Stepwise Methane-to-Methanol Conversion on CuO/SBA-15

Chemistry. 2018 Aug 27;24(48):12592-12599. doi: 10.1002/chem.201801135. Epub 2018 Jul 23.

Abstract

The direct partial oxidation of methane to methanol is a challenging scientific and economical objective to expand the application of this abundant fuel gas as a major resource for one-step production of value-added chemicals. Despite substantial efforts to commercialize this synthetic route, to date no heterogeneous catalyst can selectively oxidize methane to methanol by O2 with an economically acceptable conversion. Cu-exchanged zeolites have been recently highlighted as one of the most promising bioinspired catalysts toward the direct production of methanol from methane under mild conditions. In this work, Cu-based catalysts were prepared using mesoporous silica SBA-15 as an alternative support and their activity for this conversion was investigated. The results demonstrate that highly dispersed CuO species on SBA-15 are able to react with methane and subsequently produce methanol with high selectivity (>84 %) through water-assisted extraction. Furthermore, it was confirmed that the main intermediate formed after interaction of the catalyst with methane is a methoxyl species, which can be further converted to methanol or dimethyl ether on extraction with water or methanol, respectively.

Keywords: copper; heterogeneous catalysis; mesoporous materials; oxidation; supported catalysts.