Shape Memory and Self-Healing Behavior of 4D-Printed Electroactive Polycaprolactone/Polylactic Acid/Graphene Nanocomposite: Structure-Properties Relations

The 4D printing of thermo-responsive shape-memory multicomponent polymer composites, which possess the ability to change shape by exposure to heat, has attracted much attention in recent years because of their scientific and technological significance. In the present study, we investigate shape memory performance of a polylactic acid-polycaprolactone-graphene nanocomposite activated directly by increasing the environmental temperature and indirectly, by Joule heating. The incorporation of graphene within the shape-memory biopolymer blend allowed formation of a programmable conduction path, whose electric properties are intimately coupled to thermo-mechanical processes. Advanced rheological, thermal, and thermo-mechanical properties were evaluated and related to the structure of nanocomposite. The electrically and thermally stimulated shape memory and self-healing behavior of the nanocomposite based on polycaprolactone/poly(lactic) acid blend reinforced with graphene nanoplatelets (PCL/PLA/GNP) were investigated. The shape memory tests revealed a good reversibility of 76% between the temporary and permanent states of the samples bent to 180 degrees and a high healing efficiency of 96% if stimulated by Joule heating. The highly electroactive nanocomposite demonstrated a great potential for 4D-printing of objects with complex structures, shapes, and electrically-stimulated shape-memory and self-healing functions. The nanocomposite is biodegradable, recyclable, and reusable, which may reduce the carbon footprint of the rapidly developing additive technology.