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1.
CO2 reforming of CH4 was performed using Ni catalyst supported on La-hexaaluminate which has been an well-known material for high-temperature combustion. La-hexaaluminate was synthesized by sol-gel method at various conditions where different amount of Ni (5–20 wt%) was loaded. Ni/La-hexaaluminate experienced 72 h reaction and its catalytic activity was compared with that of Ni/Al2O3, Ni/La-hexaaluminate shows higher reforming activity and resistance to coke deposition compared to the Ni/Al2O3 model catalyst. Coke deposition increases proportionally to Ni content. Consequently, Ni(5)/La-hexaaluminate(700) is the most efficient catalyst among various Ni/La-hexaaluminate catalysts regarding the cost of Ni in Ni(X)/La-hexaaluminate catalysts. BET surface area, XRD, EA, TGA and TPO were performed for surface characterization. This work was presented at the 6 th Korea-China Workshop on Clean Energy Technology held at Busan, Korea, July 4–7, 2006.  相似文献   

2.
A co-precipitation method was employed to prepare Ni/Al2O3-ZrO2, Co/Al2 O3-ZrO2 and Ni-Co/Al2O3-ZrO2 catalysts. Their properties were characterized by N2 adsorption (BET), thermogravimetric analysis (TGA), temperature-programmed reduction (TPR), temperature-programmed desorption (CO2-TPD), and temperature-programmed surface reaction (CH4-TPSR and CO2-TPSR). Ni-Co/Al2O3-ZrO2 bimetallic catalyst has good performance in the reduction of active components Ni, Co and CO2 adsorption. Compared with mono-metallic catalyst, bimetallic catalyst could provide more active sites and CO2 adsorption sites (C + CO2 = 2CO) for the methane-reforming reaction, and a more appropriate force formed between active components and composite support (SMSI) for the catalytic reaction. According to the CH4-CO2-TPSR, there were 80.9% and 81.5% higher CH4 and CO2 conversion over Ni-Co/Al2O3-ZrO2 catalyst, and its better resistance to carbon deposition, less than 0.5% of coke after 4 h reaction, was found by TGA. The high activity and excellent anti-coking of the Ni-Co/Al2O3-ZrO2 catalyst were closely related to the synergy between Ni and Co active metal, the strong metal-support interaction and the use of composite support.  相似文献   

3.
Two types of CeO2-modified Ni/Al2O3 catalysts were prepared by a consecutive impregnation method with different sequences in the impregnation of Ni and CeO2, and their performance in autothermal reforming (ATR) of isooctane was investigated. Catalysts prepared by adding CeO2 prior to the addition of Ni, Ni/CeO2-Al2O3, produced larger amounts of hydrogen than those obtained using catalysts prepared by adding the two components in an opposite sequence, Ni-CeO2/Al2O3. The results of H2 chemisorption and temperature-programmed reduction revealed that added CeO2 increased the dispersion of the Ni species on Al2O3 and suppressed the formation of NiAl2O4 in the catalyst such that large amounts of Ni species were present as NiO, the active species for the ATR. The elemental and thermogravimetric analyses of deactivated catalysts indicated that Ni/CeO2-Al2O3, which showed a longer lifetime than Ni-CeO2/Al2O3, contained lesser amounts and different types of coke on the surface.  相似文献   

4.
A K-promoted 10Ni-(x)K/MgAl2O4 catalyst was investigated for the combined H2O and CO2 reforming (CSCR) of coke oven gas (COG) for syngas production. The 10Ni-(x)K/MgAl2O4 catalyst was prepared by co-impregnation, and the K content was varied from 0 to 5 wt%. The BET, XRD, H2-chemisorption, H2-TPR, and CO2-TPD were performed for determining the physicochemical properties of prepared catalysts. Except under the condition of a K/Ni=0.1 (wt%/wt%), the Ni crystal size and dispersion decreased with increasing K/Ni. The coke resistance of the catalyst was investigated under conditions of CH4: CO2: H2: CO:N2=1 : 1 : 2 : 0.3 : 0.3, 800 °C, 5 atm. The coke formation on the used catalyst was examined by SEM and TG analysis. As compared to the 10Ni/MgAl2O4 catalyst, the Kpromoted catalyst exhibited superior activity and coke resistance, attributed to its strong interaction with Ni and support, and the improved CO2 adsorption characteristic. The 10Ni-1K/MgAl2O4 catalyst exhibited optimum activity and coke resistance with only 1wt% of K.  相似文献   

5.
A series of Zr-doped ordered mesoporous Al2O3 with various Zr contents were synthesized by evaporation-induced self-assembly strategy and the Ni-based catalysts supported on these Al2O3 materials were prepared by impregnation method. These catalysts with large specific surface area, big pore volume, uniform pore size possess excellent catalytic performance for the low-temperature carbon dioxide reforming of methane. The activities of these catalysts were tested in carbon dioxide reforming of methane reaction with temperature increasing from 500 to 650?°C and the stabilities of these catalysts were evaluated for long time reaction at 650?°C. It was found that when Zr/(Zr?+?Al) molar ratio?=?0.5%, the Ni/0.5ZrO2–Al2O3 catalyst showed the highest activity, and exhibited superior stabilization compared to the Ni-based catalyst supported on traditional ordered mesoporous Al2O3. The “confinement effect” from mesoporous channels of alumina matrix is helpful to stabilize the Ni nanoparticles. As a promoter, Zr could stabilize the ordered mesoporous framework by reacting with Al2O3 to form ZrO2–Al2O3 solid solution. Since ZrO2 enhances the dissociation of carbon dioxide, more oxygen intermediates are given to remove the carbon formed during the reaction.  相似文献   

6.
The effect of preparation method on the catalytic performance of V-promoted Ni/Al2O3 catalysts for synthetic natural gas (SNG) production via CO methanation has been investigated. The Ni-V/Al2O3 catalysts were prepared by co-impregnation (CI) method, deposition precipitation (DP) method as well as two sequential impregnation (SI) methods with different impregnation sequence. Among the prepared catalysts, the one prepared by CI method exhibited the best catalytic performance due to its largest H2 uptake and highest metallic Ni dispersion. In a 91h-lifetime test, this catalyst showed high stability at high temperature and weight hourly space velocity. This work demonstrates that the catalytic performance of the V-promoted Ni/Al2O3 catalysts can be improved by carefully controlling the preparation method/conditions.  相似文献   

7.
A series of Mn-promoted 15 wt-% Ni/Al2O3 catalysts were prepared by an incipient wetness impregnation method. The effect of the Mn content on the activity of the Ni/Al2O3 catalysts for CO2 methanation and the comethanation of CO and CO2 in a fixed-bed reactor was investigated. The catalysts were characterized by N2 physisorption, hydrogen temperature-programmed reduction and desorption, carbon dioxide temperature-programmed desorption, X-ray diffraction and highresolution transmission electron microscopy. The presence of Mn increased the number of CO2 adsorption sites and inhibited Ni particle agglomeration due to improved Ni dispersion and weakened interactions between the nickel species and the support. The Mn-promoted 15 wt-% Ni/Al2O3 catalysts had improved CO2 methanation activity especially at low temperatures (250 to 400 °C). The Mn content was varied from 0.86% to 2.54% and the best CO2 conversion was achieved with the 1.71Mn-Ni/Al2O3 catalyst. The co-methanation tests on the 1.71Mn-Ni/Al2O3 catalyst indicated that adding Mn markedly enhanced the CO2 methanation activity especially at low temperatures but it had little influence on the CO methanation performance. CO2 methanation was more sensitive to the reaction temperature and the space velocity than the CO methanation in the co-methanation process.
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8.
Two mesoporous material Ni/γ-Al2O3 catalysts were prepared and characterized by ICP-AES, XRD, and TPR. The differences in reaction activity between Ni-in-Al2O3 and Ni-on-Al2O3 were investigated for hydrotreating of crude 2-ethylhexanol. The results show that the Ni species (Ni-on-Al2O3) exhibit excellent hydrogenation activities at a wide range of H2 pressure and space velocity, while the Ni species (Ni-in-Al2O3) exhibit similar activities with those of Ni-on-Al2O3 only at higher H2 pressure and lower space velocity. Due to the presence of extensively exposed Ni species on the Ni-on-Al2O3 catalyst, its hydrogenation performance was increased significantly because of the low interphase mass transfer resistance.  相似文献   

9.
Properties of Pt0.5M0.5 nanopowders (M = Fe, Co, Ni) of alloys obtained via the decomposition of double complex salts [Pt(NH3)5Cl][Fe(C2O4)3] ? 4H2O, [Pt(NH3)4][Co(C2O4)2(H2O)2] ? 2H2O, and [Pt(NH3)4][Ni(C2O4)2(H2O)2] ? 2H2O, respectively, are studied in the reaction of preferential CO oxidation. It is shown that bimetallic Pt0.5M0.5 catalysts (M = Fe, Co, Ni) are much more active in the low temperature range than Pt nanopowder. The activity of the catalysts decreases in the order Pt0.5M0.5 ≥ Pt0.5M0.5 > Pt0.5M0.5 @ Pt. The higher activity of bimetallic Pt0.5M0.5 catalysts in the reaction of preferential CO oxidation in the low-temperature range under conditions of dense Pt surface coverage by adsorbed CO molecules is most likely caused by the activation of CO on Pt atoms, the activation of O2 on atoms of the second metal (Fe, Co, Ni), and the reaction that occurs at the sites of contact between the atoms of platinum and the atoms of the second metal on the surfaces of the alloy’s nanoparticles. The bimetallic systems investigated in this work can be used to improve catalysts of practically important preferential CO oxidation reaction. These systems have considerable potential in the afterburning reactions of CO and hydrocarbons; hydrogenation reactions; electrochemical reactions; and many others. The means used in the preparation of bimetallic nanopowders based on the decomposition of double complex salts is simple, does not require the use of expensive or complex reagents, and can be easily adapted to produce supported catalysts containing Pt0.5M0.5 metal alloys (M = Fe, Co, Ni).  相似文献   

10.
The concept of “waste-to-wealth” is spreading awareness to prevent global warming and recycle the restrictive resources. To contribute towards sustainable development, hydrogen energy is obtained from syngas (CO and H2) generated from waste gasification, followed by CO oxidation and CO2 removal. In H2 generation, it is key to produce more purified H2 from syngas using heterogeneous catalysts. In this respect, we prepared Pt/Al2O3 catalyst with nanoporous structure using precipitation method, and compared its catalytic activity with commercial alumina (Degussa). Based on the results of XRD and TEM, it was found that metal particles did not aggregate on the alumina surface and showed high dispersion. Optimum condition for CO conversion was 1.5 wt% Pt loaded on Al2O3 support, and pure hydrogen was obtained after removal of CO2 gas.  相似文献   

11.
In this paper, a novel multifunctional superamphiphobic coating for anticorrosion was successfully prepared on aluminum substrate via a simple spraying technique. Al2O3 nanoparticles were chemically grafted onto montmorillonite (MMT) nanosheets via coupling effect of NH2-C3H6-Si(OC2H5)3 (KH-550) and then modified by low surface energy material polydimethylsiloxane (PDMS). The ethylene tetrafluoroethylene (ETFE) composite coating with 25 wt% MMT/Al2O3-PDMS binary nanocomposite exhibited well-designed nano/μ structures and possessed superamphiphobicity with high contact angles towards water (164°), glycerol (158°) and ethylene glycol (155°). This coating demonstrated outstanding self-cleaning ability and strong adhesive ability (Grade 1 according to the GB/T 9286). The superhydrophobicity could be maintained after 8000 times abrasion or annealing treatment for 2 h under 350 °C. The coating still retained high water-repellence after immersion in 1 mol/L HCl (146°), 1 mol/L NaOH (144°) and 3.5 wt% NaCl (151°) solutions for 30 d. It should be noted that this superamphiphobic coating revealed excellent long-term corrosion protection with extremely low corrosion rate (4.3 × 10?3 μm/year) and high protection performance (99.999%) after 30 d immersion in 3.5 wt% NaCl solutions based on electrochemical corrosion measurements. It is believed that such integrated functional coating could pave new way for self-cleaning and anticorrosion applications under corrosive/abrasive environment.  相似文献   

12.
Hierarchical porous NiO/Al2O3 composites were successfully prepared by two-steps. First, the core-shell structured Al2O3 microspheres were prepared via a template-free hydrothermal route using KAl(SO4)2·12H2O and Al2(SO4)3·18H2O as aluminum source. Then, the NiO/Al2O3 composites with micro- and nano-hierarchical structures were prepared by a hydrothermal method combining the subsequent calcination process. The obtained characterization result presented that the morphology of hierarchical Al2O3 microsphere tuned to irregular platelets by simply varying Ni/Al ratios. The BET analysis showed that the special surface area from 52.12m2 g?1 to 214.8m2 g?1 after two hydrothermal complex process. Effects of Ni/Al ratio, adsorbent dosage, Congo red (CR) concentration, coexisting ions, adsorption time and temperature were investigated. The obtained results indicated that NiO/Al2O3 composite had the high adsorption efficiency (99.6%) and great adsorption capacity (186.9mg g?1) under the optimum conditions. The adsorption isotherm and kinetics data were found to be well fitted and in good agreement with the Langmuir isotherm model and pseudo-second order model, respectively. The hierarchical porous NiO/Al2O3 composites presented remarkably higher adsorption efficiency during five recycling, which showed their potential as the highly efficient adsorbent for removal of CR in wastewater.  相似文献   

13.
The novel half-titanocene catalyst bearing reactive functional amino group, η5-pentamethylcyclopentadienyltri(p-amino-phenoxyl) titanium [CpTi(p-OC6H4NH2)3], was easily synthesized by the reaction of η5-pentamethylcyclopentadienyltrichloride titanium (CpTiCl3) with p-amino phenol in the presence of triethyl amine (NEt3). CpTi(p-OC6H4NH2)3 covalently anchored on MgCl2/AlEtn(OEt)3-n support obtained from the reaction of triethylaluminium (AlEt3) with the adduct of magnesium chloride (MgCl2) and ethanol (EtOH), has been investigated and used to catalyze syndiospecific polymerization of styrene. Influences of the support structure, cocatalyst, and the molar ratio of Al in methylaluminoxane (MAO) and Ti (AlMAO/Ti) on catalytic activity, syndiotacticity and molecular weight of the resultant polystyrene were investigated. Compared with the corresponding CpTi(p-OC6H4NH2)3 homogeneous catalyst, a considerable increase in activity and molecular weight of syndiotactic polystyrene (sPS) was observed for the CpTi(p-OC6H4NH2)3-MgCl2/AlEtn(OEt)3-n supported catalyst even at a relatively low AlMAO/Ti ratio of 50, and the kinetics of polymerization was stable during the reaction process.  相似文献   

14.
We investigated the correlation between vanadium surface density and VOx structure species in the selective catalytic reduction of NOx by NH3. The properties of the VOx/TiO2 catalysts were investigated using physicochemical measurements, including BET, XRD, Raman spectroscopy, FE-TEM, UV-visible DRS, NH3-TPD, H2-TPR, O2-On/Off. Catalysts were prepared using the wet impregnation method by supporting 1.0-3.0 wt% vanadium on TiO2 thermally treated at various calcination temperatures. Through the above analysis, we found that VOx surface density was 3.4 VOx/nm2, and the optimal V loading amounts were 2.0-2.5 wt% and the specific surface area was 65-80m2/g. In addition, it was confirmed that the optimal VOx surface density and formation of vanadium structure species correlated with the reaction activity depending on the V loading amounts and the specific surface area size.  相似文献   

15.
The effect of La2O3 content in Ni-La-Zr catalyst was investigated for the autothermal reforming (ATR) of CH4. The catalysts were prepared by the coprecipitation method and had a mesoporous structure. Temperature programmed reduction (TPR) and X-ray photoelectron spectroscopy (XPS) indicated that a strong interaction developed between Ni species and the support with the addition of La2O3. Thermogravimetric analysis (TGA) and H2-pulse chemisorption showed that the addition of La2O3 led to well dispersed NiO molecules on the support. Ni-La-Zr catalysts gave much higher CH4 conversion than Ni-Zr catalyst. The Ni-La-Zr containing 3.2 wt% La2O3 showed the highest activity. The optimum conditions for maximal CH4 conversion and H2 yield were H2O/CH4=1.00, O2/CH4=0.75. Under these conditions, CH4 conversion of 83% was achieved at 700 °C. In excess O2 (O2/CH4>0.88), the catalytic activity was decreased due to sintering of the catalyst.  相似文献   

16.
Zeolite Mazzite (MAZ) analogue was synthesized directly using piperazine as a structure directing agent. The reactive gel composition used was (5.0–7.0) piperazine:(6.0–7.0) Na2O:Al2O3:20.0SiO2:400H2O. Using this composition, the reaction time was shortened greatly to 4 days and the crystallization time was reduced as well. The DTA data showed that piperazine, in as-synthesized zeolite omega decomposed easily. The decomposition of the piperazine occurred at 400–480°C. NH3-TPD analysis proved that zeolite H-omega from piperazine had strong surface acidity with ammonia desorption temperature up to 590°C.  相似文献   

17.
A new green chemical route was designed in this paper for the synthesis of high-silica EU-1 molecular sieve in TEAOH–SiO2–Al2O3–HMBr2–H2O system in which tetraethylammonium hydroxide (TEAOH) substituted for sodium hydroxide (NaOH) as an alkali source. The physicochemical properties of the synthesized samples characterized by such means as X-ray powder diffraction (XRD), electrophoresis apparatus, precise pH meter, scanning electron microscope, Fourier infrared spectrometer (FT-IR), thermo gravimetric analyzer (TG) and temperature programmed desorption (NH3-TPD). The research results showed that the SiO2/Al2O3 ratio of EU-1 molecular sieve could reach 706 with TEAOH as an alkali source. The SiO2/Al2O3 ratio of the product was improved greatly to 1046 with the template agent increasing. The new synthetic route has also significantly expanded the synthetic phase region. The absolute value of zeta potential of the TEAOH sol system was obviously higher than that of the NaOH sol system, indicating the thermodynamic stability of the former sol system was higher and better for the synthesis of pure high-silica EU-1 molecular sieve. The FT-IR spectra and TG/DTG diagrams of products indicated that TEA+ occluded in the final products could balance electronegative framework. The amount of strong, weak and the total acidity reduced with the increase of SiO2/Al2O3 ratio. The catalytic results of methanol-to-hydrocarbon demonstrated that the molecular sieve prepared by the new method has better catalytic performance.  相似文献   

18.
The formation of N2O has been studied by means of isothermal lean-rich experiments at 150, 180 and 250 °C over Pt–Ba/Al2O3 and Pt/Al2O3 catalysts with H2 and/or C3H6 as reductants. This allows to provide further insights on the mechanistic aspects of N2O formation and on the influence of the storage component. Both gas phase analysis and surface species studies by operando FT-IR spectroscopy were performed. N2O evolution is observed at both lean-to-rich (primary N2O) and rich-to-lean (secondary N2O) transitions. The production of both primary and secondary N2O decreases by increasing the temperature. The presence of Ba markedly decreases secondary N2O formation. FT-IR analysis shows the presence of adsorbed ammonia at the end of the rich phase only for Pt/Al2O3 catalyst. These results suggest that: (i) primary N2O is formed when undissociated NO in the gas phase and partially reduced metal sites are present; (ii) secondary N2O originates from reaction between adsorbed NH3 and residual NOx at the beginning of the lean phase. Moreover, N2O reduction was studied performing temperature programming temperature experiments with H2, NH3 and C3H6 as reducing agents. The reduction is completely selective to nitrogen and occurs at temperature higher than 250 °C in the case of Pt–Ba/Al2O3 catalyst, while lower temperatures are detected for Pt/Al2O3 catalyst. The reactivity order of the reductants is the same for the two catalysts, being hydrogen the more efficient and propylene the less one. Having H2 a high reactivity in the reduction of N2O, it could react with N2O when the regeneration front is developing. Moreover, also ammonia present downstream to the H2 front could react with N2O, even if the reaction with stored NOx seems more efficient.  相似文献   

19.
An Al2O3-ZrO2 xerogel (AZ-SG) was prepared by a sol-gel method for use as a support for a nickel catalyst. The Ni/AZ-SG catalyst was then prepared by an impregnation method, and was applied to hydrogen production by steam reforming of LNG. A nickel catalyst supported on commercial alumina (A-C) was also prepared (Ni/A-C) for comparison. The hydroxyl-rich surface of the AZ-SG support increased the dispersion of nickel species on the support during the calcination step. The formation of a surface nickel aluminate-like phase in the Ni/AZ-SG catalyst greatly enhanced the reducibility of the Ni/AZ-SG catalyst. The ZrO2 in the AZ-SG support increased the adsorption of steam onto the support and the subsequent spillover of steam from the support to the active nickel sites in the Ni/AZ-SG catalyst. Both the high surface area and the well-developed mesoporosity of the Ni/AZ-SG catalyst improved the gasification of adsorbed surface hydrocarbons in the reaction. In the steam reforming of LNG, the Ni/AZ-SG catalyst showed a better catalytic performance than the Ni/A-C catalyst. Moreover, the Ni/AZ-SG catalyst showed strong resistance toward catalyst deactivation.  相似文献   

20.
In this study, the influence of different weight percentages of alumina oxide (Al2O3) and silicon carbide (SiC) reinforcement on the mechanical properties of Polyamide (PA6) composite is investigated. Test specimens of pure PA6, 85 wt% PA6 + 10 wt% Al2O3 + 5 wt% SiC and 85 wt% PA6 +10 wt% SiC + 5 wt% Al2O3 are prepared using an injection molding machine. To investigate the mechanical behaviors tensile test, impact test, flexural test, and hardness test were conducted in accordance with ASTM standards. Experimental results indicated that the mechanical properties, such as tensile, impact, hardness, and flexural strength were considerably higher than the pure PA6. The tensile fracture morphology and the characterization of PA6 hybrid composites were observed by scanning electron microscope and Fourier transform infrared spectroscopic method. Further, thermogravimetric analysis confirms the thermal stability of PA6 hybrid composites. The reinforcing effects of Al2O3 and SiC on the mechanical properties of PA6 hybrid composites were compared and interpreted in this paper. Improved mechanical and thermal characteristics were observed by the addition of small amount of Al2O3 and SiC simultaneously reinforced with the pure PA6.  相似文献   

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