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1.
The CO methanation was studied over zeolite NaY supported Ni, Co3O4, ZrO2 catalysts. The XRD, N2 physisorption and SEM analysis were used in order to characterize the catalysts. Catalytic activities were carried out under a feed composition of 1% CO, 50% H2 and 49% He between the 125 °C to 375 °C. Except for the Ni/Co3O4/NaY catalyst, all catalysts gave high surface area because of the presence of zeolite NaY. Average pore diameter of the catalysts fell into the mesopore diameter range. The highest CO methanation activity was obtained with Ni/ZrO2/NaY catalyst at which the CO methanation was started after 175 °C and 100% CO conversion was obtained at 275 °C using the same catalyst.  相似文献   

2.
In this study, a group of Ni catalysts supported on mesoporous nanocrystalline γ-Al2O3 with high surface area and with different Ni contents was prepared and employed in carbon dioxide methanation reaction. The obtained results showed increasing in nickel content from 10 to 25 wt.% decreased the specific surface area of catalysts from 177 to 130 m2/g and increased the nickel crystallite size from 12 to 24 nm. In addition, increasing in nickel content increased the reducibility of catalyst. The catalytic results revealed that the catalyst with 20 wt.% of Ni possessed high activity and stability in CO2 methanation reaction.  相似文献   

3.
The catalytic performances of 12 wt.% Co/MgO catalyst pre-calcined at 873 K and of Ni catalysts for the steam reforming of naphthalene were investigated. The results of characterizations (TPR, XRD, and CO adsorption) for Ni catalysts showed that Ni metal particles were formed over the catalysts pre-calcined at 873 K with high Ni loading via reduction of NiO–MgO phases. A few Ni metal particles were obtained over the catalysts pre-calcined at 1173 K with all Ni loading values.The catalytic performance data showed that Co/MgO catalyst had higher activity (conv., 23%, 3 h) than any kinds of Ni/MgO catalysts tested in this study, under lower steam/carbon mole ratio (0.6) and higher concentration of fed naphthalene (3.5 mol%) than those used in the other works. The steam reforming of naphthalene proceeded when there was a stoichiometric ratio between the carbon atoms of naphthalene and H2O over Co catalyst; however, the activation of excess H2O happened over the Ni catalyst and this phenomenon can lead to having lower activity than Co catalyst. We concluded that these observations should be attributed to different catalytic performances between Co/MgO and Ni/MgO catalysts.  相似文献   

4.
A novel plate-type anodic alumina supported 17.9 wt% Ni/Al2O3/alloy showed a quick deactivation in daily start-up and shut down (DSS) steam reforming of methane (SRM) at 700 °C, because of the Ni oxidation reaction with steam. When 0.078 wt% Pt was doped, the catalyst exhibited self-activation and self-regeneration ability, while 3000 h continual and 500-time DSS stability was testified. Further, this Pt–Ni catalyst also showed excellent reactivity during carbon dioxide reforming of methane (CMR) and partial oxidation of methane reaction (POM). According to the TPR and XRD analyses, the H2 spillover effect and the formation of Pt–Ni alloy were believed to be the main reason for the reactivity improvement of this catalyst.  相似文献   

5.
Highly efficient non-noble metal based catalysts (Zr1  xNixO2) showed outstanding catalytic performance at lower temperature for selective CO methanation. The characterization techniques revealed that Zr1  xNixO2 catalyst contained uniformly dispersed Ni particles with strong interaction between Ni and ZrO2.  相似文献   

6.
The effect of a range of operation variables such as pressure, low temperature and H2/CO molar feed ration the catalytic performance of 80%Co/20%Ni/30 wt% La2O3/1 wt% Cs catalyst was investigated. It was found that the optimum operating conditions is a H2/CO = 2/1 molar feed ratio at 260 °C temperature and 2 bar pressure. Reaction rate equations were derived on the basis of the Langmuir–Hinshelwood–Hougen–Watson (LHHW) type models for the Fischer–Tropsch reactions. The activation energy obtained was 59.69 kJ/mol for optimal kinetic model.  相似文献   

7.
Ni(0.4)-MnOx catalyst was prepared by citrate combustion, which showed high catalytic performance for NH3-SCR reaction. After the resistance tests of SO2 and H2O, Ni(0.4)-MnOx-SH showed better NH3-SCR activity than that of Ni(0.4)-MnOx, when the temperature was > 240 °C. The characterizations suggest that Ni(0.4)-MnOx-SH has more acid sites for ammonia adsorption and far weaker oxidation capacity for NH3, which resulted in the high catalytic activity at middle-temperature.  相似文献   

8.
Mesoporous nickel (30 wt%)–iron (5 wt%)–alumina (denoted as NiFeAl–X) catalysts were prepared by a coprecipitation method with a variation of precipitation agent (X = (NH4)2CO3, Na2CO3, NH4OH, and NaOH), and they were applied to the methane production from CO2 and H2. Metal particle size of reduced NiFeAl–X catalysts decreased in the order of NiFeAl–NaOH > NiFeAl–NH4OH > NiFeAl–Na2CO3 > NiFeAl–(NH4)2CO3. In the methanation of CO2, yield for CH4 increased in the order of NiFeAl–NaOH < NiFeAl–NH4OH < NiFeAl–Na2CO3 < NiFeAl–(NH4)2CO3. This indicates that the catalytic performance in the methanation of CO2 was strongly influenced by the identity of precipitation agent.  相似文献   

9.
《Fuel》2005,84(12-13):1462-1468
Several Ni-based catalysts supported on a mixture of MgO, La2O3, and Al2O3 were prepared. The catalytic performance in the steam reforming of m-cresol was evaluated. In the investigation of the effect of Ru loading added to the Ni-catalyst, it was found that the presence of Ru strongly enhances the catalytic performance of the Ni-based catalyst when increasing Ru loading up to 2 wt%. Effect of Ni loading to the Ru-based catalyst system was also investigated. It was found that the addition of nickel to the Ru-based catalyst up to 15 wt% enhanced significantly the catalytic activity of the catalyst. The lifetime of the Ru–Ni catalysts in the reforming of m-cresol was further tested at 750 °C. In agreement with general observations of the use of Ni monometallic catalyst, deactivation of the catalyst due to the carbon deposition reaction already occurred in the reforming of the oxygenated compound. On the other hand, a reasonable high resistant on the carbon deposition in the reforming of m-cresol was given by the 2 wt% Ru–15 wt% Ni catalyst system. An effort in improving the strength of the catalyst support with this catalyst system was also conducted, and the catalyst showed significant increase in the stability of the reforming of oxygenated aromatic compound.  相似文献   

10.
Catalytic combustion of CO over perovskite-type oxides LaCo0.5M0.5O3 (M = Mn, Cr, Fe, Ni, Cu) and LaCo0.5Mn0.5O3 supported on cordierite were investigated. The catalysts were synthesized by impregnation method with citrate and characterized by XRD, SEM and TPR. The LaCo0.5Mn0.5O3 catalyst showed much higher activity in CO oxidation compared with LaCo0.5M0.5O3 (M = Cr, Fe, Ni, Cu) due to different kinds of valence state and lattice oxygen content. When LaCo0.5Mn0.5O3 was supported on cordierite, the activity was improved significantly. However, calcining temperature and the presence of water vapor affected the catalytic activity due to sintering and competition of H2O with CO for adsorption, respectively.  相似文献   

11.
A bifunctional CaO-Zr/Ni (13, 18, and 20.5 wt% NiO) sorbent–catalyst was developed using the wet-mixing/sonication technique and applied for hydrogen production by sorption-enhanced steam methane reforming (SESMR), an intensified process that integrates hydrogen production with CO2 capture. The material was characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM), and N2 physisorption (BET). CO2 sorption efficiency of the developed materials was evaluated during 25 CO2 sorption/regeneration cycles. The prepared sorbent–catalysts were then applied in the SESMR during 10 reaction cycles. The results showed that the bifunctional sorbent–catalyst with 20.5 wt% NiO loading presented the most suitable activity. The H2 yield of ∼91% at the end of the 10th SESMR cycle is considerably higher than equilibrium H2 yield that could be obtained by traditional steam methane reforming.  相似文献   

12.
A sample with a composition of 84 wt% MgH2–10 wt% Ni–2 wt% NaAlH4–2 wt% Ti–2 wt% CNT (named MgH2–10Ni–2NaAlH4–2Ti–2CNT) was prepared by milling in a planetary ball mill under H2. Activation of the sample was not required. At the first cycle, the sample absorbed 3.75 wt% H for 10 min, and 4.17 wt% H for 60 min at 593 K under 12 bar H2. Reactive mechanical grinding of Mg with Ni, NaAlH4, Ti, and CNT is thought to create defects on the surface and in the interior of Mg, as well as to reduce Mg particle size.  相似文献   

13.
The kinetic of the Fischer–Tropsch synthesis over a Fe–Ni/Al2O3 catalyst was investigated in a fixed bed micro reactor. Experimental conditions were varied as follow: reaction pressure 2–10 bar, H2/CO feed ratio of 2/1 and space velocity of 96–450 cm3(STP)/h/gramcatalyst at the temperature range 523–573 K. On the basis of carbide-enol mechanism and Langmuir–Hinshelwood–Hougen–Watson (LHHW) type rate equations, seventeen kinetic expressions for CO consumption were tested and interaction between adsorption HCO and dissociated adsorption hydrogen as the controlling step gave the most plausible kinetic model. The activation energy was 46.5 kJ/mole for optimal kinetic model.  相似文献   

14.
Nanocrystalline titania was prepared by solvothermal reaction of titanium butoxide in toluene at 300 °C for 2 h. Thus obtained-powder was calcined at 300 °C in box furnace for 1 h and then quenched in various media at different temperature. The physiochemical properties of samples were investigated by using X-ray diffraction (XRD), nitrogen adsorption, CO2-Temperature Programmed Desorption (CO2-TPD), UV–visible scanning spectrophotometer, Transmission electron microscopy (TEM) and electron spin resonance spectroscopy (ESR) techniques. All physical properties such as phase, BET surface area and crystal size were not changed after quenching processes. While the CO2-TPD and ESR results indicate the changing of Ti3+ contents on the surface of TiO2 after quenching process. The amounts of Ti3+ increased as the quenching temperature decreased. Photocatalytic decomposition of water was carried out to evaluate the catalytic activity of quenched TiO2. The activity of quenched-powder increased corresponding to the increasing of Ti3+ contents increased by following order: air at 77 K > air at RT > air at 373 K > 30 wt% H2O2 at RT = 30 wt% H2O2 at 373 K > H2O at RT > H2O at 373 K.  相似文献   

15.
《Journal of Catalysis》2007,245(1):144-155
Hysteresis of catalytic performance with respect to temperature increasing and decreasing in oxidative steam reforming of methane (CH4/H2O/O2/Ar = 40/30/20/10) over the monometallic Ni catalysts disappeared by the modification with Pt, and the additive effect of Pt by the sequential impregnation method (Pt/Ni) was much more significant than that by the co-impregnation method (Pt + Ni) in terms of catalytic performance and catalyst bed temperature profile. Characterization results by means of TEM, TPR, EXAFS, and FTIR suggest that the Pt atoms on the Pt/Ni catalysts were located more preferably on the surface to form a PtNi alloy than those on the Pt + Ni catalysts. The modification of Ni with Pt suppressed the oxidation of Ni species near the bed inlet in the oxidative steam reforming of methane at 1123 K, although the species on the monometallic Ni catalysts were oxidized under similar conditions. This can be due to the decreased oxidation rate of the species and the increased reduction rate caused by the surface modification of Ni with Pt. Consequently, the PtNi species can be maintained in the metallic state near the bed inlet, and the species can be the active site for the reforming reaction as well as the combustion reaction, which this leads to a lower bed temperature and smaller temperature gradient than those seen for the monometallic Ni catalysts.  相似文献   

16.
Hexagonal boron nitride (BN), with a graphite-type structure and with surface area of 184 m2/g was used as a support for palladium oxide (PdO/BN). About 1 wt% of palladium was deposited on BN by incipient wetness method by using palladium nitrate as precursor. The support and the catalyst were characterized by BET, TEM, XRD, XPS, ICP, TG, TPD, in situ ac electrical conductivity and by ammonia adsorption microcalorimetry. Oxidation of propylene and methane were used as model reactions to study the catalytic properties of the PdO/BN catalyst. The BN support was practically inactive in propylene oxidation up to 400 °C, while the onset of the oxidation was detected around 200 °C on PdO/BN, which points out the role of the palladium in adsorption of the reactive hydrocarbon species. At the same time, this temperature is coincident with the increase of the electronic conductivity on both BN and PdO/BN samples, which is important for oxygen adsorption/activation as electrophilic species. The catalyst was inactive in methane oxidation below 400 °C. Only about 2% CH4 conversion was observed at 400 °C, increasing sharply up to 87% at 550 °C with methane transformation only to CO2 and water.  相似文献   

17.
A new preparation method of Au/α-Fe2O3 catalyst for CO oxidation reaction was proposed in this paper. The method includes only a simple modification of the conventional coprecipitation method, adding HAuCl4 solution after the growth of iron hydroxide grain to a certain size, but significantly influenced the catalytic activity in the reaction. In the characterization study, XRD (X-ray diffractometer) analysis, TEM (transmission electron microscope) observation, and N2 adsorption measurement showed similar results among the samples calcined at the same temperature, but the effect of the preparation method appeared in the CO adsorption measurement among the samples calcined at 200 °C. Catalysts having high CO adsorption ability also performed well in CO oxidation tests. The CO adsorption and oxidation studies indicated that the proposed preparation method results in stable and effective loading of Au, compared to the conventional coprecipitation method. In the CO oxidation test, the catalyst prepared by the proposed mixing scheme achieved complete CO conversion for more than 3000 h at 25 °C, space velocity 100,000 h?1, and 500 ppm CO. The selectivity for the CO oxidation was confirmed using reformed gas containing excess H2. In addition, the NO reduction reaction was favored over CO oxidation by the catalyst. Thus, we were able to load Au on the α-Fe2O3 effectively and demonstrate its potential as an environmental catalyst.  相似文献   

18.
A sample of 86 wt% MgH2–10 wt% Ni–2 wt% NaAlH4–2 wt% Ti (named MgH2–10Ni–2NaAlH4–2Ti) was prepared by reactive mechanical grinding. Activation of the sample was not required at 573 K. At the first hydriding–dehydriding cycle (n = 1), the sample absorbed more than 5 wt% H at 573 K under 12 bar H2 for 60 min. The hydriding rate increased as the temperature increased from 423 K to 553 K. MgH2–10Ni–2NaAlH4–2Ti showed quite high hydridng rates at relatively low temperatures of 423 K and 473 K under 12 bar H2, absorbing 4.02 wt% H for 60 min at 473 K.  相似文献   

19.
Nickel-based catalysts supported on mesoporous nanocrystalline gamma Al2O3 promoted with various promoters (CeO2, MnO2, ZrO2, La2O3) were prepared and employed in the carbon dioxide methanation reaction. It was found that the addition of promoters to the catalyst varied the specific surface area from 139.4 to 147.4 m2/g and CeO2 and MnO2 improved the reducibility of catalyst. The catalytic results showed that the catalyst with 2 wt% of cerium promoter possessed high activity and stability in CO2 methanation reaction and showed a high CO2 conversion of 80.3% at 350 °C.  相似文献   

20.
《Fuel》2006,85(12-13):1708-1713
Ni–La and Ni–La–K catalysts supported on cordierite were prepared for steam reforming of kerosene to produce hydrogen. All these catalysts were tested in a fixed-bed reactor under different conditions. The catalysts obtained under different calcination temperatures and different reaction temperatures were characterized by TG–DTG and XRD techniques respectively. The influence of NiO and La2O3 contents on the activity of catalysts for steam reforming of kerosene to produce hydrogen was also investigated in our experiments. The experimental results indicate that the calcination temperature has much more influence on catalyst activity. The catalyst supported the promoter 5 wt% K2O, 25 wt% NiO and 10 wt% La2O3, is the optimal catalyst under 773 K of reaction temperature and 2300 h−1 of space velocity. Composition of Ni is highly dispersed on the catalyst surface. And through the duration test, the catalyst activity and stability are very satisfactory at 873 K of the reaction temperature.  相似文献   

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