Driving macro-scale transformations in three-dimensional-printed biopolymers through controlled induction of molecular anisotropy at the nanoscale.

Motivated by the need to harness the properties of renewable and biodegradable polymers for the design and manufacturing of multi-scale structures with complex geometries, we have employed our additive manufacturing platform that leverages molecular self-assembly for the production of metre-scale structures characterized by complex geometries and heterogeneous material composition. As a precursor material, we used chitosan, a chemically modified form of chitin, an abundant and sustainable structural polysaccharide. We demonstrate the ability to control concentration-dependent crystallization as well as the induction of the preferred orientation of the polymer chains through the combination of extrusion-based robotic fabrication and directional toolpathing. Anisotropy is demonstrated and assessed through high-resolution micro-X-ray diffraction in conjunction with finite element simulations. Using this approach, we can leverage controlled and user-defined small-scale propagation of residual stresses to induce large-scale folding of the resulting structures.

Sequential Multimaterial Additive Manufacturing of Functionally Graded Biopolymer Composites.

Cellulose, chitin, and pectin are three of the most abundant natural materials on Earth. Despite this, large-scale additive manufacturing with these biopolymers is used only in limited applications and frequently relies on extensive refinement processes or plastic additives. We present novel developments in a digital fabrication and design approach for multimaterial three-dimensional printing of biopolymers. Specifically, our computational and digital fabrication workflow-sequential multimaterial additive manufacturing-enables the construction of biopolymer composites with continuously graded transitional zones using only a single extruder. We apply this method to fabricate structures on length scales ranging from millimeters to meters. Transitional regions between materials created using these methods demonstrated comparable mechanical properties with homogenous mixtures of the same composition. We present a computational workflow and physical system support a novel and flexible form of multimaterial additive manufacturing with a diverse array of potential applications.