Molecular Accessibility and Diffusion of Resorufin in Zeolite Crystals.

Autor: Erik Maris JJ; 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.; Optical Materials Engineering Laboratory, ETH Zürich, Leonhardstrasse 21, 8092, Zürich, Switzerland., Parker LA; 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.; TNO, Princetonlaan 6, 3584 CB, Utrecht (The, Netherlands., Stanciakova K; 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., Nikolopoulos N; 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., Berendsen KMH; 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., van Blaaderen A; Soft Condensed Matter Group, Utrecht University, Debye Institute for Nanomaterials Science, Princetonplein 1, 3584 CC, Utrecht (The, Netherlands., Meirer F; 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., Rabouw FT; 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.; Soft Condensed Matter Group, Utrecht University, Debye Institute for Nanomaterials Science, Princetonplein 1, 3584 CC, Utrecht (The, Netherlands., Weckhuysen BM; 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.
Jazyk: angličtina
Zdroj: Chemistry (Weinheim an der Bergstrasse, Germany) [Chemistry] 2024 Jan 02; Vol. 30 (1), pp. e202302553. Date of Electronic Publication: 2023 Nov 09.
DOI: 10.1002/chem.202302553
Abstrakt: We 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  m 2  s -1 . Furthermore, we saw that diffusion through the straight pores of zeolite-β is impeded when crossing the boundaries between zeolite subunits.
(© 2023 The Authors. Chemistry - A European Journal published by Wiley-VCH GmbH.)
Databáze: MEDLINE