Thermadapt Shape Memory Polymers Enabling Spatially Regulated Plasticity

Converting planar polymer films into sophisticated 3D structures with a facile and effective method is highly challenging yet desirable for device applications in the real world. Dynamic covalent polymer networks enable permanent shape transformations from 2D sheets to 3D structures, but either sophisticated molecular design or a complex fabrication method is required. Here, we report a shape memory polymer cross-linked by ester bonds, which can be activated upon heating after photoexposure to release the catalyst for the transesterification. The region that is activated via the bond exchange can be patterned due to the spatial-temporal selectivity of the photoexposure. Accordingly, the material presents a localized heterogeneity in stress relaxation upon stretching. The exposed and the unexposed regions show respectively plastic deformation and elastic recovery after removal of the external force, which finally make the 2D sheet transform into a 3D structure. The decoupling of the activated region (photoexposure) and activated condition (heating) enables facile chemical design and fabrication for 2D-to-3D shape morphing.