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 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.