Tunable Mechanics in Electrospun Composites via Hierarchical Organization

Design strategies from nature provide vital clues for the development of synthetic materials with tunable mechanical properties. Employing the concept of hierarchy and controlled percolation, a new class of polymer nano-composites containing a montmorillonite (MMT)-reinforced electrospun poly(vinyl alcohol) (PVA) filler embedded within a polymeric matrix of either poly(vinyl acetate) (PVAc) or ethylene oxide epichlorohydrin copolymer (EO-EPI) were developed to achieve a tunable mechanical response upon exposure to specific stimuli. Mechanical response and switching times upon hydration were shown to be dependent on the weight-fraction of MMT in the PVA electrospun fibers and type of composite matrix. PVA/MMT.PVAc composite films retained excellent two-way switchability for all MMT fractions; however, the switching time upon hydration was decreased dramatically as the MMT content was increased due to the highly hydrophilic nature of MMT. Additionally, for the first time, significant two-way switchability of PVA/MMT.EO-EPI composites was achieved for higher weight fractions (12 wt %) of MMT. An extensive investigation into the effects of fiber diameter, crystallinity, and MMT content revealed that inherent rigidity of MMT platelets plays an important role in controlling the mechanical response of these hierarchical electrospun composites.