From Insulator to Conductor: Tailoring Sustainable PLA/PCL Nanocomposites with Hybrid Nanostructures Based on Carbon Nanotubes and Graphene Nanoplatelets

This study aims to develop sustainable conductive nanocomposites based on poly(lactic acid) (PLA)/poly(ε-caprolactone) (PCL) blends reinforced with multi-walled carbon nanotubes (MWCNT) and graphene nanoplatelets (G), focusing on their multifunctional performance. The novelty lies in the production of hybrid nanocomposites based on PLA/PCL blends with MWCNT/G using conventional industrial processing techniques, enabling the development of eco-friendly nanocomposites with tailored electrical, mechanical, and electromagnetic properties. The nanocomposites were prepared by twin-screw extrusion followed by injection molding. Rheological, scanning electron microscopy (SEM), mechanical, thermal, thermomechanical, electrical conductivity, and electromagnetic shielding properties were systematically evaluated. From a rheological perspective, the PLA/PCL/MWCNT and PLA/PCL/MWCNT/G nanocomposites exhibited a plateau at low frequencies, associated with the formation of a percolated network. This was confirmed by the significant increase in electrical conductivity and electromagnetic shielding response. The morphology observed by SEM showed a refinement of the PCL phase in the PLA matrix with the incorporation of MWCNT. The PLA/PCL/MWCNT/G (4/2 parts per hundred resin, phr) nanocomposite showed a 309% increase in impact strength compared to neat PLA, while maintaining the heat deflection temperature (HDT). The elastic modulus exceeded 2300 MPa and accelerated the crystallization process by more than 15 °C compared to PLA, which makes it important to reduce injection molding time. Additionally, it exhibited the highest electrical conductivity level, around 6.79 × 10⁻⁵ S/cm, which resulted in improved electromagnetic shielding performance in the 8.2–18 GHz range, highlighting the synergistic effect between 1D and 2D fillers. The developed PLA/PCL/MWCNT and PLA/PCL/MWCNT/G nanocomposites demonstrate potential for antistatic applications, combining sustainability with multifunctional performance and industrial scalability.