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1.
Pb2+离子可以作为高效的催化剂用于降解糖为乳酸, 但是为了降低暴露Pb2+离子于环境中的风险,最好的办法是把铅固定在一个固体催化剂上.报道了一个简单的制备Pb(PbO2)/石墨烯复合固体催化剂的方法,可以得到石墨烯负载的纳米铅催化剂,铅颗粒的尺寸在2~5 nm.获得的催化剂可以在水中用于降解葡萄糖、果糖甚至纤维素,产物主要为乳酸.对于果糖、乳酸的产率为58.7% (433 K,2.5 MPa N2);当直接使用纤维素为原料,无额外酸、碱催化剂时,乳酸的产率可以达到31.7%.  相似文献   

2.
The heterogeneous adsorption and catalytic oxidation of benzene, toluene and o-xylene (BTX) over the spent platinum catalyst supported on activated carbon (Pt/AC) as well as the chemically treated spent catalysts were studied to understand their catalytic and adsorption activities. Sulfuric aqueous acid solution (0.1N, H2SO4) was used to regenerate the spent Pt/AC catalyst. The physico-chemical properties of the catalysts in the spent and chemically treated states were analyzed by using nitrogen adsorption-desorption isotherm and elemental analysis (EDX). The gravimetric adsorption and the light-off curve analysis were employed to study the BTX adsorption and oxidation on the spent catalyst and its modified Pt/AC catalysts. The experimental results indicate that the spent Pt/AC catalyst treated with the H2SO4 aqueous solution has a higher toluene adsorption and conversion ability than that of the spent Pt/AC catalyst. A further studies of H2SO4 treated Pt/AC catalyst on their catalytic and heterogeneous adsorption behaviours for BTX revealed that the activity of the H2SO4 treated Pt/AC catalyst follows the sequence of benzene > toluene > o-xylene. The adsorption equilibrium isotherms of BTX on the H2SO4 treated Pt/AC were measured at different temperatures ranging from 120 to 180 °C. To correlate the equilibrium data and evaluate their adsorption affinity for BTX, the two sites localized Langmuir (L2m) isotherm model was employed. The heterogeneous surface feature of the H2SO4 treated Pt/AC was described in detail with the information obtained from the results of isosteric enthalpy of adsorption and adsorption energy distributions. Furthermore, the activity of H2SO4 treated Pt/AC about BTX was found to be directly related to the Henry's constant, isosteric enthalpy of adsorption and adsorption energy distribution functions.  相似文献   

3.
Radiochemical separation experiments have been performed in order to realize a novel reprocessing method based on chromatography techniques using a novel pyridine resin. The newly synthesized tertiary pyridine resin with two functions of ion exchanger and soft-donor was dedicated to the experiments, where highly irradiated mixed oxide fuel from the experimental fast reactor JOYO was used as a reference spent fuel. With a 3-step separation, pure Am and Cm were individually obtained as minor actinide products, and 106Ru group, lanthanides with 137Cs group and Pu group were fractionated, respectively. The decontamination factor of 137Cs and trivalent lanthanides (155Eu, 144Ce) against the Am product exceeded 3.9 × 104 and 1.0 × 105, respectively. The decontamination factor as the mutual separation of 243Cm was larger than 2.2 × 103 against the Am product. Moreover, the content of 137Cs, trivalent lanthanides and 243Cm in Am product did not exceed 2 ppm. The tertiary pyridine resin method is a candidate separation system for an “advanced ORIENT process”, where enhanced separation, transmutation and utilization of actinides, long-lived fission products and rare metal fission product would be oriented.  相似文献   

4.
In this paper, a novel method, hydrodynamic cavitation (HC) combined with Fe3+-doped TiO2, for the degradation of organic pollutants in aqueous solution is reported. The venturi tubes with different geometric parameters (size, shape and half divergent angle) are designed to obtain a strong HC effect. The structure, morphology and chemical composition of prepared Fe3+-doped TiO2 as catalyst are characterized via using XRD, SEM, TEM, XPS, UV-vis DRS and PL methods. The effects of added TiO2 (heat-treated at different temperatures for different times) and Fe3+-doped TiO2 (with different mole ratios of Fe and Ti) on the HC catalytic degradation of RhB are discussed. The influences of operation parameters including inlet pressure, initial RhB concentration and operating temperature on the HC catalytic degradation of RhB are studied by Box-Behnken design (BBD) and response surface methodology (RSM). Under 3.0 bar inlet pressure for 10 mg/L initial concentration of RhB solution at 40 °C operating temperature in the presence of Fe3+-doped TiO2 with 0.05:1.00 M ratio of Fe and Ti, the best HC degradation ratio can be obtained (91.11%). Furthermore, a possible mechanism of HC degradation of organic pollutants in the presence of Fe3+-doped TiO2 is proposed. Perhaps, this study may provide a feasible method for a large-scale treatment of dye wastewater.  相似文献   

5.
An atmospheric-pressure plasma jet (APPJ) was directly irradiated at a gas-liquid interface under ambient conditions. The reactive oxygen species (ROS) like hydroxyl radicals (OH), hydrogen peroxide (H2O2) and ozone (O3) and also reactive nitrogen species (RNS) such as nitrogen oxides (NOx) and nitric acid (HNO3) formed during the plasma discharge were quantified under various experimental parameters. In a chemical dosimetry method, terephthalic acid (TA) was employed for the quantification of OH and titanium sulfate was used to quantify the H2O2. Quantitative determination of NO3 was carried out by using Ion chromatography (IC). The changes in the solution pH were studied during the plasma treatment. Strong acidification along with the production of dominant reactive nitrogen species and ozone formation were observed with air. The effect of various gases, gas flow rate, various applied voltage and catalyst were studied to optimize the experimental conditions for the best performance. The influence of catalyst Fe2+ salt, TiO2 on the formation of reactive species were studied. The efficiency of the plasma device for the degradation of crystal violet (CV) was also investigated with TiO2 and Fe2+ salt.  相似文献   

6.
Zinc tungstate (ZnWO4) was previously used as a photocatalyst. In this paper, for the first time as an sonocatalyst, the performance of ZnWO4 for sonocatalytic degradation of meloxicam (MEL) under ultrasonic irradiation were studied. Firstly, ZnWO4 nanomaterials were synthesized at different acidity (pH = 5, 6, 7, 8, 9) via the hydrothermal method. Utilizing SEM, XRD and EDS techniques to characterize composition and morphology of each product, the same crystal forms, but different morphologies (nano-sheet, nano-microspheres or nano-rod) of ZnWO4 could be obtained. Secondly, the sonocatalytic activities of ZnWO4 on degradation of MEL were studied. It was found that the degradation ratio varied with the synthetic pH values, with ZnWO4 under synthetic pH = 6 exhibiting the best sonocatalytic performance (75.7%). While being synthesized at this pH value, ZnWO4 nano-microspheres had the largest BET surface area (27.068 m2/g), the smallest particle size (40–60 nm) so as to provide more active sites on its surface, which were able to produce more reactive oxygen species (ROS) and holes under ultrasonic irradiation. These ROS and holes had a positive effect on the degradation of MEL into CO2, H2O and inorganic. Thirdly, various influential factors including ultrasonic power intensity, ultrasonic time, catalyst addition dosage, initial concentration of MEL solution and reusability of catalyst were also explored. Under the condition of 10 mg/L MEL concentration, 20 mg catalyst dosage, 120 min irradiation time, 0.278 W/cm2 ultrasonic power intensity, the degradation ratio on MEL reached 75.7%. Finally, the presence of hydroxyl radical (OH) and singlet molecular oxygen (1O2) in the reaction was confirmed by adding ROS scavenger. The experimental results suggested that ZnWO4 nanoparticle could be used not only as an effective photocatalyst, but also, under the condition of ultrasonic irradiation, a promising sonocatalyst for degradation of organic pollutants in aqueous media.  相似文献   

7.
The synthesis, luminescence properties, experimental determination and theoretical calculation of the emission quantum yield of Eu(NTA)3.2L complexes, where NTA is naphtoiltri-fluroacetone and L denotes H2O or DMSO (dimethyl sulphoxide), were reported. The compounds were characterized by elemental analysis (carbon, hydrogen and europium), thermal analysis, UV-visible absorption and photoluminescence spectroscopies. The experimental quantum yields were determined based on a method previously proposed by Bril and collaborators. The Eu(NTA)3.2DMSO compound shows a high value for the Ω2 intensity parameter (35.8 × 10?20 cm2), reflecting the hypersensitive nature of the 5D07F2 transition and indicating that the lanthanide ion is in a highly polarizable chemical environment. The experimental quantum yield measured for that compound, 0.75, is one of the highest so far reported for solid-state europium complexes. The theoretical calculations of the quantum yield were carried out by solving an appropriate set of rate equations and by using empirical spectroscopic parameters and energy transfer rates. The theoretical results agree well with the experimental data for both complexes. The photostability of Eu(NTA)3.2DMSO at 358K was evaluated in order to verify whether this complex can be applied as a phosphor for blue light emitting devices.  相似文献   

8.
In this article, a catalytic-ion assisted hydrothermal method has recently been developed for synthesis of hierarchical manganese dioxide nanostructures. In this study, various shapes of hierarchical MnO2 (nanorod, nanothorn sphere, sphere) were successfully synthesized using the hydrothermal method with quantitative control of Al3+ in solution. The aspect ratio of aligned nanorods on the nanothorn sphere was easily controlled by the amount of Al3+ in the MnSO4 and (NH4)2S2O8 aqueous solution. Furthermore, we found that Al3+ species in the solution acted as a functional doping species into 2 × 2 tunnels of α-MnO2 and also as a catalyst. The formation mechanism of hierarchical MnO2 structures as a function of Al3+ concentration during hydrothermal reaction was sufficiently investigated, and the role of Al3+ as catalyst and doping species in the solution was discussed.  相似文献   

9.
The study is an extension of our previous work on sonolytic and sonocatalytic decomposition of Diclofenac-Na (DCF) to depict and highlight further operation parameters of significance, and to assess the effect of a novel home-made catalyst made of magnetic nanoparticles of zero-valent iron (ZVI). It was found that high-frequency was more effective than power ultrasound (20 kHz), and the efficiency was a maximum at 861 kHz, acetate-buffered pH 3.0 and air bubbling provided that samples were prepared from a pre-heated stock solution to enhance solubility of the compound. As such, 40-min sonication rendered nearly complete transformation of DCF to intermediate products that were more biodegradable than itself, but with little mineralization of organic carbon. Catalytic sono-treatment showed that the effect of the catalyst was largest in a non-buffered acidic solution and the rate of DCF elimination increased with increasing concentrations of solids up to a “critical” mass, above which it declined via the coalescence of particles and bubbles. Sonocatalysis using the “effective” solid mass also enhanced the overall degradation or mineralization of the compound as portrayed by the accumulation of chloride and nitrate ions in solution after prolonged contact. The production of excess H2O2 during catalysis with ZVI was attributed to the presence of additional and major routes of OH and/or H2O2 formation (other than water pyrolysis). The initial rate of DCF degradation in the presence of nanoparticles was found highly sensitive to the mass of solids in solution, declining sharply as the mass exceeded a “critical” effective level. A catalyst efficacy factor was defined as a function of the initial mass ratio of Fe0 to DCF and found to be one order of magnitude larger than that obtained by using commercial microparticles with a threefold larger Fe content. The result signifies that the role of aqueous Advanced Fenton reactions (Fe0/H2O2) was less significant in the presence of nanoparticles relative to that of heterogeneous reactions with reactive Fe and oxygen species on the massive surface areas with enriched reaction/adsorption and nucleation sites.  相似文献   

10.
4‐Stilbenecarboxaldehyde (4SCA) at pH 3 was added to TiO2 anatase to form a new catalyst where the aldehyde carbonyl group reacts with the TiO2‐OH to form the corresponding acetal (4SCA‐TiO2). 4SCA‐TiO2 significantly retards the electron recombination when it is illuminated with ultraviolet B light because of the formation of a stable radical anion·?4SCA‐TiO2 that we have detected spectroelectrochemically. The light excited electron on the catalysis is transferred relatively slow to solution. Therefore, the electron transfer to solution is the rate‐limiting step for water‐dissolved organic compound degradation when 4SCA‐TiO2 is used as photocatalyst. For instance, degradation rate constants using naphthalene (Naph) and p‐nitrophenol (PNP) in an ample pH range support the proposal. Accordingly, rate constants are faster when the standard redox potential of the involved electron acceptor in the solution increases. In fact, this condition can be tuned to promote reactivity. The affinity between the organics being degraded and 4SCA‐TiO2 also influences on the degradation rate constants.  相似文献   

11.
Ni species on the spent NiMo catalyst from ultra‐deep hydrodesulfurization of gas oil in a commercial plant were studied by Ni K‐edge EXAFS and TEM measurement without contact of the catalysts with air. The Ni–Mo coordination shell related to the Ni–Mo–S phase was observed in the spent catalyst by quasi in situ Ni K‐edge EXAFS measurement with a newly constructed high‐pressure chamber. The coordination number of this shell was almost identical to that obtained by in situ Ni K‐edge EXAFS measurement of the fresh catalyst sulfided at 1.1 MPa. On the other hand, large agglomerates of Ni3S2 were observed only in the spent catalyst by quasi in situ TEM/EDX measurement. MoS2‐like slabs were sintered slightly on the spent catalyst, where they were destacked to form monolayer slabs. These results suggest that the Ni–Mo–S phase is preserved on the spent catalyst and Ni3S2 agglomerates are formed by sintering of Ni3S2 species originally present on the fresh catalyst.  相似文献   

12.
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   

13.
The photocatalytic degradation of methylene blue is a straightforward and cost-effective solution for water decontamination. Although many materials have been reported so far for this purpose, the proposed solutions inflicted high fabrication costs and low efficiencies. Here, we report on the synthesis of tetragonal (1T) and hexagonal (2H) mixed molybdenum disulfide (MoS2) heterostructures for an improved photocatalytic degradation efficiency by means of a single-step chemical vapor deposition (CVD) technique. We demonstrate that the 1T-MoS2/2H-MoS2 heterostructures exhibited a narrow bandgap ∼ 1.7 eV, and a very low reflectance (<5%) under visible-light, owing to their particular vertical micro-flower-like structure. We exfoliated the CVD-synthesised 1T-MoS2/2H-MoS2 films to assess their photodegradation properties towards the standard methylene blue dye. Our results showed that the photo-degradation rate-constant of the 1T-MoS2/2H-MoS2 heterostructures is much greater under UV excitation (i.e., 12.5 × 10−3 min−1) than under visible light illumination (i.e., 9.2 × 10−3 min−1). Our findings suggested that the intermixing of the conductive 1T-MoS2 with the semi-conducting 2H-MoS2 phases favors the photogeneration of electron-hole pairs. More importantly, it promotes a higher efficient charge transfer, which accelerates the methylene blue photodegradation process.  相似文献   

14.
An ultrasound-assisted method was used for synthesizing nanosized Pt-graphene oxide (GO)-TiO2 photocatalyst. The Pt-GO-TiO2 nanoparticles were characterized by diffused reflectance spectroscopy, X-ray diffraction, N2 BET adsorption-desorption measurements, atomic force microscopy and transmission electron microscopy. The photocatalytic and sonophotocatalytic degradation of a commonly used anionic surfactant, dodecylbenzenesulfonate (DBS), in aqueous solution was carried out using Pt-GO-TiO2 nanoparticles in order to evaluate the photocatalytic efficiency. For comparison purpose, sonolytic degradation of DBS was carried out. The Pt-GO-TiO2 catalyst degraded DBS at a higher rate than P-25 (TiO2), prepared TiO2 or GO-TiO2 photocatalysts. The mineralization of DBS was enhanced by a factor of 3 using Pt-GO-TiO2 compared to the P-25 (TiO2). In the presence of GO, an enhanced rate of DBS oxidation was observed and, when doped with platinum, mineralization of DBS was further enhanced. The Pt-GO-TiO2 catalyst also showed a considerable amount of degradation of DBS under visible light irradiation. The initial solution pH had an effect on the rate of photocatalytic oxidation of DBS, whereas no such effect of initial pH was observed in the sonochemical or sonophotocatalytic oxidation of DBS. The intermediate products formed during the degradation of DBS were monitored using electrospray mass spectrometry. The ability of GO to serve as a solid support to anchor platinum particles on GO-TiO2 is useful in developing new photocatalysts.  相似文献   

15.
In light of growing environmental concerns over emerging contaminants in aquatic environments, antibiotics in particular, have prompted the development of a new generation of effective sonocatalytic systems. In this study, a new type of nano-laminated material, Ti2SnC MAX phase, is prepared, characterized, and evaluated for the sonocatalytic degradation of oxytetracycline (OTC) antibiotic. A variety of identification analyses, including X-ray diffraction, scanning electron microscopy, energy-dispersive X-ray spectrometry, Brunauer-Emmett-Teller, and diffuse reflectance spectroscopy, were conducted to determine the physicochemical properties of the synthesized catalyst. By optimizing the operating factors, total degradation of OTC occurs within 120 min with 1 g L-1 catalyst, 10 mg L-1 OTC, at natural pH of 7.1 and 150 W ultrasonic power. The scavenger studies conclude that the singlet oxygen and superoxide ions are the most active species during the sonocatalytic reaction. Based on the obtained data and GC–MS analysis, a possible sonocatalytic mechanism for the OTC degradation in the presence of Ti2SnC is proposed. The catalyst reusability within eight consecutive runs reveals the proper stability of Ti2SnC MAX phase. The results indicate the prospect for MAX phase-based materials to be developed as efficient sonocatalysts in the treatment of antibiotics, suggesting a bright future for the field.  相似文献   

16.
以天然木棉为模板,利用造孔及纳米颗粒自组装两步法合成了分级多孔的Cafe2O4/C复合催化剂. Cafe2O4/C复合催化剂保留了木棉模板的中空纤维形貌,且该中空纤维是由碳及均匀分布在碳表面的Cafe2O4纳米颗粒组成. 该复合催化剂具有较强的甲基紫微波催化降解活性. 研究了Cafe2O4负载量、微波功率、催化剂用量、甲基紫的初始浓度和pH值对微波诱导甲基紫降解的影响. 结果表明,Cafe2O4/C微波降解甲基紫的催化反应具有较高的反应速率和较短的反应时间. 其降解反应符合一级动力学模型. Cafe2O4/C 高的催化活性得益于催化反应和吸附特性之间的协同作用.  相似文献   

17.
Removal of p-xylene and effects of various parameters on the removal efficiency in aqueous solution with plasma are studied. Results indicate that the degradation rate can be effectively raised by decreasing the diameter of discharge electrode and electric conductivity of the aqueous solution, or by increasing the pH of the solution. The addition of H2O2, and especially FeSO4 is found to significantly enhance p-xylene degradation, but the presence of Na2CO3, Ce(SO4)2 and n-butanol inhibited the degradation of p-xylene. Some major intermediate products were detected by HPLC.  相似文献   

18.
Hierarchical structured ZnFe2O4@reduced graphite oxide@TiO2 (ZnFe2O4@RGO@TiO2) nanocomposite was prepared by an electrostatic layer-by-layer route, which played a synthetic effect of Fenton oxidation of ZnFe2O4 and photocatalytic oxidation of TiO2 to degrade fulvic acid (FA) solution under visible-light irradiation. In this method, RGO, as the middle layer, can effectively promote the photo-induced electron flow between the ZnFe2O4 and TiO2 and further improve the efficiency of the photo-Fenton oxidation. The influencing factors on photo-Fenton oxidation, including solution pH, catalyst, and H2O2 dosage, have also been investigated. The results illustrated that the ternary composite presented the enhanced catalytic performance. Under visible light irradiation, the degradation efficiency of the sample on the FA solution can reach 95.4% within 3 h. In addition, the catalyst exhibited superior stability and reusability, and its degradation efficiency was still up to 90% after 5 cycles. Therefore, the composite will be a kind of efficient photocatalyst and had a promising application for visible-light driven destruction of organic pollutants.  相似文献   

19.
This study proposes a novel and simple in-house design of a nanoparticle tracking analysis (NTA) device for the online characterization of nanoparticles in an aqueous solution. The particle size distribution of two sets of model nanoparticles, for example, transparent (SiO2) and opaque (TiO2) materials with respect to water as a dispersion medium could be successfully analyzed. Experiments are conducted using two different laser wavelengths of 632.8 (red) and 510 nm (green) and a range of concentrations. The accuracy of the green laser is larger compared to the red laser for all particle concentrations used. The measured average diameter using the presented in-house NTA setup is in the acceptable range compared to the electron microscopy data. The average diameter of the transparent (SiO2) and opaque (TiO2) samples is calculated as 36.29 and 27.26 nm using NTA, 36.44 and 27.8 nm analyzing field emission scanning electron microscopy images, and 23.97 and 19.7 nm analyzing transmission electron microscopy images. In the new viewing sample holder, nanoparticles undergo mere Brownian motion with no bulk drift velocity. The effect of solid concentration and wavelength of the laser light on the performance of the NTA sensor is investigated, and the optimal concentration range for model particles is reported.  相似文献   

20.
The sonocatalytic performance of CeO2 nanoparticles synthesized by a hydrothermal method (CeO2-H) and CeO2@biochar (CeO2-H@BC) nanocomposite, were evaluated for the degradation of Reactive Red 84 (RR84) under ultrasonic irradiation. For comparison purposes the corresponding performance of bare biochar (BC) and commercial CeO2 (CeO2-C) samples were also assessed. A complementary characterization study, involving scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), Transmission electron microscopy (TEM), dynamic light scattering (DLS), X-ray diffraction (XRD), N2 adsorption at −196 °C (Brunauer–Emmett–Teller (BET) method) and Fourier transform infrared spectroscopy (FT-IR) was undertaken to gain insight into the structure-performance relationships. The effect of various parameters such as initial RR84 concentration, solution pH, catalyst amount and ultrasonic power on the sonodegradation of RR84 was studied in detail. The results indicated that the CeO2-H@BC nanocomposite exhibited the best RR84 degradation efficiency, which is enhanced with the increase of CeO2-H@BC amount and ultrasonic power but diminished with the increment in RR84 concentration and pH value. A 98.5% degradation was obtained with a CeO2-H@BC amount of 1 g/L, ultrasonic power of 450 W, pH of 6.5 and initial RR84 concentration of 10 mg/L. The quenching effects of various scavengers proposed that OH radical plays the key role in the process. Analyses of intermediates by Gas chromatography-Mass spectroscopy (GC–MS) identified several by-products and accordingly the main pathway was proposed.  相似文献   

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