Gas-phase epoxidation of propylene by molecular oxygen over Ag-Cu-Cl/BaCO₃ catalyst: Effects of Cu and Cl loadings

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• 作者：Qing Zhang ; Yanglong Guo ; ^{ylguo@ecust.edu.cn} ; Wangcheng Zhan ; Yun Guo ; Li Wang ; Yunsong Wang ; Guanzhong Lu ; ^{gzhlu@ecust.edu.cn}
• 关键词：Epoxidation of propylene ; Propylene oxide ; Molecular oxygen ; Ag-based catalyst ; Copper ; Chlorine
• 刊名：Chinese Journal of Catalysis
• 出版年：2017
• 出版时间：January 2017
• 年：2017
• 卷：38
• 期：1
• 页码：65-72
• 全文大小：700 K
• 卷排序：38

文摘

Ag-Cu-Cl/BaCO3 catalysts with different Cl and Cu loadings, prepared by the reduction deposition impregnation method, were investigated for gas-phase epoxidation of propylene by molecular oxygen and characterized by X-ray diffraction, X-ray photoelectron spectroscopy and O2 temperature programmed desorption. Ag-Cu-Cl/BaCO3 catalyst with 0.036 wt% Cu and 0.060 wt% Cl exhibited the highest catalytic performance for gas-phase epoxidation of propylene by molecular oxygen. A propylene oxide selectivity of 83.7% and propylene conversion of 1.2% were achieved under the reaction conditions of 20% C3H6-10% O2-70% N2, 200 °C, 0.1 MPa and 3000 h−1. Increasing the Cl loading allowed Ag to ensemble easier, whereas changing the Cu loading showed little effect on Ag crystallite size. The appropriate Cl loading of Ag-Cu-Cl/BaCO3 catalyst can reduce the dissociation adsorption of oxygen to atomic oxygen species leading to the combustion of propylene to CO2, which benefits epoxidation of propylene by molecular oxygen. Excessive Cl loading of Ag-Cu-Cl/BaCO3 catalyst decreases propylene conversion and propylene oxide selectivity remarkably because of Cl poisoning. The appropriate Cu loading of Ag-Cu-Cl/BaCO3 catalyst is efficient for the epoxidation of propylene by molecular oxygen, and an excess Cu loading decreases propylene oxide selectivity because the aggregation of Cu species increases the exposed surfaces of Ag nanoparticles, which was shown by slight increases in atomic oxygen species adsorbed. The appropriate loadings of Cu and Cl of Ag-Cu-Cl/BaCO3 catalyst are important to strike the balance between molecular oxygen and atomic oxygen species to create a favorable epoxidation of propylene by molecular oxygen.