Three-Dimensional Printing of Shape Memory Liquid Crystalline Thermoplastic Elastomeric Composites Using Fused Filament Fabrication.

Liquid crystalline elastomers (LCEs) are stimuli-responsive materials utilised in shape memory applications. The processability of these materials via advanced manufacturing is being paid increasing attention to advance their volume production on an industrial scale. Fused filament fabrication (FFF) is an extrusion-based additive manufacturing (AM) technique that offers the potential to address this. The critical challenge, however, is the rheological characteristics of LCEs that need to be tuned to achieve a facile processability through the extrusion-based method. In this work, new filaments of liquid crystalline thermoplastic elastomer (LCTPE) and its composites with lignin were made by the ternary system of LCE, thermoplastic polyurethane (TPU), and lignin. The results showed that TPU improves the melt flow index of the LCTPE system to approximately 10.01 g/10 min, while adding lignin further enhances the value of this index for the composites up to 21.82 g/10 min. The microstructural analysis indicated that the effective distribution of lignin and reduced domain size of the LCEs in the ternary blend contribute to the enhanced flowability of this filament through 3D printing. Samples of 3D-printed LCTPE and LCTPE/lignin composites maintained their shape memory characteristics via thermomechanical activation. Full shape recovery of the new LCTPE matrix and its composites with lignin was achieved in 39 s and 32 s at 130 °C, followed by 28 s and 24 s at 160 °C, respectively. The successful fabrication of LCTPE and LCTPE/lignin composite samples through 3D printing demonstrates a potential procedure for processing these shape memory materials using the FFF technique, and lignin offers a sustainable and cost-effective material solution that enhances the properties of this composite material.

A bioinspired 3D-printable flexure joint with cellular mechanical metamaterial architecture for soft robotic hands.

Compliant flexure joints have been widely used for cable-driven soft robotic hands and grippers due to their safe interaction with humans and objects. This paper presents a soft and compliant revolute flexure joint based on the auxetic cellular mechanical metamaterials with a heterogeneous structure. The heterogeneous architecture of the proposed metamaterial flexure joint (MFJ), which is inspired by the human finger joints, provides mechanically tunable multi-stiffness bending motion and large range of bending angle in comparison to conventional flexure joints. The multi-level variation of the joint stiffness over the range of bending motion can be tuned through the geometrical parameters of the cellular mechanical metamaterial unit cells. The proposed flexure joints are 3D printed with single flexible material in monolithic fashion using a standard benchtop 3D printer. The application of the MFJ is demonstrated in robotic in-hand manipulation and grasping thin and deformable objects such as wires and cables. The results show the capability and advantages of the proposed MFJ in soft robotic grippers and highly functional bionic hands.

Stress-gradient-induced polymer migration in Taylor-Couette flow.

We apply our recent continuum theory for stress-gradient-induced migration of polymers in solution (G. Zhu et al., J. Rheol., 2016, 60, 327-343) to rotational shearing flow in the gap between concentric cylinders (the so-called Taylor-Couette flow), where we have also accounted for the effect of polymer depletion from the solid boundaries on migration patterns. The steady-state distribution of dilute solutions of polymer dumbbells, obtained both using a systematic perturbation analysis in terms of the Weissenberg number (Wi) and by solving numerically the transport problem coupled to the upper-convected Maxwell equation, shows accumulation of polymers near the inner cylinder. This accumulation becomes so strong that most polymers are driven near the inner cylinder once Wi > 4. We also show that there is no first-order contribution to the polymer migration in Taylor-Couette flow due to the absence of a velocity component in the r-direction. Brownian dynamics (BD) simulations for a Hookean dumbbell give a concentration distribution in good agreement with the theoretical predictions of our theory, confirming the accuracy of the theory when the dumbbell radius of gyration is around an order of magnitude or much smaller than the gap. The demonstration of the accuracy of our continuum theory by direct molecular simulation opens the door to application of the theory to journal bearing and other lubrication flows containing polymers that may migrate due to stress gradients.

A molecular dynamics investigation of the planar elongational rheology of chemically identical dendrimer-linear polymer blends.

The structure and rheology of model polymer blends under planar elongational flow have been investigated through nonequilibrium molecular dynamics simulations. The polymeric blends consist of linear polymer chains (187 monomers per chain) and dendrimer polymers of generations g = 1 - 4. The number fraction, x, of the dendrimer species is varied (4%, 8%, and 12%) in the blend melt. We study the effect of extension rate, dendrimer generation, and dendrimer number fraction on pair distribution functions for different blend systems. We also calculate the extension-rate dependent radius of gyration and ratios of the eigenvalues of the gyration tensor to study the elongation-induced deformation of the molecules in the blend. Melt rheological properties including the first and second extensional viscosities are found to fall into the range between those of pure dendrimer and pure linear polymer melts, which are correlated with the mass fraction and generation of the dendrimers in the blend.

Shear rheology and structural properties of chemically identical dendrimer-linear polymer blends through molecular dynamics simulations.

We present nonequilibrium molecular dynamics (NEMD) simulation results for the miscibility, structural properties, and melt rheological behavior of polymeric blends under shear flow. The polymeric blends consist of chemically identical linear polymer chains (187 monomers per chain) and dendrimer polymers of generations g = 1-4. The number fraction x of the dendrimer species is varied (4%, 8%, and 12%) in the blend melt. The miscibility of blend species is measured, using the pair distribution functions gDL, gLL, and gDD. All the studied systems form miscible blend melts under the conditions investigated. We also study the effect of shear rate γ̇ and dendrimer generation on inter-penetration between blend species for different blend systems. The results reveal that shear flow increases the interpenetration of linear chains toward the core of the dendrimers. We also calculate the shear-rate dependent radius of gyration and ratios of the eigenvalues of the gyration tensor to study the shear-induced deformation of the molecules in the blend. Melt rheological properties including the shear viscosity and first and second normal stress coefficients obtained from NEMD simulations at constant pressure are found to fall into the range between those of pure dendrimer and pure linear polymer melts.