Direct Ink Writing of Recyclable Supramolecular Soft Actuators

Direct ink writing (DIW) of liquid crystal elastomers (LCEs) has rapidly paved its way into the field of soft actuators and other stimuli-responsive devices. However, currently used LCE systems for DIW require postprinting (photo)­polymerization, thereby forming a covalent network, making the process time-consuming and the material nonrecyclable. In this work, a DIW approach is developed for printing a supramolecular poly­(thio)­urethane LCE to overcome these drawbacks of permanent cross-linking. The thermo-reversible nature of the supramolecular cross-links enables the interplay between melt-processable behavior required for extrusion and formation of the network to fix the alignment. After printing, the actuators demonstrated a reversible contraction of 12.7% or bending and curling motions when printed on a passive substrate. The thermoplastic ink enables recyclability, as shown by cutting and printing the actuators five times. However, the actuation performance diminishes. This work highlights the potential of supramolecular LCE inks for DIW soft circular actuators and other devices.