Chemical Imaging of Hierarchical Porosity Formation within a Zeolite Crystal Visualized by Small-Angle X-Ray Scattering and In-Situ Fluorescence Microscopy

Matthias Filez; Martin Vesely; Ivan Garcia-Torregrosa; Marianna Gambino; Özgün Attila; Florian Meirer; Eugene A. Katrukha; Maarten B.J. Roeffaers; Jan Garrevoet; Lukas C. Kapitein; Bert M. Weckhuysen

doi:10.1002/anie.202101747

Chemical Imaging of Hierarchical Porosity Formation within a Zeolite Crystal Visualized by Small-Angle X-Ray Scattering and In-Situ Fluorescence Microscopy

Matthias Filez, Martin Vesely, Ivan Garcia-Torregrosa, Marianna Gambino, Özgün Attila, Florian Meirer, Eugene A. Katrukha, Maarten B.J. Roeffaers, Jan Garrevoet, Lukas C. Kapitein, Bert M. Weckhuysen^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › Academic › peer-review

Abstract

Introducing hierarchical porosity to zeolites is vital for providing molecular access to microporous domains. Yet, the dynamics of meso- and macropore formation has remained elusive and pore space ill-characterized by a lack of (in situ) microscopic tools sensitive to nanoporosity. Here, we probe hierarchical porosity formation within a zeolite ZSM-5 crystal in real-time by in situ fluorescence microscopy during desilication. In addition, we introduce small-angle X-ray scattering microscopy as novel characterization tool to map intracrystal meso- and macropore properties. It is shown that hierarchical porosity formation initiates at the crystal surface and propagates to the crystal core via a pore front with decreasing rate. Also, hierarchical porosity only establishes in specific (segments of) subunits which constitute ZSM-5. Such space-dependent meso- and macroporosity implies local discrepancies in diffusion, performance and deactivation behaviors even within a zeolite crystal.

Original language	English
Pages (from-to)	13803-13806
Number of pages	4
Journal	Angewandte Chemie - International Edition
Volume	60
Issue number	25
DOIs	https://doi.org/10.1002/anie.202101747
Publication status	Published - 14 Jun 2021

Bibliographical note

Funding

M.F. acknowledges a European Union's Horizon 2020 research and innovation program under the Marie Sklodowska-Curie grant agreement (No. 748563). B.M.W. acknowledges financial support from the Netherlands Organisation for Scientific Research (NWO) in the form of a Gravitation Program, called Multiscale Catalytic Energy Conversion (MCEC). M.V. and F.M. acknowledge support from the NWO VIDI Grant No. 723.015.007. We acknowledge DESY (Hamburg, Germany), a member of the Helmholtz Association HGF, for the provision of experimental facilities. Parts of this research was carried out at the P06 beamline of Petra III. The research leading to this result has been supported by the project CALIPSOplus under the Grant Agreement 730872 from the EU Framework Programme for Research and Innovation HORIZON 2020. M.F. acknowledges a European Union's Horizon 2020 research and innovation program under the Marie Sklodowska‐Curie grant agreement (No. 748563). B.M.W. acknowledges financial support from the Netherlands Organisation for Scientific Research (NWO) in the form of a Gravitation Program, called Multiscale Catalytic Energy Conversion (MCEC). M.V. and F.M. acknowledge support from the NWO VIDI Grant No. 723.015.007. We acknowledge DESY (Hamburg, Germany), a member of the Helmholtz Association HGF, for the provision of experimental facilities. Parts of this research was carried out at the P06 beamline of Petra III. The research leading to this result has been supported by the project CALIPSOplus under the Grant Agreement 730872 from the EU Framework Programme for Research and Innovation HORIZON 2020.

Keywords

desilication
hierarchical nanoporosity
in situ fluorescence microscopy
small-angle X-ray scattering microscopy
zeolite

Access to Document

10.1002/anie.202101747Licence: CC BY

anie.202101747Final published version, 1.46 MBLicence: CC BY

Cite this

Filez, M., Vesely, M., Garcia-Torregrosa, I., Gambino, M., Attila, Ö., Meirer, F., Katrukha, E. A., Roeffaers, M. B. J., Garrevoet, J., Kapitein, L. C., & Weckhuysen, B. M. (2021). Chemical Imaging of Hierarchical Porosity Formation within a Zeolite Crystal Visualized by Small-Angle X-Ray Scattering and In-Situ Fluorescence Microscopy. Angewandte Chemie - International Edition, 60(25), 13803-13806. https://doi.org/10.1002/anie.202101747

@article{226d9042de204d6884ff394ba900edb2,

title = "Chemical Imaging of Hierarchical Porosity Formation within a Zeolite Crystal Visualized by Small-Angle X-Ray Scattering and In-Situ Fluorescence Microscopy",

abstract = "Introducing hierarchical porosity to zeolites is vital for providing molecular access to microporous domains. Yet, the dynamics of meso- and macropore formation has remained elusive and pore space ill-characterized by a lack of (in situ) microscopic tools sensitive to nanoporosity. Here, we probe hierarchical porosity formation within a zeolite ZSM-5 crystal in real-time by in situ fluorescence microscopy during desilication. In addition, we introduce small-angle X-ray scattering microscopy as novel characterization tool to map intracrystal meso- and macropore properties. It is shown that hierarchical porosity formation initiates at the crystal surface and propagates to the crystal core via a pore front with decreasing rate. Also, hierarchical porosity only establishes in specific (segments of) subunits which constitute ZSM-5. Such space-dependent meso- and macroporosity implies local discrepancies in diffusion, performance and deactivation behaviors even within a zeolite crystal.",

keywords = "desilication, hierarchical nanoporosity, in situ fluorescence microscopy, small-angle X-ray scattering microscopy, zeolite",

author = "Matthias Filez and Martin Vesely and Ivan Garcia-Torregrosa and Marianna Gambino and {\"O}zg{\"u}n Attila and Florian Meirer and Katrukha, {Eugene A.} and Roeffaers, {Maarten B.J.} and Jan Garrevoet and Kapitein, {Lukas C.} and Weckhuysen, {Bert M.}",

note = "{\textcopyright} 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.",

year = "2021",

month = jun,

day = "14",

doi = "10.1002/anie.202101747",

language = "English",

volume = "60",

pages = "13803--13806",

journal = "Angewandte Chemie - International Edition",

issn = "1433-7851",

publisher = "John Wiley and Sons Ltd",

number = "25",

}

Filez, M, Vesely, M, Garcia-Torregrosa, I, Gambino, M, Attila, Ö, Meirer, F , Katrukha, EA, Roeffaers, MBJ, Garrevoet, J, Kapitein, LC & Weckhuysen, BM 2021, 'Chemical Imaging of Hierarchical Porosity Formation within a Zeolite Crystal Visualized by Small-Angle X-Ray Scattering and In-Situ Fluorescence Microscopy', Angewandte Chemie - International Edition, vol. 60, no. 25, pp. 13803-13806. https://doi.org/10.1002/anie.202101747

Chemical Imaging of Hierarchical Porosity Formation within a Zeolite Crystal Visualized by Small-Angle X-Ray Scattering and In-Situ Fluorescence Microscopy. / Filez, Matthias; Vesely, Martin; Garcia-Torregrosa, Ivan et al.
In: Angewandte Chemie - International Edition, Vol. 60, No. 25, 14.06.2021, p. 13803-13806.

Research output: Contribution to journal › Article › Academic › peer-review

TY - JOUR

T1 - Chemical Imaging of Hierarchical Porosity Formation within a Zeolite Crystal Visualized by Small-Angle X-Ray Scattering and In-Situ Fluorescence Microscopy

AU - Filez, Matthias

AU - Vesely, Martin

AU - Garcia-Torregrosa, Ivan

AU - Gambino, Marianna

AU - Attila, Özgün

AU - Meirer, Florian

AU - Katrukha, Eugene A.

AU - Roeffaers, Maarten B.J.

AU - Garrevoet, Jan

AU - Kapitein, Lukas C.

AU - Weckhuysen, Bert M.

PY - 2021/6/14

Y1 - 2021/6/14

N2 - Introducing hierarchical porosity to zeolites is vital for providing molecular access to microporous domains. Yet, the dynamics of meso- and macropore formation has remained elusive and pore space ill-characterized by a lack of (in situ) microscopic tools sensitive to nanoporosity. Here, we probe hierarchical porosity formation within a zeolite ZSM-5 crystal in real-time by in situ fluorescence microscopy during desilication. In addition, we introduce small-angle X-ray scattering microscopy as novel characterization tool to map intracrystal meso- and macropore properties. It is shown that hierarchical porosity formation initiates at the crystal surface and propagates to the crystal core via a pore front with decreasing rate. Also, hierarchical porosity only establishes in specific (segments of) subunits which constitute ZSM-5. Such space-dependent meso- and macroporosity implies local discrepancies in diffusion, performance and deactivation behaviors even within a zeolite crystal.

AB - Introducing hierarchical porosity to zeolites is vital for providing molecular access to microporous domains. Yet, the dynamics of meso- and macropore formation has remained elusive and pore space ill-characterized by a lack of (in situ) microscopic tools sensitive to nanoporosity. Here, we probe hierarchical porosity formation within a zeolite ZSM-5 crystal in real-time by in situ fluorescence microscopy during desilication. In addition, we introduce small-angle X-ray scattering microscopy as novel characterization tool to map intracrystal meso- and macropore properties. It is shown that hierarchical porosity formation initiates at the crystal surface and propagates to the crystal core via a pore front with decreasing rate. Also, hierarchical porosity only establishes in specific (segments of) subunits which constitute ZSM-5. Such space-dependent meso- and macroporosity implies local discrepancies in diffusion, performance and deactivation behaviors even within a zeolite crystal.

KW - desilication

KW - hierarchical nanoporosity

KW - in situ fluorescence microscopy

KW - small-angle X-ray scattering microscopy

KW - zeolite

UR - http://www.scopus.com/inward/record.url?scp=85104684784&partnerID=8YFLogxK

U2 - 10.1002/anie.202101747

DO - 10.1002/anie.202101747

M3 - Article

C2 - 33725373

AN - SCOPUS:85104684784

SN - 1433-7851

VL - 60

SP - 13803

EP - 13806

JO - Angewandte Chemie - International Edition

JF - Angewandte Chemie - International Edition

IS - 25

ER -

Chemical Imaging of Hierarchical Porosity Formation within a Zeolite Crystal Visualized by Small-Angle X-Ray Scattering and In-Situ Fluorescence Microscopy

Abstract

Bibliographical note

Funding

Keywords

Access to Document

Other files and links

Fingerprint

Cite this