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Systematic study on FRET-pair functionalization of mesoporous thin films for correlation of pH-sensing and ionic mesopore accessibility

Stanzel, Mathias ; Brilmayer, Robert ; Langhans, Markus ; Meckel, Tobias ; Andrieu-Brunsen, Annette (2022)
Systematic study on FRET-pair functionalization of mesoporous thin films for correlation of pH-sensing and ionic mesopore accessibility.
In: Microporous and Mesoporous Materials, 2019, 282
doi: 10.26083/tuprints-00021738
Article, Secondary publication, Postprint

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Abstract

Ordered mesoporous silica materials (OMS) are relevant in various applications such as separation, catalysis, or drug delivery. Thereby their performance is mainly dependent on mesopore accessibility and molecular transport within mesopores which is strongly influenced by the spatial confinement. This is especially relevant in case of charged mesopore walls and thus electrostatically controlled transport. Therefore, it is highly important to monitor charged states of functionalized mesopores. In this study we adapt pH-probing strategies, known from pH-monitoring e.g. in cells, to mesoporous thin films aiming to monitor mesopore charge and correlate this to mesopores ionic permselectivity. Therefore, grafting of a FRET dye pair, consisting of a pH-sensitive dye (fluorescein isothiocyanate (FITC)) and a pH-insensitive reference dye (rhodamine B isothiocyanate (RITC)), to the mesopore wall is optimized. The grafted FITC-RITC FRET pair allows to monitor mesopore “pH” over a broad range of up to six pH-units after optimization of FRET pair functionalization. Thereby, “pH” monitoring is performed based on absorption and fluorescence readout using confocal microscopy baring the potential of localized detection. The detected pH-dependent absorption and fluorescence emission is in good agreement with the pH-dependent ionic mesopore permselectivity, and thus with the influence of mesopore confinement on ionic permselectivity as detected by cyclic voltammetry. In addition, this study not only shows the possibility of using FRET dye pairs for monitoring charged states in mesopores but as well the influence of these probing dye molecules on the mesopores characteristics, such as ionic permselectivity, indicating the need of optimizing functionalization with probe molecules.

Item Type: Article
Erschienen: 2022
Creators: Stanzel, Mathias ; Brilmayer, Robert ; Langhans, Markus ; Meckel, Tobias ; Andrieu-Brunsen, Annette
Type of entry: Secondary publication
Title: Systematic study on FRET-pair functionalization of mesoporous thin films for correlation of pH-sensing and ionic mesopore accessibility
Language: English
Date: 2022
Place of Publication: Darmstadt
Year of primary publication: 2019
Publisher: Elsevier
Journal or Publication Title: Microporous and Mesoporous Materials
Volume of the journal: 282
Collation: 24 Seiten
DOI: 10.26083/tuprints-00021738
URL / URN: https://tuprints.ulb.tu-darmstadt.de/21738
Corresponding Links:
Origin: Secondary publication service
Abstract:

Ordered mesoporous silica materials (OMS) are relevant in various applications such as separation, catalysis, or drug delivery. Thereby their performance is mainly dependent on mesopore accessibility and molecular transport within mesopores which is strongly influenced by the spatial confinement. This is especially relevant in case of charged mesopore walls and thus electrostatically controlled transport. Therefore, it is highly important to monitor charged states of functionalized mesopores. In this study we adapt pH-probing strategies, known from pH-monitoring e.g. in cells, to mesoporous thin films aiming to monitor mesopore charge and correlate this to mesopores ionic permselectivity. Therefore, grafting of a FRET dye pair, consisting of a pH-sensitive dye (fluorescein isothiocyanate (FITC)) and a pH-insensitive reference dye (rhodamine B isothiocyanate (RITC)), to the mesopore wall is optimized. The grafted FITC-RITC FRET pair allows to monitor mesopore “pH” over a broad range of up to six pH-units after optimization of FRET pair functionalization. Thereby, “pH” monitoring is performed based on absorption and fluorescence readout using confocal microscopy baring the potential of localized detection. The detected pH-dependent absorption and fluorescence emission is in good agreement with the pH-dependent ionic mesopore permselectivity, and thus with the influence of mesopore confinement on ionic permselectivity as detected by cyclic voltammetry. In addition, this study not only shows the possibility of using FRET dye pairs for monitoring charged states in mesopores but as well the influence of these probing dye molecules on the mesopores characteristics, such as ionic permselectivity, indicating the need of optimizing functionalization with probe molecules.

Uncontrolled Keywords: Mesoporous thin films, pH-detection, Confinement effects, FRET dye pair, Ionic permselectivity, Ionic mesopore accessibility
Status: Postprint
URN: urn:nbn:de:tuda-tuprints-217385
Classification DDC: 500 Science and mathematics > 540 Chemistry
Divisions: 10 Department of Biology
10 Department of Biology > Membrane Dynamics
07 Department of Chemistry
07 Department of Chemistry > Ernst-Berl-Institut
07 Department of Chemistry > Ernst-Berl-Institut > Fachgebiet Makromolekulare Chemie
Date Deposited: 21 Jul 2022 13:06
Last Modified: 03 Jul 2024 02:39
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