Direct-Writable and Thermally One-Step Curable “Water-Stained” Epoxy Composite Inks

In this study, a simple method for preparing direct-writable and thermally one-step curable epoxy composite inks was proposed. Specifically, colloidal inks containing a mixture of ordinary epoxy resin and anhydride-type hardener with the suspended alumina microplates, as exemplary fillers, are “stained” with small amounts of water. This increases the elasticity of the ink via the interparticle capillary attraction and promotes curing of the epoxy matrix in low-temperature ranges, causing the three-dimensional (3D) printed ink to avoid structural disruption during one-step thermal curing without the tedious pre-curing step. The proposed mechanisms for the shape retention of thermally cured water-stained inks were discussed with thorough analyses using shear rheometry, DSC, FTIR, and SEM. Results of the computer-vision numerical analysis of the SEM images reveal that the particles in water-stained inks are oriented more in the vertical direction than those in water-free samples, corroborating the proposed mechanisms. The suggested concept is extremely simple and does not require any additional cost to the one required for the preparation of the common epoxy–filler composites, which is thus expected to be well-exploited in various applications where 3D printing of epoxy-based formulations is necessary.