Molecular Accessibility and Diffusion of Resorufin in Zeolite Crystals

Author:

Erik Maris J. J.12ORCID,Parker Luke A.13ORCID,Stanciakova Katarina1ORCID,Nikolopoulos Nikolaos1ORCID,Berendsen Koen M. H.1ORCID,van Blaaderen Alfons4ORCID,Meirer Florian1ORCID,Rabouw Freddy T.14ORCID,Weckhuysen Bert M.1ORCID

Affiliation:

1. Inorganic Chemistry and Catalysis Group Utrecht University Debye Institute for Nanomaterials Science and Institute for Sustainable and Circular Chemistry Universiteitsweg 99 3584 CG Utrecht (The Netherlands

2. Optical Materials Engineering Laboratory, ETH Zürich Leonhardstrasse 21 8092 Zürich Switzerland

3. TNO Princetonlaan 6 3584 CB Utrecht (The Netherlands

4. Soft Condensed Matter Group Utrecht University Debye Institute for Nanomaterials Science Princetonplein 1 3584 CC Utrecht (The Netherlands

Abstract

AbstractWe have used confocal laser scanning microscopy on the small, fluorescent resorufin dye molecule to visualize molecular accessibility and diffusion in the hierarchical, anisotropic pore structure of large (~10 μm‐sized) zeolite‐β crystals. The resorufin dye is widely used in life and materials science, but only in its deprotonated form because the protonated molecule is barely fluorescent in aqueous solution. In this work, we show that protonated resorufin is in fact strongly fluorescent when confined within zeolite micropores, thus enabling fluorescence microimaging experiments. We find that J‐aggregation guest–guest interactions lead to a decrease in the measured fluorescence intensity that can be prevented by using non‐fluorescent spacer molecules. We characterized the pore space by introducing resorufin from the outside solution and following its diffusion into zeolite‐β crystals. The eventual homogeneous distribution of resorufin molecules throughout the zeolite indicates a fully accessible pore network. This enables the quantification of the diffusion coefficient in the straight pores of zeolite‐β without the need for complex analysis, and we found a value of 3×10−15 m2 s−1. Furthermore, we saw that diffusion through the straight pores of zeolite‐β is impeded when crossing the boundaries between zeolite subunits.

Funder

Nederlandse Organisatie voor Wetenschappelijk Onderzoek

Army Research Office

Publisher

Wiley

Subject

General Chemistry,Catalysis,Organic Chemistry

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