985 resultados para Catalysis.


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The role of acid strength of zeolites in liquid-phase alkylation of benzene with ethylene was studied over beta, MCM-22, and USY zeolites by means of adsorbing NH3 at different temperatures. The strong acid sites are active centers, while the weak acid sites are inactive. The selectivity behavior of the strong acid sites varies with the relative acid strength as well as the types of the zeolites.

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A comparison of methane dehydroaromatization (MDA) on 6Mo/MCM-22 and 6Mo/ZSM-5 was carried out using a gas mixture of 90%CH4, 2%CO2 and 8%Ar as the feed. The results indicate that the stability of 6Mo/MCM-22 is better than that of 6Mo/ZSM-5. A detailed study reveals that the ability for coke accommodation and the retention of the shape selectivity for aromatics formation is responsible for the stability of a MDA catalyst.

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The transformation of olefin to aromatics over ZSM-5 catalysts with different K-loadings has been investigated both in a continuous flow fixed-bed reactor and in a pulse microreactor. Investigation of variation of olefin aromatization activity with K-loadings shows that strong acid sites are indispensable for the converting of olefin to aromatics. As intermediates of olefin aromatization process, butadiene and cyclopentene not only show much higher aromatization activity than mono-olefins, but also can be transformed into aromatics over relatively weak acid sites of K/ZSM-5. A proposal is put forward, stating that among all the steps experienced in olefins aromatization, the formation of diene or cycloolfin from mono-olefins through hydrogen transfer is the key step and can be catalyzed by strong acid sites.

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The effect of space velocity on reaction performance and coke deposition over 6Mo/MCM-22 catalyst in methane dehydro-aromatization (MDA) with CO2 were studied. The characterization of catalysts reacted at different space velocity after the same amount of methane feed by TG, TPO and Benzene/NH3-TPD techniques suggested that the inert coke maybe responsible for the deactivation of catalyst because of its blockage effect for pore system.

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The reaction performance for CO hydration on a TiO2 catalyst under different calcination temperatures was investigated. Under reaction conditions of T = 573 K, P = 0.5 MPa, CO flow rate of 30 ml min(-1), TOS = 12 h, and CO/H2O (g) = 3/2 (mol), the TiO2 catalyst with a futile content of 18% shows a maximum alcohols STY of 1.81 Mg m(-2) h(-1). In addition, the catalyst deactivation and regeneration were discussed.

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The oxidative dehydrogenation of ethane (ODE) with CO2 to C2H4 has been studied over a series of Cr-based catalysts using SiO2, Al2O3, (MCM-41 zeolite) MCM-41, MgO and Silicate-2 (Si-2) as the supports. TPR, NH3-TPD, and EPR characterizations of catalysts were carried out to investigate the reduction property of Cr species on different supports, the acidities of catalysts and Cr species of 6Cr/SiO2 catalysts, respectively.

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ZrO2-A and ZrO2-B catalysts were prepared by two different coprecipitation methods and their performance of CO hydrogenation was studied. The results indicated that ZrO2 and Li-, Pd- and Mn-modified ZrO2 catalysts exhibited good selectivity and high STY to higher alcohols. The surface characteristics of ZrO2-A and ZrO2-B samples were investigated by means of BET, NH3-TPD, XRD and UV Raman technique. The tetragonal zirconia on the surface region of ZrO2-A and Li-Pd-Mn/ZrO2-A catalysts may be responsible for the high selectivity towards ethanol, while the monoclinic zirconia on the surface of ZrO2-B and Li-Pd-Mn/ZrO2-B catalysts may be crucial to the high isobutanol selectivity.

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Colloidal alumina was used to improve the activity of an In/HZSM-5 catalyst for the selective reduction of NO with CH4 in the excess of oxygen. Compared with In/HZSM-5, the In/HZSM-5/Al2O3 catalyst showed higher activity in a wide range of reaction temperatures. It is visualized that a synergetic effect between In/HZSM-5 and Al2O3 enhances the conversion of NOx. The addition of Al2O3 improved the conversion of NO to NO2 and facilitated the activation of methane. An In/HZSM-5/Al2O3 pre-treated with steam for 15 h at 700 degreesC still showed a high activity for the removal of NOx with methane, while an In/HZSM-5 similarly pre-treated with steam showed a lower activity than the fresh sample. The activity of the In/HZSM-5/Al2O3 catalyst could be restored completely after water vapor was removed from the feed gas. Furthermore, it was found that the In/HZSM-5/Al2O3 remained fairly active under high GHSV and O-2 concentration conditions. It was also interesting to find that an increase in NO content could enhance the conversion of methane, and this illustrates that the existence of NO is beneficial for the activation of methane. (C) 2002 Elsevier Science B.V. All rights reserved.

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The reduction of NO with CO in the presence of excess oxygen was investigated over different noble metal catalysts for probing the relationship between catalytic properties and adsorption behaviors. Among the four precious metal catalysts investigated, Ir/ZSM-5 was found to be the only active one for NO reduction with CO under lean conditions. With the decreasing of the Ir content, higher NO conversion and CO selectivity was obtained. Temperature-programmed reaction (TPR) studies of NO/H-2/O-2 and NO/CO/O-2 showed that the Pt/ZSM-5 was active when H-2 was used as the reductant, whereas, the Ir/ZSM-5 was active when CO was the reducing agent. This difference is due to the different mechanisms of the two reactions. Temperature-programmed desorption (TPD) of NO, CO and O-2 showed that NO could dissociate more easily over the Ir/ZSM-5 than on the Pt/ZSM-5, while the oxidation of CO by O-2 proceeded more rapidly on the Pt/ZSM-5 than on the Ir/ZSM-5. The presence of excess O-2 inhibited drastically the dissociation of NO, which is considered as the key step for the NO-CO reaction. The high dissociation rate of NO over the Ir/ZSM-5 is visualized as the key factor for its superior high activity in NO reduction with CO under lean conditions. (C) 2002 Elsevier Science B.V. All rights reserved.

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The reduction of NO by CH4 in the presence of excess O-2 over Co/HZSM-5, Ni/HZSM-5 and Mn/HZSM-5 catalysts with microwave heating was studied. By comparing the activities of the catalysts in the microwave heating mode with that in the conventional reaction mode, it was demonstrated that microwave heating could greatly reduce the reaction temperature, and could clearly expand the temperature window of the catalysts. Especially for the Co/HZSM-5 catalyst, the maximum conversion of NO to N-2 in the conventional reaction mode was consistent with that in the microwave heating mode. However, the temperature window for the maximum conversion in the microwave heating mode was from 260 to 360degreesC instead of a temperature of 420degreesC in the conventional reaction mode. The results suggest that microwave heating has a novel effect in the reduction of NO.