Extra-Large-Pore Zeolites with UTL Topology: Control of the Catalytic Activity by Variation in the Nature of the Active Sites

Authors

  • Dr. Mariya V. Shamzhy,

    1. J. Heyrovský Institute of Physical Chemistry, Academy of Sciences of Czech Republic v.v.i Dolejškova 3, 182 23 Prague 8 (Czech Republic)
    2. L. V. Pisarzhevskiy Institute of Physical Chemistry, National Academy of Sciences of Ukraine, 31 pr. Nauky, Kyiv 03028 (Ukraine)
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  • Dr. Oleksiy V. Shvets,

    1. J. Heyrovský Institute of Physical Chemistry, Academy of Sciences of Czech Republic v.v.i Dolejškova 3, 182 23 Prague 8 (Czech Republic)
    2. L. V. Pisarzhevskiy Institute of Physical Chemistry, National Academy of Sciences of Ukraine, 31 pr. Nauky, Kyiv 03028 (Ukraine)
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  • Dr. Maksym V. Opanasenko,

    1. J. Heyrovský Institute of Physical Chemistry, Academy of Sciences of Czech Republic v.v.i Dolejškova 3, 182 23 Prague 8 (Czech Republic)
    2. L. V. Pisarzhevskiy Institute of Physical Chemistry, National Academy of Sciences of Ukraine, 31 pr. Nauky, Kyiv 03028 (Ukraine)
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  • Lenka Kurfiřtová,

    1. J. Heyrovský Institute of Physical Chemistry, Academy of Sciences of Czech Republic v.v.i Dolejškova 3, 182 23 Prague 8 (Czech Republic)
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  • Dr. David Kubička,

    1. Research Institute of Inorganic Chemistry, UniCRE-RENTECH, Chempark Litvínov, 436 70 Litvínov (Czech Republic)
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  • Prof. Jiří Čejka

    Corresponding author
    1. J. Heyrovský Institute of Physical Chemistry, Academy of Sciences of Czech Republic v.v.i Dolejškova 3, 182 23 Prague 8 (Czech Republic)
    • J. Heyrovský Institute of Physical Chemistry, Academy of Sciences of Czech Republic v.v.i Dolejškova 3, 182 23 Prague 8 (Czech Republic)

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Abstract

The catalytic behavior of isomorphously substituted B-, Al-, Ga-, and Fe-containing extra-large-pore UTL zeolites was investigated in the acylation of p-xylene with benzoyl chloride and Beckmann rearrangement of 1-indanone oxime. The clear synergism between the Brønsted acidity (i.e., the concentration and the strength of protonic acid sites) of UTL catalysts and their activity in benzoylation was established. (Ga)UTL zeolite containing the Brønsted acid sites of medium strength is characterized by the optimum activity and selectivity in the benzoylation of p-xylene. Because of a higher accessibility of active centers, (Al)UTL zeolite appears to be a more active and selective catalyst than (Al)BEA in the benzoylation of p-xylene. In contrast to (B), (Ga), and (Al)UTL, the leaching of active sites occurs in the benzoylation over (Fe)UTL. All UTL zeolites showed 100 % selectivity in the Beckmann rearrangement of 1-indanone oxime, which provides the target 3,4-dihydroquinolin-2(1H)-one. (B) and (Fe)UTL zeolites containing the weakest acid centers were found to be more active in the Beckmann rearrangement of 1-indanone oxime than (Ga) and (Al)UTL: 100 % yield of the target amide was achieved in 240 min of the reaction time over (B) and (Fe)UTL.

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