180 resultados para catalytic partial oxidation


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In our previous work, it was shown that LiLaNiO/gamma-Al2O3 was an excellent catalyst for partial oxidation of heptane to syngas in a fixed-bed reactor at high temperature and the selectivity of CO was about 93%. However, pure oxygen was used as the oxidant. We have developed a dense oxygen permeation membrane Ba0.5Sr0.5Co0.8Fe0.2O3 that can supply pure oxygen for the reaction. In this work, the membrane was combined with the catalyst LiLaNiO/gamma-Al2O3 in one rector for the partial oxidation of heptane that is typical component of gasoline. A good performance of the membrane reactor has been obtained, with 100% n-heptane conversion and >94% hydrogen selectivity at the optimized reaction conditions. (C) 2004 Elsevier B.V. All rights reserved.

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Partial oxidation of n-heptane (POH) for hydrogen generation was studied over several catalysts between 700 and 850degreesC. Modified Ni-based/gamma-Al2O3 catalyst exhibited not only good catalytic activity but also good carbon deposition resistance ability. Under the modified reaction conditions, 100% n-heptane conversion and 93% hydrogen selectivity can be obtained.

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The ignition processes for the catalytic partial oxidation of methane (POM) to synthesis gas over oxidic nickel catalyst (NiO/Al2O3), reduced nickel catalyst (Ni-0/Al2O3), and Pt-promoted oxidic nickel catalyst (Pt-NiO/Al2O3) were studied by the temperature-programmed surface reaction (TPSR) technique. The complete oxidation of methane usually took place on the NiO catalyst during the CH4/O-2 reaction, even with a pre-reduced nickel catalyst, and Ni-0 is inevitably first oxidized to NiO if the temperature is below the ignition temperature. It is above a certain temperature that Ni-0 is formed again, which leads to the start of the POM. The POM can be initiated at a much lower temperature on a Pt-NiO catalyst because of Pt promotion of the reduction of NiO. The POM in a fluidized bed can be easily initiated due to the addition of Pt.

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The deposition of carbon on catalysts during the partial oxidation of methane to syngas has been investigated in a fluidized bed. It was found that the relative rate of carbon deposition follows the order NiP > >d > Pt, Rh. Although the rate of carbon deposition in the fluidized bed was much lower than that in the fixed bed, carbon deposition could still be detected in the fluidized bed if a CH4/O-2 ratio in greater than 2.3 was used.

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Gas phase partial oxidation of toluene over V/Ti oxide catalysts has been successfully performed in a microchannel reactor, which provides very good mass and heat transfer conditions. With the elimination of hot spots, which are known as the most negative factors for partial oxidation of hydrocarbons, steady and uniform reaction conditions can be achieved in the catalyst bed by using, the microreactor. Since the best performance of the catalysts might be exploited, the selectivity of partial oxidation products of toluene has remarkably increased compared to the traditional packed fixed-bed reactor, even without the bother of modifying the catalysts, diluting the reactants or catalysts with inert contents to avoid hot spots or improve the diffusion and mixing. Furthermore, in virtue of its inherent safety features, when using pure oxygen as oxidant, the reactions were handled safety within the explosion limits in the microreactor. With TiO2 carried V2O5 as catalysts, the total selectivity of benzaldehyde and benzoic acid reaches around 60%, and the toluene conversion is about 10%. The conversion can go up without violent decline of selectivity, unlike most fixed bed reactors. Space time yield of 3.12 kg h(-1) L-1 calculated on the basis of the channel volume has been achieved. The influence of operating conditions has been investigated in detail in the microreactor. (c) 2005 Elsevier B.V. All rights reserved.

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The catalytic partial oxidation of methane to syngas over Ni/Al2O3, Pt/Al2O3 and a series of Pt - Ni/Al2O3 catalysts was investigated. It was found that Pt - Ni/Al2O3 catalysts exhibit higher activity and stability than Ni/Al2O3 and Pt/Al2O3. TPR and TPD methods were used to characterize Pt - Ni bimetallic interactions in the catalysts. A series of Pt - Ni/Al2O3 catalysts and unsupported Pt - Ni samples were studied by XRD and XPS. It was found the formation of Pt - Ni alloy in the Pt - Ni/Al2O3 catalysts and the enrichment of platinum on the surface of the catalysts. It is concluded that the higher activity and stability of Pt - Ni/Al2O3 catalysts were caused by Pt - Ni bimetallic interactions.

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The catalytic oxidation of methane to syngas has been carried out over Pt/Al2O3 and Pt/CeO2/Al2O3. It was found that the catalysts with ceria exhibit a higher activity and selectivity than those without ceria. The catalysts were characterized by means of TPR, TPD, SEM-EDX and XRD. There is a strong interaction between ceria and platinum under the reaction condition, which increase the dispersion of platinum over catalysts, preventing the sinter of the Pt particles. As a result of the synergistic;effect between Pt and ceria, the activity of Pt/Al2O3 for combustion reaction was suppressed, the activity and selectivity :For partial oxidation were improved greatly. Another role of ceria in the catalyst is the enhancing of the WGSR, which leads to the increase of the selectivity of catalyst for hydrogen and accelerating the equilibrium of the reaction.

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An in-situ modified sol-gel method for the preparation of a Ni-based monolith-supported catalyst is reported. With the presence of a proper amount of plasticizer and binder, and at an optimized pH value, the stable boehmite sol was modified with metal ions (Ni, Li, La) successfully without distinct growth of the particle size. Monolith-supported Ni-based/gamma-Al2O3 catalysts were obtained using the modified sol as the coating medium with several cycles of dip-coating and calcination. Combined BET, SEM-EDS, XRD and H-2-TPR investigations demonstrated that the derived monolith catalysts had a high specific surface area, a relatively homogeneous surface composition, and a high extent of interaction between the active component and the support. These catalysts showed relatively stable catalytic activities for partial oxidation of methane (POM) to syngas under atmospheric pressure. The monolith catalysts prepared by this sol-gel method also demonstrated an improved resistance to sintering and loss of the active component during the reaction process.

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A novel and ideal dense catalytic membrane reactor for the reaction of partial oxidation of methane to syngas (POM) was constructed from the stable mixed conducting perovskite material of BaCo0.4Fe0.4Zr0.2O3-delta and the catalyst of LiLaNiO/gamma-Al2O3. The POM reaction was performed successfully. Not only was a short induction period of 2 h obtained, but also a high catalytic performance of 96-98% CH4 conversion, 98-99% CO selectivity and an oxygen permeation flux of 5.4-5.8 ml cm(-2) min(-1) (1.9-2.) mumol m(-2) S-1 Pa-1) at 850 degreesC were achieved. Moreover, the reaction has been steadily carried out for more than 2200 h, and no interaction between the membrane material and the catalyst took place.

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The catalytic activity, thermal stability and carbon deposition of various modified NiO/gamma-Al2O3 and unmodified NiO/gamma-Al2O3 catalysts were investigated with a flow reactor, XRD, TG and UVRRS analysis. The activity and selectivity of the NiO/gamma-Al2O3 catalyst showed little difference from those of the modified nickel-based catalysts. However, modification with alkali metal oxide (Li, Na, K) and rare earth metal oxide (La, Ce, Y, Sm) can improve the thermal stability of the NiO/gamma-Al2O3 and enhance its ability to suppress carbon deposition during the partial oxidation of ethane (POE). The carbon deposition contains graphite-like species that were detected by UVRRS. The nickel-based catalysts modified by alkali metal oxide and rare earth metal oxide have excellent catalytic activities (C2H6 conversion of similar to 100%, CO selectivity of similar to 94%, 7x 10(4) l/(kg h), 1123 K), good thermal stability and carbon-deposition resistance.