Authors:	Jangizehi, Amir Ahmadi, Mostafa Pschierer, Sarah Nicolella, Paola Li, Hailong Amann-Winkel, Katrin Seiffert, Sebastian
Title:	Metal–ligand complexation and clustering in mussel-inspired side-chain functionalized supramolecular hydrogels
Online publication date:	18-Apr-2024
Year of first publication:	2022
Language:	english
Abstract:	Byssus threads of mussels have high resistance against abrasion in wave-swept habitats because of their outer cuticle, which is rich in amino acid dopa complexes with Fe3+ ions. This stems from the transient nature of metal–ligand complexes that creates extra relaxation mechanisms. Inspired by this concept, in this work, supramolecular hydrogels based on poly(acrylic acid) functionalized with nitrocatechol groups are synthesized. Polymer chains are physically crosslinked via nitrocatechol–Fe3+ complexes. The hydrogels have different polymer volume fractions as well as different nitrocatechol : Fe3+ molar ratios. The strength of the supramolecular crosslinks strongly depends on the pH of the medium. The dynamics of these hydrogels are studied by stress relaxation experiments followed by calculation of the relaxation time spectrum. Generally, samples have three relaxation modes, including dissociation of distinct metal–ligand complexes, reptation of sticky polymer chains, and disengagement of network segments from supramolecular aggregates and clusters. Such clusters hinder the terminal relaxation and potentially increase the stability of supramolecular hydrogels.
DDC:	540 Chemie 540 Chemistry and allied sciences
Institution:	Johannes Gutenberg-Universität Mainz
Department:	FB 09 Chemie, Pharmazie u. Geowissensch.
Place:	Mainz
ROR:	https://ror.org/023b0x485
DOI:	http://doi.org/10.25358/openscience-10305
Version:	Published version
Publication type:	Zeitschriftenaufsatz
Document type specification:	Scientific article
License:	CC BY
Information on rights of use:	https://creativecommons.org/licenses/by/4.0/
Journal:	Soft matter 18 36
Pages or article number:	6836 6847
Publisher:	Royal Society of Chemistry
Publisher place:	London
Issue date:	2022
ISSN:	1744-6848
Publisher DOI:	10.1039/d2sm00666a
Appears in collections:	DFG-491381577-H