IRFI 東京工業大学国際先駆研究機構



【論文】WRH 横井俊之准教授とHermann Gies特任教授の共著論文 “Direct Oxidation of Methane to Methanol over Transition-Metal-Free Ferrierite Zeolite Catalysts”が掲載されました。


科学技術創成研究院横井俊之准教授とHermann Gies特任教授の論文が、Journal of the American Chemical Society (J. Am. Chem. Soc.)に掲載されました。
“Direct Oxidation of Methane to Methanol over Transition-Metal-Free Ferrierite Zeolite Catalysts
DOI :10.1021/jacs.4c00646

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 N2O 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, N2O adsorption FTIR spectra, and 27Al 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 CH4 and N2O as resources and will open new avenues for methane oxidation.




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