Herein,
3D printable polymer-toughened epoxy resin composites are
reported. Epoxy resins are widely used due to their excellent properties,
such as thermal and chemical stability. However, their applications
are limited by traditional mold-based manufacturing and their high
brittleness. Mixtures of homopolymers, diblock copolymers, and triblock
copolymers composed of poly(phenylene ether), poly(styrene), poly(methyl
methacrylate), and poly(ethylene oxide) that self-assemble into micelles
in the uncured resin are employed, providing a balance of structure,
creep resistance, and flowability that enables 3D printing processing
techniques and retention of shape from the time of printing throughout
the cured state. The precured ink is solid at room temperature and
has strong shear-thinning behavior at elevated temperature for printing.
As the printed parts cure, the polymer morphology evolves via reaction-induced
phase separation to yield finished composites with enhanced mechanical
properties, including a 40% increase in the impact strength compared
to the neat epoxy, without compromising thermal properties.