Membrane reactor for homogeneous catalysis in supercritical carbon dioxide

E.L.V. Goetheer, A.W. Verkerk, L.J.P. Broeke, van den, E. Wolf, de, B.J. Deelman, G. Koten, van, J.T.F. Keurentjes

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    42 Citations (Scopus)

    Abstract

    A membrane reactor is presented for homogeneous catalysis in supercrit. carbon dioxide with in situ catalyst sepn. This concept offers the advantages of benign high-d. gases, i.e., the possibility of achieving a high concn. of gaseous reactants in the same phase as the substrates and catalyst as well as easy catalyst localization by means of a membrane. For the sepn. of the homogeneous catalyst from the products an inorg. microporous membrane is used. The concept is demonstrated for the hydrogenation of 1-butene using a fluoro deriv. of Wilkinson's catalyst [RhCl{P-(C6H4-p-SiMe2CH2CH2C8F17)3}3]. The size of Wilkinson's catalyst, 2-4 nm, is clearly larger than the pore diam., 0.5-0.8 nm, of the silica membrane. The membrane will, therefore, retain the catalyst, while the substrates and products diffuse through the membrane. Stable operation and continuous prodn. of n-butane has been achieved at a temp. of 353 K and a pressure of 20 MPa. A turnover no. of 1.2*105 has been obtained during 32 h of reaction. The retention of the catalyst was checked using UV-vis spectroscopy and ICP-AAS; no rhodium or phosphorous species were detected at the permeate side of the membrane.
    Original languageEnglish
    Pages (from-to)126-133
    Number of pages8
    JournalJournal of Catalysis
    Volume219
    Issue number1
    DOIs
    Publication statusPublished - 2003

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