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Selective mild oxidation of methane to methanol or formic acid on Fe-MOR catalysts

Abstract

The controllable methane oxidation directly into value-added products under mild conditions is still the remaining challenge. Herein, an active Fe/MOR catalyst has been synthesized by the simple solid-state ion exchange, which was intensively investigated for selective oxidation of methane with H2O2 in aqueous phase. The octahedral dimer Fe3+ species [Fe2(μ-O)2] in extra framework was confirmed as the initial active site by X-ray photoelectron spectroscopy, X-ray absorption near-edge structure and extended X-ray absorption fine structure, UV-Vis diffuse-reflectance spectra, and high-angle annular dark field and scanning transmission electron microscopy with the combination of DFT calculations. DFT calculations indicate that the methanol formation via methyl peroxide (CH3OOH*) on [Fe2(μ-OH)2O2] is most favorable pathway compared to direct formation of methanol via CH3O*. The formed CH3OH was easily further oxidized by hydroxyl radical (●OH) to result in non-selective methane oxidation. In contrast, The Fe/MOR catalyst can produce a high methanol selectivity of 71.3% by the presence of homogeneous Cu2+ precursor that can efficiently suppress the over-oxidation of methanol, and a high formic acid selectivity up to 81-82% by just slightly higher reaction temperature that can mildly shift the oxidation of methanol and formaldehyde to the target product.

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Publication details

The article was received on 16 Aug 2019, accepted on 04 Nov 2019 and first published on 05 Nov 2019


Article type: Paper
DOI: 10.1039/C9CY01640F
Catal. Sci. Technol., 2019, Accepted Manuscript

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    Selective mild oxidation of methane to methanol or formic acid on Fe-MOR catalysts

    Z. Fang, H. Murayama, Q. Zhao, B. Liu, F. Jiang, Y. Xu, M. Tokunaga and X. Liu, Catal. Sci. Technol., 2019, Accepted Manuscript , DOI: 10.1039/C9CY01640F

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