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The directional deformation of liquid crystalline elastomers (LCEs) is predicated on alignment, enforced by various processing techniques. Specifically, surface-aligned LCEs can exhibit higher temperature thermomechanical responses and weakened strain−temperature coupling in comparison to LCEs subjected to mechanical or rheological alignment. Recently, we reported enhanced stimuli response of mechanically aligned LCEs containing supramolecular liquid crystals. Here, we prepare supramolecular LCEs via surface-enforced alignment to study the impact of the supramolecular bond strength and intermolecular forces. This was evaluated using oxybenzoic acid (OBA) derivatives with and without pendant methyl groups as well as via oxybenzoic acid-pyridine complexes. Increased incorporation of supramolecular mesogens reduces the isotropic transition temperature and generally increases the strain−temperature coupling. The number of elastically active strands per unit volume, hydrogen bond conformations, and network morphology are affected by the supramolecular mesogens and influence the observed stimuli response. Overall, reduced intermolecular interactions correlate with more desirable actuation properties, demonstrating the influence of the supramolecular mesogen’s structure.
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This content will become publicly available on September 1, 2026
Enhanced Thermomechanical Response in Supramolecular Liquid Crystalline Elastomers With End‐On Mesogens
Liquid crystalline elastomers (LCEs) exhibit reversible macroscopic shape changes in response to a temperature change. Mechanistically, the thermomechanical response of LCEs is associated with the thermotropic nature of the liquid crystalline units (i.e., mesogens) in the polymer network. Upon heating, the mesogen‐mesogen interaction in the LCE is disrupted, which transitions the organization of the polymer network from an ordered to a disordered state. The disruption in order affects the volumetric distribution of macromolecular chains in the polymer network and results in a large directional contraction along the alignment axis. Prior reports detail that the magnitude of actuation depends strongly on the connectivity of LC mesogens (i.e., main‐chain or pendant) within the network. In this study, pendant end‐on mesogens are introduced into a primarily main‐chain supramolecular LCE composition to further reduce crosslink density while preserving overall LC concentration. The introduction of pendant end‐on mesogens to supramolecular LCE compositions further improves thermomechanical properties by enhancing strain‐temperature coupling and reducing actuation temperatures. By systematically varying the concentrations of end‐on and supramolecular mesogens, direct relationships are established between mesogen composition, polymer architecture, and the resulting thermomechanical performance of LCEs.
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- Award ID(s):
- 2105369
- PAR ID:
- 10642803
- Publisher / Repository:
- Wiley
- Date Published:
- Journal Name:
- Journal of Polymer Science
- Volume:
- 63
- Issue:
- 17
- ISSN:
- 2642-4150
- Page Range / eLocation ID:
- 3546 to 3556
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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