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Highly Selective Supported Alkali Chloride Catalysts for the Oxidative Dehydrogenation of Ethane

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Abstract

Binary, ternary and quaternary molten eutectic alkali chloride catalysts, supported on mildly redox active oxides, were investigated for the oxidative dehydrogenation of ethane. The influence of different support oxides, on the catalytic performance, as well as that of different anions (bromide vs. chloride) and cations in a chloride eutectic system were studied. Metal oxides which react with chlorides are not suitable and lead to substantial deactivation. Especially supports forming volatile chlorides induce irreversible chloride depletion. Bromides catalyze oxidative dehydrogenation of ethane with higher rates, but lower olefin selectivities, highlighting the similarities and differences of Cl− and Br− in the redox cycle. Two catalysts were identified having olefin selectivities up to 98 % at 70 % ethane conversion, which ranges among the highest selectivities reported for ethane ODH.

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Acknowledgments

The authors gratefully acknowledge SOLVAY for financial support to conduct this work. We especially thank Dr. Armin Liebens, Dr. Marco Piccinini and Dr. Paul Degraeve, SOLVAY, as well as Prof. Andreas Jentys, TUM and Prof. Angeliki Lemonidou, Aristotle University Thessaloniki for fruitful discussions. We further thank Johannes Simböck, Sabine Frischhut, Katharina Freitag, Michael Eckbauer and Thomas Bartesch for assistance with experiments. We are also grateful to Xaver Hecht for BET and Martin Neukamm for AAS measurements. C. G. thanks the TUM Graduate School and the Graduate Center Chemistry for support.

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  1. Department Chemie and Catalysis Research Center, Technische Universität München, Lichtenbergstr. 4, 85747, Garching, Germany

    Christian A. Gärtner, Andre C. van Veen & Johannes A. Lercher

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  1. Christian A. Gärtner
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  2. Andre C. van Veen
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  3. Johannes A. Lercher
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Correspondence to Johannes A. Lercher.

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Gärtner, C.A., van Veen, A.C. & Lercher, J.A. Highly Selective Supported Alkali Chloride Catalysts for the Oxidative Dehydrogenation of Ethane. Top Catal 57, 1236–1247 (2014). https://doi.org/10.1007/s11244-014-0277-5

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