Solid-conversion synthesis of three-dimensionally ordered mesoporous ZSM-5 catalysts for the methanol-to-propylene reaction

Abstract

A facile synthesis of hierarchical ZSM-5 with the three-dimensionally ordered mesoporosity (3DOm ZSM-5) was achieved by solid conversion (SC) of SiO₂ colloidal crystals to high-crystalline ZSM-5. The products of 3DZ5_S/C and 3DZ5_S, which were severally transformed from the carbon-padded SiO₂ colloidal crystals and the initial SiO₂ 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 SiO₂ 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 SiO₂ 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.

Key words： hierarchical zeolite; three-dimensionally ordered mesoporosity; ZSM-5; solid conversion; methanol-to-propylene

Competing interests

The authors declare that they have no competing interests.

Acknowledgements

This work was 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) and the Key R&D Program of Shaanxi Province (Grant No. 2024GX-YBXM-426)

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://dx.doi.org/10.1007/s11705-024-2446-9 and is accessible for authorized users.

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