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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, 282
doi: 10.26083/tuprints-00021738
Artikel, Zweitveröffentlichung, Postprint

Kurzbeschreibung (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.

Typ des Eintrags: Artikel
Erschienen: 2022
Autor(en): Stanzel, Mathias ; Brilmayer, Robert ; Langhans, Markus ; Meckel, Tobias ; Andrieu-Brunsen, Annette
Art des Eintrags: Zweitveröffentlichung
Titel: Systematic study on FRET-pair functionalization of mesoporous thin films for correlation of pH-sensing and ionic mesopore accessibility
Sprache: Englisch
Publikationsjahr: 2022
Ort: Darmstadt
Verlag: Elsevier
Titel der Zeitschrift, Zeitung oder Schriftenreihe: Microporous and Mesoporous Materials
Jahrgang/Volume einer Zeitschrift: 282
Kollation: 24 Seiten
DOI: 10.26083/tuprints-00021738
URL / URN: https://tuprints.ulb.tu-darmstadt.de/21738
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Herkunft: Zweitveröffentlichungsservice
Kurzbeschreibung (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.

Freie Schlagworte: Mesoporous thin films, pH-detection, Confinement effects, FRET dye pair, Ionic permselectivity, Ionic mesopore accessibility
Status: Postprint
URN: urn:nbn:de:tuda-tuprints-217385
Sachgruppe der Dewey Dezimalklassifikatin (DDC): 500 Naturwissenschaften und Mathematik > 540 Chemie
Fachbereich(e)/-gebiet(e): 10 Fachbereich Biologie
10 Fachbereich Biologie > Membrane Dynamics
07 Fachbereich Chemie
07 Fachbereich Chemie > Ernst-Berl-Institut > Fachgebiet Makromolekulare Chemie
Hinterlegungsdatum: 21 Jul 2022 13:06
Letzte Änderung: 22 Jul 2022 06:08
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