TY - JOUR
T1 - Unravelling Channel Structure-Diffusivity Relationships in Zeolite ZSM-5 at the Single-Molecule Level
AU - Fu, Donglong
AU - Maris, J J Erik
AU - Stanciakova, Katarina
AU - Nikolopoulos, Nikolaos
AU - van der Heijden, Onno
AU - Mandemaker, Laurens D B
AU - Siemons, Marijn E
AU - Pastene, Desiree Salas
AU - Kapitein, Lukas C
AU - Rabouw, Freddy T
AU - Meirer, Florian
AU - Weckhuysen, Bert Marc
N1 - Funding Information:
We would like to thank Eugene Y. Katrukha (Utrecht University, UU), Martin Vesely (UU), and Zoran Ristanović (Leiden University) for fruitful discussions. This work was supported by a European Research Council (ERC) Advanced Grant (No. 321140), the Netherlands Centre for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation program funded by the Ministry of Education, Culture and Science of the government of the Netherlands, and the Netherlands Technology Foundation (STW‐13941). Part of this work was carried out on the Dutch national e‐infrastructure with the support of SURF Cooperative. F.T.R. acknowledges financial support from The Netherlands Organization for Scientific Research NWO (VENI Grant 722.017.002). F.M. acknowledges funding from a Netherlands Organization for Scientific Research (NWO) VIDI Grant (No. 723.015.007).
Funding Information:
We would like to thank Eugene Y. Katrukha (Utrecht University, UU), Martin Vesely (UU), and Zoran Ristanović (Leiden University) for fruitful discussions. This work was supported by a European Research Council (ERC) Advanced Grant (No. 321140), the Netherlands Centre for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation program funded by the Ministry of Education, Culture and Science of the government of the Netherlands, and the Netherlands Technology Foundation (STW-13941). Part of this work was carried out on the Dutch national e-infrastructure with the support of SURF Cooperative. F.T.R. acknowledges financial support from The Netherlands Organization for Scientific Research NWO (VENI Grant 722.017.002). F.M. acknowledges funding from a Netherlands Organization for Scientific Research (NWO) VIDI Grant (No. 723.015.007).
Publisher Copyright:
© 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH
PY - 2022/1/26
Y1 - 2022/1/26
N2 - 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.
AB - 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.
KW - Diffusion
KW - Single-molecule studies
KW - Thin films
KW - ZSM-5
KW - Zeolites
UR - http://www.scopus.com/inward/record.url?scp=85120434376&partnerID=8YFLogxK
U2 - 10.1002/anie.202114388
DO - 10.1002/anie.202114388
M3 - Article
C2 - 34788496
SN - 1433-7851
VL - 61
SP - 1
EP - 5
JO - Angewandte Chemie-International Edition
JF - Angewandte Chemie-International Edition
IS - 5
M1 - e202114388
ER -