Direct Oxidation of Methane to Methanol over Transition-Metal-Free Ferrierite Zeolite Catalysts

Abstract

Direct oxidation of methane to methanol was reported to be highly dependent on the transition-or noble-metal-loading catalysts in the past decades. Here, we show that the transition-metal-free aluminosilicate ferrierite (FER) zeolite effectively catalyzed methane and N 2 O to methanol for the first time. The distorted tetracoordinated Al in the framework and pentacoordinated Al on the extra framework formed during calcination, activation, and reaction processes were confirmed as the potential active centers. The possible reaction pathway similar to the Fe-containing zeolites was advocated based on the reaction results using different oxidants, N 2 O adsorption FTIR spectra, and 27 Al MAS NMR spectra. The stable and efficient methanol production capacity of FER zeolite was ascribed to the two-dimensional straight channels and its distinctive Al distribution of FER zeolite (CP914C) from Zeolyst. The transition-metal-free FER zeolite performed better than the record in the literature and our recent results using transition-metalcontaining catalysts in terms of selectivity and formation rate of methanol and stability. This work has great significance and prospects for utilizing CH 4 and N 2 O as resources and will open new avenues for methane oxidation.

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“…Ferrierites are commonly found as metamorphic minerals in basaltic rocks 24 , 25 . In recent years, ferrierite was used as catalyst and catalyst support for the preparation of efficient and reusable catalysts 22 , 26 , 27 . Also, magnetization of catalysts gives them a good separation ability under an external magnetic field.…”