Synergy in bio-inspired hybrid composites with hierarchically structured fibrous reinforcements

[Display omitted] •Self-Assembled Bio-inspired Hierarchical Reinforcement induces Synergistic Effects.•Maximizing the Density of Covalent GnPs Bonds onto GFs Maximizes Synergistic Effect.•Synergy correlates with Exceptional Mechanical Performance leading to Weight-Saving.•Theoretical Framework reveals Origins of Synergy in Hierarchical Hybrid Composites.•EV Battery Casings Satisfy Stringent Mechanical Requirements and Weight Constraints. In response to the global energy crisis, high-performance transportation sectors are rapidly embracing lightweight materials to enhance energy efficiency and sustainability, while grappling with the persistent challenges of developing structural materials that meet stringent safety standards with robust mechanical performance and ease of scalability. Thus, this work presents a combined experimental and theoretical framework to develop a profound understanding of the synergistic effect in hybrid composites with bio-inspired fibrous reinforcements, by elucidating the interfacial interactions across multiple length-scales, encompassing atomic covalent bonding to micro-morphology. A model hybrid composite system, containing a self-assembled fibrous reinforcement consisting of nano-sized Graphene Nanoplatelets (GnP) covalently bonded onto chemically-modified micro-sized Glass Fibers (GF), was utilized to showcase the synergistic effect and highlight its associated mechanisms. The interfacial interactions of the reinforcement were optimized by obtaining the maximum density of covalent bonds, which was achieved with 0.5 wt% GnP for the hybrid composites containing 10 wt% GF, increasing the work of adhesion by 33 %, compared to the biphasic GF composites. The composite’s morphology contains minimal agglomeration with ∼68 % of GnPs oriented with the melt flow, supressing high-stress concentration areas, while the formed crystalline microstructure, with ∼18 % β-crystals, allows the matrix to absorb substantial energy. Furthermore, the increased trans-crystallization encapsulating the hierarchical reinforcement induced nanoscale stiffness variations, increasing rigidity, and forming an ∼16 µm gradient interphase that facilitates load transfer. The greatest synergistic effect observed was ∼54 %, ∼37 %, and ∼75 % for the tensile modulus, tensile strength, and impact strength, respectively. Additionally, a theoretical framework accounting for the synergistic effect was formulated, using a two-step core/shell homogenization model, which