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期刊论文 1

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2022 1

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An investigation of the CHOH and CO selectivity of CO hydrogenation over Cu–Ce–Zr catalysts

《化学科学与工程前沿（英文）》 2022年 第16卷 第6期   页码 950-962 doi: 10.1007/s11705-022-2162-2

摘要： A series of Cu–Ce–Zr catalysts with different Ce contents are applied to the hydrogenation of CO2 to CO/CH3OH products. The Cu–Ce–Zr catalyst with 2 wt% Ce loading shows higher CO selectivity (SCO = 0.0%–87.8%) from 200–300 °C, while the Cu–Ce–Zr catalyst with 8 wt% Ce loading presents higher CO2 conversion ( XCO2 = 5.4%–15.6%) and CH3OH selectivity ( SCH3OH = 97.8%–40.6%). The number of hydroxyl groups and solid solution nature play a significant role in changing the reaction pathway. The solid solution enhances the CO2 adsorption ability. At the CO2 adsorption step, a larger number of hydroxyl groups over the Cu–Ce–Zr catalyst with 8 wt% Ce loading leads to the production of H-containing adsorption species. At the CO2 hydrogenation step, a larger number of hydroxyl groups assists in encouraging the further hydrogenation of intermediate species to CH3OH and improving the hydrogenation rate. Hence, the Cu–Ce–Zr catalyst with 8 wt% Ce loading favors CH3OH selectivity and CO2 activation, while CO is preferred on the Cu–Ce–Zr catalyst with 2 wt% Ce loading, a smaller number of hydroxyl groups and a solid solution nature. Additionally, high-pressure in situ diffuse reflectance infrared Fourier transform spectroscopy shows that CO is produced from formate decomposition and that both monodentate formate and bidentate formate are active intermediate species of CO2 hydrogenation to CH3OH.

关键词： CO2 hydrogenation     Cu–Ce–Zr     hydroxyls     CO/CH3OH selectivity    

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An investigation of the CHOH and CO selectivity of CO hydrogenation over Cu–Ce–Zr catalysts

期刊论文