3D printing of shape memory hydrogels with tunable mechanical properties

Utilization of soft material like hydrogels for task-specific applications such as in soft robotics requires freedom in the manufacturing process and designability. Here, we have developed highly robust thermoresponsive poly(dimethyl acrylamide-co-stearyl acrylate and/or lauryl acrylate) (PDMAAm-co-SA and/or LA)-based shape memory gels (SMGs) using a customized optical 3D gel printer. This process enabled rapid and moldless fabrication of SMGs with a variety of shapes and sizes. By varying the compositions of the constituent monomers, a wide variety of SMGs with tunable mechanical, thermal, optical and swelling properties have been obtained. Printed SMGs with excellent fixity and recovery ratios have exhibited a wide range of values of Young's modulus (0.04-17.35 MPa) and strain (612-2363%) at room temperature when the acrylate co-monomer (SA and LA) content was varied and the value of strain has been found to be enhanced at elevated temperatures. Thermogravimetric analysis (TGA) of the SMGs shows one step peak degradation (407-417 °C) regardless of composition after an initial mass loss due to water evaporation. Dynamic mechanical analysis (DMA) and differential scanning calorimetry (DSC) revealed variable transition temperatures (29-49.5 °C) depending on the SA and LA content. SMGs with all of the composition ratios possess high transparency with variable swelling degrees in water and different organic solvents and exhibit refractive index values in the range of intraocular lenses, making them suitable for applications in the optical field. These unique properties of 3D printed SMGs with free formability and tunable properties are expected to generate rapid demand in a variety of sectors in biomedicine, robotics and sensing applications.