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

IF 4.3 3区工程技术 Q2 ENGINEERING, CHEMICAL Frontiers of Chemical Science and Engineering Pub Date : 2024-05-20 DOI:10.1007/s11705-024-2446-9

Weilong Chun, Chenbiao Yang, Xu Wang, Xin Yang, Huiyong Chen

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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.

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固体转化合成用于甲醇制丙烯反应的三维有序介孔 ZSM-5 催化剂

通过将二氧化硅胶体晶体固态转化（SC）为高晶ZSM-5，实现了具有三维有序介孔（3DOm ZSM-5）的分层ZSM-5的简便合成。与传统密闭空间结晶方法获得的 3DZ5_C 相比，由碳填充的 SiO2 胶体结晶和初始 SiO2 胶体结晶转化而来的 3DZ5_S/C 和 3DZ5_S 产物不仅具有相似的有序结构和酸度，而且结晶度更高，中孔/微孔组合更均衡。三种合成的 3DZ5 催化剂都比市售的微孔 ZSM-5（CZ5）具有更好的甲醇制丙烯性能，具体表现在使用寿命延长了五倍，丙烯选择性和丙烯/乙烯比（P/E）更高，焦炭耐受性更好，焦炭形成率（Rcoke）更低。此外，在所有三种 3DZ5 催化剂中，由 SiO2 胶体晶体原位转化的 3DZ5_S 催化剂对丙烯（42.51%）和轻烯烃（74.6%）的选择性最高。SiO2 胶体晶体的高效合成和原位利用表明，所提出的 SC 策略不仅能高效、环保地高产生产 3DOm ZSM-5，还能高产生产其他类型的分层沸石。

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来源期刊

Frontiers of Chemical Science and Engineering ENGINEERING, CHEMICAL-

CiteScore

7.60

自引率

6.70%

发文量

868

审稿时长

1 months

期刊介绍： Frontiers of Chemical Science and Engineering presents the latest developments in chemical science and engineering, emphasizing emerging and multidisciplinary fields and international trends in research and development. The journal promotes communication and exchange between scientists all over the world. The contents include original reviews, research papers and short communications. Coverage includes catalysis and reaction engineering, clean energy, functional material, nanotechnology and nanoscience, biomaterials and biotechnology, particle technology and multiphase processing, separation science and technology, sustainable technologies and green processing.