Partial oxidation of methane over the perovskite oxides

Ba0.5Sr0.5Co0.8Fe0.2O3-delta and Ba0.5Sr0.5Co0.8Ti0.2O3-delta oxides were synthesized by a combined EDTA-citrate complexing method. The catalytic behavior of these two oxides with the perovskite structure was studied during the reaction of methane oxidation. The pre-treatment with methane has different effect on the catalytic activities of both the oxides. The methane pre-treatment has not resulted in the change of the catalytic activity of BSCFO owing to its excellent reversibility of the perovskite structure resulting from the excellent synergistic interaction between Co and Fe in the oxide. However, the substitution with Ti on Fe-site in the lattice makes the methane pre-treatment have an obvious influence on the activity of the formed BSCTO oxide.

A novel process for converting coalmine-drained methane gas to syngas over nickel-magnesia solid solution catalysts

A novel process is developed in this paper for utilizing the coalmine-drained methane gas that is usually vented straight into the atmosphere in most coalmines worldwide. It is expected that low-cost syngas can be produced by the combined air partial oxidation and CO2 reforming of methane, because this process utilizes directly the methane, air, and carbon dioxide in the coalmine-drained gas without going through the separation step. For this purpose, a nickel-magnesia solid solution catalyst was prepared and its catalytic performance for the proposed process was investigated. It was found that calcination temperature has significant influence on the catalytic performance due to the different extent of solid solution formation in the catalysts. A uniform nickel-magnesia solid solution catalyst exhibits higher stability than the catalysts in which NiO has not completely formed solid solution with MgO. Its catalytic activity and selectivity remain stable during 120 h of reaction. The product H-2/CO ratio is mainly dependent on the feed gas composition. By changing CO2/air ratio of the feed gases, syngas with a H-2/CO ratio between 1 and 1.9 can be obtained. The influences of reaction temperature and nickel loading on the catalytic performance were also investigated. (c) 2004 Elsevier B.V All rights reserved.

High-throughput screening of HZSM-5 supported metal-oxides catalysts for the coupling of methane with CO to benzene and naphthalene

High-throughput screening of HZSM-5 supported metal-oxides catalysts were carried out for the coupling reaction of methane with CO to aromatics in a multi-stream reactor system. Zn/HZSM-5 and Mo/HZSM-5 were observed to be rather effective for the catalytic formation of aromatics from the coupling reaction of methane with CO. Temperature-programmed reaction has further proven the efficiency of the coupling of methane and CO over Zn/HZSM-5 catalyst. The results were also validated in a conventional fixed-bed reactor coupled with GC. The results propose that the coupling methane with CO toward benzene and naphthalene can be catalyzed by Zn/HZSM-5 at 500 ° C. Both methane and CO are needed for the formation of reactive coke on the catalyst, and the reactive coke may be the initial product in the producing of hydrocarbons. © 2005 Elsevier B.V. All rights reserved.

Combined single-pass conversion of methane via oxidative coupling and dehydro-aromatization

A single-pass process with the combination of oxidative coupling (OCM) and dehydro-aromatization (MDA) for the direct conversion of methane is carried out. With the assistance of the OCM reaction over the SrO-La2O3/CaO catalyst loaded on top of the catalyst bed, the duration of the dehydro-aromatization reaction catalyzed by a 6Mo/HMCM-49 catalyst shows a significant improvement, and. the initial deactivation rate constant of the overall process revealed about 1.5 x 10(-6) s(-1). Up to 72 h on stream, the yield of aromatics was still maintained at 5.0% with a methane conversion of 9.6%, which is obviously higher than that reported for the conventional MDA process with single catalyst. Upon the TPR results, this wonderful enhancement would be attributed to an in-situ formation of CO2 and H2O through the OCM reaction, which serves as a scavenger for actively removing the coke formed during the MDA reaction via a reverse Boudouard reaction and the water gas reaction as well.

The synergic effect between Mo species and acid sites in Mo/HMCM-22 catalysts for methane aromatization

The acid properties of Mo/HMCM-22 catalyst, which is the precursor form of the working catalyst for methane aromatization reaction, and the synergic effect between Mo species and acid sites were studied and characterized by various characterization techniques. It is concluded that Bronsted and Lewis acidities of HMCM-22 are modified due to the introduction of molybdenum. We suggest a monomer of Mo species is formed by the exchange of Mo species with the Bronsted acid sites. On the other hand, coordinate unsaturated sites (CUS) are suggested to be responsible for the formation of newly detected Lewis acid sites. Computer modelling is established and coupling with experimental results, it is then speculated that the effective activation of methane is properly accomplished on Mo species accommodated in the 12 MR supercages of MCM-22 zeolite whereas the Bronsted acid sites in the same channel system play a key role for the formation of benzene. A much more pronounced volcano-typed reactivity curve of the Mo/HMCM-22 catalysts, as compared with that of the Mo/HZSM-5, with respect to Mo loading is found and this can be well understood due to the unique channel structure of MCM-22 zeolite and synergic effect between Mo species and acid sites.