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Authors: Stach, Oliver S.
Breul, Katharina
Berač, Christian M.
Urschbach, Moritz
Seiffert, Sebastian
Besenius, Pol
Title: Bridging rigidity and flexibility : modulation of supramolecular hydrogels by metal complexation
Online publication date: 27-Oct-2022
Year of first publication: 2022
Language: english
Abstract: The combination of complementary, noncovalent interactions is a key principle for the design of multistimuli responsive hydrogels. In this work, an amphiphilic peptide, supramacromolecular hydrogelator which combines metal-ligand coordination induced gelation and thermoresponsive toughening is reported. Following a modular approach, the incorporation of the triphenylalanine sequence FFF into a structural (C3EG) and a terpyridine-functionalized (C3Tpy) C3-symmetric monomer enables their statistical copolymerization into self-assembled, 1D nanorods in water, as investigated by circular dichroism (CD) spectroscopy and transmission electron microscopy (TEM). In the presence of a terpyridine functionalized telechelic polyethylene glycol (PEG) cross-linker, complex formation upon addition of different transition metal ions (Fe2+, Zn2+, Ni2+) induces the formation of soft, reversible hydrogels at a solid weight content of 1 wt% as observed by linear shear rheology. The viscoelastic behavior of Fe2+ and Zn2+ cross-linked hydrogels are basically identical, while the most kinetically inert Ni2+ coordinative bond leads to significantly weaker hydrogels, suggesting that the most dynamic rather than the most thermodynamically stable interaction supports the formation of robust and responsive hydrogel materials.
DDC: 540 Chemie
540 Chemistry and allied sciences
Institution: Johannes Gutenberg-Universität Mainz
Department: FB 09 Chemie, Pharmazie u. Geowissensch.
Place: Mainz
Version: Published version
Publication type: Zeitschriftenaufsatz
License: CC BY
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Journal: Macromolecular rapid communications
Pages or article number: 2100473
Publisher: Wiley-VCH
Publisher place: Weinheim
Issue date: 2022
ISSN: 1521-3927
Publisher DOI: 10.1002/marc.202100473
Appears in collections:JGU-Publikationen

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