We present a new 4D printing approach that can create high resolution (up to a few microns), multimaterial shape memory polymer (SMP) architectures. The approach is based on high resolution projection microstereolithography (PμSL) and uses a family of photo-curable methacrylate based copolymer networks. We designed the constituents and compositions to exhibit desired thermomechanical behavior (including rubbery modulus, glass transition temperature and failure strain which is more than 300% and larger than any existing printable materials) to enable controlled shape memory behavior. We used a high resolution, high contrast digital micro display to ensure high resolution of photo-curing methacrylate based SMPs that requires higher exposure energy than more common acrylate based polymers. An automated material exchange process enables the manufacture of 3D composite architectures from multiple photo-curable SMPs. In order to understand the behavior of the 3D composite microarchitectures, we carry out high fidelity computational simulations of their complex nonlinear, time-dependent behavior and study important design considerations including local deformation, shape fixity and free recovery rate. Simulations are in good agreement with experiments for a series of single and multimaterial components and can be used to facilitate the design of SMP 3D structures.

Recent advances in three dimensional (3D) printing technology that allow multiple materials to be printed within each layer enable the creation of materials and components with precisely controlled heterogeneous microstructures. In addition, active materials, such as shape memory polymers, can be printed to create an active microstructure within a solid. These active materials can subsequently be activated in a controlled manner to change the shape or configuration of the solid in response to an environmental stimulus. This has been termed 4D printing, with the 4th dimension being the time-dependent shape change after the printing. In this paper, we advance the 4D printing concept to the design and fabrication of active origami, where a flat sheet automatically folds into a complicated 3D component. Here we print active composites with shape memory polymer fibers precisely printed in an elastomeric matrix and use them as intelligent active hinges to enable origami folding patterns. We develop a theoretical model to provide guidance in selecting design parameters such as fiber dimensions, hinge length, and programming strains and temperature. Using the model, we design and fabricate several active origami components that assemble from flat polymer sheets, including a box, a pyramid, and two origami airplanes. In addition, we directly print a 3D box with active composite hinges and program it to assume a temporary flat shape that subsequently recovers to the 3D box shape on demand.

An epoxy ink and its 3D printing method were developed to allow printed parts to be recycled and reprinted.

The three-dimensional (3D) printing of flexible and stretchable materials with smart functions such as shape memory (SM) and self-healing (SH) is highly desirable for the development of future 4D printing technology for myriad applications, such as soft actuators, deployable smart medical devices, and flexible electronics. Here, we report a novel ink that can be used for the 3D printing of highly stretchable, SM, and SH elastomer via UV-light-assisted direct-ink-write printing. An ink containing urethane diacrylate and a linear semicrystalline polymer is developed for the 3D printing of a semi-interpenetrating polymer network elastomer that can be stretched by up to 600%. The 3D-printed complex structures show interesting functional properties, such as high strain SM and SM -assisted SH capability. We demonstrate that such a 3D-printed SM elastomer has the potential application for biomedical devices, such as vascular repair devices. This research paves a new way for the further development of novel 4D printing, soft robotics, and biomedical devices.

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In this work, we advance printed active composites by combining 3D printing, printed electronics, and liquid crystal elastomers (LCEs) to achieve soft actuators with free-standing two-way shape changing behaviors. Incorporated LCE strips are activated by Joule heating produced by printed conductive wires, while uniaxial deformation of the LCE strip is utilized as a driving force to achieve bending in the printed composite. The bending behavior of laminated hinges is first characterized in order to obtain a precise control of actuation, which is then exploited to actuate four demonstrative designs: a morphing airplane, a miura-ori structure, a cubic box, and a soft crawler. The soft morphing airplane and miura-ori structure are designed and fabricated with multiple laminated hinges to demonstrate the synergistic actions during actuation. The cubic box is constructed to show the capability of sequential folding by implementing multiple groups of conductive wires to achieve accurately addressable heating with temporal control. Finally, the two-way transformation is utilized as a driving force for the locomotion of a soft crawler stimulated by a periodic rectangular wave current. These examples show the great potential of using the hybrid 3D printing and pick-and-place method and using LCEs to achieve controllable shape change structures for a variety of potential practical applications.

Pure cellulose nanocrystal (CNC) aerogels with controlled 3D structures and inner pore architecture are printed using the direct ink write (DIW) technique. While traditional cellulosic aerogel processing approaches lack the ability to easily fabricate complete aerogel structures, DIW 3D printing followed by freeze drying can overcome this shortcoming and can produce CNC aerogels with minimal structural shrinkage or damage. The resultant products have great potential in applications such as tissue scaffold templates, drug delivery, packaging, etc., due to their inherent sustainability, biocompatibility, and biodegradability. Various 3D structures are successfully printed without support material, and the print quality can be improved with increasing CNC concentration and printing resolution. Dual pore CNC aerogel scaffolds are also successfully printed, where the customizable 3D structure and inner pore architecture can potentially enable advance CNC scaffold designs suited for specific cell integration requirements.

A method for 3D printing of complicated structures using a photopolymer with high porosity was developed.