Double Networks of Liquid-Crystalline Elastomers with Enhanced Mechanical Strength

Liquid-crystalline elastomers (LCEs) are frequently used in soft actuator development. However, applications are limited because LCEs are prone to mechanical failure when subjected to heavy loads and high temperatures during the working cycle. A mechanically tough LCE system offers larger work capacity and lower failure rate for the actuators. Herein, we adopt the double-network strategy, starting with a siloxane-based exchangeable LCE and developing a series of double-network liquid-crystalline elastomers (DN-LCEs) that are mechanically tougher than the initial elastomer. We incorporate diacrylate reacting monomers to fabricate DN-LCEs, some of which have the breaking stress of 40 MPa. We incorporate thermoplastic polyurethane to fabricate a DN-LCE, achieving an enormous ductility of 90 MJ/m³. We have also attempted to utilize the aza-Michael chemistry to make a DN-LCE that retains high plasticity because of several bond-exchange mechanisms; however, it failed to produce a stable reprocessable LCE system using conventional ester-based reactive mesogens. Each of these DN-LCEs exhibits unique features and characteristics, which are compared and discussed.