期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 34, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202205716
关键词
Facet-Shaped; Hierarchical Structure; Methanol-to-Propylene Reaction; ZSM-5; Zeolites
资金
- National Key Research and Development Program of China [2021YFA1501202]
- National Natural Science Foundation of China [21920102005, 21835002, 21621001]
- 111 Project [B17020]
- ShanghaiTech University [EM02161943]
This study successfully synthesized single-crystalline hierarchical ZSM-5 zeolites with hexagonal mesopores formed within the microporous framework. Due to their unique texture properties and more accessible acid sites, these zeolites exhibited longer lifetime and higher propylene selectivity in the methanol-to-propylene reaction.
Hierarchical zeolites integrating intrinsic micropores with secondary meso- and/or macropores afford superior catalytic properties for enhanced mass transportation and more accessible active sites. The mesopores generated by using mesoporogens or framework etching are usually irregular with abundant defective sites and low hydrothermal stability. Here, using protozeolite nanoparticles as seeds, we succeeded in the synthesis of single-crystalline hierarchical ZSM-5 zeolites with hexagonal mesopores faceted by complete microporous frameworks. The protozeolites played a key role in the formation of faceted mesopores achieved via intraparticle ripening process. Thanks to the unique texture properties and more accessible acid sites at the open location, the as-prepared zeolites exhibited remarkedly long lifetime (18 h) and high propylene selectivity (52.7 %) with propylene/ethylene ratio of 3.64 in the methanol-to-propylene reaction (WHSV=12.5 h(-1)) compared to the counterparts.
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