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1.
Aqueous phase reforming of glycerol over the Pd loaded Ni/Al2O3 catalysts   总被引:1,自引:0,他引:1  
Bifunctional catalysts containing (0.5-1.5 wt%) palladium and 15 wt% of Nickel supported on gamma-Al2O3 were prepared via an impregnation technique and catalysts were characterzed by XRD BET surface area and SEM, respectively. The aqueous phase reforming of glycerol (APR) was conducted over alumina-supported catalysts at different reaction conditions for catalytic activity. Finally, we concluded that the 1.0 wt% Pd 15 wt% Ni/gamma-Al2O3 catalyst evidences higher conversion, hydrogen selectivity, lower alkane selectivity and CO production. This indicate that Pd loaded Ni/gamma-Al2O3 could be a potential catalyst for the APR of glycerol.  相似文献   

2.
Steam reforming (SR) of glycerol for the production of hydrogen was investigated over the nano-sized Ni-based catalysts. The Ni-based catalysts were prepared by solid phase crystallization and impregnation methods, and characterized by N2 physisorption, CO chemisorption, XRD, SEM, and TEM techniques. The Ni/gamma-Al2O3 catalyst showed higher conversion and H2 selectivity. However, it was slowly deactivated due to the carbon formation on the surface of catalyst and the sintering. It was found that the Ni based hydrotalcite-like catalyst (spc-Ni/MgAl) showed higher catalytic activity to prevent carbon formation than Ni/gamma-Al2O3 catalyst in the SR of glycerol.  相似文献   

3.
Characteristics of carbon deposition by CH4 and carbon elimination by CO2 over conventional and nanoscale Ni/gamma-Al2O3 catalysts were investigated by using a pulse reaction, as well as by TGA, TEM, TPO-MS, H2-TPR and H2-chemisorption techniques. It was found that the behaviors of carbon deposition by CH4 decomposition and carbon elimination by CO2 depend on the active metal dispersion and the metal-support interaction. The filamentous carbon was formed on the conventional Ni/gamma-Al2O3 catalyst with low metal dispersion and relatively large particles, this type of filamentous carbon was far from the active centers and difficult to eliminate by CO2. On the other hand, the carbon deposition originated from CH4 decomposition on the nanoscale Ni/gamma-Al2O3 catalyst would mainly cover the surface of active centers, this type of highly active carbon was easily eliminated by CO2 because it is close to the active center Ni atoms. As a result, the improvement of coking-resistance was ascribed to the high metal dispersion and strong metal-support interaction, a model of CH4 decomposition carbon deposition on Ni/gamma-Al2O3 catalyst was proposed.  相似文献   

4.
Catalytic oxidation of VOC (toluene) over a copper based catalyst was carried out to assess its properties and performance. The Brunauer Emmett Teller (BET) method, X-ray diffraction (XRD), temperature programmed reduction (TPR), N2O pulse titration and energy dispersive spectroscopy (EDS) were used to characterize a series of 5 wt% Cu/gamma-Al2O3 catalysts modified with silver. The experimental results revealed that the addition of silver to 5 wt% Cu/gamma-Al2O3 catalyst highly enhanced its catalytic activity. With increasing addition amount of silver, the light-off curve for complete oxidation of toluene shifted to lower temperature. In addition, the increase of the addition amount of silver caused the copper particle size of 5 wt% Cu/gamma-Al2O3 catalyst to gradually increase. Subsequently, it demonstrated that the increase in the copper particle size is closely associated with the increase in catalytic activity.  相似文献   

5.
In order to find a catalyst with high activity and stability for catalytic wet peroxide oxidation (CWPO) process under normal condition, with Fe(2)O(3)/gamma-Al(2)O(3) and Fe(2)O(3)-CeO(2)/gamma-Al(2)O(3) catalysts prepared by impregnation method, the effect of CeO(2) doping on the structure and catalytic activity of Fe(2)O(3)/gamma-Al(2)O(3) for catalytic wet peroxide oxidation of azo dyes at 25 degrees C and atmospheric pressure is evaluated using BET, SEM, XRF, XRD, XPS and chemical analysis techniques, and test results show that, better dispersion and smaller size of Fe(2)O(3) crystal can be achieved by adding CeO(2), and the content of chemisorbed oxygen can also be increased on the surface of catalyst. CWPO experimental results indicate that azo dyes in simulated wastewater can be efficiently mineralized and the catalytic activity of Fe(2)O(3)-CeO(2)/gamma-Al(2)O(3) can be increased by about 10% compared with that of Fe(2)O(3)/gamma-Al(2)O(3) because of the promotion of the structural and redox properties of the ferric oxide by ceria doped. Leaching tests indicate that Fe(2)O(3)/gamma-Al(2)O(3) and Fe(2)O(3)-CeO(2)/gamma-Al(2)O(3) are stable with a negligible amount of irons found in the aqueous solution after reaction for 2h. It can therefore be concluded from results and discussion that in comparison with Fe(2)O(3)/gamma-Al(2)O(3), Fe(2)O(3)-CeO(2)/gamma-Al(2)O(3) is a suitable catalyst, which can effectively degrade contaminants at normal temperature and atmospheric pressure.  相似文献   

6.
The catalytic oxidation of aromatic hydrocarbons over supported metal oxide   总被引:9,自引:0,他引:9  
The catalytic activity of metals (Cu, Mn, Fe, V, Mo, Co, Ni, Zn)/gamma-Al2O3 was investigated to bring about the complete oxidation of benzene, toluene and xylene (BTX). Among them, Cu/gamma-Al2O3 was found to be the most promising catalyst based on activity. X-ray diffraction (XRD), Brunauer Emmett Teller method (BET), electron probe X-ray micro analysis (EPMA) and temperature programmed reduction (TPR) by H2 were used to characterize a series of supported copper catalysts. Increasing the calcination temperature resulted in decreasing the specific surface areas of catalysts and, subsequently, the catalytic activity. Copper loadings on gamma-Al2O3 had a great effect on catalytic activity, and 5 wt.% Cu/gamma-Al2O3 catalyst was observed to be the most active, which might be contributed to the well-dispersed copper surface phase. Using TiO2 (anatase), TiO2 (rutile), SiO2 (I) and SiO2 (II) as support instead of gamma-Al2O3, the activity sequence of 5 wt.% Cu with respect to the support was gamma-Al2O3 > TiO2 (rutile) > TiO2 (anatase)>SiO2 (I) > SiO2 (II), and this appeared to be correlated with the distribution of copper on support rather than with the specific surface area of the catalyst. The smaller particle size of copper, due to its high dispersion on support, had a positive effect on catalytic activity. The activity of 5 wt.% Cu/gamma-Al2O3 with respect to the VOC molecule was observed to follow this sequence: toluene > xylene > benzene. Increasing the reactant concentration exerted an inhibiting effect on the catalytic activity.  相似文献   

7.
The preferential CO oxidation in the presence of excess hydrogen was studied over Pt-Co/gamma-Al2O3. CO chemisorption, X-ray diffraction (XRD), transmission electron microscopy (TEM), energy dispersive X-ray spectrometer (EDX) and temperature programmed reduction (TPR) were conducted to characterize active catalysts. The catalytic activity for CO oxidation and methanation at low temperatures increased with the amounts of cobalt in Pt-Co/gamma-Al2O3. This accompanied the TPR peak shift to lower temperatures. The optimum molar ratio between Co and Pt was determined to be 10. The co-impregnated Pt-Co/gamma-Al2O3 appeared to be superior to Pt/Co/gamma-Al2O3 and Co/Pt/gamma-Al2O3. The reductive pretreatment at high temperature such as 773 K increased the CO2 selectivity over a wide reaction temperature. The bimetallic phase of Pt-Co seems to give rise to high catalytic activity in selective oxidation of CO in H2-rich stream.  相似文献   

8.
The performance of Ni/delta-Al2O3 catalyst in propane autothermal reforming (ATR) for hydrogen production was investigated in the present study. The catalysts were characterized using XRD, TEM, and SEM. The activity of the Ni/delta-Al2O3 catalyst manufactured by the water-alcohol method was better than those of the catalysts manufactured by the impregnation and chemical reduction methods. The Ni/delta-Al2O3 catalysts were modified by the addition of promoters such as Mg, La, Ce, and Co, in order to improve their stability and yield. Hydrogen production was the largest for the Ni-Co-CeO2/Al2O3, catalyst.  相似文献   

9.
Multiwalled carbon nanotubes (MWCNTs)-supported nickel catalysts with different metal-loading contents were synthesized trough deposition–precipitation (DP) method for its subsequent performance study on steam reforming reaction of propane. The metal-loading content was set at 5, 10, 20, and 25% of nickel. Results showed that 20 wt% nickel oxide over MWCNTs (20% NiO/MWCNTs) had the best performance, on the propane steam reforming reaction, in terms of H2 conversion comparing with the rest of the NiO/MWCNTs catalysts (5, 10, 25 wt% Ni) and a nickel over alumina (Ni/Al2O3) commercial catalyst. The features of the NiO/MWCNTs catalysts were studied trough FT-IR, Raman spectroscopy, N2 adsorption–desorption isotherms, X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscopy, and field emission scanning electron microscopy measurements. The results evidenced that optimum relation between Ni content, Ni dispersion, and particle size played a main role in the catalyst performance, rendering the 20% NiO/MWCNT as the most promising, among the catalysts studied, for the steam reforming of propane.  相似文献   

10.
Autothermal reforming of propane for hydrogen over Ni catalysts supported on a variety of perovskites was performed in an atmospheric flow reactor. Perovskite is known for its higher thermal stability and oxygen storage capacity, but catalytic activity of itself is low. A sites of the ABO3 structured perovskites were occupied by La while B sites by one of Fe, Co, Ni, and Al by citrate method. The composition of the reactant mixture was H2O/C/O2 = 8.96/1.0/1.1. The changes in the states of the catalysts after reaction were analyzed by XRD, TPD, and TGA. Ni/LaAlO3 catalyst maintained the perovskite structure after reaction. It showed higher hydrogen yield and thermal stability compared to those of the catalysts with Fe, Co, or Ni in B sites. Catalysts prepared by deposition-precipitation (DP) method showed higher activity than those prepared by impregnation method, presumably due to the smaller sizes of the NiO crystal particles.  相似文献   

11.
In this study, Al_2O_3-washcoated SiC(Al_2O_3–SiC) foams and Al_2O_3 powder were employed as the supports of a Ni catalyst for the liquid-phase hydrogenation of benzaldehyde. A series of Ni/Al_2O_3–SiC foam catalysts and Ni/Al_2O_3 powder catalysts with a Ni loading from 10 wt% to 37 wt% of the weight of Al_2O_3 were first prepared by a deposition–precipitation(DP) method. The catalytic activity and recyclability of both kinds of catalysts were then compared. Although it had a smaller accessible surface area with the reactant, the foam catalyst with a Ni loading of 16 wt% exhibited a slightly higher conversion of benzaldehyde after 6 h(of 99.3%) in comparison with the Ni/Al_2O_3 catalyst with identical Ni loading(conversion of 97.5%). When the Ni loading increased from 16 wt% to 37 wt%, the reaction rate obtained with the foam catalyst increased significantly from 0.108 to 0.204 mol L~(-1)h~(-1), whereas the reaction rate obtained with the powder catalyst increased from 0.106 to 0.123 mol L~(-1)h~(-1). Furthermore, the specific activity(moles of benzaldehyde consumed by 1 g min~(-1)of Ni) of the foam catalyst with a Ni loading above 30 wt% was superior to that of the powder catalyst because of its smaller Ni-particle size and higher mass-transfer rate. The foam catalyst displayed a high recyclability as a function of run times owing to the strong interaction between the Ni component and the Al_2O_3 coating. The conversion of benzaldehyde over the foam catalyst remained almost unchanged after being used 8 times. In comparison, a drop of 43% in the conversion of benzaldehyde with the powder catalyst was observed after being used 7 times due to the leaching of the Ni component.  相似文献   

12.
Epoxidation of 1-butene-3-ol (1B3O) with 30 wt% hydrogen peroxide over TS-2 catalyst has been studied with methanol as a solvent and at elevated pressure (autogenic). The influence of temperature in the range of 20-120 degrees C, the molar ratio of 1B3O/H(2)O(2) 1:1-5:1, methanol concentration 5-90 wt%, TS-2 catalyst concentration 0.1-5.0 wt% and the reaction time 0.5-5.0 h have been investigated. The process was described by the following functions: the selectivity of transformation to 1,2-epoxybutane-3-ol (1,2EB3) in relation to 1B3O consumed, the selectivity of transformation to organic compounds in relation to H(2)O(2) consumed and the conversions of 1B3O and hydrogen peroxide. The major product of epoxidation is 1,2EB3, a compound with many applications.  相似文献   

13.
Catalytic oxidation is one of the cost-effective technologies to solve the troublesome volatile organic compounds. This study treated methyl-isobutyl-ketone (MIBK) by a commercial catalyst, Pt/gamma-Al(2)O(3), in a fixed-bed reactor. The effects of operating factors, such as operating temperature, MIBK concentration, space velocity, and O(2) concentration, on the performance of the catalyst were investigated. The products and reactants distributions from the oxidation of MIBK over Pt/gamma-Al(2)O(3) were observed. The results show that the products containing carbon atoms are CO, CO(2), and C(3)H(6)O. Two catalyst life-tests were also carried out to characterize the deactivation effect of MIBK. The result shows that the deactivation effect may be due to the coke on the catalyst surface at 423 K. From the statistical analysis, the operating temperature is the most effective factor on the conversion of MIBK. The catalysts were also characterized by surface area analysis and elemental analysis before and after the test. The results show that the catalytic deactivation may be due to carbon coating. At low temperature (423 K), the phenomenon of carbon coating was more obvious than that at high temperature (573 K). The product distributions from the oxidation of MIBK over Pt/gamma-Al(2)O(3) were analyzed by GC. The results indicate that the C(3)H(6)O is formed from the beginning, presenting a peak at 423 K, 6.54 ppm. The CO concentration also peaked at the same temperature, 6.84 ppm.  相似文献   

14.
High gravimetric energy density, earth-abundance, and environmental friendliness of hydrogen sources have inspired the utilization of hydrogen fuel as a clean alternative to fossil fuels. Hydrogen evolution reaction (HER), a half reaction of water splitting, is crucial to the low-cost production of pure H2 fuels but necessitates the use of electrocatalysts to expedite reaction kinetics. Owing to the availability of low-cost oxygen evolution reaction (OER) catalysts for the counter electrode in alkaline media and the lack of low-cost OER catalysts in acidic media, researchers have focused on developing HER catalysts in alkaline media with high activity and stability. Nickel is well-known as an HER catalyst and continuous efforts have been undertaken to improve Ni-based catalysts as alkaline electrolyzers. In this review, we summarize earlier studies of HER activity and mechanism on Ni surfaces, along with recent progress in the optimization of the Ni-based catalysts using various modern techniques. Recently developed Ni-based HER catalysts are categorized according to their chemical nature, and the advantages as well as limitations of each category are discussed. Among all Ni-based catalysts, Ni-based alloys and Ni-based hetero-structure exhibit the most promising electrocatalytic activity and stability owing to the fine-tuning of their surface adsorption properties via a synergistic nearby element or domain. Finally, selected applications of the developed Ni-based HER catalysts are highlighted, such as water splitting, the chloralkali process, and microbial electrolysis cell.
  相似文献   

15.
In order to develop a catalyst with high activity and stability for microwave assisted ClO2 catalytic oxidation, we prepared CuOn-La2O3/gamma-Al2O3 by impregnation-deposition method, and determined its properties using BET, XRF, XPS and chemical analysis techniques. The test results show that, better thermal ability of gamma-Al2O3 and high loading of Cu in the catalyst can be achieved by adding La2O3. The microwave assisted ClO2 catalytic oxidation process with CuOn-La2O3/gamma-Al2O3 used as catalyst was also investigated, and the results show that the catalyst has an excellent catalytic activity in treating synthetic wastewater containing 100 mg/L phenol, and 91.66% of phenol and 50.35% of total organic carbon (TOC) can be removed under the optimum process conditions. Compared with no catalyst process, CuOn-La2O3/gamma-Al2O3 can effectively degrade contaminants in short reaction time and with low oxidant dosage, extensive pH range. The comparison of phenol removal efficiency in the different process indicates that microwave irradiation and catalyst work together to oxidize phenol effectively. It can therefore be concluded from results and discussion that CuOn-La2O3/gamma-Al2O3 is a suitable catalyst in microwave assisted ClO2 catalytic oxidation process.  相似文献   

16.
The catalytic combustion of carbon tetrachloride (CCl4) by metal oxide catalysts coated on the monolith support was investigated. The prepared catalysts were tested at temperatures between 300 and 800 degrees C and at varying gas hourly space velocity (GHSV) values with an excess air ratio of 3100%. The catalyst, whose composition was 18% Cr2O3, 2% Ce2O3 and 80% gamma-Al2O3, was found to almost completely oxidize CCl4. The operating conditions proposed are 5702 h(-1) for GHSV, 3100% excess air and a temperature slightly higher than 800 degrees C. The reaction rate expression was found to be independent of oxygen partial pressure but strongly dependent on CCl4 partial pressure.  相似文献   

17.
采用固相法制备氮掺杂SrTiO3,并用浸渍氢气还原法制备了不同NiO、CoO负载量的N-SrTiO3异质结复合光催化剂,采用XRD、SEM、荧光光谱(FS)、紫外可见漫反射光谱(UV-Vis DRS)对其进行表征和分析,考察了在模拟太阳光下产氢活性及其变化规律,同时探讨了负载物的不同处理方法对光催化剂产氢活性的影响. 结果表明,氧化物的负载先氢还原后氧化处理较直接氧化处理有更高的光催化活性;所制备的NiO/N-SrTiO3、CoO/N-SrTiO3复合催化剂较单一催化剂有更高的产氢活性,当负载量分别为1.0wt%、0.5wt%时达最佳产氢活性,6h内的产氢量分别是未改性N-SrTiO3样品的4.2、4.9倍. 导致产氢率提高的主要原因是由于负载金属氧化物在两相界面处形成的异质结成为光催化反应中光生电子和空穴的单向转移通道,促使光生电荷有效分离,提高了复合催化剂的光催化活性.  相似文献   

18.
分别以碳纳米管(CNTs)和活性氧化铝(Al2O3)为载体,通过浸渍法制备了负载型镍基催化剂和钙改性的镍基催化剂,用二氧化碳甲炕化反应评价其催化性能,通过X射线衍射(XRD)、程序升温还原(H2-TPR)、程序升温脱附(H2-TPD)和氮气等温吸附脱附等手段对催化剂进行表征,结果表明,Ni/CNTs催化剂中的镍物种比Ni/Al2O3中的镍物种容易还原,同时钙改性Ni/CNTs催化剂更能促进镍物种的还原,添加钙可以促进CNTs载体催化剂的分散度,这些特性能提高钙改性Ni/CNTs催化剂的催化活性和稳定性。  相似文献   

19.
吴军良  夏启斌  刘治猛  李忠 《功能材料》2012,43(10):1332-1335,1340
采用等体积浸渍法制备了MnOx/γ-Al2O3、FeOx/γ-Al2O3和CuOx/γ-Al2O3催化剂,测定了不同催化剂在低温等离子体场内分解甲苯的活性,用X射线衍射(XRD)、氢气程序升温还原(H2-TPR)技术对催化剂进行表征。结果表明催化剂分解甲苯的活性的顺序是MnOx/γ-Al2O3>FeOx/γ-Al2O3>CuOx/γ-Al2O3。催化剂分解臭氧的实验表明,不同催化活性组分对臭氧的催化分解性能顺序与对甲苯的分解性能顺序是一致的。MnOx/γ-Al2O3催化剂的Mn负载量对其催化活性有明显影响,Mn的含量为1%(质量分数)时,催化剂的活性最高,当能量密度为19J/L时,其对甲苯催化氧化的转化率接近100%。催化剂表征结果表明当Mn含量为1%(质量分数)时,氧化锰在载体γ-Al2O3上最接近单层分散量,此时活性组分与载体表面的相互结合力最强,在载体上有很好的分散性,从而表现出对甲苯分解的最好性能。  相似文献   

20.
Colloidal Pt nanoparticles are prepared using H2PtCl6 as a precursor, polyvinylpyrrolidone (PVP: molecular weight = 10,000 and 40,000) and hydrogen as a stabilizing agent and a reducing agent, respectively. The amounts of the precursor and the stabilizing agent and the molecular weight of PVP have an effect on the formation of Pt nanoparticles. Supported Pt catalyst (CSPt) is prepared from colloidal Pt nanoparticles and y-Al2O3. Another supported Pt catalyst (ISPt) is prepared by using the conventional incipient wetness impregnation method with an aqueous H2PtCl6 solution and gamma-Al2O3. The catalytic activities of CSPt and ISPt catalysts are compared for VOC (toluene) oxidation. Transmission Electron Microscopy (TEM), UV-vis, X-ray diffraction (XRD) and temperature programmed reduction (TPR) are used to characterize CSPt and ISPt catalysts. The experimental results reveal that the catalytic activity of CSPt is superior to that of ISPT.  相似文献   

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