This study reports the synthesis of size-controlled Fe-MFI （Fe-substituted zeolites with the MFI topology） and their catalytic performances for DTO （dimethyl ether-to-olefins） reaction. The amount of HC1 and aging...This study reports the synthesis of size-controlled Fe-MFI （Fe-substituted zeolites with the MFI topology） and their catalytic performances for DTO （dimethyl ether-to-olefins） reaction. The amount of HC1 and aging temperature were decisive factors to control the particle size of Fe-MFI in the range of 50 nm to 600 nm. The introduction of Fe3＋ ions into the zeolitic framework was confirmed by UV （ultraviolet）-visible spectroscopy. In addition, it was observed that the strength of acid site in prepared Fe-MFI was weaker than that of commercial ZSM-5. With decrease in the particle size, the amount of deposited coke decreased so that the catalyst life for the DTO reaction was well promoted. The present catalysts showed the higher light-olefin selectivity （C2= ＋ C3= ＋ C4=） than commercial ZSM-5 catalysts mainly due to the suppression of the formation of paraffins; however, the Fe-MFI catalysts were deactivated rapidly because of their low activity for the cracking of alkenes.展开更多
Two flexible click-based porous organic polymers （CPP-F1 and CPP-F2） have been readily synthesized. SEM images show CPP-F1 is a 3D network, while CPP-F2 exhibits a granular morphology. Pd（OAc）2 can be easily incor...Two flexible click-based porous organic polymers （CPP-F1 and CPP-F2） have been readily synthesized. SEM images show CPP-F1 is a 3D network, while CPP-F2 exhibits a granular morphology. Pd（OAc）2 can be easily incorporated into CPP-F1 and CPP-F2 to form Pd@CPP-F1 and Pd@CPP-F2, respectively. The interactions between the polymers and palladium are confirmed by solid-state 13C NMR, IR and XPS. Palladium nanoparticles （NPs） are formed after hydrogenation of olefins and nitrobenzene. Palladium NPs in CPP-F1 are well dispersed on the external surface of the polymer, while palladium NPs in CPP-F2 are located in the interior pores and on the external surface. In comparison with NPs in CPP-F1, the dual distribution of palladium NPs in CPP-F2 results in higher selectivity in the hydrogenation of 1,3-cyclohexadiene to cyclohexane. The catalytic systems can be recycled several times without obvious loss of catalytic activity or agglomeration of palladium NPs. Hot filtration, mercury drop tests and ICP analyses suggest that the catalytic systems proceed via a heterogeneous pathway.展开更多
文摘This study reports the synthesis of size-controlled Fe-MFI （Fe-substituted zeolites with the MFI topology） and their catalytic performances for DTO （dimethyl ether-to-olefins） reaction. The amount of HC1 and aging temperature were decisive factors to control the particle size of Fe-MFI in the range of 50 nm to 600 nm. The introduction of Fe3＋ ions into the zeolitic framework was confirmed by UV （ultraviolet）-visible spectroscopy. In addition, it was observed that the strength of acid site in prepared Fe-MFI was weaker than that of commercial ZSM-5. With decrease in the particle size, the amount of deposited coke decreased so that the catalyst life for the DTO reaction was well promoted. The present catalysts showed the higher light-olefin selectivity （C2= ＋ C3= ＋ C4=） than commercial ZSM-5 catalysts mainly due to the suppression of the formation of paraffins; however, the Fe-MFI catalysts were deactivated rapidly because of their low activity for the cracking of alkenes.
文摘Two flexible click-based porous organic polymers （CPP-F1 and CPP-F2） have been readily synthesized. SEM images show CPP-F1 is a 3D network, while CPP-F2 exhibits a granular morphology. Pd（OAc）2 can be easily incorporated into CPP-F1 and CPP-F2 to form Pd@CPP-F1 and Pd@CPP-F2, respectively. The interactions between the polymers and palladium are confirmed by solid-state 13C NMR, IR and XPS. Palladium nanoparticles （NPs） are formed after hydrogenation of olefins and nitrobenzene. Palladium NPs in CPP-F1 are well dispersed on the external surface of the polymer, while palladium NPs in CPP-F2 are located in the interior pores and on the external surface. In comparison with NPs in CPP-F1, the dual distribution of palladium NPs in CPP-F2 results in higher selectivity in the hydrogenation of 1,3-cyclohexadiene to cyclohexane. The catalytic systems can be recycled several times without obvious loss of catalytic activity or agglomeration of palladium NPs. Hot filtration, mercury drop tests and ICP analyses suggest that the catalytic systems proceed via a heterogeneous pathway.
