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Constructing Intrapenetrated Hierarchical Zeolites with Highly Complete Framework via Protozeolite Seeding |
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| Authors: | Yinghao Liu Xingxing Wang Dr Junyan Li Dr Qiang Zhang Zijian Niu Dr Sen Wang Yanjing Gao Mingkun Gao Dr Risheng Bai Dr Yida Zhou Dr Weibin Fan Prof Osamu Terasaki Prof Jun Xu Prof Jihong Yu |
| Institution: | 1. State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Qianjin Street 2699, Changchun, 130012 P. R. China;2. State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Qianjin Street 2699, Changchun, 130012 P. R. China
National Centre for Magnetic Resonance in Wuhan, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan, 430071 P. R. China;3. State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Qianjin Street 2699, Changchun, 130012 P. R. China Center for High-resolution Electron Microscopy (C?EM), School of Physical Science and Technology, ShanghaiTech University, 393 Middle Huaxia Road, Pudong, Shanghai, 201210 P.R. China;4. State Key Laboratory of Coal Conversion Institute of Coal Chemistry, Chinese Academy of Sciences Taiyuan, Shanxi, 030001 P. R. China;5. Center for High-resolution Electron Microscopy (C?EM), School of Physical Science and Technology, ShanghaiTech University, 393 Middle Huaxia Road, Pudong, Shanghai, 201210 P.R. China;6. National Centre for Magnetic Resonance in Wuhan, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan, 430071 P. R. China |
| Abstract: | Creation of intrapenetrated mesopores with open highway from external surface into the interior of zeolite crystals are highly desirable that can significantly improve the molecular transport and active sites accessibility of microporous zeolites to afford enhanced catalytic properties. Here, different from traditional zeolite-seeded methods that generally produced isolated mesopores in zeolites, nanosized amorphous protozeolites with embryo structure of zeolites were used as seeds for the construction of single-crystalline hierarchical ZSM-5 zeolites with intrapenetrated mesopores (mesopore volume of 0.51 cm3 g?1) and highly complete framework. In this strategy, in contrast to the conventional synthesis, only a small amount of organic structure directing agents and a low crystallization temperature were adopted to promise the protozeolites as the dominant growth directing sites to induce crystallization. The protozeolite nanoseeds provided abundant nucleation sites for surrounding precursors to be crystallized, followed by oriented coalescence of crystallites resulting in the formation of intrapenetrated mesopores. The as-prepared hierarchical ZSM-5 zeolites exhibited ultra-long lifetime of 443.9 hours and a high propylene selectivity of 47.92 % at a WHSV of 2 h?1 in the methanol-to-propylene reaction. This work provides a facile protozeolite-seeded strategy for the synthesis of intrapenetrated hierarchical zeolites that are highly effective for catalytic applications. |
| Keywords: | Hierarchical Structure Intrapenetrated Mesopores Methanol-to-Propylene Reaction Protozeolite Seed |