Design-encoded dual shape-morphing and shape-memory in 4D printed polymer parts toward cellularized vascular grafts†

Current additive manufacturing technologies wherein as-printed simple two-dimensional (2D) structures morph into complex tissue mimetic three-dimensional (3D) shapes are limited to multi-material hydrogel systems, which necessitates multiple fabrication steps and specific materials. This work utilizes a single shape memory thermoplastic polymer (SMP), PLMC (polylactide-co-trimethylene carbonate), to achieve programmable shape deformation through anisotropic design and infill angles encoded during 3D printing. The shape changes were first computationally predicted through finite element analysis (FEA) simulations and then experimentally validated through quantitative correlation. Rectangular 2D sheets could self-roll into complete hollow tubes of specific diameters (ranging from ≈6 mm to ≈10 mm) and lengths (as long as 40 mm), as quantitatively predicted from FEA simulations within one minute at relatively lower temperatures (≈80 °C). Furthermore, shape memory properties were demonstrated post-shape change to exhibit dual shape morphing at temperatures close to physiological levels. The tubes (retained as the permanent shape) were deformed into flat sheets (temporary shape), seeded with endothelial cells (at T < T_g), and thereafter triggered at ≈37 °C back into tubes (permanent shape), utilizing the shape memory properties to yield bioresorbable tubes with cellularized lumens for potential use as vascular grafts with improved long-term patency. Additionally, out-of-plane bending and twisting deformation were demonstrated in complex structures by careful control of infill angles that can unprecedently expand the scope of cellularized biomimetic 3D shapes. This work demonstrates the potential of the combination of shape morphing and SMP behaviors at physiological temperatures to yield next-generation smart implants with precise control over dimensions for tissue repair and regeneration.