4.8 Article

Construction of Single-Crystalline Hierarchical ZSM-5 with Open Nanoarchitectures via Anisotropic-Kinetics Transformation for the Methanol-to-Hydrocarbons Reaction

期刊

出版社

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202200677

关键词

Methanol-to-Hydrocarbons Reaction; Nanocages; Open Nanostructures; ZSM-5; Zeolites

资金

  1. National Key Research and Development Program of China [2021YFA1501202]
  2. National Natural Science Foundation of China [21920102005, 21835002, 21621001]
  3. 111 Project [B17020]

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We present an anisotropic-kinetics transformation strategy for preparing single-crystalline aluminosilicate MFI zeolites with highly open nanoarchitectures and hierarchical porosities. The strategy involves in situ etching and recrystallization of pure-silica MFI zeolite nanotemplates under hydrothermal conditions. The resulting ZSM-5 nanocages exhibit enhanced catalytic lifetime and lower coking rate in the methanol-to-hydrocarbons reaction compared to conventional microcrystals and nanocrystals.
We report an anisotropic-kinetics transformation strategy to prepare single-crystalline aluminosilicate MFI zeolites (ZSM-5) with highly open nanoarchitectures and hierarchical porosities. The methodology relies on the cooperative effect of in situ etching and recrystallization on the evolution of pure-silica MFI zeolite (silicalite-1) nanotemplates under hydrothermal conditions. The strategy enables a controllable preparation of ZSM-5 nanostructures with diverse open geometries by tuning the relative rate difference between etching and recrystallization processes. Meanwhile, it can also be extended to synthesize other heteroatom-substituted MFI zeolite nanocages. Compared with conventional ZSM-5 microcrystals, nanocrystals, and nanoboxes, the ZSM-5 nanocages with single-crystalline nature, highly open nanoarchitectures, and hierarchical porosities exhibit remarkably enhanced catalytic lifetime and low coking rate in the methanol-to-hydrocarbons (MTH) reaction.

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