Direct Methylation of Benzene with Methane Catalyzed by Co/MFI Zeolite

Cobalt‐loaded MFI zeolite showed distinct activity for direct methylation of benzene with methane into toluene. High activity was found at around 0.6 of Co/Al molar ratio. Incorporation of carbon from methane into the methyl group of toluene was confirmed with isotope tracer experiments and mass spe...

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Published inChemCatChem Vol. 10; no. 17; pp. 3806 - 3812
Main Authors Nakamura, Koshiro, Okuda, Akihito, Ohta, Kiyotaka, Matsubara, Hitoshi, Okumura, Kazu, Yamamoto, Kana, Itagaki, Ryosuke, Suganuma, Satoshi, Tsuji, Etsushi, Katada, Naonobu
Format Journal Article
LanguageEnglish
Published Germany Wiley Subscription Services, Inc 07.09.2018
John Wiley and Sons Inc
Subjects
Absorption
Acidic oxides
Ammonia
Benzene
Cobalt
Fine structure
Hydrocarbons
Ion exchange
Mass spectroscopy
Methane
Methylation
MFI Zeolite
Oxidation
Spectrum analysis
Toluene
Transmission electron microscopy
Valence
Zeolites
Methane
MFI Zeolite
Methylation
Cobalt
Benzene
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Summary:Cobalt‐loaded MFI zeolite showed distinct activity for direct methylation of benzene with methane into toluene. High activity was found at around 0.6 of Co/Al molar ratio. Incorporation of carbon from methane into the methyl group of toluene was confirmed with isotope tracer experiments and mass spectroscopy. Ammonia infrared‐mass spectroscopy temperature‐programmed desorption, transmission electron microscopy, X‐ray absorption near edge spectroscopy and extended X‐ray absorption fine structure indicated that Lewis acidic divalent (+II of oxidation state) Co species mono‐atomically dispersed on the ion exchange site of MFI zeolite was the active species. Efficient methane conversion: For the direct methylation of benzene with methane, Co/MFI zeolite showed distinct catalytic activity compared to various elements/zeolites. The active species was identified to be Lewis acidic Co (oxidation state +II) species mono‐atomically dispersed on the ion exchange site of MFI zeolite.
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ISSN:1867-3880
1867-3899
DOI:10.1002/cctc.201800724