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Optical Monitoring of Supramolecular Interactions in Polymers.

Derek J Kiebala^1,2,3, Andrea Dodero^1,2, Christoph Weder^1,2

¹Adolphe Merkle Institute (AMI), University of Fribourg, Chemin des Verdiers 4, 1700, Fribourg, Switzerland.

Angewandte Chemie (International Ed. in English)

|June 11, 2024

Summary

Researchers developed a new supramolecular material that visually indicates its assembly and disassembly. This allows direct correlation between molecular changes and macroscopic properties in stimuli-responsive polymers.

Keywords:

cross-linking mechanofluorescence optical monitoring stimuli-responsive supramolecular assembly

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Area of Science:

Materials Science
Polymer Chemistry
Supramolecular Chemistry

Background:

Stimuli-responsive materials utilize reversible supramolecular binding for functions like self-healing and switchable adhesion.
Directly linking molecular-level supramolecular binding changes to macroscopic material behavior remains a significant challenge.

Purpose of the Study:

To develop a novel supramolecular binding motif with integrated indicators for real-time monitoring of assembly.
To establish direct correlations between molecular-level binding events and macroscopic material properties in stimuli-responsive polymers.

Main Methods:

Designed a novel ureido-4-pyrimidinone (UPy) motif functionalized with pyrene fluorophores.
Utilized pyrene excimer formation as an optical indicator for supramolecular dimerization.
Incorporated the motif as cross-linkers in poly(methyl acrylate) to study mechanoresponsive behavior.

Main Results:

The pyrene-functionalized UPy motif enables straightforward optical quantification of supramolecular assembly.
Stimuli-induced dissociation of hydrogen bonds is dependent on initial cross-link density.
Force-induced dissociation in polymer films correlates with applied stress or strain, influenced by cross-link density.

Conclusions:

Introduced a robust tool for in situ study of dynamic supramolecular assembly and disassembly mechanisms.
Provided new insights into the mechanoresponsive behavior of supramolecular materials.
Demonstrated the utility of integrated binding indicators for bridging molecular and macroscopic scales.