Chirality-Enhanced Mechanics in a Dynamic Polymer Network

High Resolution Image Download MS PowerPoint Slide In recent decades, polymer research has focused on developing dynamic polymer materials that harness noncovalent interactions to engineer self-healing behavior. Herein, we examine the impact of introducing chiral 1,2-disubstituted cyclohexyl thioureas (TUCyH) into ethylene glycol-based copolymers to explore the role of chirality and supramolecular order in governing mechanics and self-healing. We find that raising the TUCyH fraction leads to the controlled formation of rigid domains bearing a well-packed structure reinforced by hydrogen bonds that is critical for the material’s thermal stability and tensile strength. Importantly, the enantioenriched 20% TUCyH copolymers outperform their racemic analogues in tensile strength tests after heat-activated self-healing, demonstrating the relevance of chirality for augmenting the mechanics of the materials. These findings establish the chiral TUCyH hydrogen bonding unit as a promising building block for the development of polymer materials that require robustness, durability, yet are self-healing, and highlight chirality as a design element that can be harnessed to modulate their mechanical behavior.