3 resultados para catalytic partial oxidation of methane


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Gas-to-liquid processes are generally used to convert natural gas or other gaseous hydrocarbons into liquid fuels via an intermediate syngas stream. This includes the production of liquid fuels from biomass-derived sources such as biogas. For example, the dry reforming of methane is done by reacting CH4 and CO2, the two main components of natural biogas, into more valuable products, i.e., CO and H2. Nickel containing perovskite type catalysts can promote this reaction, yielding good conversions and selectivities; however, they are prone to coke laydown under certain operating conditions. We investigated the addition of high oxygen mobility dopants such as CeO2, ZrO2, or YSZ to reduce carbon laydown, particularly using reaction conditions that normally result in rapid coking. While doping with YSZ, YDC, GDC, and SDC did not result in any improvement, we show that a Ni perovskite catalyst (Na0.5La0.5Ni0.3Al0.7O2.5) doped with 80.9 ZrO2 15.2 CeO2 gave the lowest amount of carbon formation at 800 °C and activity was maintained over the operating time.

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The initial rate of the photocatalysed oxidation of methylene blue, MB, by dissolved oxygen in solution, ri(MB), is measured for a series of titania on glass samples exhibiting a wide range of activities.  The samples used include two different types of commercial self-cleaning glass and a lab-made sol-geltitania film.  The activities of these samples are also assessed using a resazurin-based photocatalyst activity indicator ink, i.e. Rz paii, for which the initial rates of the photocatalysed reduction of Rz were measured, ri(Rz).  A plot of ri(MB)vs. ri(Rz) reveals a goodstraight line, thereby demonstrating a linear correlation (for TiO2films on glass at least) between the slow (usually hours) photocatalysed oxidation of organic materials, such as MB, and the fast (typically minutes) photocatalysed irreversible reduction of a dye, like Rz, in a paii.  The possible use of paii technology for assessing, in a simple, quick and inexpensive manner, photocatalytic films both in the laboratory and in situ is discussed briefly.  

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Baeyer–Villiger oxidation of cyclic ketones, using H2O2 as the oxidising agent, was systematically studied using a range of metal chlorides in different solvents, and in neat chlorogallate(III) ionic liquids. The extremely high activity of GaCl3 in promoting oxidation with H2O2, irrespective of solvent, was reported for the first time. The activity of all other metal chlorides was strongly solvent-dependent. In particular, AlCl3 was very active in a protic solvent (ethanol), and tin chlorides, SnCl4 and SnCl2, were active in aprotic solvents (toluene and dioxane). In order to eliminate the need for volatile organic solvent, a Lewis acidic chlorogallate(III) ionic liquid was used in the place of GaCl3, which afforded typically 89–94% yields of lactones in 1–120 min, at ambient conditions. Raman and 71Ga NMR spectroscopic studies suggest that the active species, in both GaCl3 and chlorogallate(III) ionic liquid systems, are chlorohydroxygallate(III) anions, [GaCl3OH]−, which are the products of partial hydrolysis of GaCl3 and chlorogallate(III) anions; therefore, the presence of water is crucial.