CO2 hydrogenation to methanol over Cu/CeO2 and Cu/ZrO2 catalysts:Tuning methanol selectivity via metal-support interaction
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摘要:
Copper-based catalysts for CO2 hydrogenation to methanol are supported on ZrO2 and CeO2,respectively.Reaction results at 3.0MPa and temperatures between 200 and 300 ℃ reveal that Cu catalysts supported on ZrO2 and CeO2 exhibit better activity and selectivity than pure Cu catalyst due to Cu-support (ZrO2 and CeO2) interaction.Combining the structural characterizations with in-situ diffuse reflectance infrared Fourier transform spectroscopy (in-situ DRIFTS),Cu/CeO2 shows the higher methanol selectivity due to the formation of main carbonates intermediates,which are closely related with the oxygen vacancies over Cu/CeO2.In contrast,bicarbonate and carboxyl species are observed on Cu/ZrO2,which originates from the hydroxyl groups presented on catalyst surfaces.Difference in CO2 adsorption intermediates results in the distinct methanol selectivity over the two catalysts.