then they decreased. Two empirical models: WA = 90.46 + 125.04[PU]-319.96[PU]2 and T = 9.09 + 96.07[PU]-235.11[PU]2, were obtained. With the increase of CoFe2O4 content, the saturation magnetization increased from 5.5 to 14.2 emu · g?1, and remanence increased from 1.7 to 3.7 emu · g?1, while coercivity decreased from 875 to 763 Oe.  相似文献   

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