Elucidating the Pivotal Role of Thermodynamics and Nanofiller Geometry on the Stereocomplexation of Polylactide Nanocomposites Filled With Graphene Oxide, Carbon Nanotubes, and Their Hybrid

ABSTRACT Incorporating nanoparticles can meaningfully alter the stereocomplexation of polylactide systems. In the current study, the stereocomplex crystallization behavior, microstructure, electrical conductivity, wettability, and thermal stability performance of stereocomplexed‐polylactide nanocomposites loaded with graphene oxide, carbon nanotubes, and their nanohybrid system (1:1) from an interface‐geometry combinational point of view was systematically investigated. After the nanocomposites were analyzed via transmission electron microscopy, electrical conductivity test, differential scanning calorimetry, thermogravimetric analysis, contact angle measurements, and surface energy calculations, it was concluded that two factors, thermodynamic (dispersion/filler–polymer interaction) and nanofiller geometry, are determinant in modulating the degree of stereocomplexation and thermal stability. By introducing only 0.25 wt.% graphene oxide, 33.0% stereocomplex crystals with a melting temperature 14 K higher than that of the neat stereocomplexed‐polylactide and an 11 K higher thermal degradation temperature were obtained, which was attributed to the simultaneous presence of stereocomplex crystals and graphenic platelets. For the first time, a mechanism for the stereocomplexation of polylactide enantiomeric chains on the surface of graphenic platelets and carbon nanotubes in their hybrid system was proposed. Our results pave the way toward a feasible engineering of the interface to control the stereocomplexation for the desired application of stereocomplexed‐polylactide‐filled hybrid nanocomposites.