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    1) New catalysts using ionic liquids were developed for selectively hydrogenating acetylene in ethylene production. 2) Pd-Ag shell catalysts were impregnated with different ionic liquids and tested under industrial tail-end conditions. 3) The results showed that ionic liquid loadings decreased acetylene conversion by an order of magnitude while increasing ethylene selectivity for low Ag shell catalysts and decreasing undesirable C4 hydrocarbon selectivity for high Ag catalysts.

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    New Catalysts for Selective Hydrogenation of Acetylene

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    New Catalysts for Selective Hydrogenation of Acetylene

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    1) New catalysts using ionic liquids were developed for selectively hydrogenating acetylene in ethylene production. 2) Pd-Ag shell catalysts were impregnated with different ionic liquids and tested under industrial tail-end conditions. 3) The results showed that ionic liquid loadings decreased acetylene conversion by an order of magnitude while increasing ethylene selectivity for low Ag shell catalysts and decreasing undesirable C4 hydrocarbon selectivity for high Ag catalysts.

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    New Catalysts For Selective Hydrogenation of Acetylene

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    1) New catalysts using ionic liquids were developed for selectively hydrogenating acetylene in ethylene production. 2) Pd-Ag shell catalysts were impregnated with different ionic liquids and tested under industrial tail-end conditions. 3) The results showed that ionic liquid loadings decreased acetylene conversion by an order of magnitude while increasing ethylene selectivity for low Ag shell catalysts and decreasing undesirable C4 hydrocarbon selectivity for high Ag catalysts.

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    New catalysts for selective hydrogenation of acetylene: SCILL type systems

    T. Herrmann, L. Rmann, M. Lucas, P. Claus Ernst-Berl-Institute/Technical Chemistry II TU Darmstadt, Petersenstrae 20, 64287 Darmstadt, Germany

    Introduction Ethylene is worldwide one of the most important petrochemicals: its production exceeded 100106 t/a in 2008[1] and it is primarily used as a chemical building block for the production of plastics. Ethylene itself is mainly produced by thermal cracking of naphtha and the so obtained C2-cut contains trace impurities of acetylene which poisons the downstream polymerization catalysts. In commercial ethylene plants acetylene is removed by selective hydrogenation on Pd based catalysts. Ideally, this only leads to ethylene but in practice the formation of ethane and byproducts also occur. Rapid deactivation of the catalysts due to the formation of green oils, which partially cover the catalyst surface, therefore, still remains one of the main drawbacks in tail-end hydrogenation.[2] In recent years, ionic liquids attracted much attention as additives, solvents or catalyst coatings due to their non-volatility. SCILL catalysts for example show high activities and improved selectivities towards the intermediate product in semihydrogenation reactions of citral or COD.[3,4] The aim of this work was to expand this catalyst concept on the selective hydrogenation of acetylene under industrial conditions and to increase the selectivity to ethylene, thus reducing the formation of C4-hydrocarbons which act as precursors for green oil formation. Experimental Catalyst preparation: For the preparation of the SCILL catalysts industrial Pd-Ag shell catalysts were impregnated with ionic liquids via incipient wetness methods. Catalytic testing: The selective hydrogenation under tail-end conditions was carried out in a so-called monoline reactor developed in our laboratory which allows for the use of intact catalyst pellets (Figure 1). The reaction was carried out between 40 and 80 C and at a pressure of 10 bar. As reaction gas a typical tail-end acetylene/ethylene mixture was used (1 Vol% C2H2, H2, C3H8 each, 30 Vol% C2H4

    in Ar). The analysis of the product gas was carried out online with a gaschromatograph (Hewlett Packard 5890 Series II).

    SCILL catalyst

    packing material

    tubular reactor

    heating shell

    thermocouple

    Teflon tube

    Fig. 1: Catalyst alignment during the catalytic testing.

    Results For the hydrogenation reaction Pd-Ag shell catalysts with different Pd:Ag ratios were impregnated with ionic liquids. During the preparation procedure the type of the IL and the loading were varied in a broad range. The activity measurements show that with increasing IL loadings the conversion rate of acetylene decreases roughly about one order of magnitude with reference to the untreated Pd-Ag shell catalyst. For shell catalysts with high Ag contents ionic liquids decrease the selectivity of C4hydrocarbons with increasing IL loadings, whereas for shell catalysts with low Ag content the ethylene selectivity is improved with increasing IL loadings.

    [1]

    H. Zimmermann, R. Walzl in: Ullmanns Encyclopedia of Industrial Chemistry, online Edition, VCH,

    Weinheim, 2010, DOI: 10.1002/14356007.


    [2] [3] [4]

    A. Borodzinski, G.C. Bond, Catal. Rev. 2006, 48, 91. J. Arras, M. Steffan, Y. Shayeghi, P. Claus, Chem. Commun. 2008, 4058. U. Kernchen, B. Etzold, W. Korth, A. Jess, Chem.-Ing.-Tech. 2007, 79, 807.

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