Thermosets comprised of cross-linked polymers demonstrate enhanced thermal, solvent, chemical, and dimensional stability as compared to their non-cross-linked counterparts. However, these often-desirable material properties typically come at the expense of reprocessability, recyclability, and healability. One solution to this challenge comes from the construction of polymers that are reversibly cross-linked. We relied on lessons from Nature to prepare polymer networks comprised of either cooperative Janus-faced hydrogen bonded cross-links or associative dynamic-covalent cross-links based on a variety of chemistries. Rheological experiments and dynamic mechanical analysis were employed to investigate the flow behavior of these systems, wherein the reversible cross-linkable moieties were distributed either homogeneously or in microphase-separated regions to gain insight into the role of morphology on reprocessability, recyclability, and healability.

Dynamic-covalent and supramolecular networks with unprecedented properties

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ACS Spring 2023

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