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Selective Formation of Active Cobalt Species for Direct Methylation of Benzene with Methane on MFI Zeolite by Co-presence of Secondary Elements

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Abstract

The catalytic activity for methylation of benzene was found on Co/MFI zeolite; the activity was generated by loading of Co in the region of Co/Al molar ratio in the final solid = 0.2–0.6 (significantly increased at 0.3–0.4) on a support MFI with [Al] = 1.3 mol kg−1. It has been found that the low activity at Co/Al > 0.6 was ascribed to the cobalt oxide aggregate formation, but even in the region of Co/Al < 0.6 where cobalt was mono-atomically dispersed, the presence of at least two types of cobalt species, active and inactive ones formed at Co/Al > 0.2 and Co/Al < 0.2, respectively, is suggested. Even in the low Co/Al region, addition of typical divalent elements such as Mg, Zn, Pb and Ca during the Co loading process was found to generate the catalytic activity. It is speculated that the active cobalt species were selectively formed.

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Acknowledgements

This study was partly supported by JST CREST Grant Number JPMJCR17P1, Japan.

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Authors and Affiliations

  1. Center for Research on Green Sustainable Chemistry, Tottori University, 4-101 Koyama-cho Minami, Tottori, 680-8552, Japan

    Hitoshi Matsubara, Etsushi Tsuji, Yasumi Moriwaki, Kana Yamamoto, Koshiro Nakamura, Satoshi Suganuma & Naonobu Katada

  2. Department of Applied Chemistry, Faculty of Engineering, Kogakuin University, 2665-1 Nakano-machi, Hachioji, Tokyo, 192-0015, Japan

    Kazu Okumura

Authors
  1. Hitoshi Matsubara
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  2. Etsushi Tsuji
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  3. Yasumi Moriwaki
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  4. Kazu Okumura
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  5. Kana Yamamoto
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  6. Koshiro Nakamura
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  7. Satoshi Suganuma
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  8. Naonobu Katada
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Correspondence to Etsushi Tsuji.

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Matsubara, H., Tsuji, E., Moriwaki, Y. et al. Selective Formation of Active Cobalt Species for Direct Methylation of Benzene with Methane on MFI Zeolite by Co-presence of Secondary Elements. Catal Lett 149, 2627–2635 (2019). https://doi.org/10.1007/s10562-019-02855-y

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  • DOI: https://doi.org/10.1007/s10562-019-02855-y

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