In situXPS study of methanol oxidation over a copper catalyst derived from layered double hydroxides

Autor: Panafidin, Maxim A., Bukhtiyarov, Andrey V., Fedorov, Alexey Yu., Bukhtiyarova, Marina V., Prosvirin, Igor P., Bukhtiyarov, Valerii I.
Zdroj: Catalysis Science & Technology; 2024, Vol. 14 Issue: 17 p4986-4996, 11p
Abstrakt: Copper nanoparticles supported on alumina have been synthesized from CuAl-layered double hydroxide by heat treatment at 450 °C and have been characterized by thermal analysis, X-ray diffraction, transmission electron microscopy, and X-ray photoelectron spectroscopy. Methanol oxidation at different molar ratios of the components of the reaction feed (CH3OH : O2= 1 : 1, 3 : 1, 6 : 1 and 1 : 3, Ptotal= 0.012 mbar) over the prepared CuAlOxcatalyst has been studied by in situX-ray photoelectron spectroscopy and mass-spectrometry. It was revealed that methanol oxidation takes place at temperatures higher than 250 °C. The conversion of methanol and selectivities towards CH2O and CO2were found to depend on the molar ratio of the reaction mixture components and reaction temperature. A quantitative estimation of the surface composition for the CuAlOxcatalyst under different experimental conditions was performed based on the deconvolution of copper Auger spectra using a linear combination of individual components. It was shown that treatment of the as-loaded CuAlOxcatalyst in hydrogen at 300 °C led to a partial reduction of Cu+to Cu0. However, there were only Cu0species on the surface in the CH3OH : O2= 1 : 1 reaction mixture at 400 °C indicating the formation of active sites directly during the catalytic reaction. Metallic copper was shown to be an active component for the production of formaldehyde under the conditions of methanol excess in the reaction mixture.
Databáze: Supplemental Index