Copper-modified zeolites and silica for conversion of methane to methanol

• 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 SiO2 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 O2, N2 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/SiO2 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.

Ämnesord

TEKNIK OCH TEKNOLOGIER  -- Kemiteknik -- Kemiska processer (hsv//swe)

ENGINEERING AND TECHNOLOGY  -- Chemical Engineering -- Chemical Process Engineering (hsv//eng)

NATURVETENSKAP  -- Fysik -- Den kondenserade materiens fysik (hsv//swe)

NATURAL SCIENCES  -- Physical Sciences -- Condensed Matter Physics (hsv//eng)

NATURVETENSKAP  -- Kemi -- Materialkemi (hsv//swe)

NATURAL SCIENCES  -- Chemical Sciences -- Materials Chemistry (hsv//eng)

Nyckelord

Cu-SSZ-13

Cu-ZSM-5

Cu/SiO

DCMM

In situ infrared spectroscopy

Methane partial oxidation

Methoxy reaction intermediate species

Supported copper ions

methoxy reaction intermediate species

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