Preparation and Characterization of Poly(Acrylic Acid)-Based Self-Healing Hydrogel for 3D Shape Fabrication via Extrusion-Based 3D Printing.

The three-dimensional (3D) printing of hydrogel is an issue of interest in various applications to build optimized 3D structured devices beyond 2D-shaped conventional structures such as film or mesh. The materials design for the hydrogel, as well as the resulting rheological properties, largely affect its applicability in extrusion-based 3D printing. Here, we prepared a new poly(acrylic acid)-based self-healing hydrogel by controlling the hydrogel design factors based on a defined material design window in terms of rheological properties for application in extrusion-based 3D printing. The hydrogel is designed with a poly(acrylic acid) main chain with a 1.0 mol% covalent crosslinker and 2.0 mol% dynamic crosslinker, and is successfully prepared based on radical polymerization utilizing ammonium persulfate as a thermal initiator. With the prepared poly(acrylic acid)-based hydrogel, self-healing characteristics, rheological characteristics, and 3D printing applicability are deeply investigated. The hydrogel spontaneously heals mechanical damage within 30 min and exhibits appropriate rheological characteristics, including G'1075 Pa and tan δ0.12, for extrusion-based 3D printing. Upon application in 3D printing, various 3D structures of hydrogel were successfully fabricated without showing structural deformation during the 3D printing process. Furthermore, the 3D-printed hydrogel structures exhibited excellent dimensional accuracy of the printed shape compared to the designed 3D structure.