Biomimetic Color-Changing Hierarchical and Gradient Hydrogel Actuators Based on Salt-Induced Microphase Separation

There have been more challenges for hydrogel actuators to meet the combined requirement of discoloration, complex deformation, and simple preparation. Structural coloration is widely used to fabricate discolored hydrogel via microrearrangement of photonic crystals in the hydrogel framework. However, precise regulation is usually required. Besides, the macro-optical properties are unstable. Herein, we develop a hierarchical and gradient hydrogel actuator with complex deformation and color-changing functions using an electrophoresis method. A simple but effective strategy is presented for fabrication of hierarchical hydrogel composed of homopolymers and copolymers via salt-induced microphase separation during the polymerization of the N-isopropylacrylamide (NIPAm) and [2-(methacryloyloxy)ethyl]trimethylammonium chloride (DMC). Meanwhile a gradient distribution of DMC is also formed during the polymerization due to migration of DMC under electric field. The hierarchical and gradient structures are characterized by confocal laser scanning microscope (CLSM), small-angle X-ray scattering measurement (SAXS), temperature-variable Fourier transform infrared (FTIR), etc. The discoloration mechanism is proposed. The as-prepared hydrogel can undergo fast and complex thermo-triggered deformation and discoloration. Bionic movements of discoloration flowering and information encryption are successfully demonstrated, promising great potential in the application of biomimetic materials.