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NoElastocaloric cooling is a promising solid-state alternative to vapor-compression refrigeration. In conventional systems, such as natural rubber, deformation induces entropy change accompanied by temperature release. Unloading the material restores the entropic state and is accompanied by cooling. Inverse elastocaloric effects have been detailed in shape memory alloys, where deformation induces loss of order and cooling. Here, we report on a distinctive inverse elastocaloric effect in liquid crystalline elastomers (LCEs) containing supramolecular hydrogen bonds. Upon deformation, the supramolecular LCE exhibits initial organization but then disorganizes as the intramesogenic hydrogen bonds are broken. Due to the liquid crystalline nature of the dimeric supramolecular bonds, the mechanochemical bond breakage manifests in a disruption in order. By disrupting the extent of liquid crystallinity in the system, we hypothesize that the network disorganizes to the deformation (e.g., entropy increases) and produces an inverse elastocaloric output.t Available 

Liquid crystalline elastomers (LCEs) are soft materials that associate order and deformation. Upon deformation, mechanically induced changes order affect entropy and can produce a caloric output (elastocaloric). Elastocaloric effects in materials continue to be considered for functional use as solid state refrigerants. Prior elastocaloric investigations of LCEs and related materials have measured ≈2 °C temperature changes upon deformation (100% strain). Here, the elastocaloric response of LCEs is explored that are prepared with a subambient nematic to isotropic transition temperature. These materials are referred as “isotropic” liquid crystalline elastomers. The LCEs are prepared by a two‐step thiol‐Michael/thiol‐ene reaction. This polymer network chemistry enhances elastic recovery and reduces hysteresis compared to acrylate‐based chemistries. The LCEs exhibit appreciable elastocaloric temperature changes upon deformation and recovery (> ± 3 °C, total ΔTof 6 °C) to deformation driven by minimal force (<< 1 MPa). Notably, the strong association of deformation and order and the resulting temperature change attained at low force achieves a responsivity of 14 °C MPa⁻¹which is seven times greater than natural rubber. 

Liquid crystalline elastomers (LCEs) are anisotropic soft materials capable of large dimensional changes when subjected to a stimulus. The magnitude and directionality of the stimuli‐induced thermomechanical response is associated with the alignment of the LCE. Recent reports detail the preparation of LCEs by additive manufacturing (AM) techniques, predominately using direct ink write printing. Another AM technique, digital light process (DLP) 3D printing, has generated significant interest as it affords LCE free‐forms with high fidelity and resolution. However, one challenge of printing LCEs using vat polymerization methods such as DLP is enforcing alignment. Here, we document the preparation of aligned, main‐chain LCEs via DLP 3D printing using a 100 mT magnetic field. Systematic examination isolates the contribution of magnetic field strength, alignment time, and build layer thickness on the degree of orientation in 3D printed LCEs. Informed by this fundamental understanding, DLP is used to print complex LCE free‐forms with through‐thickness variation in both spatial orientations. The hierarchical variation in spatial orientation within LCE free‐forms is used to produce objects that exhibit mechanical instabilities upon heating. DLP printing of aligned LCEs opens new opportunities to fabricate stimuli‐responsive materials in form factors optimized for functional use in soft robotics and energy absorption.