摘要
Copper-based catalysts for CO2 hydrogenation to methanol are supported on ZrO2 and CeO2,respectively.Reaction results at 3.0 MPa and temperatures between 200 and 300°C 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.
Copper-based catalysts for CO2 hydrogenation to methanol are supported on ZrO2 and CeO2, respectively.Reaction results at 3.0 MPa and temperatures between 200 and 300 °C 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.
基金
financially supported by the National Natural Science Foundation of China (21577014, 21876019, 21825203, 21688102)
Programme of Introducing Talents of Discipline to Universities (B13012)
the fund of the State Key Laboratory of Catalysis in DICP (Y401010502)
