The magnetic perovskite-supported palladium catalysts Pd/Lal_xPbxMnO3 (x = 0.2-0.7) were prepared and used for the oxidative carbonylation of phenol to diphenyl carbonate. The synthesized catalysts were characterize...The magnetic perovskite-supported palladium catalysts Pd/Lal_xPbxMnO3 (x = 0.2-0.7) were prepared and used for the oxidative carbonylation of phenol to diphenyl carbonate. The synthesized catalysts were characterized by the X-ray diffraction (XRD), surface area measurement BET, vibration sample magnetometer (VSM) and tem- perature-programmed reduction (TPR). The experimental results demonstrated that the magnetic Pd/La1-xPbxMnO3 (x = 0.4-0.5) obtain relative better catalytic activity. It can be explained by higher concentration of oxygen vacan- cies, larger amount and better mobility of lattice oxygen of their support. Furthermore, these samples possess suffi- cient saturated magnetization. Thus, Pd/La1-xPbxMnO3 (x = 0.4-0.5) may be suitable for operation in the magneti- cally stabilized bed reactor.展开更多
Glycerol carbonate was synthesized by the oxidative carbonylation of glycerol catalyzed by the commercial Pd/C with the aid of NaI. High conversion of glycerol (82.2%), selectivity to glycerol carbonate (〉99%), a...Glycerol carbonate was synthesized by the oxidative carbonylation of glycerol catalyzed by the commercial Pd/C with the aid of NaI. High conversion of glycerol (82.2%), selectivity to glycerol carbonate (〉99%), and TOF (900 h-1) were obtained under the conditions of 5 MPa (Pco:Po2 = 2:1), 140 C, 2 h. The highly active palladium species were generated in situ by dissolution from the carbon support and stabilized by re-deposition onto the support surface after the reaction was finished. Palladium dissolution and re-deposition were crucial and inherent parts of the catalytic cycle, which involved heterogeneous reactions. This Pd/C catalyst could be recycled and efficiently reused for four times with a gradual decrease in activity. Moreover, the in- fluences of various parameters, e.g., types of catalysts, solvents, additives, reaction temperature, pressure, and time on the conversion of glycerol were investigated. A reaction mechanism was proposed for oxidative carbonylation of glycerol to glyc- erol carbonate.展开更多
基金Supported by the Key Program of National Natural Science Foundation of China(20936003)the Foundation for Innovation Research Groups of the Natural Science Foundation of Hubei Province(2008CDA009)
文摘The magnetic perovskite-supported palladium catalysts Pd/Lal_xPbxMnO3 (x = 0.2-0.7) were prepared and used for the oxidative carbonylation of phenol to diphenyl carbonate. The synthesized catalysts were characterized by the X-ray diffraction (XRD), surface area measurement BET, vibration sample magnetometer (VSM) and tem- perature-programmed reduction (TPR). The experimental results demonstrated that the magnetic Pd/La1-xPbxMnO3 (x = 0.4-0.5) obtain relative better catalytic activity. It can be explained by higher concentration of oxygen vacan- cies, larger amount and better mobility of lattice oxygen of their support. Furthermore, these samples possess suffi- cient saturated magnetization. Thus, Pd/La1-xPbxMnO3 (x = 0.4-0.5) may be suitable for operation in the magneti- cally stabilized bed reactor.
基金supported by the National Natural Science Foundation of China(20976101)the Program for Key Science&Technology Innovation Team of Shaanxi Province(2012KCT-21)the Program for Changjiang Scholars and Innovative Research Team in University of China(IRT1070)
文摘Glycerol carbonate was synthesized by the oxidative carbonylation of glycerol catalyzed by the commercial Pd/C with the aid of NaI. High conversion of glycerol (82.2%), selectivity to glycerol carbonate (〉99%), and TOF (900 h-1) were obtained under the conditions of 5 MPa (Pco:Po2 = 2:1), 140 C, 2 h. The highly active palladium species were generated in situ by dissolution from the carbon support and stabilized by re-deposition onto the support surface after the reaction was finished. Palladium dissolution and re-deposition were crucial and inherent parts of the catalytic cycle, which involved heterogeneous reactions. This Pd/C catalyst could be recycled and efficiently reused for four times with a gradual decrease in activity. Moreover, the in- fluences of various parameters, e.g., types of catalysts, solvents, additives, reaction temperature, pressure, and time on the conversion of glycerol were investigated. A reaction mechanism was proposed for oxidative carbonylation of glycerol to glyc- erol carbonate.