Reduction of NO by CH4 with microwave heating

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.

Gasoline-range hydrocarbon synthesis over cobalt-based Fischer-Tropsch catalysts supported onSiO2/HZSM-5

Two types of SiO2 with different mesopore size and HZSM-5 zeolite were used to prepare hybrid supported cobalt-based catalysts. The textual and structural properties of the catalysts were studied using N-2 physisorption, X-ray diffraction (XRD), and H-2 temperature-programmed reduction (TPR) techniques. Fischer-Tropsch synthesis (FTS) performances of the catalysts were carried out in a fixed-bed reactor. The combination effects of the meso- and micropores of the supports as well as the interaction between supports and cobalt particles on FTS activity are discussed. The results indicate that the catalyst supported on the tailor-made SiO2 and HZSM-5 hybrid maintained both meso- and micropore pores during the preparation process without HZSM-5 particles agglomerating. The mesopores provided quick mass transfer channels, while the micropores contributed to high metal dispersion and accelerated hydrocracking/hydroisomerization reaction rate. High CO conversion of 83.9% and selectivity to gasoline-range hydrocarbons (C-5-C-12) of 55%, including more than 10% isoparaffins, were achieved simultaneously on this type of catalyst.

Methane dehydroaromatization over Mo/HZSM-5 catalysts: The reactivity of MoCx species formed from MoOx associated and non-associated with Bronsted acid sites

The catalytic performances of methane dehydroaromatization (MDA) under non-oxidative conditions over 6 wt.% Mo/HZSM-5 catalysts calcined for different durations of time at 773 K have been investigated in combination with ex situ H-1 MAS NMR characterization. Prolongation of the calcination time at 773 K is in favor of the diffusion of the Mo species on the external surface and the migration of Mo species into the channels, resulting in a further decrease in the number of Bronsted acid sites, while causing only a slight change in the Mo contents of the bulk and in the framework structure of the HZSM-5 zeolite. The MoQ(x) species associated and non-associated with the Bronsted acid sites can be estimated quantitatively based on the 1H MAS NMR measurements as well as on the assumption of a stoichiometry ratio of 1: 1 between the Mo species and the Bronsted acid sites. Calcining the 6 wt.% Mo/HZSM-5 catalyst at 773 K for 18 h can cause the MoOx species to associate with the Bronsted acid sites, while a 6 Wt-% MO/SiO2 sample can be taken as a catalyst in which all MoOx species are non-associated with the Bronsted acid sites. The TOF data at different times on stream on the 6 wt.% Mo/HZSM-5 catalyst calcined at 773 K for 18 h and on the 6 Wt-% MO/SiO2 catalyst reveal that the MoCx species formed from MoOx associated with the Bronsted acid sites are more active and stable than those formed from MoOx non-associated with the Bronsted acid sites. An analysis of the TPO profiles recorded on the used 6 wt.% Mo/HZSM-5 catalysts calcined for different durations of time combined with the TGA measurements also reveals that the more of the MoCx species formed from MoOx species associated with the Br6nsted acid sites, the lower the amount of coke that will be deposited on it. The decrease of the coke amount is mainly due to a decrease in the coke burnt-off at high temperature. (c) 2005 Elsevier B.V. All rights reserved.

Effect of Ru addition to CO/SiO2/HZSM-5 catalysts on Fischer-Tropsch synthesis of gasoline-range hydrocarbons

Microporous HZSM-5 zeolite and mesoporous SiO2 supported Ru-Co catalysts of various Ru adding amounts were prepared and evaluated for Fischer-Tropsch synthesis (FTS) of gasoline-range hydrocarbons (C-5-C-12). The tailor-made Ru-Co/SiO2/HZSM-5 catalysts possessed both micro- and mesopores, which accelerated hydrocracking/hydroisomerization of long-chain products and provided quick mass transfer channels respectively during FTS. In the same time. Ru increased Cor reduction degree by hydrogen spillover, thus CO conversion of 62.8% and gasoline-range hydrocarbon selectivity of 47%, including more than 14% isoparaffins, were achieved simultaneously when Ru content was optimized at 1 wt% in Ru-Co/SiO2/HZSM-5 catalyst.

Post-steam-treatment of Mo/HZSM-5 catalysts: An alternative and effective approach for enhancing their catalytic performances of methane dehydroaromatization

Post-steam-treatment is a facile and effective method for improving the catalytic performances of Mo/HZSM-5 catalysts in methane dehydroaromatization under nonoxidative conditions. The treatment can enhance the stability of the catalyst and also give a higher methane conversion and a higher yield of light aromatics, as well as a decrease in the formation rate of carbonaceous deposits. (27)Al, (29)Si, and (1)H multinuclear magic angle spinning nuclear magnetic resonance, X-ray photoelectron spectroscopy, X-ray diffraction, X-ray fluorescence spectroscopy, and thermogravimetric analysis measurements as well as catalytic reaction evaluations were employed to conduct comparative studies on the properties of the catalysts before and after the post-steam-treatment. The results revealed that the number of free Bronsted acid sites per unit cell decreased, while more Mo species migrated into the HZSM-5 channels for the 6Mo/HZSM-5 catalysts after the post-steam-treatment. In addition, the average pore diameter was also larger for the post-steam-treated catalysts, and this was advantageous for mass transport of the reaction products. However, a severe post-steam-treatment, i.e., with longer treating time, of the 6Mo/HZSM-5 catalyst will lead to the formation of the Al(2)(MoO(4))(3) phases, which is detrimental to the reaction.

A Mossbauer study of In-Fe2O3/HZSM-5 catalysts for the selective catalytic reduction of NO by methane

The selective catalytic reduction of NO by CH4 was compared over In-Fe2O3/HZSM-5 catalysts prepared by impregnation and co-impregnation methods. It was found that the catalyst preparation method greatly affected the catalyst activity. The impregnated catalyst was very active, but the co-impregnated one showed poor activity. The In Fe2O3/HZSM-5 catalysts were investigated by Mossbauer spectroscopy. The results showed that indium cations entered into the iron oxide lattice in the co-impregnated catalyst, while the impregnated catalyst exhibited a more stable structure, when both of the catalysts were treated severely in the reaction atmosphere. Characterization by means of combined in situ temperature programmed reduction (TPR)- Mossbauer spectroscopy further revealed that the performances of the two catalysts were different in the TPR processes.