4.8 Article

Unravelling Channel Structure-Diffusivity Relationships in Zeolite ZSM-5 at the Single-Molecule Level

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 5, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202114388

Keywords

Diffusion; Single-molecule studies; Thin films; Zeolites; ZSM-5

Funding

  1. European Research Council (ERC) [321140]
  2. Netherlands Centre for Multiscale Catalytic Energy Conversion (MCEC)
  3. NWO Gravitation program - Ministry of Education, Culture and Science of the government of the Netherlands
  4. Netherlands Technology Foundation [STW-13941]
  5. SURF Cooperative
  6. Netherlands Organization for Scientific Research NWO (VENI Grant) [722.017.002]
  7. Netherlands Organization for Scientific Research (NWO) VIDI Grant [723.015.007]

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This study utilizes advanced techniques to track the diffusion of single molecules in zeolite materials, revealing different motion behaviors of guest molecules in different zeolite channels, with the geometry of the zeolite channels determining diffusion anisotropy. Additionally, the study shows that the addition of secondary pore networks primarily enhances the diffusivity of sinusoidal zeolite channels, alleviating diffusion limitations of microporous zeolites.
The development of improved zeolite materials for applications in separation and catalysis requires understanding of mass transport. Herein, diffusion of single molecules is tracked in the straight and sinusoidal channels of the industrially relevant ZSM-5 zeolites using a combination of single-molecule localization microscopy and uniformly oriented zeolite thin films. Distinct motion behaviors are observed in zeolite channels with the same geometry, suggesting heterogeneous guest-host interactions. Quantification of the diffusion heterogeneities in the sinusoidal and straight channels suggests that the geometry of zeolite channels dictates the mobility and motion behavior of the guest molecules, resulting in diffusion anisotropy. The study of hierarchical zeolites shows that the addition of secondary pore networks primarily enhances the diffusivity of sinusoidal zeolite channels, and thus alleviating the diffusion limitations of microporous zeolites.

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