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1.
The catalytic performance of nanostructured Ni-Co/Al2O3-ZrO2 catalysts, prepared by ultrasound-assisted impregnation method was examined in the dry reforming of methane. The effect of irradiation power and irradiation time have been studied by changing time (0, 20, 80 min) and power of the sonication (30, 60, 90 W) during the synthesis which resulted in different physiochemical properties of the nanocatalyst. The nanocatalysts were characterized by XRD, FESEM, PSD, EDX, TEM, TPR-H2, BET, FTIR and TG analyses. Based on the characterization results, ultrasound treatment endowed the sample with more uniform and smaller nanoparticles; higher surface area, stronger metal-support interaction and more homogenous dispersion. Moreover, the analyses exhibited smaller particles with higher surface area and less population of particle aggregates at longer and highly irradiated nanocatalysts. The nanocatalyst irradiated at 90 W for 80 min (the longest irradiation time and the most intense power) showed a uniform morphology and a very narrow particles size distribution. More than 65% of particles of this nanocatalyst were in the range of 10–30 nm. Activity tests demonstrated that employing ultrasound irradiation during impregnation improves feed conversion and products yield, reaching values close to equilibrium. Among sonicated nanocatalysts, with increasing power and time of irradiation, the nanocatalyst represents higher activity. The superior performance amongst the various bimetallic catalysts tested was observed over the catalyst with 90 W and 80 min ultrasonic irradiation which is stable in 24 h time on stream test. The excellent anti-coking performance of this bimetallic catalyst, confirmed by TG and FESEM analyses of spent catalyst, is closely related to the promoting effect of sonication on the metal-support interaction, Ni dispersion and particle size; and probably, the synergy between metallic species.  相似文献   

2.
Fe3O4 magnetic nanoparticles (Fe3O4 MNPs) with much improved peroxidase-like activity were successfully prepared through an advanced reverse co-precipitation method under the assistance of ultrasound irradiation. The characterizations with XRD, BET and SEM indicated that the ultrasound irradiation in the preparation induced the production of Fe3O4 MNPs possessing smaller particle sizes (16.5 nm), greater BET surface area (82.5 m2 g?1) and much higher dispersibility in water. The particle sizes, BET surface area, chemical composition and then catalytic property of the Fe3O4 MNPs could be tailored by adjusting the initial concentration of ammonia water and the molar ratio of Fe2+/Fe3+ during the preparation process. The H2O2-activating ability of Fe3O4 MNPs was evaluated by using Rhodamine B (RhB) as a model compound of organic pollutants to be degraded. At pH 5.4 and temperature 40 °C, the sonochemically synthesized Fe3O4 MNPs were observed to be able to activate H2O2 and remove ca. 90% of RhB (0.02 mmol L?1) in 60 min with a apparent rate constant of 0.034 min?1 for the RhB degradation, being 12.6 folds of that (0.0027 min?1) over the Fe3O4 MNPs prepared via a conventional reverse co-precipitation method. The mechanisms of the peroxidase-like catalysis with Fe3O4 MNPs were discussed to develop more efficient novel catalysts.  相似文献   

3.
A recyclable heterogeneous catalyst has been successfully developed for application in a Fenton-type advanced oxidation process without adding external H2O2. LaFeO3 was prepared from Fe(NO3)3·9H2O and La(NO3)·6H2O by a simple sol-gel method and its catalytic efficiency was evaluated for mineralization of 4-chlorophenol using a Fenton-like process. The mineralization process was carried out under ultrasonication in presence of heterogeneous LaFeO3 catalyst with H2O2 that was produced during ultrasonication. The mineralization process was monitored through total organic carbon (TOC) analysis. Very importantly, utmost 5-fold synergism was evidenced by the ultrasound mediated LaFeO3-catalyzed system. Besides, more than twofold synergism was observed by combining the ultrasound assisted LaFeO3 catalytic process and potassium persulfate (KPS) assisted advanced oxidation process. It is worth to mention that complete mineralization (∼96%) of 4-chlorophenol (initial concentration of 1.25 × 10−4 M) was observed within 1 h in the presence of LaFeO3 (0.5 g L−1) and KPS (1.0 mmol) under ultrasonication (40 kHz). Even after four cycles, the activity of LaFeO3 remained intact which proved its recyclability. Extremely reusable heterogeneous LaFeO3 catalyst makes the system more interesting from both economic and environmental points of view.  相似文献   

4.
Nanostructured CuO–ZnO–Al2O3/HZSM-5 was synthesized from nitrate and acetate precursors using ultrasound assisted co-precipitation method under different irradiation powers. The CuO–ZnO–Al2O3/HZSM-5 nanocatalysts were characterized using XRD, FESEM, BET, FTIR and EDX Dot-mapping analyses. The results indicated precursor type and irradiation power have significant influences on phase structure, morphology, surface area and functional groups. It was observed that the acetate formulated CuO–ZnO–Al2O3/HZSM-5 nanocatalyst have smaller CuO crystals with better dispersion and stronger interaction between components in comparison to nitrate based nanocatalysts. Ultrasound assisted co-precipitation synthesis method resulted in nanocatalyst with more uniform morphology compared to conventional method and increasing irradiation power yields smaller particles with better dispersion and higher surface area. Additionally the crystallinity of CuO is lower at high irradiation powers leading to stronger interaction between metal oxides. The nanocatalysts performance were tested at 200–300 °C, 10–40 bar and space velocity of 18,000–36,000 cm3/g h with the inlet gas composition of H2/CO = 2/1 in a stainless steel autoclave reactor. The acetate based nanocatalysts irradiated with higher levels of power exhibited better reactivity in terms of CO conversion and DME yield. While there is an optimal temperature for CO conversion and DME yield in direct synthesis of DME, CO conversion and DME yield both increase with the pressure increase. Furthermore ultrasound assisted co-precipitation method yields more stable CuO–ZnO–Al2O3/HZSM-5 nanocatalyst while conventional precipitated nanocatalyst lost their activity ca. 18% and 58% in terms of CO conversion and DME yield respectively in 24 h time on stream test.  相似文献   

5.
In this study, the synthesis of Ce0.8Sm0.2O1.9 (SDC) solid electrolyte by the ultrasound assisted co-precipitation method was accomplished to explore the effects of ultrasound power, ultrasound pulse ratio and probe type upon the ionic conductivity of SDC as well as the lattice parameter, the microstructure and the density. Fine powders of uniform crystallite sizes (average 11.70 ± 0.62 nm) were obtained, needing lower sintering temperature. The SDC powders were successfully sintered to a relative density of over 95% at 1200 °C (5 °C min?1) for 6 h. The micrograph of SDC pellets showed non-agglomerated and well-developed grains with average size of about 200 nm. X-ray diffraction analysis showed that the lattice parameter increased with increasing acoustic intensity and reached a maximum for the 14.94 W cm?2. Further, a linear relationship was detected between the lattice parameter and the ionic conductivity, inspiring a dopant like effect of US on the electrolyte properties. The highest ionic conductivity as σ800°C = 3.07 × 10?2 S cm?1 with an activation energy Ea = 0.871 kJ mol?1 was obtained with pulsed ultrasound for an acoustic intensity of 14.94 W cm?2, using 19 mm probe and 8:2 pulse ratio.  相似文献   

6.
The present work establishes in depth study of ultrasound assisted preparation of performic acid (PFA) in a continuous flow microstructured reactor. The influence of various parameters viz. formic acid: hydrogen peroxide molar ratio, flow rate, temperature and catalyst loading on the PFA formation were studied in a continuous flow microstructured reactor. In a continuous microstructured reactor in the presence of ultrasonic irradiation, the formation of PFA was found to be dependent on the molar ratio of formic acid: hydrogen peroxide, flow rate of reactants, temperature and catalyst loading (Amberlite IR-120H). The optimized parameter values are 1:1 M ratio, 50 mL/h, 40 °C and 471 mg/cm3 respectively. Further, the performance of Amberlite IR-120H catalyst was evaluated for three successive cycles in continuous microstructured reactor. The performance of catalyst was found to be decreased with the usage of the catalyst and is attributed to neutralization of the sulfonic acid groups, catalyst shrinkage, or loss in pore sites. The experimental results revealed that, for an ultrasound assisted synthesis of PFA in continuous microstructured reactor the observed reaction time was even less than 10 min. The observed intensification in the PFA synthesis process can be attributed to the intense collapse of the cavities formed at low temperature during ultrasonic irradiations, which further improved the heat and mass transfer rates with the formation of H2O2 during the reaction. The combined use of ultrasound and a continuous flow microstructured reactor has proved beneficial process of performic acid synthesis.  相似文献   

7.
《Current Applied Physics》2010,10(3):947-951
Carbon aerogel was prepared by polycondensation of resorcinol and formaldehyde using sodium carbonate as a catalyst with a resorcinol to catalyst ratio of 500. Co-doped carbon aerogels were then prepared by an impregnation method with a variation of cobalt content (1, 3, 5, 7, 10, and 15 wt.%), and their performance for supercapacitor electrode was investigated by measurement of specific capacitance in 1 M H2SO4 electrolyte at a scan rate of 10 mV/s. Among the samples prepared, 7 wt.% Co-doped carbon aerogel showed the highest capacitance (100 F/g) and stable cyclability. The enhanced capacitance of Co-doped carbon aerogel was attributed to the faradaic redox reactions of cobalt oxide. On the basis of this result, 7 wt.% Cu-, Fe-, Mn-, and Zn-doped carbon aerogels were also prepared by an impregnation method for use as a supercapacitor electrode. Among the metal-doped carbon aerogels, Mn-doped carbon aerogel showed the highest capacitance (107 F/g) while Cu- and Fe-doped carbon aerogels exhibited the most stable cyclability.  相似文献   

8.
In the present research work deals with the preparation of 1-butoxy-4-nitrobenzene was successfully carried out by 4-nitrophenol with n-butyl bromide using aqueous potassium carbonate and catalyzed by a new multi-site phase-transfer catalyst (MPTC) viz., N1,N4-diethyl-N1,N1,N4,N4-tetraisopropylbutane-1,4-diammonium dibromide, under ultrasonic (40 kHz, 300 W) assisted organic solvent condition. The pseudo first-order kinetic equation was applied to describe the overall reaction. Under ultrasound irradiation (40 kHz, 300 W) in a batch reactor, it shows that the overall reaction greatly enhanced with ultrasound irradiation than without ultrasound. The present study provides a method to synthesize nitro aromatic ethers by ultrasound assisted liquid–liquid multi-site phase-transfer catalysis condition.  相似文献   

9.
《Current Applied Physics》2010,10(2):521-525
Nanocrystalline hydroxyapatite (HAp) powders were synthesized by a simple method using aloe vera plant extracted solution. To obtain nanocrystalline HAp, the prepared precursor was calcined in air at 400–800 °C for 2 h. The phase composition of the calcined samples was studied by X-ray diffraction (XRD) technique. The XRD results confirmed the formation of HAp phase. With increasing calcination temperature, the crystallite of the HAp increased, showing the hexagonal structure of HAp with the lattice parameter, a, in a range of 0.9520–0.9536 nm and c of 0.6739–0.6928 nm. The particle sizes of the powder were obtained to be 43–171 nm. The optical properties of the calcined powders were characterized by Raman and FTIR spectroscopies. The Raman spectra showed a main peak of the phosphate vibration mode (ν1(PO4)) at ∼963 cm−1 for all the calcined samples. The peaks of the phosphate carbonate and hydroxyl vibration modes were observed in the FTIR spectra for all the calcined powders. The morphology tends to change from a spherical shape to a rod-like shape with increasing calcination temperature as revealed by TEM.  相似文献   

10.
Sono-dispersion of Ni, Co and Ni–Co over Al2O3–MgO with Al/Mg ratio of 1.5 was prepared and tested for dry reforming of methane. The samples were characterized by XRD, FESEM, PSD, EDX, TEM, BET and FTIR analyses. In order to assess the effect of ultrasound irradiation, Ni–Co/Al2O3–MgO with Co content of 8% prepared via sonochemistry and impregnation methods. The sono-synthesized sample showed better textural properties and higher activity than that of impregnated one. Comparison of XRD patterns indicated that the NiO peaks became broader by increasing Co content over the support. The FESEM images displayed the particles are small and well-dispersed as a result of sonochemistry method. Also, EDX analysis demonstrated better dispersion of Ni and Co as a result of sonochemistry method in confirmation of XRD analysis. The sono-synthesized Ni–Co/Al2O3–MgO as a superior nanocatalyst with Co content of 3% illustrates much higher conversions (97.5% and 99% for CH4 and CO2 at 850 °C), yields (94% and 96% for H2 and CO at 850 °C) and 0.97 of H2/CO molar ratio in all samples using an equimolar feed ratio at 850 °C. During the 1200 min stability test, H2/CO molar ratio remained constant for the superior nanocatalyst.  相似文献   

11.
In this study, ultrasound assisted dispersive solid-phase micro extraction combined with spectrophotometry (USA-DSPME-UV) method based on activated carbon modified with Fe2O3 nanoparticles (Fe2O3-NPs-AC) was developed for pre-concentration and determination of safranin O (SO). It is known that the efficiency of USA-DSPME-UV method may be affected by pH, amount of adsorbent, ultrasound time and eluent volume and the extent and magnitude of their contribution on response (in term of main and interaction part) was studied by using central composite design (CCD) and artificial neural network-genetic algorithms (ANN-GA). Accordingly by adjustment of experimental conditions suggested by ANN-GA at pH 6.5, 1.1 mg of adsorbent, 10 min ultrasound and 150 μL of eluent volume led to achievement of best operation performance like low LOD (6.3 ng mL−1) and LOQ (17.5 ng mL−1) in the range of 25–3500 ng mL−1. In following stage, the SO content in real water and wastewater samples with recoveries between 93.27–99.41% with RSD lower than 3% was successfully determined.  相似文献   

12.
《Ultrasonics sonochemistry》2014,21(6):1964-1968
Through an ultrasound assisted method, TiO2/WO3 nanoparticles were synthesized at room temperature. The XRD pattern of as-prepared TiO2/WO3 nanoparticles matches well with that of pure monoclinic WO3 and rutile TiO2 nanoparticles. TEM images show that the prepared TiO2/WO3 nanoparticles consist of mixed square and hexagonal shape particles about 8–12 nm in diameter. The photocatalytic activity of TiO2/WO3 nanoparticles was tested for the degradation of a wastewater containing methylene blue (MB) under visible light illumination. The TiO2/WO3 nanoparticles exhibits a higher degradation rate constant (6.72 × 10−4 s−1) than bare TiO2 nanoparticles (1.72 × 10−4 s−1) under similar experimental conditions.  相似文献   

13.
Photocatalytic degradation of methylene blue (MB) in water was examined using Er3+-doped TiO2 (Er–TiO2) nanorods prepared by a sol–gel derived electrospinning, calcination, and subsequent mechanical grinding. Different concentrations of Er dopant in the range of 0–1.0 mol% were synthesized to evaluate the effect of Er content on the photocatalytic activity of TiO2. Among Er3+–TiO2 catalysts, the 0.7 mol% Er3+–TiO2 catalyst showed the highest MB degradation rate. The degradation kinetic constant (k) increased from 1.0 × 10?3 min?1 to 5.1 × 10?3 min?1 with the increase of Er3+ doping from 0 to 0.7 mol%, but decreased down to 2.1 × 10?3 min?1 when Er3+ content was 1.0 mol%. It can be concluded that the degradation of MB under UV radiation was more efficient with Er3+–TiO2 catalyst than with pure TiO2. The higher activity might be attributed to the transition of 4f electrons of Er3+ and red shifts of the optical absorption edge of TiO2 by erbium ion doping.  相似文献   

14.
InNbO4 was prepared by the solid-state reaction method. Various cocatalysts were added on InNbO4 by the incipient-wetness impregnation method. The effects of co-catalyst and pretreatment conditions on the photocatalytic activity of InNbO4 for photoreduction of carbon dioxide were investigated. NiO–InNbO4 and Co3O4–InNbO4 were pretreated by reduction at 500 °C for 2 h and subsequent oxidation at 200 °C for 1 h. The catalysts were characterized by X-ray diffraction, scanning electron microscopy, X-ray photoelectron spectroscopy, and UV–vis diffuse reflectance spectroscopy. The characterization results of NiO–InNbO4 catalysts after pretreatment showed the presence of highly crystalline NiO and monoclinic Nb2O5. NiO–InNbO4 with reduction–oxidation pretreatment exhibited the highest activity due to the presence of core–shell type Ni0 and NiO on the surface and the presence of a small amount of Nb2O5 as a promoter.  相似文献   

15.
The thermodynamics and kinetics of traditional and simultaneous dual frequency energy-gathered ultrasound (SDFU) assisted enzymolysis of potato protein were investigated to get the knowledge of the mechanisms on the SDFU’s promoting efficiency during enzymolysis. The concentration of potato protein hydrolysate and parameters of thermodynamic and kinetic during traditional and SDFU assisted enzymolysis were determined. The results showed that potato protein hydrolysate concentration of SDFU assisted enzymolysis was higher than traditional enzymolysis at the hydrolysis time of 60 min (p < 0.05) whereas not significantly different at 120 min (p > 0.05). In some cases, SDFU assisted enzymolysis took less hydrolysis time than traditional enzymolysis when the similar conversion rates of potato protein were obtained. The thermodynamic papameters including the energy of activation (Ea), enthalpy of activation (△H), entropy of activation (△S) were reduced by ultrasound pretreatment while Gibbs free energy of activation (△G) increased little (1.6%). Also, kinetic papameters including Michaelis constant (KM) and catalytic rate constant (kcat) decreased by ultrasound pretreatment. On the contrary, reaction rate constants (k) of SDFU assisted enzymolysis were higher than that of traditional enzymolysis (p < 0.05). It was indicated that the efficiency of SDFU assisted enzymolysis was higher than traditional enzymolysis in a limited time. The higher efficiency of SDFU assisted enzymolysis was related with the decrease of Ea and KM by lowering the energy barrier between ground and active state and increasing affinity between substrate and enzyme.  相似文献   

16.
In the present research, the degradation of an emerging pharmaceutical micro-pollutant, Ibuprofen (IBP) by using Pd@Fe3O4 and a hybrid sono-electrolytical (US/EC) treatment system has been demonstrated for the first time. The magnetically separable nanocomposite, Pd@Fe3O4 catalyst was synthesized following co-precipitation method to enhance the efficiency of US/EC system. The synthesized catalyst showed a strong reusable property even after applying for five times and in all the five cases, 100% degradation of IBP was maintained. It not only enhanced the IBP degradation rate, but also reduced the energy consumption of the system by ∼35%. Its strong magnetization value of 64.27 emu g−1 made it easily separable. Hence, a comprehensive knowledge on the application of combined energy based US/EC system and magnetically separable multifunctional catalysts for degradation of intractable pollutants like Ibuprofen was achieved, assuring that US/EC can be an effective option for IBP treatment.  相似文献   

17.
《Current Applied Physics》2010,10(1):333-336
Observation of room temperature ferromagnetism in Fe doped In2O3 samples (In1−xFex)2O3 (0  x  0.07) prepared by co-precipitation technique is reported. Lattice parameter obtained from powder X software shows distinct shrinkage of the lattice constant indicating an actual incorporation of Fe ions into the In2O3 lattice. X-ray diffraction data measurements show that the entire sample exhibits single phase polycrystalline behavior. SEM micrographs showed the prepared powder was in the range 25–36 nm. SEM EDS mapping showed the presence of Fe and In ions in the Fe doped In2O3 sample. The highest remanence magnetization moment (6.624 × 10−4 emu/g) is reached in the sample with x = 0.03.  相似文献   

18.
In this study, the effects of ultrasound with different ultrasonic frequencies on the properties of sodium alginate (ALG) were investigated, which were characterized by the means of the multi-angle laser light scattering photometer analysis (GPC-MALLS), rheological analysis, circular dichroism (CD) spectrometer and scanning electron microscope (SEM). It showed that the molecular weight (Mw) and molecular number (Mn) of the untreated ALG was 1.927 × 105 g/mol and 4.852 × 104 g/mol, respectively. The Mw of the ultrasound treated ALG was gradually increased from 3.50 × 104 g/mol to 7.34 × 104 g/mol while the Mn of ALG was increased and then decreased with the increase of the ultrasonic frequency. The maximum value of Mn was 9.988 × 104 g/mol when the ALG was treated by ultrasound at 40 kHz. It indicated that ultrasound could induce ALG degradation and rearrangement. The number of the large molecules and small molecules of ALG was changed by ultrasound. The value of dn/dc suggested that the ultrasound could enhance the stability of ALG. Furthermore, it was found that ALG treated by ultrasound at 50 kHz tended to be closer to a Newtonian behavior, while the untreated and treated ALG solutions exhibited pseudoplastic behaviours. Moreover, CD spectra demonstrated that ultrasound could be used to improve the strength of the gel by changing the ratio of M/G, which showed that the minimum ratio of M/G of ALG treated at 135 kHz was 1.34. The gel-forming capacity of ALG was correlated with the content of G-blocks. It suggested that ALG treated by ultrasound at 135 kHz was stiffer in the process of forming gels. The morphology results indicated that ultrasound treatment of ALG at 135 kHz increased its hydrophobic interaction and interfacial activity. This study is important to explore the effect of ultrasound on ALG in improving the physical properties of ALG as food additives, enzyme and drug carriers.  相似文献   

19.
In the present work, kinetics of synthesis of 1,3-bis(allyloxy)benzene was successfully carried out by O-allylation of resorcinol with allyl bromide using aqueous potassium hydroxide and catalyzed by a new multi-site phase-transfer catalyst viz., 1,3,5,7-tetrabenzylhexamethylenetetraammonium tetrachloride, MPTC under ultrasonic (40 kHz, 300 W) assisted organic solvent condition. The pseudo first-order kinetic equation was applied to describe the overall reaction. Under ultrasound irradiation (40 kHz, 300 W) in a batch reactor, it shows that the overall reaction rate can be greatly enhanced to seven fold faster with ultrasound irradiation than without ultrasound. The present study provides a method to synthesize ethers by ultrasound assisted liquid–liquid phase-transfer catalysis condition.  相似文献   

20.
《Ultrasonics sonochemistry》2014,21(5):1805-1814
The ultrasound assisted preparation of 1-(benzyloxy)-4-nitrobenzene from the reaction of 4-chloronitrobenzene (CNB) and benzyl alcohol was carried out successfully using potassium hydroxide and catalyzed by a new multi-site phase-transfer catalyst (MPTC) viz., 1,3,5-triethyl-1,3,5-trihexyl-1,3,5-triazinane-1,3,5-triium trichloride in a solid–liquid reaction condition (SL-MPTC). The advantage of using SL-MPTC is to avoid a serious hydration of potassium salt of benzyl alcohol in the reaction between 4-chloronitrobenzene (CNB) and benzyl alcohol. The reaction is greatly enhanced in the solid–liquid system, catalyzed by multi-site quaternary ammonium salt (MPTC) and ultrasound irradiation (40 kHz, 300 W) in a batch reactor, it shows that the overall reaction greatly enhanced with ultrasound irradiation than without ultrasound. The reaction mechanism is proposed and verified by examining the experimental evidence. A kinetic model is proposed in which a pseudo first-order rate law is sufficient to describe the results, such as the effects of agitation speed, ultrasound, different phase transfer catalysts and the effect of organic solvents, the amount of newly prepared MPTC, the effect of temperature, the amount of water, the concentration of 4-chloronitrobenzene (CNB) and potassium hydroxide concentrations. The apparent rate constant (kapp) were investigated in detail. Rational explanations to account for the phenomena on the results were made.  相似文献   

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