Hierarchical Self-Assembly and Multidynamic Responsiveness of Fluorescent Dynamic Covalent Networks Forming Organogels

Smart stimuli-responsive fluorescent materials are of interest in the context of sensing and imaging applications. In this project, we elaborated multidynamic fluorescent materials made of a tetraphenylethene fluorophore displaying aggregation-induced emission and short cysteine-rich C-hydrazide pep...

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Veröffentlicht in:Biomacromolecules 2022-01, Vol.23 (1), p.431-442
Hauptverfasser: Suárez-Picado, Esteban, Coste, Maëva, Runser, Jean-Yves, Fossépré, Mathieu, Carvalho, Alain, Surin, Mathieu, Jierry, Loïc, Ulrich, Sébastien
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Sprache:eng
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Zusammenfassung:Smart stimuli-responsive fluorescent materials are of interest in the context of sensing and imaging applications. In this project, we elaborated multidynamic fluorescent materials made of a tetraphenylethene fluorophore displaying aggregation-induced emission and short cysteine-rich C-hydrazide peptides. Specifically, we show that a hierarchical dynamic covalent self-assembly process, combining disulfide and acyl-hydrazone bond formation operating simultaneously in a one-pot reaction, yields cage compounds at low concentration (2 mM), while soluble fluorescent dynamic covalent networks and even chemically cross-linked fluorescent organogels are formed at higher concentrations. The number of cysteine residues in the peptide sequence impacts directly the mechanical properties of the resulting organogels, Young’s moduli varying 2500-fold across the series. These materials underpinned by a nanofibrillar network display multidynamic responsiveness following concentration changes, chemical triggers, as well as light irradiation, all of which enable their controlled degradation with concomitant changes in spectroscopic outputsself-assembly enhances fluorescence emission by ca. 100-fold and disassembly quenches fluorescence emission.
ISSN:1525-7797
1526-4602
DOI:10.1021/acs.biomac.1c01389