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Synthesis of a Thiol Building Block for the Crystallization of a Semiconducting Gyroidal Metal-sulfur Framework

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Dynamic Chalcogen Squares for Material and Topological Control over Macromolecules.

Aaron H Bui¹, Anne D Fernando Pulle¹, Aaron S Micallef^1,2

¹School of Chemistry and Physics, Centre for Materials Science, Queensland University of Technology, 2 George Street, Brisbane, QLD, 4000, Australia.

Angewandte Chemie (International Ed. in English)

|March 7, 2024

Summary

New dynamic supramolecular bonding interactions using selenadiazole motifs create advanced soft matter materials. These chalcogen-bonded networks exhibit enhanced properties and autonomous self-healing capabilities.

Keywords:

chalcogen chemistry multicomponent chemistry polymer chemistry soft matter materials

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Area of Science:

Materials Science
Polymer Chemistry
Supramolecular Chemistry

Background:

Dynamic covalent chemistry and supramolecular interactions are crucial for developing advanced materials.
Chalcogen bonding is an emerging non-covalent interaction with potential applications in materials science.

Purpose of the Study:

To introduce chalcogen squares via selenadiazole motifs as a novel class of dynamic supramolecular bonding interactions.
To explore the use of these interactions for modifying and controlling soft matter materials.

Main Methods:

Synthesis of supramolecular networks using tandem step-growth/Passerini multicomponent reactions (MCRs).
Incorporation of selenadiazole motifs into polymer chains.
Post-polymerization modification using the Biginelli MCR.

Main Results:

Selenadiazole-containing networks showed increased glass transition temperatures and moduli compared to controls.
Elastomeric networks demonstrated autonomous self-healing at room temperature, retaining up to 83% of tensile strength.
Post-polymerization modification allowed for controlled topology in solution.

Conclusions:

Chalcogen squares via selenadiazoles represent a new and exciting exchange mechanism for dynamic materials.
This approach enables the design of soft matter with enhanced mechanical properties and self-healing abilities.