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1.
The methane autothermal reforming in the present of oxygen was studied over cerium-and zirconium-promoted Ni/SiO2 catalysts in a fluidized bed reactor. The addition of CeZrO2 resulted in a significant improvement in the initial activity of the catalysis as well as an in-crease in the stability. The long-term activity of the promoted catalyst was dependent upon the rapid redox properties between the oxidative zone and the reductive zone in a fluidized bed reactor. H2 temperature-programmed reduction (H2-TPR) and temperature-progranmaed sur-face reaction (TPSR) studies demonstrated that addition of the CeZrO2 resulted in an increase in the reducibility and oxygen transfer ability of the support, Ni/Ce0.5ZrO0.5O2-SiO2 showed improved redox properties compared with Ni/SiO2 due to a low-temperature reduction. X-ray diffraction (XRD) of the fresh and spent catalysts showed that the promoter enhanced the nickel dispersion and retarded metal particle growth during reaction at high temperature, and surface Ni was gradually oxidized by remaining O2, leading to Ni deactivation.  相似文献   

2.
The effects of Ce-ZrOx, Ce-LaOx, Ce-SmOx and Ce-GdOx additions to Rh/Al2O3 catalysts on methane autothermal re-forming were investigated. Activity tests showed that the addition of Ce-ZrOx could significantly reduce the concentration of CO in reformats. When Ce/Zr atomic ratio was 1:1, C%.5Zr0.5O2 solid solution with high thermal stability was obtained, which could effec- tively improve the catalytic performance effectively. The additives of alkaline-earth metals (Mg, K and Ca) on the catalytic properties were also studied. The results of experiments showed that the addition of MgO to Rh/Ce0.5Zr0.5O2/Al2O3 improved the stable per- formance and the carbon resistance of the catalyst. The optimized catalyst was 0.1%Rh/2.0%MgO/40%Ce0.5Zr0.5O2/Al2O3, which showed a highly stable performance for methane autothermal reforming.  相似文献   

3.
Y2O3-Al2O3 with different mole ratios of Y:Al were prepared by co-precipitation method. Catalysts Ni/Y2O3, Ni/Al2O3 and Ni/ Y2O3-Al2O3 were prepared by impregnation method. The result of BET showed that Al2O3 with relative high surface area was in favor of Ni distribution, whilst the TPR test demonstrated that composite support had appropriate synergistic effect between active constituent and sup-port, and NiO could be reduced more easily than loaded on the single support. H2-TPD test indicated that the catalyst NYA11 had lots of ac-tivity sites where H could be desorbed easily, which led to hydrogen-rich production over the catalyst. Composite support catalysts exhibited high activity for ethanol steam reforming (SRE), and the supported catalyst with composite of 1:1 mole ratio of Y:Al exhibited the optimum catalytic properties for SRE. Ethanol could be completely converted over catalyst NYA11 even at 450 °C, and there had no inactivation after 60 h continuous reaction, hydrogen yield appeared maximum 35.9% at 400 °C, and tended to increase with increasing H2O/EtOH molar ratio and feed flow rate.  相似文献   

4.
Chemical-looping steam methane reforming (CL-SMR) is a novel process towards the production of pure hydrogen and syngas, consisting ofa syngas production reaction and a hydrogen production reaction. Macroporous CeQ-ZrO2 oxygen carders with different pore sizes prepared by colloidal crystal templating method and characterized by techniques of scalming electron microscopy (SEM), transmission electron microscopy (TEM), Brunauer-Emmett-Teller (BET), X-ray diffraction (XRD) and temperature pro- grammed reduction (H2-TPR) were tested in CL-SMR process. For comparison, nonporous CeO2-ZrO2 oxygen carrier prepared by precipitation method was also investigated. It was found that macroporous CeO2-ZrO2 oxygen carriers owned higher reducibility and reactivity in CL-SMR process than nonporous samples. For the macroporous CeO2-ZrO2 sample, the decline of pore size could im- prove the reducibility and reactivity. The macroporous sample with a pore size of 100 nm (labeled as Ce-Zr-100) showed the highest performance for the co-production of syngas and hydrogen during the successive CL-SMR redox cycles. After 10 redox cycles, it still retained good porous structure and reducibility. It was found that the porous structure could accelerate the oxygen release from bulk to surface, leading to a good mobility of oxygen and higher reducibility. In addition, it was also favorable for diffusion and penetration of methane and water steam into the sample particles to accelerate the reaction rate.  相似文献   

5.
The nickel-based catalysts were prepared by the sol-gel method and used for the CH4 reforming with CO2. The effects of the sol-gel method on the specific surface area, catalytic activity, desorption, and reduction performances of catalysts were investigated with BET, TPR, and TPD. Compared with the catalyst prepared by the impregnation method, the results indicated that the catalysts prepared by the sol-gel method had larger specific surface area, showing higher catalytic activities and exhibiting perfect desorption and reduction performances. In addition, the modification effects of adding La were studied, and it was found that the 0.75NLBT catalyst constituted of 5wt.%Ni-0.75wt.%La was optimal.  相似文献   

6.
Characteristics of carbon deposition of CH4 and C2H4 decomposition over supported Ni and Ni-Ce catalysts were studied by using a pulse reaction as well as BET, TPR, XPS and hydrogen chemisorption techniques. It is found that there is a metal-semiconductor interaction (MScI) in the Ni-Ce catalyst, and the effect of MScI on the carbon deposition of CH4 decomposition is opposite to that of C2H4. A novel model of carbon deposition of CH4 or C2H4 decomposition was proposed.  相似文献   

7.
MgO,CeO2 and MgO-CeO2 with different mole ratio of Mg:Ce were prepared by solid-phase burning method.Catalysts Ni/MgO,Ni/CeO2 and Ni/MgO-CeO2 were prepared by impregnation method.The catalytic properties were evaluated in ethanol steam reforming(ESR) reaction.Specific surface areas of the supports were measured by nitrogen adsorption-desorption at 77 K,and the catalysts were characterized with X-ray diffraction(XRD),temperature programmed reduction(TPR) and thermogravimetric(TG).The results showed that well...  相似文献   

8.
A series of Ni-Sm/sepiolite catalysts were prepared by impregnation. The modification of Sm2O3 for Ni/sepiolite was investigated by TPR, XPS and poisoning of CS2, respectively. The results indicate that the addition of Sm2O3 improves the activity of hydrogenation and anti-poisoning ability of Ni/sepiolite catalyst, and it also increases the dispersion of nickel atoms over support and the amount of active nickel atoms in catalyst. Effect of Sm203 on Ni/sepiolite catalyst ineludes not only electronic effect but also steric effect, whereas electronic effect seems to be principal.  相似文献   

9.
High surface area CeO2 was prepared by the surfactant-assisted route and was employed as catalyst support. The 0-3 at.% Cu doped Cu-Ni/CeO2 catalysts with 10 wt.% and 15 wt.% of total metal loading were prepared by an impregnation-coprecipitation method. The influence of Cu atomic content on the catalytic performance was investigated on the steam reforming of ethanol (SRE) for H2 production and the catalysts were characterized by N2 adsorption, inductively coupled plasma (ICP), X-ray diffraction (XRD), transmission electron microscopy (TEM), temperature-programmed rerduction (TPR) and H2-pulse chemisorption techniques. The activity and products distribution behaviors of the catalysts were significantly affected by the doped Cu molar content based on the promotion effect on the dispersion of NiO particles and the interactions between Cu-Ni metal and CeO2 support. Significant increase in the ethanol conversion and hydrogen selectivity were obtained when moderate Cu metal was doped into the Ni/CeO2 catalyst. Over both of the 10Ni98.5Cu1.5/CeO2 and 15Ni98.5Cu1.5/CeO2 catalysts, more than 80% of ethanol conversion and 60% of H2 selectivity were obtained in the ethanol steam-reforming when the reaction temperature was above 450 ℃.  相似文献   

10.
Nickel catalysts supported on CeO2-ZrO2-CeO2,ZrO2-Al2O3 and Al2O3 were prepared and characterized by means of X-ray diffraction(XRD),BET areas,H2 temperature-programmed reduction(H2-TPR),and X-ray photoelectron spectroscopy(XPS).Through the test of catalytic partial oxidation of methane(CPOM),Ni/CeO2-ZrO2-Al2O3 displayed the highest activity,which resulted from its largest BET area and best NiO dispersion.Furthermore,Ni/CeO2-ZrO2-Al2O3 maintained a long-time stability in CPOM,which was attributed to its best coking resistance among all the prepared catalysts.  相似文献   

11.
Two-step steam reforming of methane(SRM)is a novel chemical looping process towards the production of pure hydrogen and syngas(synthesis gas),consisting ofa syngas production step and a water-splitting step.Renewable energy can be used to drive this process for hydrogen production,especially solar energy.CeO2-Fe2O3 complex oxide oxygen carrier was prepared by the impregnation method and characterized by means of X-ray diffractometer(XRD),Raman spectroscopy(Raman)and hydrogen programmed reduction(H2-TPR).CH4temperature programmed and isothermal reactions were adopted to test syngas production reactivity,and water splitting reaction was employed to investigate water-splitting activity.Moreover,two-step SRM performance was evaluated by a successive redox cycle.The results showed that CO-uncontaminated H2 and highly selective syngas(with H2/CO ratio close to 2)could be respectively obtained from two steps,and CeFeO3 formation was found in the first redox cycle and proved to be enhanced by the redox treatment.After 10 successive cycles,obvious CeFeO3 phase was detected,which may be responsible for favorable successive redox cycle performances.  相似文献   

12.
NiO/Ce0.7Pr0.3O2 catalysts were prepared by co-precipitation method and used for steam reforming of ethanol to produce hydrogen. The influence of nickel content and the doping of Pr on the catalytic performance were investigated. The catalysts were characterized by using temperature programmed reduction (TPR), X-ray diffraction (XRD) and thermal analysis techniques. 15 wt.%NiO/Ce0.7Pr0.3O2 catalyst was highly active and selective for steam reforming of ethanol to produce hydrogen. With the doping of Pr, the anti-carbon deposition property of the catalyst and the anti-sintering stability of metal nickel were effectively improved. The improvement of the anti-carbon deposition is attributed to generation of oxygen vacancies resulted from the Pr doping; while the improvement of anti sintering is ascribed to the intensified interaction between the nickel species and the support which is owing to the Pr-doping resulted incorporation of some nickel ions into ceria lattice.  相似文献   

13.
La modified Ni/γ-Al2O3 catalysts prepared by co-precipitation method using NaOH-Na2CO3 as a precipitator show high activity and selectivity for the partial oxidation of methane (POM). Meanwhile, the addition of La is beneficial for the formation of an active component and stability of support. We investigated some factors including calcining temperature, nickel content, and space velocity, which turned out to have a strong influence on catalytic activity and selectivity. By XRD and TPR, it is concluded that Ni0 reduced from amorphous NiAl2O4 is the major active component for POM.  相似文献   

14.
Syngas production from CO2 reforming of ethanol over an Ir/Ce O2 catalyst was investigated. Catalysts characterization was conducted by X-ray diffraction(XRD), temperature programmed reduction(TPR), transmission electron microscopy(TEM) and temperature programmed oxidation(TPO). The Ir/Ce O2 catalyst was more active and stable toward syngas formation(molar ratio ~1). The superior catalytic performance was interpreted in terms of the strong interaction between Ir particles and ceria support which was crucial for efficient ethanol/CO2 activation and coke removal on the catalyst surface.  相似文献   

15.
La modified Ni/T-Al2O3 catalysts prepared by co-precipitation method using NaOH-Na2CO3 as a precipitator show high activity and selectivity for the partial oxidation of methane (POM). Meanwhile, the addition of La is beneficial for the formation of an active component and stability of support. We investigated some factors including calcining temperature, nickel content, and space velocity, which turned out to have a strong influence on catalytic activity and selectivity. By XRD and TPR, it is concluded that Ni^0 reduced from amorphous NiAl2O4 is the major active component for POM.  相似文献   

16.
The organic rare earth complex was embedded in silica spheres to form inorganic-organic hybrid. Photoactiver are earth complexes with various organic ligands exhibit intense narrow emission band, and the silica is an excellent matrix for inorganic-organic structure. The transmission electron microscope image presents the hybrid nanospheres. The diameter of the hybrid is about 100 nm. The europium complex that incorporated into silica sphere is also proved by the IR spectra, the excitation and emission spectra. The lifetimes of the Eu3 ions in the hybrid nanospheres and in the pure europium complex were also detected. This hybrid with inhomogeneous compositions exhibits specifically tailored chemical and optical properties, such as perfect thermal and mechanical stability, colorimetric purity and so on. It can be used as luminescent and optical material in EL and PL fields.  相似文献   

17.
Monometallic catalyst Pt/SAPO-11 was prepared by impregnation method.Bimetallic catalysts LaPt/SAPO-11 or CePt/SAPO-11 was prepared by sequential impregnation method.The catalysts were characterized by X-ray diffraction(XRD),nitrogen adsorption,temperature-programmed desorption of ammonia(NH3-TPD),and Fourier transform infrared spectroscopy(FT-IR) techniques.The results showed that with the addition of rare earths the BET surface areas,pore volume,the amount of Bronsted acid and the total acidity of catalys...  相似文献   

18.
Pd/CeO2 catalysts with flower-like morphology were fabricated via an ultrasonic-assisted membrane reduction (UAMR) and hydrothermal methods. The catalysts were physically characterized and evaluated fo...  相似文献   

19.
A different method was employed for the preparation of a metal supported perovskite catalyst for the catalytic combustion of methane.The prepared metallic catalysts were characterized by means of X-ray diffractometer(XRD),scanning electron microscopy(SEM),transmission electron microscopy(TEM),and also by ultrasonic and thermal shock tests and catalytic activity.It was found that the process factors during the preparation,e.g.the preparation of the catalyst precursor and the coating slurry,the calcination te...  相似文献   

20.
Water-gas shift(WGS)is a critical step in fuelprocessors for preli minary COclean-up and additionalhydrogen generation prior to the CO clean-up stage,which opened up new potential applications for WGScatalysts.Recently several formulations of noble-met-al…  相似文献   

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