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Interfacial slip mechanisms of strain energy dissipation and vibration damping of highly aligned carbon nanotube (CNT) reinforced polymer composites were studied through experimentation and complementary micromechanics modeling. Experimentally, we have developed CNT-polystyrene (PS) composites with a high degree of CNT alignment via a combination of twin-screw extrusion and hot-drawing. The aligned nanocomposites enabled a focused study of the interfacial slip mechanics associated with shear stress concentrations along the CNT-PS interface induced by the elastic mismatch between the filler and matrix. The variation of storage and loss modulus suggests the initiation of the interfacial slip occurs at axial strains as low as 0.028%, primarily due to shear stress concentration along the CNT-PS interface. Through micromechanics modeling and by matching the model with the experimental results at the onset of slip, the interfacial shear strength was evaluated. The model was then used to provide additional insight into the experimental observations by showing that the nonlinear variation of damping with dynamic strain can be attributed to slip-stick behavior. The dependence of the interfacial load-transfer reversibility on the dynamic strain history and characteristic time scale was experimentally investigated to demonstrate the relative contribution of van der Waals (vdW) interactions, mechanical interlocking, and covalent bonding to shear interactions.

Soft robotics is an emerging field enabled by advances in the development of soft materials with properties commensurate to their biological counterparts, for the purpose of reproducing locomotion and other distinctive capabilities of active biological organisms. The development of soft actuators is fundamental to the advancement of soft robots and bio-inspired machines. Among the different material systems incorporated in the fabrication of soft devices, ionic hydrogelelastomer hybrids have recently attracted vast attention due to their favorable characteristics, including their analogy with human skin. Here, we demonstrate that this hybrid material system can be 3D printed as a soft dielectric elastomer actuator (DEA) with a unimorph configuration that is capable of generating high bending motion in response to an applied electrical stimulus. We characterized the device actuation performance via applied (i) ramp-up electrical input, (ii) cyclic electrical loading, and (iii) payload masses. A maximum vertical tip displacement of 9.78 ± 2.52 mm at 5.44 kV was achieved from the tested 3D printed DEAs. Furthermore, the nonlinear actuation behavior of the unimorph DEA was successfully modeled using analytical energetic formulation and a finite element method (FEM).

Soft materials with widely tailorable mechanical properties throughout the material's volume can shape the future of soft robotics and wearable electronics, impacting both consumer and defense sectors. Herein, a platform of 3D printable soft polymer networks with unprecedented tunability of stiffness of nearly three orders of magnitude (MPa to GPa) and an inherent capability to interbond is reported. The materials are based on dynamic covalent polymer networks with variable density of crosslinkers attached to prepolymer backbones via a temperature‐reversible Diels–Alder (DA) reaction. Inherent flexibility of the prepolymer chains and controllable crosslinking density enable 3D printed networks with glass transition temperatures ranging from just a few degrees to several tens of degrees Celsius. Materials with an elastomeric network demonstrate a fast and spontaneous self‐healing behavior at room temperature both in air and under water—a behavior difficult to achieve with other crosslinked materials. Reversible dissociation of DA networks at temperatures exceeding ≈120 °C allows for reprintability, while control of the stereochemistry of DA attachments enables reprogrammable shape memory behavior. The introduced platform addresses current major challenges including control of polymer interbonding, enhanced mechanical performance of printed parts, and reprocessability of 3D‐printed crosslinked materials in the absence of solvent.