A facile synthesis of hierarchical ZSM-5 with the three-dimensionally ordered mesoporosity(3DOm ZSM-5)was achieved by solid conversion(SC)of SiO_(2)colloidal crystals to high-crystalline ZSM-5.The products of 3DZ5_S/C...A facile synthesis of hierarchical ZSM-5 with the three-dimensionally ordered mesoporosity(3DOm ZSM-5)was achieved by solid conversion(SC)of SiO_(2)colloidal crystals to high-crystalline ZSM-5.The products of 3DZ5_S/C and 3DZ5_S,which were severally transformed from the carbon-padded SiO_(2)colloidal crystals and the initial SiO_(2)colloidal crystals,exhibited not only a similar ordered structure and acidity but also higher crystallinity and more balanced meso-/micropore combination in comparison with 3DZ5_C obtained by the conventional confined space crystallization approach.All three synthesized 3DZ5 catalysts showed improved methanol-to-propylene performance than the commercially microporous ZSM-5(CZ5),embodied in five times longer lifetime,higher propylene selectivity and S_(propylene)/S_(ethylene) ratio(P/E),and superior coke toleration with lower formation rate of coke(R_(coke)).Moreover,the 3DZ5_S catalyst in situ converted from SiO_(2)colloidal crystals presented the highest selectivities of propylene(42.51%)and light olefins(74.6%)among all three 3DZ5 catalysts.The high efficiency in synthesis and in situ utilization of SiO_(2)colloidal crystals demonstrate the proposed SC strategy to be more efficiently and eco-friendly for the high-yield production of not only 3DOm ZSM-5 but also other types of hierarchical zeolites.展开更多
基金supported by the National Natural Science Foundation of China(Grant No.21978238)the Natural Science Foundation of Shaanxi Provincial Department of Education(Grant No.21JY041)the Key R&D Program of Shaanxi Province(Grant No.2024GX-YBXM-426)。
文摘A facile synthesis of hierarchical ZSM-5 with the three-dimensionally ordered mesoporosity(3DOm ZSM-5)was achieved by solid conversion(SC)of SiO_(2)colloidal crystals to high-crystalline ZSM-5.The products of 3DZ5_S/C and 3DZ5_S,which were severally transformed from the carbon-padded SiO_(2)colloidal crystals and the initial SiO_(2)colloidal crystals,exhibited not only a similar ordered structure and acidity but also higher crystallinity and more balanced meso-/micropore combination in comparison with 3DZ5_C obtained by the conventional confined space crystallization approach.All three synthesized 3DZ5 catalysts showed improved methanol-to-propylene performance than the commercially microporous ZSM-5(CZ5),embodied in five times longer lifetime,higher propylene selectivity and S_(propylene)/S_(ethylene) ratio(P/E),and superior coke toleration with lower formation rate of coke(R_(coke)).Moreover,the 3DZ5_S catalyst in situ converted from SiO_(2)colloidal crystals presented the highest selectivities of propylene(42.51%)and light olefins(74.6%)among all three 3DZ5 catalysts.The high efficiency in synthesis and in situ utilization of SiO_(2)colloidal crystals demonstrate the proposed SC strategy to be more efficiently and eco-friendly for the high-yield production of not only 3DOm ZSM-5 but also other types of hierarchical zeolites.