Thermodynamic control over energy dissipation modes in dual-network hydrogels based on metal-ligand coordination

Abstract

<p>Multiple energy dissipating modes are introduced into a model network hydrogel by metallo-supramolecular bonds and regulated by their association thermodynamics.</p>

Autoren

Mostafa Ahmadi
Sebastian Seiffert

DOI

10.1039/c9sm02149c

eISSN

1744-6848

ISSN

1744-683X

Ausgabe der Veröffentlichung

9

Zeitschrift

Soft Matter

Sprache

en

Online publication date

2020

Paginierung

2332 - 2341

Status

Published online

Herausgeber

Royal Society of Chemistry (RSC)

Herausgeber URL

http://dx.doi.org/10.1039/c9sm02149c

Datum der Datenerfassung

2024

Titel

Thermodynamic control over energy dissipation modes in dual-network hydrogels based on metal–ligand coordination

Ausgabe der Zeitschrift

16

Datenquelle: Crossref

Abstract

Modern polymeric hydrogels use reversible bonds to mimic biological functionalities. However, true biological materials benefit from several supramolecular elements and deliver multiple functions at the same time. To approach similar creation and control of multiple different functional elements in a synthetic soft material, we develop a model dual-network hydrogel in which multiple energy dissipating modes are formed by metal-ligand coordination and regulated by their association thermodynamics. This idea is realized by using linear and tetra-arm poly(ethylene glycol) (PEG) precursors with complementary reactive end groups. The former also carries terpyridine ligands on both ends, which form metallo-supramolecular bonds upon addition of metal ions. Multiple relaxation modes are provided by a combination of different metal ions. The timescale and amplitude of energy dissipating elements are characterized by oscillatory shear deformation. These studies suggest that the composition of metal ions controls the contribution of the corresponding relaxation modes in a linear fashion. A molecular-level confirmation is provided by following the UV-vis absorbance of the linear precursor in combination with mixtures of metal ions, accompanied by a theoretical study on the kinetics of the reversible association process. These results show that the linearity of the aforementioned dependence holds for such systems in which the utilized combination of metal ions and ligands exclusively form stable bis-complexes. By contrast, in many other cases, especially when the ions may compete to form mono-, bis-, or tris-complexes with the ligand, deviation from linearity is expected.

Addresses

Department of Polymer Engineering and Color Technology, Amirkabir University of Technology, Tehran, Iran and Institute of Physical Chemistry, Johannes Gutenberg-Universität Mainz, Duesbergweg 10-14, D-55128 Mainz, Germany. sebastian.seiffert@uni-mainz.de.

Autoren

Mostafa Ahmadi
Sebastian Seiffert

DOI

10.1039/c9sm02149c

eISSN

1744-6848

Externe Identifier

PubMed Identifier: 32053126

Funding acknowledgements

Alexander von Humboldt-Stiftung: Georg Förster fellowship

Open access

false

ISSN

1744-683X

Ausgabe der Veröffentlichung

9

Zeitschrift

Soft matter

Sprache

eng

Medium

Print

Paginierung

2332 - 2341

Datum der Veröffentlichung

2020

Status

Published

Datum der Datenerfassung

2020

Titel

Thermodynamic control over energy dissipation modes in dual-network hydrogels based on metal-ligand coordination.

Sub types

Journal Article

Ausgabe der Zeitschrift

16

Datenquelle: Europe PubMed Central

Abstract

Modern polymeric hydrogels use reversible bonds to mimic biological functionalities. However, true biological materials benefit from several supramolecular elements and deliver multiple functions at the same time. To approach similar creation and control of multiple different functional elements in a synthetic soft material, we develop a model dual-network hydrogel in which multiple energy dissipating modes are formed by metal-ligand coordination and regulated by their association thermodynamics. This idea is realized by using linear and tetra-arm poly(ethylene glycol) (PEG) precursors with complementary reactive end groups. The former also carries terpyridine ligands on both ends, which form metallo-supramolecular bonds upon addition of metal ions. Multiple relaxation modes are provided by a combination of different metal ions. The timescale and amplitude of energy dissipating elements are characterized by oscillatory shear deformation. These studies suggest that the composition of metal ions controls the contribution of the corresponding relaxation modes in a linear fashion. A molecular-level confirmation is provided by following the UV-vis absorbance of the linear precursor in combination with mixtures of metal ions, accompanied by a theoretical study on the kinetics of the reversible association process. These results show that the linearity of the aforementioned dependence holds for such systems in which the utilized combination of metal ions and ligands exclusively form stable bis-complexes. By contrast, in many other cases, especially when the ions may compete to form mono-, bis-, or tris-complexes with the ligand, deviation from linearity is expected.

Autoren

Mostafa Ahmadi
Sebastian Seiffert

Autoren-URL

https://www.ncbi.nlm.nih.gov/pubmed/32053126

DOI

10.1039/c9sm02149c

eISSN

1744-6848

Ausgabe der Veröffentlichung

9

Zeitschrift

Soft Matter

Sprache

eng

Country

England

Paginierung

2332 - 2341

Datum der Veröffentlichung

2020

Status

Published

Titel

Thermodynamic control over energy dissipation modes in dual-network hydrogels based on metal-ligand coordination.

Sub types

Journal Article

Ausgabe der Zeitschrift

16

Datenquelle: PubMed

Thermodynamic control over energy dissipation modes in dual-network hydrogels based on metal-ligand coordination

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