Mechanisms and impact of fiber–matrix compatibilization techniques on the material characterization of PHBV/oak wood flour engineered biobased composites

Fully biobased composite materials were fabricated using a natural, lignocellulosic filler, namely oak wood flour (OWF), as particle reinforcement in a biosynthesized microbial polyester matrix derived from poly(β-hydroxybutyrate)-co-poly(β-hydroxyvalerate) (PHBV) via an extrusion injection molding process. The mechanisms and effects of processing, filler volume percent (vol%), a silane coupling agent, and a maleic anhydride (MA) grafting technique on polymer and composite morphologies and tensile mechanical properties were investigated and substantiated through calorimetry testing, scanning electron microscopy, and micromechanical modeling of initial composite stiffness. The addition of 46 vol% silane-treated OWF improved the tensile modulus of neat PHBV by 165%. Similarly, the tensile modulus of MA-grafted PHBV increased 170% over that of neat PHBV with a 28 vol% addition of untreated OWF. Incorporation of OWF reduced the overall degree of crystallinity of the matrix phase and induced embrittlement in the composites, which led to reductions in ultimate tensile stress and strain for both treated and untreated specimens. Deviations from the Halpin–Tsai/Tsai–Pagano micromechanical model for composite stiffness in the silane and MA compatibilized specimens are attributed to the inability of the model both to incorporate improved dispersion and wettability due to fiber–matrix modifications and to account for changes in neat PHBV and MA-grafted PHBV polymer morphology induced by the OWF.