Physiologically responsive, mechanically adaptive bio-nanocomposites for biomedical applications.

We report mechanically adaptive bionanocomposites based on poly(vinyl alcohol) (PVOH) and cellulose nanocrystals (CNCs), whose mechanical properties change significantly upon exposure to simulated physiological conditions. These nanocomposites were made using CNCs derived from tunicates (t-CNCs) and cotton (c-CNCs) to explore how aspect ratio, surface charge density, and filler content influence the mechanical properties. Dynamic mechanical analysis data reveal a significant enhancement of the tensile storage modulus (E') upon introduction of CNCs, which scaled with the CNC type and content. For example, in the dry, glassy state at 25 °C, E' increased up to 23% (for c-CNCs) and 88% (for t-CNCs) compared to the neat polymer. Exposing the materials to simulated physiological conditions caused a drastic softening of the materials, from 9.0 GPa to 1 MPa for c-CNCs and from 13.7 GPa to 160 MPa for t-CNCs. The data show that the swelling characteristics of the nanocomposites and the extent of mechanical switching could be influenced via the amount and type of CNCs and also the processing conditions. The high stiffness in the dry state and the ability to tailor the mechanical contrast via composition and processing makes the new materials particularly useful as basis for adaptive biomedical implants.