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1.
A series of cobalt–magnesium oxide solid solution catalysts (CoMgO) have been prepared using urea combustion methods, and characterised by X-ray diffraction (XRD) and laser Raman (LR). The catalytic activities for methane combustion have been tested in a continuous-flow microreactor. The Co content has a significant effect on the activity of the cobalt–magnesium oxide solid solution catalysts. The catalysts containing 5 and 10% Co have the lowest light-off temperature in methane combustion. In the preparation of cobalt–magnesium oxide solid solution catalysts, higher urea to metal ratio favors the formation of the catalysts with smaller crystal particles and leads to a better catalytic performance for methane combustion. Addition of lanthanum nitrate to the solution of Co and Mg nitrate depressed the formation of the cobalt–magnesium oxide solid solution and decreased the activity of the catalysts for methane combustion. The cobalt–magnesium oxide solid solution catalysts are very stable when the calcination or reaction temperature is no more than 900°C. However, the catalytic activity decreases rapidly after high temperature (>1000°C) calcination, possibly due to sintering of the catalyst and thus decrease of the surface area.  相似文献   

2.
Poly[bis(-phenoxyethoxy)phosphazene] [PBPEP] had been shown in our previous paper to be a very useful polymer for investigating the crystallization mechanism of polymers, as the crystallization rate of PBPEP is extraordinarily small when isothermally crystallized from the melt. The crystallization of the low molecular weight oligomers of PBPEP was first studied in comparison to the high molecular weight polymers. The oligomer-rich fraction was obtained by fractionation of the as-polymerized sample, which had a broad molecular weight distribution. The fractions thus obtained were characterized by solution viscometry and size exclusion chromatography. The melting temperature and the growth rate of the spherulite from the melt were investigated by differential scanning calorimetry and optical microscopy. The growth rate was one or two orders of magnitude smaller in the oligomer-rich fraction than in the other high molecular weight fractions. A collapsed spherulite appeared in the oligomer-rich fraction at high crystallization temperatures. It is speculated that in the oligomer-rich fraction there is an excess free energy due to defects in the crystal phase. This defect is considerably larger in the oligomer-rich fraction than in the other fractions because a large quantity of short length chains is present.  相似文献   

3.
The kinetics of catalytic hydrogenation of ortho-nitrochlorobenzene to 2,2'-dichloroazoxybenzene on platinum/carbon catalyst is investigated in a slurry reactor with the temperature range of 313-343 K, and ortho-chloroaniline is formed as a byproduct. Models based on Rideal-Eley and Langmuir-Hinshelwood mechanism have been proposed based on the rate data and the kinetic regime. The former model can be used to fit the experimental data better. Reaction controlling steps are physical adsorption of hydrogen and adsorbed ortho-nitrochlorobenzene reacted on the surface of catalyst.  相似文献   

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An alumina-supported silver composite system has been investigated in the reaction of heterogeneous catalytic ozone decomposition. Perlite loaded with silver and silver modified zeolites have also been tested as catalysts for gas phase conversion of ozone to molecular oxygen. The catalysts have been activated by calcination and the changes occurring on the catalytic surface as a result of the reaction have been characterized in details using XPS. The SEM analysis has revealеd the role of surface morphology in the process of ozone decomposition on the surface of Ag/α-Al2O3 catalyst. A catalytic cycle is proposed that supports the hypothesis about the important role of the peroxide species as intermediates participating in the process and catalyzing the complete ozone conversion into molecular oxygen. It has been found out that the maximum conversion degree, achieved with the alumina-supported silver system, is up to 90%.  相似文献   

6.
1 INTRODUCTION Poly-N-vinyl-pyrrolidone (PVP) is a non-ionic water-soluble chemical, which is widely used in many industrial fields such as pharmaceutical, cosmetic, foodstuff, electronics, printing, paper-making, deter- gent and adhesive etc.[1]. Traditional acetylene process is dangerous because of using acetylene under high temperature and pressure[2] Nowadays, it is usually produced by polymerization of N-vinyl-pyrrolidone (NVP), which is produced by cata- lytic dehydration of N-(h…  相似文献   

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Dianhua Liu  Chunfeng Yao  Dingye Fang 《Fuel》2011,90(5):1738-1742
A γ-Al2O3 catalyst was modified with metal oxide (Nb2O5) in order to improve its activity and stability for dimethyl ether (DME) synthesis from methanol. A series of modified γ-Al2O3 catalysts were prepared with Nb2O5 and characterized by X-ray diffraction and temperature programmed desorption of ammonia. Results showed that the γ-Al2O3 catalyst containing 10 wt.% of Nb2O5 exhibited the highest surface area among the modified ones. The number of acid sites of the modified catalysts was increased by the Nb2O5 modification. In the chemical reaction of DME synthesis, it was found that the Nb2O5 modified γ-Al2O3 catalyst exhibited a higher activity in the low temperature region (240 °C-260 °C) and a higher activity than did the untreated γ-Al2O3 catalyst.  相似文献   

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Mn–Ce–Mg/Al2O3 catalyst prepared by a wet impregnation method was investigated in the catalytic combustion of chlorobenzene. The addition of Mg decreased the interaction of Mn and Ce species with Al2O3 and promotes the dispersion of Mn and Ce species and the formation of Ce–Mn–O solid solution. High activity, good selectivity and desired stability of Mn–Ce–Mg/Al2O3 catalyst were observed.  相似文献   

12.
A kinetic model of the acetylene hydrochlorination over the bimetallic Au–Cu/C catalyst was obtained on the basis of kinetic data. DFT theoretical calculation and the kinetic model indicated the reaction probably proceeds via the Eley-Rideal mechanism in which gas phase HCl reacts with the adsorbed C2H2 to produce vinyl chloride. Reaction conditions were optimized according to kinetics analyses. Under the optimized reaction conditions obtained, the bimetallic Au–Cu/C showed excellent performances with more than 99.5% conversion and selectivity and did not deactivate in 200 h on stream.  相似文献   

13.
The steady-state kinetics of acetylene oxidation has been studied in the framework of automotive exhaust gas catalysis over a commercially available three-way catalyst. Experiments under cold-start conditions have been carried out in a laboratory fixed-bed reactor, which can adequately be described by the developed elementary step model and rate parameters.  相似文献   

14.
《Journal of Catalysis》2002,205(2):289-293
The reaction behavior and carbon deposition during the CO2/CH4 reforming reaction have been investigated over the γ-Al2O3-supported Co catalysts as a function of Co loading (between 2 and 20 wt%) and calcination temperature (Tc=500 or 1000°C). It was found that the stability of Co/γ-Al2O3 catalysts was strongly dependent on the Co loading and calcination temperature. For some loadings (6 wt% for Tc=500°C and 9 wt% for Tc=1000°C), stable activities have been achieved. However, over the catalysts with high Co loadings (>12 wt%), notable amounts of carbon were accumulated during reforming, and deactivation was observed. Moreover, severe deactivation was also noted over the 2 wt% catalysts, both when carbon deposition occurred (Tc=500°C) or was absent (Tc=1000°C). In the latter case, the oxidation of the metallic sites was responsible for the deactivation. Hence, there are two different deactivation mechanisms, namely, carbon deposition and oxidation of metallic sites. The activities were stable when a balance between carbon formation and its oxidation could be achieved.  相似文献   

15.
Spherical clusters of Ni(OH)2 nanosheets are directly grown on skeletons of nickel foam via a facile template-free spontaneous growth method. The obtained electrode (β-Ni(OH)2/Ni-foam) is characterized by X-ray diffractometry, scanning and transmission electron microscopy and thermal analysis. Results show that Ni(OH)2 has a β-phase structure and presents on the nickel foam skeleton mostly as spherical clusters with a diameter of ∼10 μm. The spheres are composed of nanosheets with thickness of ∼60 nm, width of ∼230 nm and length up to ∼2 μm, and the nanosheets are assembled by nanoparticles with diameter of ∼20 nm. The electrochemical performance of the β-Ni(OH)2/Ni-foam electrode is evaluated by cyclic voltammetry and galvanostatic charge–discharge tests. The difference between the oxygen evolution reaction onset potential and the anodic peak potential for this electrode (∼100 mV) is larger than that for β-Ni(OH)2 nanosheets and nanotubes powder electrode (∼65–77 mV) and much larger than that for commercial spherical β-Ni(OH)2 powder electrode (∼25–47 mV), indicating that the β-Ni(OH)2/Ni-foam electrode can be fully charged. The specific discharge capacity of β-Ni(OH)2 in the β-Ni(OH)2/Ni-foam electrode reaches 275 mAh g−1, which is close to the theoretical value, lower than that of β-Ni(OH)2 nanotubes (315 mAh g−1), but higher than that of nanosheets (219.5 mAh g−1), commercial micrometer grade spherical powders (265 mAh g−1) and microtubes (232.4 mAh g−1).  相似文献   

16.
Monte Carlo method is applied to investigate the kinetics of ammonia oxidative decomposition over the commercial propylene ammoxidation catalyst(Mo-Bi). The simulation is quite in agreement with experimental results. Monte Carlo simulation proves that the process of ammonia oxidation decomposition is a two-step reaction.  相似文献   

17.
The kinetics of reactions involved in dehydrogenation of propane to propylene over Pt–Sn/Al2O3 catalyst was studied. The simultaneous deactivation of individual dehydrogenation, hydrogenolysis and cracking sites was also studied. A model was developed to obtain the transient conversion of propane, product selectivity and catalytic site activity. The dehydrogenation reaction was considered as the main reaction governing propane and hydrogen concentrations along the reactor. Catalytic test runs were performed in a fixed-bed quartz reactor. The kinetic expressions developed for the main and side reactions were verified by integral and a combination of integral–differential analysis of reactor data, respectively, and the kinetic parameters were obtained. The deactivation of the active sites for the three reactions was found to follow a first-order independent decay law. The rate constants of deactivation were found to decrease in the order of dehydrogenation, hydrogenolysis and cracking. Noncatalytic thermal cracking was found to be comparable to the catalytic route resulting in a very low apparent deactivation rate constant for cracking reaction.  相似文献   

18.
Co/TiO2 catalysts prepared by sol–gel method were studied for gas-phase mercury oxidation in this paper. Experimental results revealed that the optimal loading of Co was 7.5%, which yielded more than 90% oxidation efficiency within the temperature range of 120–330 °C. The high activity was mainly attributed to the enrichment of well dispersed Co3O4. We also found that oxygen performed a key role in mercury oxidation process, while HCl could corrode the oxidized mercury and release it to gas phase. Thereafter, a modified Mars–Maessen mechanism was proposed and the possible simultaneous oxidization of NO and mercury was studied.  相似文献   

19.
Propane combustion was studied on Pt(0.4%)/V2O5–Al2O3 catalysts containing up to 20% V2O5. The density, strength and nature of surface acid sites were determined by TPD of NH3 and FTIR spectra of adsorbed pyridine. The sample acidity increased with the vanadium content, essentially because the addition of vanadium oxide generated Brønsted acid sites. The Pt dispersion as determined by H2 chemisorption increased with increasing V2O5 loading. The sample activity for propane combustion was evaluated through both conversion versus temperature (light-off curves) and kinetically-controlled conversion versus time catalytic tests. The propane combustion turnover rate on Pt/V2O5–Al2O3 increased with the amount of vanadium, probably because the intrinsic Pt oxidation activity increases with the sample acidity.  相似文献   

20.
This study was undertaken to know the influence of chloride ions in TiO2–ZrO2 mixed oxide and to explore chloride containing Fe2O3/TiO2–ZrO2 catalyst for oxidative dehydrogenation of ethylbenzene to styrene utilizing carbon dioxide as a soft oxidant. The TiO2–ZrO2 mixed oxide was synthesized by a co-precipitation method. Over the calcined support, a nominal 15 wt.% Fe2O3 was deposited by a wet impregnation method. The prepared catalysts were characterized using X-ray diffraction, temperature programmed desorption of NH3 and CO2, scanning electron microscopy and BET surface area methods. The catalytic activity measurements were made in a fixed-bed microreactor under normal atmospheric pressure. Characterization studies reveal that chloride ions exhibit a strong influence on the physicochemical and catalytic properties of the titania–zirconia composite oxides. The impregnated iron oxide was found to be in a highly dispersed form over the TiO2–ZrO2 support and influenced greatly on its acid–base properties. The chloride containing Fe2O3/TiO2–ZrO2 catalyst exhibited better activity and selectivity. The order of activity on various samples was found to be Fe2O3/TiO2–ZrO2 (chloride) > TiO2–ZrO2 (chloride) > TiO2–ZrO2.  相似文献   

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