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Abstract Liquid crystal elastomers (LCEs) exhibit unique mechanical properties of soft elasticity and reversible shape‐changing behaviors, and so serve as potentially transformative materials for various protective and actuation applications. This study contributes to filling a critical knowledge gap in the field by investigating the microscale mesogen organization of nematic LCEs with diverse macroscopic deformation. A polarized Fourier transform infrared light spectroscopy (FTIR) tester is utilized to examine the mesogen organizations, including both the nematic director and mesogen order parameter. Three types of material deformation are analyzed: uniaxial tension, simple shear, and bi‐axial tension, which are all commonly encountered in practical designs of LCEs. By integrating customized loading fixtures into the FTIR tester, mesogen organizations are examined across varying magnitudes of strain levels for each deformation mode. Their relationships with macroscopic stress responses are revealed and compared with predictions from existing theories. Furthermore, this study reveals unique features of mesogen organizations that have not been previously reported, such as simultaneous evolutions of the mesogen order parameter and nematic director in simple shear and bi‐axial loading conditions. Overall, the findings presented in this study offer significant new insights for future rational designs, modeling, and applications of LCE materials. 

3D printing allows for moldless fabrication of continuous fiber composites with high design freedom and low manufacturing cost per part, which makes it particularly well-suited for rapid prototyping and composite product development. Compared to thermal-curable resins, UV-curable resins enable the 3D printing of composites with high fiber content and faster manufacturing speeds. However, the printed composites exhibit low mechanical strength and weak interfacial bonding for high-performance engineering applications. In addition, they are typically not reprocessable or repairable; if they could be, it would dramatically benefit the rapid prototyping of composite products with improved durability, reliability, cost savings, and streamlined workflow. In this study, we demonstrate that the recently emerged two-stage UV-curable resin is an ideal material candidate to tackle these grand challenges in 3D printing of thermoset composites with continuous carbon fiber. The resin consists primarily of acrylate monomers and crosslinkers with exchangeable covalent bonds. During the printing process, composite filaments containing up to 30.9% carbon fiber can be rapidly deposited and solidified through UV irradiation. After printing, the printed composites are subjected to post-heating. Their mechanical stiffness, strength, and inter-filament bonding are significantly enhanced due to the bond exchange reactions within the thermoset matrix. Furthermore, the utilization of the two-stage curable resin enables the repair, reshaping, and recycling of 3D printed thermosetting composites. This study represents the first detailed study to explore the benefits of using two-stage UV curable resins for composite printing. The fundamental understanding could potentially be extended to other types of two-stage curable resins with different molecular mechanisms.