Partial oxidation of ethane to syngas in an oxygen-permeable membrane reactor

A perovskite-type oxide of Ba0.5Sr0.5Co0.8Fe0.2O3-delta (BSCFO) with mixed electronic and oxygen ionic conductivity at high temperatures was used as an oxygen-permeable membrane. A tubular membrane of BSCFO made by extrusion method has been used in the membrane reactor to exclusively transport oxygen for the partial oxidation of ethane (POE) to syngas with catalyst of LiLaNiO/gamma-Al2O3 at temperatures of 800-900 degreesC. After only 30 min POE reaction in the membrane reactor, the oxygen permeation flux reached at 8.2 ml cm(-2) min(-1). After that, the oxygen permeation flux increased slowly and it took 12 h to reach at 11.0 ml cm(-2) min(-1). SEM and EDS analysis showed that Sr and Ba segregations occurred on the used membrane surface exposed to air while Co slightly enriched on the membrane surface exposed to ethane. The oxygen permeation flux increased with increasing of concentration of C2H6, which was attributed to increasing of the driving force resulting from the more reducing conditions produced with an increase of concentration of C2H6 in the feed gas. The tubular membrane reactor was successfully operated for POE reaction at 875 degreesC for more than 100 h without failure, with ethane conversion of similar to 100%, CO selectivity of >91% and oxygen permeation fluxes of 10-11 ml cm(-2) min(-1). (C) 2002 Elsevier Science B.V. All rights reserved.

Partial oxidation of ethane to syngas over nickel-based catalysts modified by alkali metal oxide and rare earth metal oxide

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.

Development and application of oxygen permeable membrane in selective oxidation of light alkanes

In this paper, oxygen permeable membrane used in membrane reactor for selective oxidation of alkanes will be discussed in detail. The recent developments for the membrane materials will be presented, and the strategy for the selection of the membrane materials will be outlined. The main applications of oxygen permeable membrane in selective oxidation of light alkanes will be summarized, which includes partial oxidation of methane (POM) to syngas and partial oxidation of heptane (POH) to produce H-2, oxidative coupling of methane (OCM) to C-2, oxidative dehydrogenation of ethane (ODE) to ethylene and oxidative dehydrogenation of propane (ODP) to propylene. Achievements for the membrane material developments and selective oxidation of light alkanes in membrane reactor in our group are highlighted.

Gas phase catalytic partial oxidation of toluene in a microchannel reactor

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.

On the reactivity of Mo species for methane partial oxidation on Mo/HMCM-22 catalysts

By characterizing fresh and used Mo/HMCM-22 catalysts with ICP-AES, XRD, NH3-TPD technique, UV - Vis DRS and UV Raman spectroscopy, the reactivity of Mo species for methane partial oxidation into formaldehyde were directly studied with a new point of view. By comparing the fresh and used catalysts, it was found that the tetrahedral Mo species bonding chemically to the support surface were practically unchanged after the reaction, while the polymolybdate octahedral Mo species, which had a rather weak interaction with the MCM-22 zeolite, leached out during the reaction, especially when the Mo loading was high. Correspondingly, it was found from the time-on-stream reaction data that the HCHO yield remained unchanged, while COx decreased with the reaction time during the reaction. By combining the characterization results and the reaction data, it can be drawn that the isolated tetrahedral molybdenum oxo-species (T-d) is responsible for HCHO formation, while the octahedral polyoxomolybdate species (O-h) will lead to the total oxidation of methane.