Direct Oxidation of Methane to Methanol over Transition-Metal-Free Ferrierite Zeolite Catalysts
Peipei Xiao, Yong Wang, Yao Lü, Kengo Nakamura, Nobuki Ozawa, Momoji Kubo, Hermann Gies, Toshiyuki Yokoi
Abstract
High Resolution Image Download MS PowerPoint Slide 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-metal-containing 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.