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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

  • Hitoshi Matsubara
  • Etsushi TsujiEmail author
  • Yasumi Moriwaki
  • Kazu Okumura
  • Kana Yamamoto
  • Koshiro Nakamura
  • Satoshi Suganuma
  • Naonobu Katada
Article
  • 34 Downloads

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.

Graphic Abstract

Keywords

Methylation of benzene with methane Co/MFI zeolite Secondary element additive 

Notes

Acknowledgements

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

Supplementary material

10562_2019_2855_MOESM1_ESM.pdf (295 kb)
Supplementary material 1 (PDF 294 kb)

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Copyright information

© Springer Science+Business Media, LLC, part of Springer Nature 2019

Authors and Affiliations

  • Hitoshi Matsubara
    • 1
  • Etsushi Tsuji
    • 1
    Email author
  • Yasumi Moriwaki
    • 1
  • Kazu Okumura
    • 2
  • Kana Yamamoto
    • 1
  • Koshiro Nakamura
    • 1
  • Satoshi Suganuma
    • 1
  • Naonobu Katada
    • 1
  1. 1.Center for Research on Green Sustainable ChemistryTottori UniversityTottoriJapan
  2. 2.Department of Applied Chemistry, Faculty of EngineeringKogakuin UniversityHachiojiJapan

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