48 research outputs found

    Comparison of oxidizing agents for the oxidative coupling of methane over state-of-the-art catalysts

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    The synthesis of selected state-of-the-art catalysts providing high performances in the oxidative coupling of methane (OCM) with O2 was reproduced according to the respective recipes reported in literature. A reference material with identical stoichiometric composition was further synthesized by applying the cellulose templating method. This method increases the surface area and affects the phase composition and crystallite size of the catalysts as determined by N2-physisoprtion, X-ray diffraction and scanning electron microscopy. This, however, is in most cases detrimental to the catalytic OCM performance due to enhanced global activity resulting in hot spots in the catalyst bed. Catalysts were tested in the OCM under variation of temperature (973–1073 K), GHSV (3600–100,000 h−1) and oxidizing agent (O2 and N2O). In general, conversions of CH4 when using N2O are lower than in the presence of O2, however, the selectivities to C2 products ethane and ethylene are higher even at a similar level of CH4 conversion. This confirms the presence of different oxygen species formed by activation of these oxidizing agents

    Rhodium catalyzed hydrogenation reactions in aqueous micellar systems as green solvents

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    Dieser Beitrag ist mit Zustimmung des Rechteinhabers aufgrund einer (DFG geförderten) Allianz- bzw. Nationallizenz frei zugÀnglich.This publication is with permission of the rights owner freely accessible due to an Alliance licence and a national licence (funded by the DFG, German Research Foundation) respectively.The hydrogenation of itaconic acid and dimethyl itaconate is transferred from methanol to aqueous micellar solutions of several surfactants, e.g., SDS and Triton X-100, in order to facilitate the recovery of the catalyst. The reaction rate and selectivity strongly depends on the chosen surfactant and in some cases also on the surfactant concentration. In the best case the selectivity is the same as in methanol but the reaction rate is still lower because of a lower hydrogen solubility in water. Repetitive semi-batch experiments are chosen to demonstrate that high turn-over-numbers (>1000) can be reached in aqueous micellar solutions. No notable catalyst deactivation is observed in these experiments. The performance of micellar reaction systems is controlled by the partition coefficient of the substrates between the micelles and the continuous aqueous phase which can be predicted using the Conductor-like Screening Model for Real Solvents (COSMO-RS).DFG, EXC 314, Unifying Concepts in Catalysi

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