Hydrogel‐Reactive‐Microenvironment Powering Reconfiguration of Polymer Architectures

Abstract Reconfiguration of architected structures has great significance for achieving new topologies and functions of engineering materials. Existing reconfigurable strategies have been reported, including approaches based on heat, mechanical instability, swelling, origami/kirigami designs, and electromagnetic actuation. However, these approaches mainly involve physical interactions between the host materials and the relevant stimuli. Herein, a novel, easy‐manipulated, and controllable reconfiguration strategy for polymer architectures is proposed by using a chemical reaction of host material within a hydrogel reactive microenvironment. 3D printed polycaprolactone (PCL) lattices transformed in an aqueous polyacrylamide (PAAm) hydrogel precursor solution, in which ultraviolet (UV) light triggered heterogeneous grafting polymerization between PCL and AAm. In situ microscopy shows that PCL beams go through volumetric expansion and cooperative buckling, resulting in transformation of PCL lattices into sinusoidal patterns. The transformation process can be tuned easily and patterned through the adjustment of the PCL beam diameter, unit cell width, and UV light on–off state. Controlling domain formation is achieved by using UV masks. This framework enables the design, fabrication, and programming of architected materials and inspires the development of novel 4D printing approaches.