Liquid crystalline elastomers (LCEs) prepared via thiol−ene photopolymerization result in homogeneous distribution of molecular weight between cross-links. Numerous prior reports emphasize that LCEs are material actuators that undergo a thermomechanical response associated with an order−disorder transition. However, modern and widely utilized approaches to create LCEs result in heterogeneous networks. Theoretical examination suggests that network heterogeneity and high degrees of cross-linking cause a continuous association of strain with temperature, rather than a first-order, stepwise association. Alternatively, thiol−ene photopolymerization historically yields homogeneous polymers with tailorable cross-link densities. This report extends these prior studies to formulations, which are conducive to LCE preparation. Specifically, this examination copolymerizes a liquid crystalline dialkene mesogen with a tetrathiol cross-linker and dithiol chain extender via a purely thiol−ene polymerization. Notably, this composition is amenable to surface-enforced alignment. This contribution exploits the tunability of thiol−ene photopolymerization to emphasize the influence of cross-linking on the coupling of strain and temperature.
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Thermomechanically Active Electrodes Power Work-Dense Soft Actuators
The effect of chain extender structure and composition on the thermomechanical properties of liquid crystal elastomers (LCE) synthesized using thiol-acrylate Michael addition is presented. The intrinsic molecular stiffness of the thiol chain extender and its relative molar ratio to acrylate-based host mesogens determine the magnitudes of the thermomechanical strains, temperatures at which they are realized and the mechanical work-content. A non-linear structure-property relationship emerges, wherein higher concentrations of flexible extenders first magnify the thermomechanical sensitivity, but a continued increase leads to weaker actuation. Understanding this interplay leads to a composite material platform, enabling a peak specific work production of ~2 J/kg using ~115 mW of electrical power supplied at 2 V. Composites of LCE with eGaIn liquid metal (LM) are prepared, which act as heaters, while being capable of actuation themselves. The thermomechanically active electrodes convert the electrical power into Joule heat, which they efficiently couple with the neat LCE to which they are bound. This system harnesses the nascent responsiveness of the LCE using electrodes that work with them, instead of fighting against them (or passively standing in the way). Specific work generated increases when subjected to increasing levels of load, reaching a peak at loads 260x the actuator weight. These ideas are extended to tri-layered actuators, where LCE films with orthogonal molecular orientations sandwich LCE-LM composite heaters. Torsional actuation modes are harnessed to twist under load.
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- Award ID(s):
- 1635926
- PAR ID:
- 10205551
- Date Published:
- Journal Name:
- Soft Matter
- ISSN:
- 1744-683X
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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