Water‐Assisted Reprocessing and Shape Programming of Epoxy Vitrimer

Abstract Vitrimers are reprocessing and recycling thermosetting plastics. They possess reconfigurable polymer networks that allow for unlimited transformation in shape in principle. However, current strategies to reshape the vitrimers typically involve heat or light, which often induces undesirable oxidation and decomposition. To address this issue, here a water‐assisted approach is proposed for programming epoxy vitrimers’ shapes. In this design, water molecules are utilized to reversibly dissociate the hydrogen bonds in epoxy vitrimers to enable the polymer segments to move flexibly. The hydrated epoxy vitrimers can then be reprogrammed and retained into different temporary shapes by removing the water. Such samples would be recovered to their original shapes by rehydration, exhibiting water‐induced shape memory property. More than temporary deformation, the permanent figures of the hydrated vitrimers can also be permanently changed at room temperature (rt) or elevated temperatures in the presence of transesterification catalysts. Combing the shape memory and high temperature plasticity or utilizing rt plasticity, sophisticated shapes such as spiral shapes are demonstrated. It is envisioned that this water‐assisted methodology can be useful in programming cross‐linked polymers into diverse 3D structures, which has wide practical applications in soft robots, deployable devices, aerospace materials, etc.