Copper-Modified Zeolites and Silica for Conversion of Methane to Methanol

Abstract

Powder materials containing copper ions supported on ZSM-5 (Cu-Zeolite Socony Mobil-5) and SSZ-13 (Cu-Standard Oil synthesised zeolite-13), and predominantly CuO nanoparticles on amorphous SiO 2 were synthesised, characterised, wash-coated onto ceramic monoliths and, for the first time, compared as catalysts for direct conversion of methane to methanol (DCMM) at ambient pressure (1 atm) using O 2 , N 2 O and NO as oxidants. Methanol production was monitored and quantified using Fourier transform infrared spectroscopy. Methanol is formed over all monolith samples, though the formation is considerably higher for the copper-exchanged zeolites. Hence, copper ions are the main active sites for DCMM. The minor amount of methanol produced over the Cu/SiO 2 sample, however, suggests that zeolites are not the sole substrate that can host those active copper sites but also silica. Further, we present the first ambient pressure in situ infrared spectroscopic measurements revealing the formation and consumption of surface methoxy species, which are considered to be key intermediates in the DCMM reaction.

Keywords

• methane partial oxidation
• DCMM
• supported copper ions
• methoxy reaction intermediate species
• in situ infrared spectroscopy
• Cu-ZSM-5
• Cu-SSZ-13
• Cu/SiO₂