A Tailorable Family of Elastomeric-to-Rigid, 3D Printable, Interbonding Polymer Networks
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AbstractSoft 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 temperaturereversible DielsAlder (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 selfhealing behavior at room temperature both in air and under watera 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 3Dprinted crosslinked materials in the absence of solvent.
